Interlayer and moiré excitons in atomically thin double layers: from individual

quantum emitters to degenerate ensembles

Mauro Brotons-Gisbert,1, ∗ Brian D. Gerardot,1, † Alexander W. Holleitner,2, ‡ and Ursula Wurstbauer3, §

1
Institute of Photonics and Quantum Sciences, SUPA, Heriot-Watt University, Edinburgh EH14 4AS, UK
2
Walter Schottky Institute and Physics Department, Technical
University of Munich, Am Coulombwall 4a, 85748 Garching, Germany
3
Institute of Physics, University of Münster, Wilhelm-Klemm-Str. 10, 48149 Münster, Germany
(Dated: July 16, 2024)
Interlayer excitons (IXs), composed of electron and hole states localized in different layers, excel
arXiv:2407.10713v1 [cond-mat.mes-hall] 15 Jul 2024

in bilayers composed of atomically thin van der Waals materials such as semiconducting transition
metal dichalcogenides (TMDs) due to drastically enlarged exciton binding energies, exciting spin-
valley properties, elongated lifetimes, and large permanent dipoles. The latter allows modification
by electric fields and the study of thermalized bosonic quasiparticles, from the single particle level to
interacting degenerate dense ensembles. Additionally, the freedom to combine bilayers of different
van der Waals materials without lattice or relative twist angle constraints leads to layer hybridized
and moiré excitons which can be widely engineered. This review covers fundamental aspects of IXs
including correlation phenomena as well as the consequence of moiré superlattices with a strong
focus on TMD homo- and hetero-bilayers.
Keywords: 2D materials, transition metal dichalcogenides, semiconductor optics, van der Waals hetero-
structures, moiré crystals, excitons, dipolar interactions

INTRODUCTION be controlled by external stimuli such as electric fields

[5, 6], pressure [7, 8], or twist angle [9]. In this way,
Van der Waals (vdW) bilayers host a plethora of dif- the competition and coupling between intralayer, inter-
ferent exciton species with different properties and func- layer and layer-hybridized excitons emitting at the fun-
tionalities that are promising for applications. Vice damental gap as well as from higher lying states can be
versa, excitons can serve as sensitive probes for the lo- experimentally accessed [10]. While also lateral vdW
cal potential landscape in vdW hetero-structures. Such hetero-structures can host IXs [11], this review focuses
vdW stacks can be prepared from the same or different on the peculiarities of excitons in vertical vdW bilayers
two-dimensional crystals and are called homo-bilayer or prepared from semiconducting transition metal dichalco-
hetero-bilayer, respectively. As Coulomb-bound electron- genide (TMD) monolayers. With several engineering
hole pairs, excitons are very sensitive to their dielec- opportunities, TMD-based vdW stacks hold fascinat-
tric environment inside and outside of the semiconduct- ing properties that individual layers or conventional 3D
ing host materials. Moreover, the excitonic properties solids typically do not exhibit within one material: (i) de-
strongly depend on the underlying Bloch states. Like in pending on the material combination, rich IX physics can
two-dimensional monolayers, a reduced dielectric screen- be addressed including the dynamics of neutral, charged,
ing and the two-dimensional nature of the bilayers re- and layer-hybridized IXs, as well as layer-specific charac-
sults in excitonic binding energies exceeding several hun- teristics of higher-lying IXs. (ii) Stacking of two lattices
dreds of millielectron volts. Unlike monolayers, vertical with similar but not identical lattice constants and/or a
vdW double layers can host excitons with the constitut- relative twist angle results in the formation of a moiré lat-
ing electron and hole states being localized in adjacent tice. A moiré lattice is a geometrical superimposed peri-
layers. As a direct consequence, the reduced overlap of odic patterns that forms by stacking two atomically thin
the electron – hole wavefunctions results in enhanced life- commensurate with a relative twist angle, or two crystals
times, up to several 100s of nanoseconds [1, 2], allowing with different lattice constants or both together. The
the study of thermalized ensembles [3] of such interlayer long-period moiré super-lattice structure causes highly
excitons (IXs). Another peculiarity of IXs is their per- periodic potential modulations in real space [12] and
manent dipole moment, which enables one to tune their flat moiré minibands in the reciprocal space for spe-
energy and to control them by electric fields in capac- cific lattice mismatches and twist angles [13]. The zero-
itor structures [4] that can be realized even in devices dimensional potential traps can host so-called moiré exci-
prepared only from vdW materials with e.g. hBN as tons that can function as single photon emitters allowing
a dielectric material and graphene or thin graphite as for the creation of periodic networks of quantum emitters
semi-transparent electrodes. In addition to manipulat- [14, 15]. Similar to magic angle twisted bilayer graphene
ing the IX energy, momentum-dependent hybridization [16], in twisted bilayer TMDs, strongly correlated states
of the IXs with other exciton species (in particular in- can emerge by the combination of a quenched kinetic en-
tralayer excitons with strong oscillator strengths) can ergy and a high density of states in the flat minibands,
 2

which can act as sensitive probes for correlated phases of version symmetry of the TMDs lattice unit cell lead to
adjacent charge carrier systems [13, 17–20]. Compared to an effective coupling between the valley index and spin of
intralayer excitons, IXs exhibit superior sensitivity due to the electrons and holes at the ±K corners [30]. This ef-
their permanent dipolar moment [21]. In hetero-bilayers fective coupling (typically referred to as spin-valley lock-
of TMDs, excitons can not only sense correlated states, ing), results in valley-dependent optical selection rules
but also correlated excitonic states, such as an excitonic [31]: excitonic absorption and emission processes at ±K
insulator, can emerge [22–24]. Moreover, the presence of involve σ ± -polarized photons, respectively, enabling op-
strong spin-orbit coupling gives rise to even more exotic tical control of excitons [32, 33].
correlated states [25]. This high degree of tunability of
rich exciton physics makes vertical vdW double layers a
highly interesting research subject for fundamental stud- INTERLAYER EXCITONS AND DIPOLES
ies on both many-body and correlation phenomena of
low-dimensional exciton and charge carrier systems. On Interlayer excitons in natural multi-layer TMDs
a more applied perspective, such highly tunable char-
acteristics suggest various possibilities of optoelectronic Despite their indirect-gap nature, multi-layer TMDs
and quantum photonic devices such as solar cells, light preserve the direct gap at the ±K corners of the Brillioun
emitting diodes, photo-sensors or single-photon sources zone even in the bulk limit, with spin-orbit-split conduc-
operating in a largely extended spectral range covering tion bands that present a flat dispersion along the out-
the near-infrared to ultraviolet wavelength ranges. This of-plane direction (i.e., the K-H high-symmetry direc-
review article is organized as follows: After this introduc- tion) [7, 34]. Such flat band dispersion ensures that the
tion and a brief summary on the most fundamental prop- electron wave functions around ±K are highly confined
erties of TMD semiconductors, IXs and dipolar excitons within each individual layer, resulting in the formation
are discussed, followed by an introduction of excitons in of intralayer excitons, i.e. excitons in which the electron-
TMD moiré hetero-structures and hybridization of intra- hole pairs are localized in the same layer (see Figure 1A).
and interlayer excitons as well as the impact of structural In addition to intralayer excitons, the layer-localized elec-
effects. Next, interaction effects, including the formation tron wave functions in TMD multi-layers can also bind to
of degenerate IX ensembles, are considered, followed by a holes with wave functions confined within adjacent layers
discussion of IX formation and transport processes. The or that spread along several layers, giving rise to IXs with
article concludes with a brief summary and an outlook. spatially displaced wave functions [34–39]. Interlayer and
intralayer excitons coexist in multi-layer TMDs (see Fig-
ure 1A, top [40]), with both exciton species depicting
BACKGROUND momentum-direct optical transitions at ± K. The bottom
panel of figure 1A shows a schematic of the spin, band
Two-dimensional group-VI TMD semiconductors of and layer configurations of dipole-allowed intralayer and
the form MX2 (with M = Mo, W, and X = S, Se) have IXs for bilayer 2H-MoS2 , a prototypical centrosymmetric
attracted much attention due to their appealing prop- multi-layer TMD. Ground-state intralayer excitons (the
erties for a large palette of optoelectronics, spintronics, so called A excitons) show optical transitions involving
and photonics applications. The investigation of their an electron in the lowest conduction band and a hole in
structural, electronic, and optical properties constitutes the highest valence band (red arrows), while intralayer B
a very active research field in the solid-state and pho- excitons present optical transitions between the topmost
tonics communities. Consequently, the main properties spin-orbit-split conduction band and the lower spin-orbit-
of 2D TMD semiconductors are extensively covered and split valence band at ±K (blue arrows). Dipole allowed
reviewed in the literature for both their bulk and few lay- IXs present optical transitions between the topmost va-
ers forms [26, 27]. Among their main properties, TMDs lence band in one layer and the upper spin-orbit-split
monolayers are well known by their momentum-direct conduction band in the other layer (green arrows). Con-
optical band gaps with energies in the visible to near- sequently, dipole-allowed interlayer and intralayer exci-
infrared spectral range, with the band edges located at tons exhibit optical transitions with similar symmetry
the degenerate but inequivalent corners of the Brillouin properties, with the difference that the spin-valley selec-
zone (typically referred to as ±K valleys). Carriers oc- tivity characteristic of monolayer TMDs is replaced by a
cupying the conduction and valence band edges at ±K spin-layer selectivity in the optical generation of excitons
form excitons that are hydrogen-like states with a typi- with circular polarized light. As detailed below, stacking-
cal binding energy on the order of 0.5 eV [28, 29]. Due to order dependent hybridization can give rise to a hole state
their large binding energy, excitons dominate the optical that is delocalized across different layers [40, 41].
response of TMDs at both cryogenic and room tempera- Figure 1B shows differential reflectance spectra
tures. Moreover, the strong spin-orbit coupling induced (DR/R) of monolayer, bilayer and trilayer 2H-MoS2 sam-
by the heavy transition-metal atoms and the broken in- ples (black, red and blue solid lines, respectively) for a
 3

FIG. 1. Interlayer excitons in homobilayer TMDs [MoS2 (A-D) and WSe2 (E)].
(A) Top: schematics showing the intralayer and interlayer nature of the excitons in bilayer 2H-MoS2 . Bottom: sketch of the
spin, valley and layer configuration of the optical transitions corresponding to intralayer A excitons (red arrows), intralayer B
excitons (blue arrows), and IXs (green arrows) in bilayer 2H-MoS2 . (B) Differential reflectivity of ML, BL and TL 2H-MoS2
(black, red and blue solid lines, respectively) for a sample temperature of T = 4 K. (C) First derivative of the differential
reflectivity spectrum for as-grown 2H-bilayer (blue) and as-grown 3R-bilayer (red) MoS2 4 K. (D) Color map of the absorption
spectra of bilayer MoS2 showing a Stark shift of the IXs at small electric fields. The intralayer A:1s and B:1s and the two
branches of the IX resonances (IE11 and IE2 ) are labelled. (E) IX emission energy in BL WSe2 as a function of the applied
electric field for different electron doping densities. Adapted with permission from Ref. [40], Nature Publishing Group (A, C),
Ref. [42], APS (B), Ref. [37], Nature Publishing Group (B), and Ref. [35], ACS (E).

sample temperature of T = 4 K [42], in which an absorp- depicting an asymmetric interlayer coupling arising from
tion peak arising from IXs can be seen for the bilayer and a layer-dependent Berry phase effect. Such an asymmet-
trilayer samples. Despite the large spatial separation of ric coupling is also the electronic origin of spontaneous
the electron and hole wavefunctions, IXs in multi-layer polarization characteristic of R-stacked TMDs [41].
TMDs possess binding energies almost an order of mag- Moreover, the spatial displacement of the exciton car-
nitude larger compared with those in coupled III-V quan- riers in TMD homo-bilayers endows IXs with a large out-
tum wells, and of the same order of magnitude as their of-plane static electric dipole that can be tuned via the
intralayer counterparts [42]. Consequently, the optical Stark effect [37–39]. Figure 1D depicts a color map of the
transitions associated to IXs in TMDs can appear either absorption spectra of bilayer 2H-MoS2 showing a Stark
at lower or at higher energies than the intralayer A exci- shift of the IXs for applied vertical electric fields [37].
ton depending on the dark or bright nature of the ground Here, the IX resonance splits into two branches (IE1 and
IX state, respectively. Interestingly, the stacking order of IE2 ) that shift linearly to lower (higher) energy depend-
the TMD multilayers has a strong impact on the forma- ing on the parallel (anti-parallel) orientation of the elec-
tion of IXs. In Ref. [40], the authors demonstrated that tric field and the permanent electric dipole. The effects
hole delocalization over MoS2 homo-bilayers is allowed of an applied vertical electric field on the IX resonance
for 2H stacking but forbidden for 3R stacking, resulting energy and its recombination dynamics have also been in-
in the presence (absence) of IXs in 2H-MoS2 (3R-MoS2 ) vestigated in dual-gated homo-bilayer WSe2 and MoSe2
homo-bilayers (see Figure 1C [40]). However, a more re- devices [35, 43]. Via photoluminescence (PL) and time-
cent work showed the presence of IXs in R-MoS2 bilayers resolved PL spectroscopy at 10 K, the authors in Ref.
 4

[35] show that the IX emission redshifts symmetrically Single interlayer exciton moiré trapping
for both positive and negative applied vertical electric
fields. The symmetrical redshift of the exciton energy Beyond the large permanent dipole moment and the
for both positive and negative fields is attributed to the spin-valley physics, the compelling concept of a moiré
electric-field-induced redistribution of carriers among the superlattice emerges in TMD hetero-bilayers with lattice
two layers that results in a parallel alignment of the ex- mismatch and/or any relative twist angle between the
citon permanent dipole with the applied field. Figure 1E constituent monolayers [12]. The moiré superlattice cre-
summarizes the Stark shift observed under different dop- ates a periodic potential landscape for IXs [58–60], in
ing densities (positive values n for electron doping and which three high-symmetry sites (A, B, and C) with spe-
negative values for hole doping) [35]. Close to the charge cific atomic registries arise, such as Rhh (A), RX
h (B) and
neutrality point, a linear Stark effect emerges immedi- µ
RMh (C), where R h denotes an R-type stacking with the µ
ately, whereas for finite electron or hole doping densities site of the electron layer (either h the hexagon centre, X
an appreciable Stark effect is observed only for applied the chalcogen site or M the metal site) vertically aligned
gate voltages beyond a threshold value. The existence with the hexagon centre (h) of the hole layer (Figure
of a threshold gate voltage can be understood as an off- 2A). For moiré periods larger than the IX Bohr radius
set in the resulting electric field produced by an unequal that is in the order of a few nanometers [61], these moiré
distribution of carriers between the two layers as a con- high-symmetry sites can behave as smooth quantum-dot-
sequence of the applied field [35]. Beyond natural bi- like confining potentials, leading to the trapping of sin-
layer TMD systems, ground and excited-state IXs with gle electrons, holes, or IXs [58, 59]. The moiré potential
large permanent dipole moments were also been reported minima preserve the three-fold rotational (C3 ) symme-
in trilayer 2H-MoSe2 and three-, four-, five-, and seven- try [58, 59], and excitons trapped in such moiré sites
layer 2H-WSe2 , in which the wavefunctions of the carriers obey selection rules that depend on the spin configura-
forming the excitons are confined in an every-other-layer tion of the exciton carriers (spin-singlet/spin-triplet) and
configuration [43, 44]. Finally, in addition to the Stark the atomic registry of the trapping site, as theoretically
effect, the application of vertical electric fields can result predicted (see Figure 2A) [62]. Experimental evidence
in an enhancement of the IX recombination lifetime by of neutral IXs trapped in a moiré potential has been re-
more than two orders of magnitude [35]. ported in MoSe2 /WSe2 hetero-bilayers with twist angles
of around 0◦ , 21.8◦ and 60◦ at cryogenic temperatures
[14, 63–65]. Hetero-bilayers with twist angles of around
0◦ present ground IX states with spin-singlet configu-
Excitons in TMD moiré hetero-structures
rations, while hetero-bilayers with twist angles of 21.8◦
and 60◦ present ground exciton states with spin-triplet
In contrast to TMD homo-bilayers, stacking any two optical transitions. For small IX densities, polarization-
different ML TMDs creates a hetero-bilayer typically resolved PL measurements show that the moiré-trapped
with type-II band alignment while preserving atomically IXs exhibit linewidths below 100 µeV with strong helical
sharp interfaces [45–47]. Such a band alignment results in polarization due to the C3 symmetry, which results in a
the formation of IXs with smaller transition energies than notable absence of observable fine structure [14, 63, 64]
the intralayer excitons in the individual monolayers, from (Figure 2B, top). Moreover, the trapped IXs show well-
which the IXs localized at the ±K valleys inherit their defined magneto-optical properties: The g factors of the
valley-contrasting physics [4, 48–50], although indirect trapped excitons depend on the relative valley alignment
IXs with an inter-valley nature also arise in many com- (i.e., stacking configuration) between the layers hosting
binations of homo- and hetero-bilayers [51]. In addition, the carriers (Figure 2B, bottom) [14, 63, 64]. In ad-
the interlayer nature of the excitons leads to a reduced dition, the emission from the localized interlayer exci-
overlap of the electron and hole wave functions, which re- tons presents clear hallmarks of quantum-confined exci-
sults in optical dipole transitions with long radiative life- tons: power-dependent emission intensities that can be
times compared to intralayer excitons [48, 51, 52]. Sim- described by a two-level saturation model [14, 63, 64]
ilar to IXs in TMD homo-bilayers, the separation of the and photon antibunching (Figure 2C) [14]. Finally, the
exciton carriers can result in a large permanent electric large permanent dipole of the moiré-trapped IXs can be
out-of-plane dipole moment that enables a large tunabil- exploited to achieve large direct current Stark tuning of
ity of the exciton transition energy by vertically applied their emission energies up to 40 meV [14].
electric fields [4, 14, 53]. Moreover, similar to mono-
layer TMDs [54, 55], patterned substrates were shown to
lead to local strain profiles that enable exciton trapping Moiré interlayer trions
in nanoscale confinement potentials, in which the mean
number of trapped IXs can be controlled via the optical In addition to neutral IXs, the loading of additional
excitation level [56, 57]. charge carriers into the moiré lattice in gate-tunable
 5

FIG. 2. Moiré-trapped IXs in MoSe2 /WSe2 hetero-bilayers [MX2 /WX2 (A) and MoSe2 /WSe2 (B, C)].
(A) Top: schematics of the long-period moiré pattern in a R-stacked MoX2 /WX2 hetero-bilayer. Green diamond denotes the
moiré supercell. Insets show zooms of the local atomic registries in the three high-symmetry trapping sites (A, B and C) of
the moiré supercell. A, B and C have atomic registries Rhh , RhX and RhM , respectively. Bottom: schematic illustration of the
polarization selection rules, for K-valley spin-singlet and spin-triplet IX wavepackets centered at trapping sites A, B and C,
respectively. (B) Helicity-resolved PL of moiré-trapped IXs in MoSe2 /WSe2 hetero-bilayers with twist angles of 57◦ (left) and
2◦ (right) as a function of the applied out-of-plane magnetic field (top panels). The bottom panels show the Zeeman splitting
(∆ = Eσ+ − Eσ− ) from the corresponding IXs as a function of the applied magnetic field with a linear regression from which
the values of the effective Landé gef f of -15.89 and 6.72 are extracted. (C) Leftmost panel: PL spectrum showing a few moiré-
trapped IXs in MoSe2 /WSe2 . The blue and red regions shown for the PL line at 1.401 eV represent the estimated PL signal from
the emitter and the background, respectively. Second panel from the left: integrated PL intensity of the emitter highlighted
in the leftmost panel at different excitation powers. Second panel from the right: second-order photon correlation statistics
of the emitter highlighted in the leftmost panel. The red shadowed area represents the Poissonian interval error associated to
the experimental determination of g (2) (τ ). The black dashed line and the gray shadowed area represent the average and error
interval of the experimental limitation for g (2) (0), respectively, owing to the non-filtered emission background. Rightmost panel:
PL spectra of moiré-trapped IXs in a dual-gated MoSe2 /WSe2 hetero-bilayer at different gate voltages. Three representative
peaks are indicated as E1, E2, and E3.

WSe2 /MoSe2 hetero-bilayers also enables the forma- ure 3B) [67, 69], with the only differences being: i) the
tion of moiré-trapped interlayer trions, which are bound emission line widths, which are one order of magnitude
quasiparticles consisting of two electrons and a hole (neg- broader for the ensemble exciton peaks; and ii) the ab-
atively charged trion) or a single electron and two holes solute emission energies, which show an exciton-density-
(positively charged trion) [66–69]. Upon electron or hole dependent blue-shift in the ensemble exciton peaks as
doping of the hetero-bilayer, the neutral trapped IXs a consequence of the dipolar interactions [69]. More-
form on-site negatively or positively charged interlayer over, the magneto-optical properties of the neutral and
trions with an average binding energy of ∼7 and ∼6 meV, charged IXs are also identical (see Figure 3C). However,
respectively (see Figure 3A) [66–69]. Interestingly, the at high IX densities, emission from a higher energy IX
doping-dependent evolution of the IX PL shows the same ensemble peak with opposite selection rules and different
overall behavior for both low and high IX densities (Fig- effective g-factor appears, which has been attributed to
 6

FIG. 3. Moiré-trapped interlayer trions in TMD hetero-bilayers [WSe2 /MoSe2 (A-E)].

(A) Gate-dependent PL emission from a WSe2 /MoSe2 hetero-bilayer showing PL from moiré-trapped interlayer excitons and
trions. The positive (negative) gate voltage (Vg ) and carrier density correspond to the electron (hole) doping. (B) Gate-
dependent PL intensity of moiré-trapped IXs in a WSe2 /MoSe2 hetero-bilayer for excitation powers of 20 µW (top) and 20 nW
(bottom). (C) Top: PL spectra of moiré-trapped neutral (left), negatively-charged (middle), and positively-charged (right) IXs
as a function of a vertical magnetic field. Bottom: Zeeman splitting of representative IXs extracted from the corresponding top
panels. Landé gef f of -16.10, -15.75 and -16.37 are extracted for neutral IX0 , negatively charged IX− and positively charged
IX+ , respectively. (D) Gate-voltage-controlled PL of IXs in the neutral (Vg ≤ 0.1 V) and electron-doping regime (Vg ≥ 0.1 V)
for excitation powers of 20 nW (left panel) and 40 µW (right panel) at 4 K. In the right panel, the PL intensity is multiplied by
a factor 20 in the spectral range delimited by the vertical dashed area for visualization purposes. (E) Right: Logarithmic-scale
density plot showing the evolution of the PL spectrum of negative interlayer trions as a function of excitation power, in which
four different peaks can be resolved (as indicated by the arrows). Left: PL spectrum acquired for an intermediate excitation
power of 2 µW (as indicated by the white dashed line in the left panel) showing four Lorentzian peaks corresponding to various
exciton species. Bottom: Schematic representation of the charge configurations for IX− −
T,inter (left), IXT,intra (middle), and
−
IXS,inter (right) showing the optical transitions that involve a hole in the topmost valence band of WSe2 at K. Adapted with
permission from Ref. [66] (A), Ref. [67] (B), Ref. [68] (C), Nature Publishing Group, and Ref. [69] (D, E), American Physical
Society.

optical transitions involving the highest spin-orbit-split both intervalley and intravalley interlayer trions with
conduction band of MoSe2 at ±K [4, 69–71]. This higher spin-triplet optical transitions (as schematically depicted
energy ensemble exciton state can also be tuned from a in the right, central, and left panels of the bottom of
neutral to a charged regime by gate doping, with a charg- Figure 3E, respectively [69]), which result in PL spectra
ing offset very similar to the ground IX state at lower that can show up to four different PL components: the
energy (see Figure 3D)[69]. three moiré-localized negative trions with contrasting
Finally, a combination of power-dependent and spin-valley configurations plus an additional low-energy
magneto-optical measurements in a gate-tunable peak which has recently been attributed to a composite
MoSe2 /WSe2 hetero-bilayer revealed the presence of six-particle “hexciton” state [72].
three different species of moiré-localized negative trions
with contrasting spin-valley configurations: intervalley
interlayer trions with spin-singlet optical transitions, and
 7

Moiré effects on the intralayer excitons Umklapp scattering within the reduced Brillouin zone
and the presence on exotic many-body moiré excitons,
the moiré effects on the intralayer excitons in TMD
The presence of a long-range periodic exciton potential
hetero-bilayers that feature a close energy alignment of
can profoundly modify the optical spectrum of TMDs.
the band edges (such as MoSe2 /WS2 and MoTe2 /MoSe2 )
This is the case for twisted TMD homo- and hetero-
are enhanced by resonant interlayer band hybridization
bilayers, in which the moiré superlattice gives rise to
[75]. Theoretical calculations show that the resonantly
a long-range crystal structure with a reduced Brillouin
hybridized exciton energy in these TMD hetero-bilayers
zone. The reduced Brillouin zone results in a folding-
shows a sharp modulation as a function of the interlayer
induced flattening of the conduction and valence bands
twist angle (see Figure 4D) [75]. Such resonant hybridiza-
and a multitude of avoided crossings that arise as a conse-
tion between exciton bands has been experimentally ob-
quence of the interlayer hybridization [74, 77]. Recently,
served through PL measurements in WS2 /MoSe2 [76],
several groups have experimentally shown that the pe-
MoS2 /WSe2 [84] and WS2 /WSe2 [85] hetero-bilayers,
riodic moiré exciton potential leads to a mixing of mo-
which feature nearly-degenerate band edges. The hy-
mentum states separated by moiré reciprocal lattice vec-
bridized excitons in these systems exhibit a pronounced
tors, which results in the formation of satellite exciton
energy shift as a function of twist angle (see Figure 4E)
peaks (see Figure 4A) [73, 74]. Although the moiré su-
[76].
perlattice plays a key role in the formation of the satel-
lite peaks observed in these works (also referred to as
Umklapp [73] or moiré excitons [74]), the origin of the
Hybridization of intralayer and interlayer exciton
periodic exciton potential is different. In Ref. [73], the states
authors used a twisted MoSe2 /hBN/MoSe2 homo-bilayer
structure where the carrier density in the two MoSe2 lay-
ers can be controlled independently. The presence of the Intralayer and interlayer excitons in multi-layer TMDs
monolayer-thick hBN barrier layer in their device reduces can hybridize even in the absence of a moiré superlattice.
the interlayer coupling between the twisted MoSe2 lay- The large quantum-confined Stark effect of IXs in TMD
ers, which results in a weak periodic moiré potential for homo- and hetero-bilayers allows one to exploit the appli-
intralayer excitons. Therefore, in the absence of electron cation of vertical electric fields to energetically tune IXs
or hole doping, the spectrum does not show any moiré ex- into resonance with intralayer excitons, where they hy-
citon peaks (see Figure 4B). However, for unity electron bridize [5, 37–39, 43, 44, 81, 82, 86, 87]. In the case homo-
filling of the underlying moiré potential in either or both bilayer MoS2 , the results in Ref. [37] show that the Stark-
MoSe2 layers, new optical resonances appear in the reflec- split IX branches undergo clear avoided crossings with
tion spectrum (see Figure 4B). Such Umklapp or moiré both the intralayer B- and A-exciton branches, where
exciton resonances arise due to the spatially modulated the coupling orginates from hole tunnelling and from an
interactions between excitons and electrons in an incom- exchange-induced A-B exciton admixture, respectively
pressible Mott-like correlated state, which creates a peri- [86]. Similar couplings between interlayer and intralayer
odic potential for excitons with the periodicity imposed excitons have also been reported by other groups in bi-
by the moiré lattice constant [73]. In contrast to the layer 2H-MoS2 [38, 39], natural bilayer and trilayer 2H-
MoSe2 /hBN/MoSe2 device in Ref. [73], nearly-aligned MoSe2 [43], and three-, four-, five-, and seven-layer nat-
WSe2 /WS2 hetero-bilayers present a strong static moiré ural 2H-WSe2 [44]. Figure 5A shows a density plot of
potential, which leads to the formation of satellite moiré the electric field dependence of the reflectance spectrum
exciton peaks even in the absence of electron or hole dop- differentiated with respect to photon energy from trilayer
ing (see Figure 4C) [74]. The presence of such satellite 2H-WSe2 , where the hybridization of the IXs with the 1s
moiré exciton peaks is not restricted to hetero-structures and 2s states of the intralayer A exciton leads to clear
consisting of two layers, but has also been reported in anticrossings at the corresponding intralayer exciton en-
devices in which the WSe2 layer is replaced by a bilayer ergies [44].
and a trilayer [78]. In addition to the normalization of the exciton reso-
nance energy and the redistribution of oscillator strength
Moreover, the moiré pattern of TMD hetero-bilayers between the different exciton branches, the hybridiza-
has shown to result in the formation of non-trivial many- tion of interlayer and intralayer excitons in natural multi-
body excitonic states [79, 80]. Examples of such many- layer 2H-stacked TMDs has also shown to result in gate-
body moiré excitons include intralayer charge-transfer tunable g factors for the resulting hybrid exciton species
excitons [79] and an interlayer moiré exciton in which [38, 43]. Figure 5B shows the electric-field-driven evolu-
the hole’s wavefunction is surrounded by the correspond- tion of the g-factor of the hybrid excitons in a natural
ing electron’s wavefunction, which is distributed among 2H-MoSe2 bilayer [43] (bottom panel). The top panel
three adjacent moiré traps [80]. shows the electric-field-dependent normalized contribu-
In addition to the satellite spectral features caused by tions of each bare exciton state |C IX(X) |2 to the corre-
 8

FIG. 4. Effects of the moiré superlattice on the intralayer excitons [MoSe2 /hBN/MoSe2 (B), WS2 /WSe2 (C), MoSe2 /WS2
(D,E)].
(A) Left: bare dispersion of mobile excitons in a ML TMD. The linearly polarized exciton modes split into two branches
with linear (green line) and parabolic (blue line) dispersion due to the strong intervalley electron-hole exchange coupling.
The transparent lines represent higher bands arising from the mixing of states connected by reciprocal lattice vectors as a
consequence of a periodic potential. Right: dispersion bands of excitons moving in periodic moiré potential along a path in
the moiré Brillouin zone. The color bar indicates the oscillator strength of each state (saturated for all blue lines). Only a
single Umklapp band per polarization obtains sizable oscillator strength, while most states remain dark. (B) Dependence of the
differential reflectance measured in MoSe2 /hBN/MoSe2 hetero-structure as function of the chemical potential Vµ differentiated
with respect to energy E for a fixed vertical electric field VE = 0.24 V. An additional higher-energy Umklapp exciton resonance
U
Xtop is observed once the top layer is filled with one electron per moiré site (i.e., ν = 1). (C) Reflection contrast spectrum
measured in a moiré WS2 /WSe2 hetero-bilayer as a function of electron concentration. Three prominent moiré exciton peaks
are labelled. Peak I exhibits a strong blue-shift and diminishes upon doping while another lower energy peak (I′ ) emerges.
Similarly peak III shows a strong blue-shift and weakens upon doping. (D) Calculated absorption spectrum as functions of
twist angle for MoSe2 /WS2 close to parallel (bottom panel) and anti-parallel (top panel) alignment. The full low-energy exciton
spectrum is overlaid on top the absorption map by blue and yellow curves, showing multiple momentum-dark exciton states.
(E) Normalized room-temperature PL spectra of MoSe2 /WS2 hetero-bilayers with interlayer twist angles ranging from 1◦ to
59◦ . The dashed curve shows the typical room-temperature PL peak from the A exciton of ML MoSe2 (XA ), and its energy is
indicated by the vertical dashed line. Adapted with permission from Ref. [73] (A, B), Ref. [74] (C), Ref. [75] (D), Ref. [76]
(E).

sponding hybrid excitons, showing a clear evolution from intralayer excitons (see Figure 5C). In Ref. [82], hy-
pure intralayer (interlayer) to pure interlayer (intralayer) bridization of interlayer and moiré excitons in angle-
character before and after the anticrossing. aligned WSe2 /WS2 and MoSe2 /WS2 hetero-bilayers was
observed and in Ref. [87] for MoSe2 /WS2 hetero-bilayer.
The Vg -induced hybridization between intralayer and
The hybrid excitons are formed via spin-conserving res-
interlayer excitons is not restricted to natural TMD
onant tunnelling of electrons or holes between the lay-
multilayers, but can also be observed in twisted TMD
ers, and exhibit the characteristics of both interlayer
homo- and hetero-bilayers [5, 81, 82]. In Ref. [81],
(large out-of-plane electric dipole) and intralayer exci-
the coupling between intralayer and interlayer excitons
tons (appreciable oscillator strength). Figure 5D shows
in near-0◦ -twist-angle MoSe2 /MoSe2 homo-bilayers is re-
the electric-field dependence of hybrid excitons in a
ported. These homo-bilayers featured large rhombo-
WSe2 /WS2 moiré superlattice loaded with one electron
hedral AB/BA domains, which support IXs with out-
per site [82], where the energy-level anticrossing between
of-plane electric dipole moments in opposite directions
the intralayer moiré excitons (higher energy peaks) and
that can be flipped by the application of vertical electric
the IXs (lower energy peak) can be observed. Simi-
fields, resulting in field-asymmetric hybridization with
 9

FIG. 5. Hybridization of intralayer and interlayer excitons [3L 2H-WSe2 (A), 2L 2H-MoSe2 (B), twisted (t≈ 0◦ ) MoSe2 /MoSe2
(C), twisted (t≈ 60◦ ) WSe2 /WS2 (D), MoS2 /WS2 (E), MoSe2 /hBN/MoSe2 (F)].
(A) Color maps of the reflectance spectrum differentiated with respect to photon energy from trilayer 2H-WSe2 as a function
of the electric field Ez applied perpendicular to the trilayer in the spectral regions around the ground and first-excited state of
the A-exciton. (B) Electric-field-driven evolution of the g-factor of the hybrid inter- and intralayer excitons hX3 and hX4 in a
natural 2H-MoSe2 bilayer (bottom panel). The top panel shows the electric-field-dependent normalized contributions of each
bare exciton state |C IX(X) |2 to the corresponding hybrid excitons. (C) Electric-field-dependent reflectance contrast spectra of
the intralayer excitons in a near-0◦ -twist-angle MoSe2 /MoSe2 bilayer which features large rhombohedral AB/BA domains. (D)
Energy derivative of the reflectance contrast spectrum as a function of the applied out-of-plane electric field in a 60◦ aligned
WSe2 /WS2 sample at a fixed doping of one electron per moiré cell. (E) Left panel: Emission energy of the upper (IupperA ) and
lower exciton branches (Ilower
A ) in a MoS2 /WS2 hetero-bilayer embedded in an vdW field-effect structure as a function of the
applied gate voltage. Right panel: Hybridization-induced evolution of the PL lifetime corresponding to the lower exciton branch
measured at a bath temperature of 10 K. (F) Color map of the reflectance signal from a MoSe2 /hBN/MoSe2 as a function of
the applied vertical electric field (right panel) together with the corresponding schematics of the energy bands and the exciton
energy alignment (left panel). Adapted with permission from Ref. [44] (A), Ref. [43] (B), American Physical Society, Ref. [81]
(C), Ref. [82] (D), Ref. [5] (E), and Ref. [83] (F), Nature Publishing Group.

lar electric-field-induced hybridization between interlayer as 40 meV and 11 meV could be extracted, respectively,
and intralayer excitons was observed in angle-aligned demonstrating that these systems were strongly coupled
MoS2 /WS2 hetero-bilayers embedded in a vdW field- [5, 82].
effect structure (see Figure 5E) [5]. In addition to the Finally, the coupling between interlayer and intralayer
electric-field-induced energy anti-crossing between the excitons has been observed even for hetero-structures in
upper and lower exciton branches in the PL spectra, the which the interlayer exciton constituent states are located
authors in Ref. [5] also showed hybridization-induced in layers separated by a hBN tunnel barrier [83]. Using
renormalization of the PL lifetime for the lower exci- a double-gated MoSe2 /hBN/MoSe2 hetero-structure, co-
ton emission branch (see Figure 5E). The electric-field- herent coupling of interlayer and intralayer excitons via
induced renormalization of the hybrid exciton resonance hole tunnelling through the hBN barrier has been ex-
energies in all these systems can be quantitatively re- plored. Figure 5F shows a color map of the reflectance
produced by a phenomenological model in which the hy- signal from the MoSe2 /hBN/MoSe2 as a function of the
bridization between different exciton states is treated as a applied vertical electric field, where the resonances at
coupling between oscillators with resonance energies cor- 1.632 eV and 1.640 eV correspond to intralayer excitons
responding to the bare exciton states being hybridized in the top and bottom MoSe2 layers, respectively [83].
[5, 38, 82]. The black dashed lines in Figures 5D and 5E At large applied electric fields, several resonances with a
show the best fits of the experimental data to an oscilla- strong E-field dependence are observed, which originate
tor model, from which inter-/intralayer couplings as high from IXs with a large dipole moment leading to a sizeable
 10

Stark shift. The spectra for a positive top gate voltage rhombohedral AB/BA domains (see the sketch in the
(Vtg ) regime correspond to the IX↑ , which have a hole top panel of Figure 6C). The bottom panel of Figure
in the bottom layer and an electron in the top layer (see 6C shows a dark-field TEM image of one of their near-
the schematic of the energy bands and the exciton en- 0◦ -twist-angle MoSe2 /MoSe2 homo-bilayers, where al-
ergy alignment under electric fields in Figure 5F). Inter- ternating, micrometre-sized AB and BA domains can
estingly, the results in Figure 5F show that IX↑ hybridize be observed due to the effects of atomic reconstruc-
exclusively with intralayer excitons in the top layer, as tion. Further, the authors showed that the broken
seen by a multitude of avoided crossings, which unequiv- mirror/inversion symmetry exhibited by the alternating
ocally shows that the coupling originates exclusively from AB/BA domains results into an effective locking of the
spin-conserving hole tunnelling. Finally, the existence of domain atomic stacking and the orientation of the IX
multiple avoided crossings demonstrates the existence of permanent dipole moment: AB (BA) domains host IXs
a moiré superlattice in the MoSe2 /hBN/MoSe2 hetero- with permanent electric dipole pointing up (down) [81].
structure. This effect leads to opposite energy Stark shifts for IXs
in AB and BA domains under applied vertical electric
fields. Figure 6D shows electric-field-dependent PL spec-
Structural effects on the PL of interlayer excitons tra of IXs measured at three different spots in a twisted
MoSe2 /MoSe2 homo-bilayer (first three panels from the
Beyond the effects of applied external electric fields, left) [81]. As can be seen in the first two panels, the IXs
carrier doping, layer- and exciton-hybridization, and the in two of the measured spots show field-dependent Stark
moiré superlattice discussed in the previous sections, the shifts with similar magnitude but opposite signs, indicat-
structural properties of the TMD hetero-structures such ing that the excitons in the two spots presented opposite
as strain and atomic reconstruction also play an im- dipole moments (as schematically shown in the insets).
portant role on the optical and electric properties of Interestingly, these measurements also showed that the
their host IXs. Recently, it has been shown that the dipole orientation in both spots can be flipped at large
PL of IXs in TMD homo- and hetero-bilayers can be enough applied fields. The results of a third spot demon-
profoundly affected by the structural properties of the strate IX with Stark shifts with both positive (blue-shift)
hetero-structure [81, 88–90]. In Ref. [88], the authors and negative (red-shift) slopes, indicating the presence of
used real-space imaging to show how the application of both AB and BA domains inside the dimensions of the
uniaxial hetero-strain in a WSe2 /MoSe2 moiré hetero- confocal PL spot. The authors were also able to exploit
bilayer, where the weak vdW interaction between the the domain-dependent sign of the IX Stark shift to gen-
layers can result in different deformation, leads to a tran- erate a spatial map of the electric dipole moment of the
sition from a triangular moiré lattice of zero-dimensional IX in their sample (see right panel in Figure 6D).
traps into parallel stripes of one-dimensional quantum Finally, in Ref. [96] the authors showed one-to-one
wires. Figure 6A illustrates the concept and shows ex- correlations between local spectral features and sample
perimental results for a nominally unstrained (top pan- morphology in non-gated MoSe2 /WSe2 hetero-bilayers,
els) and a strained hetero-bilayer (bottom panel). In- which suggests the co-existence of domains of different
terestingly, optical spectroscopy characterization of the dimensionality and exciton characteristics. Their results
samples revealed that the IX PL changes drastically from show that reconstructed 2D domains with large lateral di-
the unstrained to the strained samples. Figure 6B shows mensions in small-twist hetero-bilayers exhibit clear lu-
representative low-temperature PL spectra measured in minescent singlet and triplet IXs while split intralayer
nominally unstrained (top) and strained hetero-bilayers exciton resonances and spectrally narrow IXs are present
(bottom) for helicity-resolved photon collection. As can in the 1D domains connecting the extended 2D domains
be seen in these plots, the PL emission from IXs in to arrays of nanometre-sized 0D domains.
strained samples (i.e., depicting one-dimensional moiré
potentials) shows linear polarization and two orders of
magnitude higher intensity than the circularly-polarized INTERACTIONS
quantum emitter-like sharp PL peaks characteristic of
the zero-dimensional moiré traps. Interlayer excitons interacting with electronic states
In addition to active approaches to modify the IX emis- in moiré hetero-structures
sion through structural modifications of the TMD hetero-
structures, intrinsic structural effects such as atomic re- First predicted theoretically in 2018 [99, 100], it has
construction and domain formation in twisted hetero- been experimentally shown that strong electronic cor-
structures [91–96] can also strongly alter the IX prop- relations can arise in the flat-bands of TMD hetero-
erties. In Ref. [81], a combination of electronic and op- structures that arise due to the moiré superlattice struc-
tical far-field spectroscopy is employed to study near-0◦ - ture [18, 19, 83, 101]. In this scenario, the flat bands
twist-angle MoSe2 /MoSe2 homo-bilayers featuring large quench the kinetic energy of the charge carriers relative
 11

FIG. 6. Structural effects on the PL of interlayer excitons [MoSe2 /WSe2 (A, B) and twisted MoSe2 /MoSe2 (C, D)].
(A) Top left: sketch of a MoSe2 /WSe2 hetero-bilayer with a twist angle of 2◦ at no applied strain. The dashed lines indicate
the supercell of the hexagonal moiré superlattice, where A, B and C represent high-symmetry points preserving the C3 sym-
metry within the supercell. Bottom left: skecth of a MoSe2 /WSe2 hetero-bilayer with a twist angle of 0.5◦ under an applied
uniaxial hetero-strain of 8%. The arrows indicate the resulting primary 1D moiré structures. Right panels: experimental
piezoresponse force microscopy (PFM) images of the same spatial spot in a MoSe2 /WSe2 hetero-bilayer with a twist angle
of ∼59◦ under no applied (top) and applied uniaxial strain (bottom). (B) Representative PL spectra from two MoSe2 /WSe2
hetero-bilayer samples with h-BN encapsulation showing circularly-polarized quantum emitter-like sharp PL peaks (top) and
linearly-polarized ensemble IX emission (bottom). The blue and orange lines represent helicity-resolved spectra for σ + and
σ − emission, respectively, under σ + excitation. (C) Top panels: top and side views of the atomic structure in a twisted
MoSe2 /MoSe2 homo-bilayer showing rhombohedral AB (left) and BA stacking configurations (right). Bottom panel: dark-field
TEM image of a near-0◦ -twist-angle MoSe2 /MoSe2 bilayer showing alternating, micrometre-sized AB and BA domains. (D)
Electric-field-dependent PL spectra of IXs measured at three different spots of a twisted MoSe2 /MoSe2 homo-bilayer (first three
panels from the left). The insets show sketches of the predominant orientation of the permanent electric dipole at each spot.
The right panel shows a map of the magnitude (PL+ -PL− )/(PL+ +PL− ), which is proportional to the orientation (up/down)
of the permanent electric dipole. PL± is the PL intensity at Ez = ±0.15 V nm−1 , integrated over the energy range below 1.36
eV. Adapted with permission from Ref. [88] (A, B), and Ref. [81] (C, D), Nature Publishing Group.

to their Coulomb interaction energy, and several stable probes, novel many-body ground states are formed via
charge ordered phases, designated as Wigner crystals and the interaction of moiré excitons and correlated electron
Mott insulators, are observed at multiple fractional fill- lattices.
ings (ν) of the moiré lattice. Selected examples of ordered
states are shown in Figure 7A. In a WSe2 /WS2 moiré hetero-structure, Liu et al. in-
vestigated the PL from IXs as a function of fractional
Initially, the charge ordered states were optically filling of the moiré lattice [21]. Abrupt changes in PL
probed using the dielectric response of IXs to the cor- intensity and photon energy are observed at a number
related electronic states [18, 19, 83, 101]. However, due of different fractional fillings corresponding to correlated
to their large permanent dipole, IXs are not only highly insulating states at ν = -2, -3/2, -8/7, -1, -1/3, -1/4,
tunable with applied electric field, but they are highly 1/4, 1/3, 2/5, 2/3, 6/7, 1, 5/4, 5/3, and 13/7. This
sensitive to their charge environment. Natural questions modulation can arise because the insulating phases have
to ask then, is how do the correlated electronic phases reduced charge screening which renormalizes the band
affect the IX emission and can one use the trapped IX gap and exciton (or trion) binding energy. Further, the
as a sensitive local probe of the electronic crystallization valley polarization is modulated by the charge ordered
in the vicinity of the IX? In addition to use IXs as local states. The degree of valley polarization is measured by
 12

FIG. 7. Excitonic insulators in moiré superlattice structures [WSe2 /hBN/MoSe2 (A-D), WSe2 /WS2 (e-I)].
(A) Schematic of dual-gated bilayer devices. Anti-symmetric gating ∆ reduces the gap energy EG . The symmetric gating Vg
tunes the electron and hole density difference. (B) Scheme of the type II band alignment of MoSe2 /WSe2 . A bias voltage
Vb reduces the charge gap. IXs can form. (C) Electrostatics simulation of the bilayer based on a parallel-plate capacitor
model. Depending on bias and gate voltages, the bilayer can be in an intrinsic (i), positively (p) and negatively (n) doped
regime. (D) Normalized penetration capacitance CP /Cgg as a function of bias and gate voltages (Cgg gate-to-gate capacitance).
Charge incompressible region is marked by red dashed lines. The estimated exciton binding energy in the limit of zero exciton
density is 25 meV. (measurements done at 15 K and ∆ = 4.6 V). (E) Schematic of a dual-gated WSe2 /WS2 hetero-bilayer.
(F) Illustration of the moiré exciton lattice with one of the moiré unit cells with double occupancy. (G) IX PL intensity as a
function of gate voltage (doping) and emission energy for low (left) and high optical excitation intensity (right). Filling factors
are labelled. With increasing excitation intensity, the PL peak IX2 (34 meV above the ground state) appears. (H) IX PL
intensity versus excitation power P . The threshold Pth for the occurrence of IX3 and IX4 is marked by dashed lines. (I)
Energy level diagram for a single moiré orbit occupied by multiple exciton dipoles. Solid (dashed) line indicates the scenario
with (without) onsite dipole–dipole interaction. Expected PL spectrum from the dipole ladder with constant energy spacing
between IX1 and IX3 . IX4 originates from the fourth exciton localized in the second moiré orbital and has hence lower energy.
Adapted with permission from Ref. [97] (A-D) and from Ref. [98] (E-I).

spectrally integrating the PL intensity ratio (IRR - IRL ) hetero-structures are reported for various material com-
/ (IRR + IRL ), where the subscripts RR and RL indi- binations [24, 98] including natural bilayers [22, 23] and
cate excitation-detection right- and left-handed circular with ultrathin hBN separation layer [97] as shown in Fig-
polarization. The degree of valley polarization clearly ure 7(A). Strong onsite dipole-dipole interaction of ex-
decreases at the transition from conducting to insulating citons occupying the same moiré lattice is reported for
states. The valley polarization is limited by intervalley WSe2 /WS2 bilayers with the interaction between those
scattering and thus dependent on the electron-hole ex- IXs given by the Hubbard U parameter [98] (see Figure
change interaction, which increases when the screening 7 (E, F)). PL measurements reveal a dipole ladder with
effect is reduced. Hence, in the insulating states, the emission peak separation of around 34 meV as summa-
intervalley scattering is increased and the valley polar- rized in Figures 7 (G-I). The authors conclude from such
ization reduced. a large Hubbard parameter that in such systems exci-
ton crystal phases can be possibly realized [98]. Signa-
tures for the formation of an incompressible IX state in
Excitonic insulators in moiré structures a MoS2 /hBN/WSe2 hetero-structure has been deduced
from capacitance measurements in Ref. [97] (see Fig-
IXs with at least one constituent residing in a moiré- ures 7 (C-D)). An incompressible state in this context
flat band are prone to form correlated bosonic states means that the chemical potential of the system increases
similar to the fermionic Mott-insulator state. Experi- discontinuously as a function of exciton density [102].
mental observations of excitonic insulator states in TMD Similarly, signatures for the formation of an incompress-
 13

ible exciton state formed in WS2 /bilayer WSe2 hetero- with a Lorentzian luminescence profile allow accessing
junction moiré superlattice for exciton filling factor ν=1 coherent phases of dense and mobile IXs, consistent with
have been observed by utilizing microwave impedance mi- the predicted quantum degeneracy at low temperature
croscopy and differential reflectance spectroscopy ∆R/R [3, 107]. In contrast, Gaussian luminescence profiles with
[22]. Those signatures exhibit a peculiar temperature possible sub-structures appear at higher temperatures
dependence and vanish above a critical temperature of and/or at the presence of additional localized excitons
about 90 K, suggesting the formation of an exciton in- (cf. Figures 8A and above sections).
sulator state of IXs at low temperatures [22]. Interest- In principle, luminescence experiments allow distin-
ingly, Xiong et al. report the phase diagram for a mixed guishing whether bosonic or fermionic interactions dom-
fermionic and bosonic correlated insulator for 60◦ -aligned inate within the ensembles of mobile IXs: for an increas-
WSe2 /WS2 [24]. The excess electron density nex and the ing exciton density, a decrease of the full-width at half
exciton density nX were experimentally controlled and maximum (FWHM) of homogeneously broadened lumi-
the mixed correlated insulator state has been observed nescence spectra is understood as a signature for a dom-
along the line of ntot = nex + ne = 1. Again, the exciton inating bosonic characteristic within the exciton ensem-
correlated insulator states are experimentally identified bles [106]. A corresponding increase of the FWHM is
by their incompressible nature determined by a special less unambiguous, pointing towards fermionic interac-
type of optical pump-probe spectroscopy in analogy to tions, but also towards the interaction with further par-
the electrical capacitance measurements [24]. ticles, such as phonons [106, 129, 130]. The temporal
coherence of the luminescence can be accessed by the
help of Michelson-Morley interferometers. The corre-
Degenerate ensembles of mobile interlayer excitons sponding coherent part of the interferometers’ signal is
expressed as the normalized first order correlation func-
At low temperatures and high exciton densities, ther- tion |g (1) (τ )| [131], with τ the time delay between the
malized ensembles of mobile IXs can be considered to be two optical paths within the interferometer (cf. Figures
degenerate in vdW hetero-bilayers, as soon as the exci- 8C). Particularly, a bi-exponential decay of |g (1) (τ )| as
tonic thermal de-Broglie wavelength exceeds the mutual in Figures 8C allows accessing the homogeneously broad-
distance between the IXs [103, 104]. The correspond- ened (Lorentzian) part of a luminescence spectrum (cf.
ing phase diagram includes this degeneracy phase with a Figures 8A and [131]). Recent work suggests that degen-
predicted local superfluidity at a temperature below 10s erate ensembles of mobile IXs in MoSe2 /WSe2 hetero-
of Kelvin and a possible Berezinskii–Kosterlitz–Thouless bilayers show such a coherent luminescence of “synchro-
transition to a phase with an expected macroscopic su- nized” emitters [3], with the temporal coherence time,
perfluidity at even lower temperatures [105]. At high ex- the FWHM of |g (1) (τ )| being in the regime of 100s of fs.
citon densities (above ∼ 1012 cm−2 ), a Mott transition to At present, this fast time scale is related to the emission
a degenerate electron-hole Fermi gas is expected wherein process of the photons. At higher temperatures, when
fermionic interactions between the electrons and holes the IX ensembles are expected to be in the phase of a
dominate [104, 105]. Recently, it was proposed that also non-degenerate, classical gas, the corresponding |g (1) (τ )|
for the degenerate phase both the fermionic and bosonic is reduced and it seems to follow a Gaussian profile (cf.
characteristics of the exciton ensembles need to be con- Figures 8C and [107]).
sidered, particularly at the presence of phonons [106]. For measuring the spatial coherence of the IXs’ lu-
The coherence of the ground state of such many-body minescence, it is essential that the spatial pattern of
ensembles can be deduced from the temporal and spa- the excitonic luminescence is isotropic in the plane of
tial coherences as measured in luminescence experiments the hetero-bilayer (e.g. Figures 8B) and that the point-
(see Figures 8A and [3, 107–115]). For such experi- spread function (PSF) of the utilized optical system both
ments, IXs are advantageous compared to intralayer ex- at the wavelength of the optical excitation and detec-
citons due to their relatively long lifetime of tens to hun- tion is thoroughly understood [107]. Then, with the
dreds of nanoseconds [1, 2, 116, 117] and a permanent help of a point-inverting Michelson-Morley interferom-
dipole moment [5] (see above sections). The long lifetime eter [132, 133], the spatial dependence of the normal-
allows performing time-resolved experiments, such that ized first order correlation function |g (1) (x, y)| can be
the IX ensembles can be considered to be thermalized imaged, with x and y the coordinates within the ref-
before they emit a photon [107, 117], while the out-of- erence frame of the hetero-bilayers (cf. Figures 8D).
plane dipole drives an in-plane expansion of the IXs. In Importantly, such spatial coherence experiments need to
turn, the IX mobility can be straight-forwardly “imaged” be performed again in a time-resolved manner, because
as soon as the spatial luminescence pattern exceeds the only when the excitation laser is off for several 100s of
optical excitation area (Figures 8B and section below, fs to ps, laser-induced coherences as well as thermal-
[118–128]). Recent experimental work on MoSe2 /WSe2 ization dynamics within the hetero-bilayers can be ex-
hetero-bilayers suggests that IX ensembles particularly cluded to impact the IXs’ luminescence [107]. The lat-
 14

FIG. 8. Degenerate ensembles of mobile IXs and the coherence of their luminescence [MoSe2 /WSe2 (A - E)].
(A) PL spectra from a MoSe2 /WSe2 hetero-bilayer with h-BN encapsulation at the bath temperature ranging from 1.7 K
to 14 K. The maximum at ∼1.38 eV corresponds to IXs. (B) Corresponding spatial PL map in a false-color plot at 1.7 K
[green (blue) equals high (low) intensity], demonstrating an isotropic expansion of the IXs in the plane of the hetero-bilayer.
Dotted circle highlights the point spread function (PSF) at the IX wavelength (1.38 eV ∼ 0.9 µm). Scale bar, 1 µm. (C)
Normalized first order correlation function |g (1) (τ )| of the IX luminescence for 1.7 K and 14 K, with τ the time delay as given
by a Michelson-Morley interferometer. (D) Spatial dependence of the normalized first order correlation function |g (1) (x, y)| at
τ = 0. (E) Temperature dependence of the spatial coherence length xc . Dotted and dashed-dotted lines represent the point
spread function PSF at the emission wavelength [as in (B)] and the excitation energy (1.94 eV ∼ 639 nm). Adapted with
permission from Ref. [107]

eral FWHM of |g (1) (x, y)|, e.g. as measured along the Dynamics of interlayer excitons: formation and
dashed line in Figure 8D, gives access to the spatial co- transport
herence length xc of the IXs’ luminescence. Recent ex-
periments on MoSe2 /WSe2 hetero-bilayers demonstrate As discussed, in most TMD-based hetero-bilayer type-
that xc can exceed the PSFs of the optical imaging appa- II band alignment with efficient IX formation upon sep-
ratus at the experimental temperature when the IXs can aration of electron and hole states in adjacent layers
be theoretically considered to be degenerate (cf. Figure is commonly reported. Already in 2014, Hong et al.
8E and [107]). Then, xc can be even equal to the over- [138] experimentally demonstrated ultrafast interlayer
all expansion of the IXs ensembles [107]. Future studies, charge transfer withing 50 fs of photo-excited carriers
e.g. on laterally patterned hetero-bilayers [121, 134–136], across the vdW gap in MoS2 /WS2 hetero-bilayers. This
might reveal whether the predicted local or macroscopic process is surprisingly fast since the photoexcited car-
superfluidity explains the extended spatial coherence of riers are supposed to live at the K-valley formed by
the luminescence. Moreover, for an unambiguous exper- transition-metal d-orbitals that are well localized within
imental evidence of a pure bosonic exciton condensation each layer such that tunneling over the vdW gap is re-
in the momentum space, back-focal plane imaging seems quired for charge transfer [139]. Combined experimen-
to be suitable, however, at temperatures significantly be- tal and theoretical effort established that this ultrafast
low 1K [137]. charge transfer is mediated by efficient intervalley phonon
scattering connecting the layer localized CB K-states
with the strongly hybridized Σ-states facilitating ultra-
 15

fast charge transfer [139–143]. By femtosecond momen- CONCLUSION AND OUTLOOK

tum microscopy together with microscopic modelling, the
authors in Ref. [143] showed that momentum indirect
We introduced the fundamental concepts of how the in-
Σ − K intralayer excitons and layer hybridized hΣ − K-
terplay of spins, valley degree of freedom, moiré superlat-
IXs form via exciton-phonon scattering in WSe2 mono-
tic formation, doping as well as exteral stimuli determine
layers and WSe2 /MoS2 hetero-bilayers, respectively. In-
the properties of exciton species in homo- and hetero-
terestingly, the relative level alignment between the di-
bilayer TMD devices. The interplay of the different de-
rect K −K- and the indirect (h)Σ−K-excitons matters in
grees of freedom is dictated by the precise details of the
the radiative decay process. If the Σ-states are energeti-
stacking of the bilayer TMDs such that their properties
cally lower compared to K as in the hetero-bilayer, an ex-
can be widely engineered. This review provides a snap-
citon cascade transfers the K−K-exciton over the hΣ−K
shot of the state-of-the-art experimental demonstrations
into a true IX [143]. For a (nearly) degenerate alignment,
in the field, including the first devices that provide tech-
as in WSe2 monolayers, the exciton occupation decays
nological implementations that exploit the novel proper-
predominantly radiatively via the bright K − K-exciton
ties of IXs in moiré materials. Altogether, these results
indicating the crucial role of level alignment that is prone
establish a strong foundation for a wide range of future
to changes by internal and external stimuli such as em-
fundamental studies and developing technologies. In the
bedding in vdW stacks that can e.g. impact interlyer hy-
following, we provide a perspective on future challenges
bridization or interlayer phonon coupling, dielectric envi-
and a few worthwhile pursuits in this rapidly emerging
ronment, doping or strain and is hence is highly tunable
topic.
[143, 144]. The crucial role of the phonons in these ultra-
fast charge transfer processes has been directly confirmed One exciting prospect is exploiting the highly tunable
from ultrafast electron diffraction visualizing the lattice properties of trapped IXs as quantum light sources. Be-
dynamics in photoexcited WSe2 /WS2 [145]. cause of the IXs’ large permanent dipole, DC Stark tun-
ing of the exciton energy over a wide range is facile.
So far, the quantum nature of the emission has been
demonstrated with individual IXs trapped via the intrin-
sic moiré potential, but an additional avenue to pursue
is extrinsic trapping of IXs for quantum light sources,
Several partially competing impact factors underlie the for example via localized strain or electrostatic poten-
transport properties of excitons species in vdW bilayer tial via tunable gating [152–154]. The externally gen-
structures resulting in a wealth of different scenarios erated potentials for trapping can enable deterministic
[6, 146–148]. Moiré superlattice potential modulation positioning and scalability for applications in quantum
can result in nearly complete localized excitons while photonics. For these applications, nanophotonic struc-
shallow twist and/or high IX densities foster tunneling tures will be required to achieve Purcell enhancement
between moiré sites resulting in hopping transport such and increased light-matter interaction efficiencies. An
that the diffusion length is highly dependent on materials open question is how coherent the generated photons can
combination and twist angle and can even reach a few be; can highly indistinguishable photons be generated in
microns in commensurate vdW bilayers [148–151]. IXs these platforms? Similarly, open questions exist about
with constituents localized in adjacent layers hold a per- the potential to exploit the spin-valley degrees of free-
manent dipolar moment such that dipole-dipole interac- dom of trapped IXs to enable a coherent spin-photon
tion, i.e. repulsion modulates exciton transport in vdW interface. On the other hand, the intrinsically high den-
bilayers and allows for long-range propagation [6, 147]. sity of precisely arranged quantum emitters in the moiré
Large linear diffusion coefficients even at low IX den- lattice provides a platform for investigations of sub- and
sities have been shown for reconstructed, low-disorder super-radiant Dicke states with applications in quantum
MoSe2 /WSe2 hetero-bilayers at cryogenic temperatures information science.
[147]. Non-linear propagation in those structures arise From a many-body physics point of view, the long life-
from nearly equally contribution from exciton-exciton re- times and strong dipolar interactions of Bosonic neutral
pulsion and annihilation [147]. Layer hybridized IXs have IXs in TMD moiré materials can yield correlated exci-
a reduced out-of plane dipolar moment and dipolar inter- tonic states, as described by the Bose-Hubbard model.
action contributes less to exciton transport. Tagarelli et Changing the band structure (determined by the material
al. demonstrate that the degree of hybridization can be combinations), moiré period and exciton density provide
tuned by electric fields enabling control of IX transport access to a wide range of the Bose-Hubbard phase dia-
in vdW hetero-bilayers [6]. Understanding and control- gram in different regimes such as non-interacting Bose
ling of exciton transport in vdW bilayer structures is im- gas phase, superfluid phase, quadrupolar and dipolar
portant for both the realization of efficient excitonic and exciton ensembles, Mott insulator phase or beyond the
optoelectronic devices. Mott transition an electron-hole plasma phase [155–159].
 16

By adding a charge to the localized, neutral excitons AUTHORS CONTRIBUTIONS

via electrostatic gating, charged Fermi-polarons can be
created, providing access to the Fermi-Hubbard model. All authors discussed the content of the manuscript
Overall, a significant goal in the field is to realize de- and wrote it together.
signer many-body Hamiltonians in moiré superlattices as
a new platform for quantum simulators. Employing IXs
as probes of these systems remains a compelling concept. FUNDING
Moreover, for MoSe2 /WSe2 hetero-bilayers, reported sig-
natures of degenerate exciton ensembles with an ex-
We gratefully acknowledge financial support from the
tended lateral coherence [3, 107] suggest that hetero-
German Science Foundation via Grants HO 3324/9-2,
bilayers also allow studying bosonic and fermionic corre-
WU 637/4-2 and 7-1, the clusters of excellence MCQST
lations in mobile exciton ensembles. In addition to tuning
(EXS-2111) and e-conversion (EXS2089), and the prior-
the phase diagram by the stacking configuration during
ity program 2244 (2DMP). M.B.-G. is supported by a
fabrication, an important target will be to in-situ tune
Royal Society University Research Fellowship. B.D.G. is
the interaction parameters. Two approaches can readily
supported by a Chair in Emerging Technology from the
be pursued: applying hetero-strain to tune the geometry
Royal Academy of Engineering and the European Re-
of the moiré lattice [160] or controlling the relative twist
search Council (grant no. 725920)
angle between the bilayers [161].

To date, most TMD moiré devices have consisted of COMPETING INTERESTS

only a handful of individual atomic layers; due to poor
fabrication yield, a device consisting of a few TMD layers
encapsulated in hBN layers and electronic gating with There is no conflict of interest.
graphene layers is considered a ‘hero’ device in many
laboratories. This limits the boundless opportunities to
DATA AVAILABILITY
freely engineer and add to the many degrees of freedom
for dipoles in multilayer devices. For instance, spin-layer
locking adds an additional layer degree of freedom in Included in cited original research papers.
the system while giant interlayer dipoles extending over
more than two-layers can in principle be engineered. Fur-
ther, multilayer devices with independently configurable
hetero-interfaces yield exciting prospects such as multi- ∗
m.brotons i [email protected]
orbital moire superlattices or multiple moiré periodicities †
[email protected]
of varying moiré potential strength. ‡
[email protected]
§
[email protected]
A final challenge, not solely confined to moiré TMD [1] Pasqual Rivera, John R. Schaibley, Aaron M. Jones, Ja-
devices but for the entire field of vdW moiré materials, son S. Ross, Sanfeng Wu, Grant Aivazian, Philip Kle-
is the development of improved fabrication techniques ment, Kyle Seyler, Genevieve Clark, Nirmal J. Ghimire,
Jiaqiang Yan, D. G. Mandrus, Wang Yao, and Xi-
that take steps towards reproducible and homogeneous aodong Xu, “Observation of long-lived interlayer exci-
moiré superlattices with deterministic periodicity. Cur- tons in monolayer MoSe2–WSe2 heterostructures,” Na-
rent state-of-the-art fabrication techniques yield signifi- ture Communications 6, 6242 (2015), number: 1 Pub-
cant inhomogeneities within the moiré superlattice, in- lisher: Nature Publishing Group.
cluding twist angle disorder and defects such as bubbles [2] Bastian Miller, Alexander Steinhoff, Borja Pano, Julian
or wrinkles. Additionally, substantial sample-to-sample Klein, Frank Jahnke, Alexander Holleitner, and Ursula
Wurstbauer, “Long-Lived Direct and Indirect Interlayer
variation presents reproducibility issues across different
Excitons in van der Waals Heterostructures,” Nano Let-
laboratories. Important questions to address include ters 17, 5229–5237 (2017), publisher: American Chem-
“How homogeneous can a moiré material be?” and “How ical Society.
does twist-angle disorder affect or determine the emer- [3] Lukas Sigl, Florian Sigger, Fabian Kronowetter,
gent physical properties of the moiré material?” Further, Jonas Kiemle, Julian Klein, Kenji Watanabe, Takashi
increased reproducibility and moiré homogeneity are es- Taniguchi, Jonathan J. Finley, Ursula Wurstbauer, and
sential to realize more complex samples and devices with Alexander W. Holleitner, “Signatures of a degener-
ate many-body state of interlayer excitons in a van
increasing number of layers and contacts. Finally, im-
der Waals heterostack,” Physical Review Research 2,
proved and reproducible low-resistance Ohmic contacts 042044 (2020), publisher: American Physical Society.
to TMDs would facilitate transport measurements on a [4] Alberto Ciarrocchi, Dmitrii Unuchek, Ahmet Avsar,
regular basis, a crucial technique which can compliment Kenji Watanabe, Takashi Taniguchi, and Andras Kis,
optical investigations of moiré TMD devices. “Polarization switching and electrical control of inter-
 17

layer excitons in two-dimensional van der Waals het- tov, “Superconductors, orbital magnets and correlated
erostructures,” Nature Photonics 13, 131–136 (2019). states in magic-angle bilayer graphene,” Nature 574,
[5] Jonas Kiemle, Florian Sigger, Michael Lorke, Bastian 653–657 (2019).
Miller, Kenji Watanabe, Takashi Taniguchi, Alexander [17] Yanhao Tang, Lizhong Li, Tingxin Li, Yang Xu,
Holleitner, and Ursula Wurstbauer, “Control of the or- Song Liu, Katayun Barmak, Kenji Watanabe, Takashi
bital character of indirect excitons in MoS2 /WS2 heter- Taniguchi, Allan H. MacDonald, Jie Shan, and
obilayers,” Physical Review B 101, 121404 (2020). Kin Fai Mak, “Simulation of hubbard model physics
[6] Fedele Tagarelli, Edoardo Lopriore, Daniel Erkensten, in wse2/ws2 moiré superlattices,” Nature 579, 353–358
Raül Perea-Causı́n, Samuel Brem, Joakim Hagel, Zhe (2020).
Sun, Gabriele Pasquale, Kenji Watanabe, Takashi [18] Yang Xu, Song Liu, Daniel A Rhodes, Kenji Watan-
Taniguchi, Ermin Malic, and Andras Kis, “Electrical abe, Takashi Taniguchi, James Hone, Veit Elser, Kin Fai
control of hybrid exciton transport in a van der waals Mak, and Jie Shan, “Correlated insulating states at
heterostructure,” Nature photonics 17, 615–621 (2023). fractional fillings of moiré superlattices,” Nature 587,
[7] Mauro Brotons-Gisbert, Alfredo Segura, Roberto Rob- 214–218 (2020).
les, Enric Canadell, Pablo Ordejón, and Juan F [19] Emma C Regan, Danqing Wang, Chenhao Jin, M Iqbal
Sánchez-Royo, “Optical and electronic properties of 2H- Bakti Utama, Beini Gao, Xin Wei, Sihan Zhao, Wenyu
MoS2 under pressure: Revealing the spin-polarized na- Zhao, Zuocheng Zhang, Kentaro Yumigeta, et al., “Mott
ture of bulk electronic bands,” Physical review materials and generalized Wigner crystal states in WSe2 /WS2
2, 054602 (2018). moiré superlattices,” Nature 579, 359–363 (2020).
[8] Paul Steeger, Jan-Hauke Graalmann, Robert Schmidt, [20] Jiaqi Cai, Eric Anderson, Chong Wang, Xiaowei Zhang,
Ilya Kupenko, Carmen Sanchez-Valle, Philipp Xiaoyu Liu, William Holtzmann, Yinong Zhang, Fen-
Marauhn, Thorsten Deilmann, Steffen Michaelis gren Fan, Takashi Taniguchi, Kenji Watanabe, Ying
de Vasconcellos, Michael Rohlfing, and Rudolf Ran, Ting Cao, Liang Fu, Di Xiao, Wang Yao, and Xi-
Bratschitsch, “Pressure dependence of intra- and aodong Xu, “Signatures of fractional quantum anoma-
interlayer excitons in 2h-mos2 bilayers,” Nano lous hall states in twisted mote2,” Nature 622, 63–68
Letters 23, 8947–8952 (2023), pMID: 37734032, (2023).
https://doi.org/10.1021/acs.nanolett.3c02428. [21] Erfu Liu, Takashi Taniguchi, Kenji Watanabe,
[9] Viviana Villafañe, Malte Kremser, Ruven Hübner, Nathaniel M Gabor, Yong-Tao Cui, and Chun Hung
Marko M. Petrić, Nathan P. Wilson, Andreas V. Stier, Lui, “Excitonic and valley-polarization signatures of
Kai Müller, Matthias Florian, Alexander Steinhoff, and fractional correlated electronic phases in a WSe2 /WS2
Jonathan J. Finley, “Twist-dependent intra- and inter- moiré superlattice,” Physical Review Letters 127,
layer excitons in moiré mose2 homobilayers,” Phys. Rev. 037402 (2021).
Lett. 130, 026901 (2023). [22] Dongxue Chen, Zhen Lian, Xiong Huang, Ying Su,
[10] Nihit Saigal and Ursula Wurstbauer, “Excitons stabilize Mina Rashetnia, Lei Ma, Li Yan, Mark Blei, Li Xiang,
above the band gap in bilayer wse2,” Nature Nanotech- Takashi Taniguchi, Kenji Watanabe, Sefaattin Ton-
nology 19, 141–142 (2024). gay, Dmitry Smirnov, Zenghui Wang, Chuanwei Zhang,
[11] Ka Wai Lau, Calvin, Zhirui Gong, Hongyi Yu, and Yong-Tao Cui, and Su-Fei Shi, “Excitonic insulator in a
Wang Yao, “Interface excitons at lateral heterojunctions heterojunction moiré superlattice,” Nature Physics 18,
in monolayer semiconductors,” Phys. Rev. B 98, 115427 1171–1176 (2022).
(2018). [23] Zuocheng Zhang, Emma C. Regan, Danqing Wang,
[12] Jun Kang, Jingbo Li, Shu-Shen Li, Jian-Bai Xia, and Wenyu Zhao, Shaoxin Wang, Mohammed Sayyad, Ken-
Lin-Wang Wang, “Electronic structural Moiré pattern taro Yumigeta, Kenji Watanabe, Takashi Taniguchi,
effects on MoS2 /MoSe2 2D heterostructures,” Nano Let- Sefaattin Tongay, Michael Crommie, Alex Zettl,
ters 13, 5485–5490 (2013). Michael P. Zaletel, and Feng Wang, “Correlated inter-
[13] Fengcheng Wu, Timothy Lovorn, Emanuel Tutuc, and layer exciton insulator in heterostructures of monolayer
A. H. MacDonald, “Hubbard model physics in tran- wse2 and moiré ws2/wse2,” Nature Physics 18, 1214–
sition metal dichalcogenide moiré bands,” Phys. Rev. 1220 (2022).
Lett. 121, 026402 (2018). [24] Richen Xiong, Jacob H. Nie, Samuel L. Brantly,
[14] H Baek, M Brotons-Gisbert, ZX Koong, A Camp- Patrick Hays, Renee Sailus, Kenji Watanabe, Takashi
bell, M Rambach, K Watanabe, T Taniguchi, and Taniguchi, Sefaattin Tongay, and Chenhao Jin, “Cor-
BD Gerardot, “Highly energy-tunable quantum light related insulator of excitons in wse2/ws2 moiré superlat-
from moiré-trapped excitons,” Science Advances 6, tices,” Science (New York, N.Y.) 380, 860–864 (2023).
eaba8526 (2020). [25] Trithep Devakul, Valentin Cr®pel, Yang Zhang, and
[15] Isaac Soltero, Mikhail A. Kaliteevski, James G. Liang Fu, “Magic in twisted transition metal dichalco-
McHugh, Vladimir Enaldiev, and Vladimir I. genide bilayers,” Nature communications 12, 6730
Fal’ko, “Competition of moiré network sites (2021).
to form electronic quantum dots in recon- [26] Hongyi Yu, Xiaodong Cui, Xiaodong Xu, and Wang
structed mox2/wx2 heterostructures,” Nano Let- Yao, “Valley excitons in two-dimensional semiconduc-
ters 24, 1996–2002 (2024), pMID: 38295286, tors,” National Science Review 2, 57–70 (2015).
https://doi.org/10.1021/acs.nanolett.3c04427. [27] Gang Wang, Alexey Chernikov, Mikhail M Glazov,
[16] Xiaobo Lu, Petr Stepanov, Wei Yang, Ming Xie, Mo- Tony F Heinz, Xavier Marie, Thierry Amand, and
hammed Ali Aamir, Ipsita Das, Carles Urgell, Kenji Bernhard Urbaszek, “Colloquium: Excitons in atomi-
Watanabe, Takashi Taniguchi, Guangyu Zhang, Adrian cally thin transition metal dichalcogenides,” Reviews of
Bachtold, Allan H. MacDonald, and Dmitri K. Efe- Modern Physics 90, 021001 (2018).
 18

[28] Alexey Chernikov, Timothy C Berkelbach, Heather M [41] Jing Liang, Dongyang Yang, Jingda Wu, Jerry I Dadap,
Hill, Albert Rigosi, Yilei Li, Ozgur Burak Aslan, Kenji Watanabe, Takashi Taniguchi, and Ziliang Ye,
David R Reichman, Mark S Hybertsen, and Tony F “Optically probing the asymmetric interlayer coupling
Heinz, “Exciton binding energy and nonhydrogenic Ry- in rhombohedral-stacked mos2 bilayer,” Physical Re-
dberg series in monolayer WS2 ,” Physical Review Let- view X 12, 041005 (2022).
ters 113, 076802 (2014). [42] Iann C Gerber, Emmanuel Courtade, Shivangi Shree,
[29] Keliang He, Nardeep Kumar, Liang Zhao, Zefang Wang, Cedric Robert, Takashi Taniguchi, Kenji Watanabe,
Kin Fai Mak, Hui Zhao, and Jie Shan, “Tightly bound Andrea Balocchi, Pierre Renucci, Delphine Lagarde,
excitons in monolayer WSe2 ,” Physical Review Letters Xavier Marie, et al., “Interlayer excitons in bilayer MoS2
113, 026803 (2014). with strong oscillator strength up to room tempera-
[30] Di Xiao, Gui-Bin Liu, Wanxiang Feng, Xiaodong Xu, ture,” Physical Review B 99, 035443 (2019).
and Wang Yao, “Coupled spin and valley physics [43] Shun Feng, Aidan Campbell, Mauro Brotons-Gisbert,
in monolayers of MoS2 and other group-VI dichalco- Daniel Andres-Penares, Hyeonjun Baek, Takashi
genides,” Physical Review Letters 108, 196802 (2012). Taniguchi, Kenji Watanabe, Bernhard Urbaszek, Iann C
[31] Xiaodong Xu, Wang Yao, Di Xiao, and Tony F Gerber, and Brian D Gerardot, “Highly Tunable
Heinz, “Spin and pseudospins in layered transition Ground and Excited State Excitonic Dipoles in Mul-
metal dichalcogenides,” Nature Physics 10, 343–350 tilayer 2H-MoSe2 ,” arXiv preprint arXiv:2212.14338
(2014). (2022).
[32] Kin Fai Mak, Keliang He, Jie Shan, and Tony F Heinz, [44] Yinong Zhang, Chengxin Xiao, Dmitry Ovchinnikov, Ji-
“Control of valley polarization in monolayer MoS2 by ayi Zhu, Xi Wang, Takashi Taniguchi, Kenji Watanabe,
optical helicity,” Nature Nanotechnology 7, 494–498 Jiaqiang Yan, Wang Yao, and Xiaodong Xu, “Every-
(2012). other-layer dipolar excitons in a spin-valley locked su-
[33] Hualing Zeng, Junfeng Dai, Wang Yao, Di Xiao, and perlattice,” Nature nanotechnology 18, 501–506 (2023).
Xiaodong Cui, “Valley polarization in MoS2 monolayers [45] Jun Kang, Sefaattin Tongay, Jian Zhou, Jingbo Li, and
by optical pumping,” Nature Nanotechnology 7, 490– Junqiao Wu, “Band offsets and heterostructures of two-
493 (2012). dimensional semiconductors,” Applied Physics Letters
[34] Ashish Arora, Matthias Drüppel, Robert Schmidt, 102, 012111 (2013).
Thorsten Deilmann, Robert Schneider, Maciej R Mo- [46] Ming-Hui Chiu, Chendong Zhang, Hung-Wei Shiu,
las, Philipp Marauhn, Steffen Michaelis de Vasconcel- Chih-Piao Chuu, Chang-Hsiao Chen, Chih-Yuan S
los, Marek Potemski, Michael Rohlfing, et al., “Inter- Chang, Chia-Hao Chen, Mei-Yin Chou, Chih-Kang
layer excitons in a bulk van der waals semiconductor,” Shih, and Lain-Jong Li, “Determination of band align-
Nature communications 8, 1–6 (2017). ment in the single-layer MoS2 /WSe2 heterojunction,”
[35] Zefang Wang, Yi-Hsin Chiu, Kevin Honz, Kin Fai Mak, Nature Communications 6, 7666 (2015).
and Jie Shan, “Electrical tuning of interlayer exciton [47] Neil R Wilson, Paul V Nguyen, Kyle Seyler, Pasqual
gases in WSe2 bilayers,” Nano Letters 18, 137–143 Rivera, Alexander J Marsden, Zachary PL Laker,
(2018). Gabriel C Constantinescu, Viktor Kandyba, Alexei
[36] Jason Horng, Tineke Stroucken, Long Zhang, Eunice Y Barinov, Nicholas DM Hine, Xiaodong Xu, and
Paik, Hui Deng, and Stephan W Koch, “Observation David H Cobden, “Determination of band offsets, hy-
of interlayer excitons in MoSe2 single crystals,” Physical bridization, and exciton binding in 2D semiconductor
Review B 97, 241404 (2018). heterostructures,” Science Advances 3, e1601832 (2017).
[37] Nadine Leisgang, Shivangi Shree, Ioannis Paradisanos, [48] Pasqual Rivera, John R Schaibley, Aaron M Jones, Ja-
Lukas Sponfeldner, Cedric Robert, Delphine Lagarde, son S Ross, Sanfeng Wu, Grant Aivazian, Philip Kle-
Andrea Balocchi, Kenji Watanabe, Takashi Taniguchi, ment, Kyle Seyler, Genevieve Clark, Nirmal J Ghimire,
Xavier Marie, et al., “Giant Stark splitting of an exciton Jiaqiang Yan, D. G. Mandrus, Wang Yao, and Xi-
in bilayer MoS2 ,” Nature Nanotechnology 15, 901–907 aodong Xu, “Observation of long-lived interlayer exci-
(2020). tons in monolayer MoSe2 -WSe2 heterostructures,” Na-
[38] Etienne Lorchat, Malte Selig, Florian Katsch, Kentaro ture Communications 6, 6242 (2015).
Yumigeta, Sefaattin Tongay, Andreas Knorr, Christian [49] Pasqual Rivera, Kyle L Seyler, Hongyi Yu, John R
Schneider, and Sven Höfling, “Excitons in Bilayer MoS2 Schaibley, Jiaqiang Yan, David G Mandrus, Wang Yao,
Displaying a Colossal Electric Field Splitting and Tun- and Xiaodong Xu, “Valley-polarized exciton dynamics
able Magnetic Response,” Physical Review Letters 126, in a 2D semiconductor heterostructure,” Science 351,
037401 (2021). 688–691 (2016).
[39] Namphung Peimyoo, Thorsten Deilmann, Freddie [50] Aubrey T Hanbicki, Hsun-Jen Chuang, Matthew R
Withers, Janire Escolar, Darren Nutting, Takashi Rosenberger, C Stephen Hellberg, Saujan V Sivaram,
Taniguchi, Kenji Watanabe, Alireza Taghizadeh, Mon- Kathleen M McCreary, Igor I Mazin, and Berend T
ica Felicia Craciun, Kristian Sommer Thygesen, et al., Jonker, “Double indirect interlayer exciton in a
“Electrical tuning of optically active interlayer excitons MoSe2 /WSe2 van der Waals heterostructure,” Acs Nano
in bilayer MoS2 ,” Nature Nanotechnology , 1–6 (2021). 12, 4719–4726 (2018).
[40] Ioannis Paradisanos, Shivangi Shree, Antony George, [51] Bastian Miller, Alexander Steinhoff, Borja Pano, Julian
Nadine Leisgang, Cedric Robert, Kenji Watanabe, Klein, Frank Jahnke, Alexander Holleitner, and Ursula
Takashi Taniguchi, Richard J Warburton, Andrey Tur- Wurstbauer, “Long-lived direct and indirect interlayer
chanin, Xavier Marie, et al., “Controlling interlayer ex- excitons in van der waals heterostructures,” Nano Let-
citons in MoS2 layers grown by chemical vapor deposi- ters 17, 5229–5237 (2017).
tion,” Nature Communications 11, 1–7 (2020).
 19

[52] Philipp Nagler, Gerd Plechinger, Mariana V Ballottin, locking of interlayer excitons trapped in moiré poten-
Anatolie Mitioglu, Sebastian Meier, Nicola Paradiso, tials,” Nature Materials 19, 630 (2020).
Christoph Strunk, Alexey Chernikov, Peter C M Chris- [65] Elyse Barré, Ouri Karni, Erfu Liu, Aidan L O’Beirne,
tianen, Christian Schüller, and Tobias Korn, “Inter- Xueqi Chen, Henrique B Ribeiro, Leo Yu, Bumho
layer exciton dynamics in a dichalcogenide monolayer Kim, Kenji Watanabe, Takashi Taniguchi, et al., “Opti-
heterostructure,” 2D Materials 4, 025112 (2017). cal absorption of interlayer excitons in transition-metal
[53] Luis A Jauregui, Andrew Y Joe, Kateryna Pistunova, dichalcogenide heterostructures,” Science 376, 406–410
Dominik S Wild, Alexander A High, You Zhou, Gio- (2022).
vanni Scuri, Kristiaan De Greve, Andrey Sushko, Che- [66] Xi Wang, Jiayi Zhu, Kyle L. Seyler, Pasqual Rivera,
Hang Yu, et al., “Electrical control of interlayer exciton Huiyuan Zheng, Yingqi Wang, Minhao He, Takashi
dynamics in atomically thin heterostructures,” Science Taniguchi, Kenji Watanabe, Jiaqiang Yan, David G.
366, 870–875 (2019). Mandrus, Daniel R. Gamelin, Wang Yao, and Xiaodong
[54] Artur Branny, Santosh Kumar, Raphaël Proux, and Xu, “Moiré trions in mose2/wse2 heterobilayers,” Na-
Brian D Gerardot, “Deterministic strain-induced arrays ture Nanotechnology 16, 1208–1213 (2021).
of quantum emitters in a two-dimensional semiconduc- [67] Erfu Liu, Elyse Barré, Jeremiah van Baren, Matthew
tor,” Nature Communications 8, 15053 (2017). Wilson, Takashi Taniguchi, Kenji Watanabe, Yong-
[55] Carmen Palacios-Berraquero, Dhiren M Kara, Alejan- Tao Cui, Nathaniel M Gabor, Tony F Heinz, Yia-
dro R-P Montblanch, Matteo Barbone, Pawel Latawiec, Chung Chang, et al., “Signatures of moiré trions
Duhee Yoon, Anna K Ott, Marko Loncar, Andrea C Fer- in WSe2 /MoSe2 heterobilayers,” Nature 594, 46–50
rari, and Mete Atatüre, “Large-scale quantum-emitter (2021).
arrays in atomically thin semiconductors,” Nature Com- [68] Hyeonjun Baek, Mauro Brotons-Gisbert, Aidan Camp-
munications 8, 15093 (2017). bell, Valerio Vitale, Johannes Lischner, Kenji Watan-
[56] Malte Kremser, Mauro Brotons-Gisbert, Johannes abe, Takashi Taniguchi, and Brian D Gerardot, “Op-
Knörzer, Janine G´’uckelhorn, Moritz Meyer, Matteo tical read-out of Coulomb staircases in a moiré super-
Barbone, Andreas V Stier, Brian D Gerardot, Kai lattice via trapped interlayer trions,” Nature Nanotech-
M´’uller, and Jonathan J Finley, “Discrete interactions nology , 1–7 (2021).
between a few interlayer excitons trapped at a MoSe2 - [69] Mauro Brotons-Gisbert, Hyeonjun Baek, Aidan Camp-
WSe2 heterointerface,” npj 2D Materials and Applica- bell, Kenji Watanabe, Takashi Taniguchi, and Brian D
tions 4, 1–6 (2020). Gerardot, “Moiré-trapped interlayer trions in a charge-
[57] Weijie Li, Xin Lu, Sudipta Dubey, Luka Devenica, and tunable WSe2 /MoSe2 heterobilayer,” Physical Review
Ajit Srivastava, “Dipolar interactions between localized X 11, 1–12 (2021).
interlayer excitons in van der Waals heterostructures,” [70] Tianmeng Wang, Shengnan Miao, Zhipeng Li, Yuze
Nature Materials 19, 624 (2020). Meng, Zhengguang Lu, Zhen Lian, Mark Blei, Takashi
[58] Hongyi Yu, Gui-Bin Liu, Jianju Tang, Xiaodong Xu, Taniguchi, Kenji Watanabe, Sefaattin Tongay, et al.,
and Wang Yao, “Moiré excitons: From programmable “Giant valley-Zeeman splitting from spin-singlet and
quantum emitter arrays to spin-orbit–coupled artificial spin-triplet interlayer excitons in WSe2 /MoSe2 het-
lattices,” Science Advances 3, e1701696 (2017). erostructure,” Nano letters 20, 694–700 (2019).
[59] Fengcheng Wu, Timothy Lovorn, and AH MacDonald, [71] Andrew Y Joe, Luis A Jauregui, Kateryna Pistunova,
“Theory of optical absorption by interlayer excitons in Andrés M Mier Valdivia, Zhengguang Lu, Dominik S
transition metal dichalcogenide heterobilayers,” Physi- Wild, Giovanni Scuri, Kristiaan De Greve, Ryan J Gelly,
cal Review B 97, 035306 (2018). You Zhou, et al., “Electrically controlled emission from
[60] Chendong Zhang, Chih-Piao Chuu, Xibiao Ren, Ming- singlet and triplet exciton species in atomically thin
Yang Li, Lain-Jong Li, Chuanhong Jin, Mei-Yin Chou, light-emitting diodes,” Physical Review B 103, L161411
and Chih-Kang Shih, “Interlayer couplings, Moiré pat- (2021).
terns, and 2D electronic superlattices in MoS2 /WSe2 [72] Dinh Van Tuan, Su-Fei Shi, Xiaodong Xu, Scott A
hetero-bilayers,” Science Advances 3, e1601459 (2017). Crooker, and Hanan Dery, “Six-body and eight-body
[61] Thorsten Deilmann, Michael Rohlfing, and Ursula exciton states in monolayer WSe2 ,” Physical Review
Wurstbauer, “Light–matter interaction in van der waals Letters 129, 076801 (2022).
hetero-structures,” Journal of Physics: Condensed Mat- [73] Yuya Shimazaki, Clemens Kuhlenkamp, Ido Schwartz,
ter 32, 333002 (2020). Tomasz Smoleński, Kenji Watanabe, Takashi Taniguchi,
[62] Hongyi Yu, Gui-Bin Liu, and Wang Yao, “Bright- Martin Kroner, Richard Schmidt, Michael Knap, and
ened spin-triplet interlayer excitons and optical selec- Ataç Imamoğlu, “Optical signatures of periodic charge
tion rules in van der Waals heterobilayers,” 2D Materi- distribution in a mott-like correlated insulator state,”
als 5, 035021 (2018). Physical Review X 11, 021027 (2021).
[63] Kyle L Seyler, Pasqual Rivera, Hongyi Yu, Nathan P [74] Chenhao Jin, Emma C Regan, Aiming Yan,
Wilson, Essance L Ray, David G Mandrus, Jiaqiang M Iqbal Bakti Utama, Danqing Wang, Sihan Zhao,
Yan, Wang Yao, and Xiaodong Xu, “Signatures of Ying Qin, Sijie Yang, Zhiren Zheng, Shenyang Shi,
moiré-trapped valley excitons in MoSe2 /WSe2 hetero- et al., “Observation of moiré excitons in WSe2 /WS2
bilayers,” Nature 567, 66–70 (2019). heterostructure superlattices,” Nature 567, 76 (2019).
[64] Mauro Brotons-Gisbert, Hyeonjun Baek, Alejandro [75] David A. Ruiz-Tijerina and Vladimir I. Fal’ko, “Inter-
Molina-Sánchez, Aidan Campbell, Eleanor Scerri, layer hybridization and moiré superlattice minibands for
Daniel White, Kenji Watanabe, Takashi Taniguchi, electrons and excitons in heterobilayers of transition-
Cristian Bonato, and Brian D Gerardot, “Spin-layer metal dichalcogenides,” Phys. Rev. B 99, 125424 (2019).
 20

[76] Evgeny M Alexeev, David A Ruiz-Tijerina, Mark 132, 076902 (2024).

Danovich, Matthew J Hamer, Daniel J Terry, [88] Yusong Bai, Lin Zhou, Jue Wang, Wenjing Wu, Leo J
Pramoda K Nayak, Seongjoon Ahn, Sangyeon Pak, Ju- McGilly, Dorri Halbertal, Chiu Fan Bowen Lo, Fang
won Lee, Jung Inn Sohn, et al., “Resonantly hybridized Liu, Jenny Ardelean, Pasqual Rivera, et al., “Excitons
excitons in moiré superlattices in van der Waals het- in strain-induced one-dimensional moiré potentials at
erostructures,” Nature 567, 81 (2019). transition metal dichalcogenide heterojunctions,” Na-
[77] Fengcheng Wu, Timothy Lovorn, and Allan H MacDon- ture Materials 19, 1068–1073 (2020).
ald, “Topological exciton bands in moiré heterojunc- [89] Shen Zhao, Zhijie Li, Xin Huang, Anna Rupp, Jonas
tions,” Physical Review Letters 118, 147401 (2017). Göser, Ilia A. Vovk, Stanislav Yu. Kruchinin, Kenji
[78] Dongxue Chen, Zhen Lian, Xiong Huang, Ying Su, Watanabe, Takashi Taniguchi, Ismail Bilgin, Anvar S.
Mina Rashetnia, Li Yan, Mark Blei, Takashi Taniguchi, Baimuratov, and Alexander Högele, “Excitons in meso-
Kenji Watanabe, Sefaattin Tongay, et al., “Tuning scopically reconstructed moiré heterostructures,” Na-
moiré excitons and correlated electronic states through ture Nanotechnology 18, 572–579 (2023).
layer degree of freedom,” Nature Communications 13, [90] Zhijie Li, Farsane Tabataba-Vakili, Shen Zhao, Anna
4810 (2022). Rupp, Ismail Bilgin, Ziria Herdegen, Benjamin März,
[79] Mit H Naik, Emma C Regan, Zuocheng Zhang, Yang- Kenji Watanabe, Takashi Taniguchi, Gabriel Ravan-
Hao Chan, Zhenglu Li, Danqing Wang, Yoseob Yoon, hani Schleder, Anvar S. Baimuratov, Efthimios Kaxi-
Chin Shen Ong, Wenyu Zhao, Sihan Zhao, et al., “In- ras, Knut Müller-Caspary, and Alexander Högele,
tralayer charge-transfer moiré excitons in van der waals “Lattice reconstruction in mose2–wse2 heterobilay-
superlattices,” Nature 609, 52–57 (2022). ers synthesized by chemical vapor deposition,” Nano
[80] Xi Wang, Xiaowei Zhang, Jiayi Zhu, Heonjoon Park, Letters 23, 4160–4166 (2023), pMID: 37141148,
Yingqi Wang, Chong Wang, William G Holtzmann, https://doi.org/10.1021/acs.nanolett.2c05094.
Takashi Taniguchi, Kenji Watanabe, Jiaqiang Yan, [91] VV Enaldiev, Viktor Zólyomi, CELAL Yelgel,
et al., “Intercell moiré exciton complexes in electron lat- SJ Magorrian, and VI Fal’ko, “Stacking domains and
tices,” Nature Materials 22, 599–604 (2023). dislocation networks in marginally twisted bilayers of
[81] Jiho Sung, You Zhou, Giovanni Scuri, Viktor Zólyomi, transition metal dichalcogenides,” Physical Review Let-
Trond I Andersen, Hyobin Yoo, Dominik S Wild, An- ters 124, 206101 (2020).
drew Y Joe, Ryan J Gelly, Hoseok Heo, et al., “Broken [92] Astrid Weston, Yichao Zou, Vladimir Enaldiev, Alex
mirror symmetry in excitonic response of reconstructed Summerfield, Nicholas Clark, Viktor Zólyomi, Abi-
domains in twisted mose2 /mose2 bilayers,” Nature Nan- gail Graham, Celal Yelgel, Samuel Magorrian, Mingwei
otechnology 15, 750–754 (2020). Zhou, et al., “Atomic reconstruction in twisted bilayers
[82] Yanhao Tang, Jie Gu, Song Liu, Kenji Watanabe, of transition metal dichalcogenides,” Nature Nanotech-
Takashi Taniguchi, James Hone, Kin Fai Mak, and nology 15, 592–597 (2020).
Jie Shan, “Tuning layer-hybridized moiré excitons by [93] Leo J McGilly, Alexander Kerelsky, Nathan R Finney,
the quantum-confined Stark effect,” Nature Nanotech- Konstantin Shapovalov, En-Min Shih, Augusto Ghiotto,
nology 16, 52–57 (2021). Yihang Zeng, Samuel L Moore, Wenjing Wu, Yusong
[83] Yuya Shimazaki, Ido Schwartz, Kenji Watanabe, Bai, et al., “Visualization of moiré superlattices,” Na-
Takashi Taniguchi, Martin Kroner, and Ataç ture Nanotechnology 15, 580–584 (2020).
Imamoğlu, “Strongly correlated electrons and hybrid ex- [94] Matthew R Rosenberger, Hsun-Jen Chuang, Madeleine
citons in a moiré heterostructure,” Nature 580, 472–477 Phillips, Vladimir P Oleshko, Kathleen M McCreary,
(2020). Saujan V Sivaram, C Stephen Hellberg, and Berend T
[84] Philipp Nagler, Fabian Mooshammer, Jens Kunst- Jonker, “Twist angle-dependent atomic reconstruction
mann, Mariana V Ballottin, Anatolie Mitioglu, Alexey and moiré patterns in transition metal dichalcogenide
Chernikov, Andrey Chaves, Frederick Stein, Nicola Par- heterostructures,” ACS Nano 14, 4550–4558 (2020).
adiso, Sebastian Meier, et al., “Interlayer excitons in [95] Trond I. Andersen, Giovanni Scuri, Andrey Sushko,
transition-metal dichalcogenide heterobilayers,” Phys- Kristiaan de Greve, Jiho Sung, You Zhou, Dominik S.
ica Status Solidi (b) 256, 1900308 (2019). Wild, Ryan J. Gelly, Hoseok Heo, Damien Bérubé, An-
[85] Ke Wu, Hongxia Zhong, Quanbing Guo, Jibo Tang, drew Y. Joe, Luis A. Jauregui, Kenji Watanabe, Takashi
Jing Zhang, Lihua Qian, Zhifeng Shi, Chendong Zhang, Taniguchi, Philip Kim, Hongkun Park, and Mikhail D.
Shengjun Yuan, Shunping Zhang, et al., “Identification Lukin, “Excitons in a reconstructed moiré potential in
of twist-angle-dependent excitons in WS2 /WSe2 heter- twisted wse2/wse2 homobilayers,” Nature materials 20,
obilayers,” National Science Review (2021). 480–487 (2021).
[86] Lukas Sponfeldner, Nadine Leisgang, Shivangi Shree, [96] Shen Zhao, Zhijie Li, Xin Huang, Anna Rupp, Jonas
Ioannis Paradisanos, Kenji Watanabe, Takashi Göser, Ilia A. Vovk, Stanislav Yu. Kruchinin, Kenji
Taniguchi, Cedric Robert, Delphine Lagarde, Andrea Watanabe, Takashi Taniguchi, Ismail Bilgin, Anvar S.
Balocchi, Xavier Marie, et al., “Capacitively-coupled Baimuratov, and Alexander Högele, “Excitons in meso-
and inductively-coupled excitons in bilayer MoS2 ,” scopically reconstructed moiré heterostructures,” Na-
arXiv preprint arXiv:2108.04248 (2021). ture Nanotechnology 18, 572–579 (2023).
[87] Borislav Polovnikov, Johannes Scherzer, Subhradeep [97] Liguo Ma, Phuong X. Nguyen, Zefang Wang, Yongxin
Misra, Xin Huang, Christian Mohl, Zhijie Li, Jonas Zeng, Kenji Watanabe, Takashi Taniguchi, Allan H.
Göser, Jonathan Förste, Ismail Bilgin, Kenji Watanabe, MacDonald, Kin Fai Mak, and Jie Shan, “Strongly
Takashi Taniguchi, Alexander Högele, and Anvar S. correlated excitonic insulator in atomic double layers,”
Baimuratov, “Field-Induced Hybridization of Moiré Ex- Nature 598, 585–589 (2021).
citons in M2 /WS2 Heterobilayers,” Phys. Rev. Lett.
 21

[98] Heonjoon Park, Jiayi Zhu, Xi Wang, Yingqi Wang, [111] Zefang Wang, Daniel A. Rhodes, Kenji Watanabe,
William Holtzmann, Takashi Taniguchi, Kenji Watan- Takashi Taniguchi, James C. Hone, Jie Shan, and
abe, Jiaqiang Yan, Liang Fu, Ting Cao, Di Xiao, Kin Fai Mak, “Evidence of high-temperature exciton
Daniel R. Gamelin, Hongyi Yu, Wang Yao, and Xi- condensation in two-dimensional atomic double layers,”
aodong Xu, “Dipole ladders with large hubbard inter- Nature 574, 76–80 (2019), number: 7776 Publisher: Na-
action in a moiré exciton lattice,” Nature Physics 19, ture Publishing Group.
1286–1292 (2023). [112] Anshul Kogar, Melinda S. Rak, Sean Vig, Ali A. Husain,
[99] Fengcheng Wu, Timothy Lovorn, Emanuel Tutuc, and Felix Flicker, Young Il Joe, Luc Venema, Greg J. Mac-
Allan H MacDonald, “Hubbard model physics in transi- Dougall, Tai C. Chiang, Eduardo Fradkin, Jasper van
tion metal dichalcogenide moiré bands,” Physical review Wezel, and Peter Abbamonte, “Signatures of exciton
letters 121, 026402 (2018). condensation in a transition metal dichalcogenide,” Sci-
[100] Mit H Naik and Manish Jain, “Ultraflatbands and shear ence 358, 1314–1317 (2017), publisher: American As-
solitons in moiré patterns of twisted bilayer transition sociation for the Advancement of Science.
metal dichalcogenides,” Physical Review Letters 121, [113] Mathieu Alloing, Mussie Beian, Maciej Lewenstein,
266401 (2018). David Fuster, Yolanda González, Luisa González,
[101] Yanhao Tang, Lizhong Li, Tingxin Li, Yang Xu, Roland Combescot, Monique Combescot, and François
Song Liu, Katayun Barmak, Kenji Watanabe, Takashi Dubin, “Evidence for a Bose-Einstein condensate of ex-
Taniguchi, Allan H MacDonald, Jie Shan, et al., “Sim- citons,” Europhysics Letters 107, 10012 (2014), pub-
ulation of hubbard model physics in wse2/ws2 moiré lisher: EDP Sciences, IOP Publishing and Società Ital-
superlattices,” Nature 579, 353–358 (2020). iana di Fisica.
[102] A. H. MacDonald, “Introduction to the physics of [114] A. A. High, J. R. Leonard, M. Remeika, L. V. Butov,
the quantum hall regime,” arXiv:cond-mat/9410047 M. Hanson, and A. C. Gossard, “Condensation of Ex-
(1994), doi.org/10.48550/arXiv.cond-mat/9410047. citons in a Trap,” Nano Letters 12, 2605–2609 (2012),
[103] John M. Blatt, K. W. Böer, and Werner Brandt, “Bose- publisher: American Chemical Society.
Einstein Condensation of Excitons,” Physical Review [115] A. Griffin, D. W. Snoke, and S. Stringari, “Bose-
126, 1691–1692 (1962), publisher: American Physical Einstein Condensation,” (1995), iSBN: 9780521464734
Society. 9780521589901 9780511524240 Publisher: Cambridge
[104] B. Laikhtman and R. Rapaport, “Exciton correlations University Press.
in coupled quantum wells and their luminescence blue [116] Aubrey T. Hanbicki, Hsun-Jen Chuang, Matthew R.
shift,” Physical Review B 80, 195313 (2009), publisher: Rosenberger, C. Stephen Hellberg, Saujan V. Sivaram,
American Physical Society. Kathleen M. McCreary, Igor I. Mazin, and Berend T.
[105] M. M. Fogler, L. V. Butov, and K. S. Novoselov, “High- Jonker, “Double Indirect Interlayer Exciton in a
temperature superfluidity with indirect excitons in van MoSe2/WSe2 van der Waals Heterostructure,” ACS
der Waals heterostructures,” Nature Communications Nano 12, 4719–4726 (2018), publisher: American
5, 4555 (2014), number: 1 Publisher: Nature Publishing Chemical Society.
Group. [117] P. Merkl, F. Mooshammer, P. Steinleitner, A. Girnghu-
[106] Manuel Katzer, Malte Selig, Lukas Sigl, Mirco Troue, ber, K.-Q. Lin, P. Nagler, J. Holler, C. Schüller, J. M.
Johannes Figueiredo, Jonas Kiemle, Florian Sigger, Ur- Lupton, T. Korn, S. Ovesen, S. Brem, E. Malic, and
sula Wurstbauer, Alexander W. Holleitner, and An- R. Huber, “Ultrafast transition between exciton phases
dreas Knorr, “Exciton-phonon scattering: Competition in van der Waals heterostructures,” Nature Materials
between the bosonic and fermionic nature of bound 18, 691–696 (2019), number: 7 Publisher: Nature Pub-
electron-hole pairs,” Physical Review B 108, L121102 lishing Group.
(2023), publisher: American Physical Society. [118] L. V. Butov, A. A. Shashkin, V. T. Dolgopolov, K. L.
[107] Mirco Troue, Johannes Figueiredo, Lukas Sigl, Chris- Campman, and A. C. Gossard, “Magneto-optics of
tos Paspalides, Manuel Katzer, Takashi Taniguchi, the spatially separated electron and hole layers in
Kenji Watanabe, Malte Selig, Andreas Knorr, Ur- gaas/alxga1-xas coupled quantum wells,” Physical Re-
sula Wurstbauer, and Alexander W. Holleitner, “Ex- view B 60, 8753–8758 (1999), publisher: American
tended Spatial Coherence of Interlayer Excitons in Physical Society.
${\mathrm{MoSe}} {2}/{\mathrm{WSe}} {2}$ Het- [119] Z. Vörös, R. Balili, D. W. Snoke, L. Pfeiffer, and
erobilayers,” Physical Review Letters 131, 036902 K. West, “Long-Distance Diffusion of Excitons in Dou-
(2023), publisher: American Physical Society. ble Quantum Well Structures,” Physical Review Letters
[108] J. P. Eisenstein and A. H. MacDonald, “Bose–Einstein 94, 226401 (2005), publisher: American Physical Soci-
condensation of excitons in bilayer electron systems,” ety.
Nature 432, 691–694 (2004), number: 7018 Publisher: [120] A. Gärtner, A. W. Holleitner, J. P. Kotthaus, and
Nature Publishing Group. D. Schuh, “Drift mobility of long-living excitons in cou-
[109] Michael Stern, Vladimir Umansky, and Israel Bar- pled GaAs quantum wells,” Applied Physics Letters 89,
Joseph, “Exciton Liquid in Coupled Quantum Wells,” 052108 (2006).
Science 343, 55–57 (2014), publisher: American Asso- [121] A. Gärtner, L. Prechtel, D. Schuh, A. W. Holleitner,
ciation for the Advancement of Science. and J. P. Kotthaus, “Micropatterned electrostatic traps
[110] Xiaomeng Liu, Kenji Watanabe, Takashi Taniguchi, for indirect excitons in coupled GaAs quantum wells,”
Bertrand I. Halperin, and Philip Kim, “Quantum Hall Physical Review B 76, 085304 (2007), publisher: Amer-
drag of exciton condensate in graphene,” Nature Physics ican Physical Society.
13, 746–750 (2017), number: 8 Publisher: Nature Pub- [122] X. P. Vögele, D. Schuh, W. Wegscheider, J. P. Kotthaus,
lishing Group. and A. W. Holleitner, “Density Enhanced Diffusion of
 22

Dipolar Excitons within a One-Dimensional Channel,” Physical Review Letters 110, 127403 (2013), publisher:
Physical Review Letters 103, 126402 (2009), publisher: American Physical Society.
American Physical Society. [135] Y. Y. Kuznetsova, P. Andreakou, M. W. Hasling, J. R.
[123] Roland Zimmermann and Christoph Schindler, “Ex- Leonard, E. V. Calman, L. V. Butov, M. Hanson, and
citon–exciton interaction in coupled quantum wells,” A. C. Gossard, “Two-dimensional snowflake trap for in-
Solid State Communications Spontaneous coherence in direct excitons,” Optics Letters 40, 589 (2015).
exciton systems, 144, 395–398 (2007). [136] Daniel N. Shanks, Fateme Mahdikhanysarvejahany,
[124] M. M. Glazov, “Phonon wind and drag of excitons in Christine Muccianti, Adam Alfrey, Michael R. Koehler,
monolayer semiconductors,” Physical Review B 100, David G. Mandrus, Takashi Taniguchi, Kenji Watan-
045426 (2019), publisher: American Physical Society. abe, Hongyi Yu, Brian J. LeRoy, and John R. Schaib-
[125] Koloman Wagner, Jonas Zipfel, Roberto Rosati, ley, “Nanoscale Trapping of Interlayer Excitons in a
Edith Wietek, Jonas D. Ziegler, Samuel Brem, Raül 2D Semiconductor Heterostructure,” Nano Letters 21,
Perea-Causı́n, Takashi Taniguchi, Kenji Watanabe, 5641–5647 (2021), publisher: American Chemical Soci-
Mikhail M. Glazov, Ermin Malic, and Alexey ety.
Chernikov, “Nonclassical Exciton Diffusion in Mono- [137] Lukas Sigl, Mirco Troue, Manuel Katzer, Malte Selig,
layer ${\mathrm{WSe}} {2}$,” Physical Review Let- Florian Sigger, Jonas Kiemle, Mauro Brotons-Gisbert,
ters 127, 076801 (2021), publisher: American Physical Kenji Watanabe, Takashi Taniguchi, Brian D. Gerardot,
Society. Andreas Knorr, Ursula Wurstbauer, and Alexander W.
[126] Zhe Sun, Alberto Ciarrocchi, Fedele Tagarelli, Holleitner, “Optical dipole orientation of interlayer
Juan Francisco Gonzalez Marin, Kenji Watanabe, excitons in ${\mathrm{MoSe}} {2}\ensuremath{-
Takashi Taniguchi, and Andras Kis, “Excitonic trans- }{\mathrm{WSe}} {2}$ heterostacks,” Physical
port driven by repulsive dipolar interaction in a van der Review B 105, 035417 (2022), publisher: American
waals heterostructure,” Nature Photonics , 1–7 (2021). Physical Society.
[127] Kanak Datta, Zhengyang Lyu, Zidong Li, Takashi [138] Xiaoping Hong, Jonghwan Kim, Su-Fei Shi, Yu Zhang,
Taniguchi, Kenji Watanabe, and Parag B. Deotare, Chenhao Jin, Yinghui Sun, Sefaattin Tongay, Junqiao
“Spatiotemporally controlled room-temperature exciton Wu, Yanfeng Zhang, and Feng Wang, “Ultrafast charge
transport under dynamic strain,” Nature Photonics 16, transfer in atomically thin mos2 /ws2 heterostructures,”
242–247 (2022), number: 3 Publisher: Nature Publish- Nature Nanotechnology 9, 682–686 (2014).
ing Group. [139] Giuseppe Meneghini, Samuel Brem, and Ermin Malic,
[128] Ruoming Peng, Adina Ripin, Yusen Ye, Jiayi Zhu, “Ultrafast phonon–driven charge transfer in van der
Changming Wu, Seokhyeong Lee, Huan Li, Takashi waals heterostructures,” Natural Sciences 2 (2022),
Taniguchi, Kenji Watanabe, Ting Cao, Xiaodong Xu, 10.1002/ntls.20220014.
and Mo Li, “Long-range transport of 2D excitons [140] Julien Madéo, Michael K. L. Man, Chakradhar Sahoo,
with acoustic waves,” Nature Communications 13, 1334 Marshall Campbell, Vivek Pareek, E. Laine Wong, Ab-
(2022), number: 1 Publisher: Nature Publishing Group. dullah Al-Mahboob, Nicholas S. Chan, Arka Karmakar,
[129] Malte Selig, Gunnar Berghäuser, Archana Raja, Philipp Bala Murali Krishna Mariserla, Xiaoqin Li, Tony F.
Nagler, Christian Schüller, Tony F. Heinz, Tobias Korn, Heinz, Ting Cao, and Keshav M. Dani, “Directly visual-
Alexey Chernikov, Ermin Malic, and Andreas Knorr, izing the momentum-forbidden dark excitons and their
“Excitonic linewidth and coherence lifetime in mono- dynamics in atomically thin semiconductors,” Science
layer transition metal dichalcogenides,” Nature Com- (New York, N.Y.) 370, 1199–1204 (2020).
munications 7 (2016), 10.1038/ncomms13279. [141] Jonas E. Zimmermann, Marleen Axt, Fabian Moosham-
[130] Galan Moody, Chandriker Kavir Dass, Kai Hao, Chang- mer, Philipp Nagler, Christian Schüller, Tobias Korn,
Hsiao Chen, Lain-Jong Li, Akshay Singh, Kha Tran, Ulrich Höfer, and Gerson Mette, “Ultrafast charge-
Genevieve Clark, Xiaodong Xu, Gunnar Berghäuser, transfer dynamics in twisted mos2/wse2 heterostruc-
Ermin Malic, Andreas Knorr, and Xiaoqin Li, “Intrinsic tures,” ACS nano 15, 14725–14731 (2021).
homogeneous linewidth and broadening mechanisms of [142] David Schmitt, Jan Philipp Bange, Wiebke Bennecke,
excitons in monolayer transition metal dichalcogenides,” AbdulAziz AlMutairi, Giuseppe Meneghini, Kenji
Nature Communications 6, 1–6 (2015). Watanabe, Takashi Taniguchi, Daniel Steil, D. Russell
[131] Rodney Loudon, The Quantum Theory of Light, 3rd ed. Luke, R. Thomas Weitz, Sabine Steil, G. S. Matthijs
(Oxford University Press, Oxford, 2000). Jansen, Samuel Brem, Ermin Malic, Stephan Hofmann,
[132] S. Savasta, O. Di Stefano, V. Savona, and W. Lang- Marcel Reutzel, and Stefan Mathias, “Formation of
bein, “Quantum Complementarity of Microcavity Po- moiré interlayer excitons in space and time,” Nature
laritons,” Physical Review Letters 94, 246401 (2005), 608, 499–503 (2022).
publisher: American Physical Society. [143] Jan Philipp Bange, Paul Werner, David Schmitt,
[133] Eunice Y. Paik, Long Zhang, G. William Burg, Rahul Wiebke Bennecke, Giuseppe Meneghini, AbdulAziz Al-
Gogna, Emanuel Tutuc, and Hui Deng, “Interlayer ex- Mutairi, Marco Merboldt, Kenji Watanabe, Takashi
citon laser of extended spatial coherence in atomically Taniguchi, Sabine Steil, Daniel Steil, R. Thomas Weitz,
thin heterostructures,” Nature 576, 80–84 (2019), num- Stephan Hofmann, G. S. Matthijs Jansen, Samuel Brem,
ber: 7785 Publisher: Nature Publishing Group. Ermin Malic, Marcel Reutzel, and Stefan Mathias, “Ul-
[134] G. J. Schinner, J. Repp, E. Schubert, A. K. Rai, trafast dynamics of bright and dark excitons in mono-
D. Reuter, A. D. Wieck, A. O. Govorov, A. W. Holleit- layer wse 2 and heterobilayer wse 2 /mos 2,” 2D Mate-
ner, and J. P. Kotthaus, “Confinement and Interac- rials 10, 035039 (2023).
tion of Single Indirect Excitons in a Voltage-Controlled [144] Iris Niehues, Philipp Marauhn, Thorsten Deilmann,
Trap Formed Inside Double InGaAs Quantum Wells,” Daniel Wigger, Robert Schmidt, Ashish Arora, Stef-
 23

fen Michaelis de Vasconcellos, Michael Rohlfing, and [152] Ke Wang, Kristiaan De Greve, Luis A Jauregui, Andrey
Rudolf Bratschitsch, “Strain tuning of the stokes shift in Sushko, Alexander High, You Zhou, Giovanni Scuri,
atomically thin semiconductors,” Nanoscale 12, 20786– Takashi Taniguchi, Kenji Watanabe, Mikhail D Lukin,
20796 (2020). et al., “Electrical control of charged carriers and exci-
[145] Aditya Sood, Jonah B. Haber, Johan CarlstrÂm, Eliza- tons in atomically thin materials,” Nature Nanotechnol-
beth A. Peterson, Elyse Barre, Johnathan D. Georgaras, ogy 13, 128–132 (2018).
Reid, Alexander H. M., Xiaozhe Shen, Marc E. Zajac, [153] Daniel N Shanks, Fateme Mahdikhanysarvejahany,
Emma C. Regan, Jie Yang, Takashi Taniguchi, Kenji Christine Muccianti, Adam Alfrey, Michael R Koehler,
Watanabe, Feng Wang, Xijie Wang, Jeffrey B. Neaton, David G Mandrus, Takashi Taniguchi, Kenji Watanabe,
Tony F. Heinz, Aaron M. Lindenberg, Felipe H. Da Jor- Hongyi Yu, Brian J LeRoy, et al., “Nanoscale trapping
nada, and Archana Raja, “Bidirectional phonon emis- of interlayer excitons in a 2d semiconductor heterostruc-
sion in two-dimensional heterostructures triggered by ture,” Nano Letters 21, 5641–5647 (2021).
ultrafast charge transfer,” Nature Nanotechnology 18, [154] Deepankur Thureja, Atac Imamoglu, Tomasz
29–35 (2023). Smoleński, Ivan Amelio, Alexander Popert, Thibault
[146] Ermin Malic, Raül Perea-Causin, Roberto Rosati, Chervy, Xiaobo Lu, Song Liu, Katayun Barmak,
Daniel Erkensten, and Samuel Brem, “Exciton trans- Kenji Watanabe, et al., “Electrically tunable quantum
port in atomically thin semiconductors,” Nature com- confinement of neutral excitons,” Nature 606, 298–304
munications 14, 3430 (2023). (2022).
[147] Edith Wietek, Matthias Florian, Jonas Göser, [155] Yevgeny Slobodkin, Yotam Mazuz-Harpaz, Sivan
Takashi Taniguchi, Kenji Watanabe, Alexander Högele, Refaely-Abramson, Snir Gazit, Hadar Steinberg, and
Mikhail M. Glazov, Alexander Steinhoff, and Alexey Ronen Rapaport, “Quantum phase transitions of tri-
Chernikov, “Nonlinear and negative effective diffusiv- layer excitons in atomically thin heterostructures,”
ity of interlayer excitons in moiré-free heterobilayers,” Physical Review Letters 125, 255301 (2020).
Phys. Rev. Lett. 132, 016202 (2024). [156] Camille Lagoin and François Dubin, “Key role of the
[148] Willy Knorr, Samuel Brem, Giuseppe Meneghini, and moiré potential for the quasicondensation of interlayer
Ermin Malic, “Exciton transport in a moiré poten- excitons in van der Waals heterostructures,” Physical
tial: From hopping to dispersive regime,” Physical Review B 103, L041406 (2021).
Review Materials 6 (2022), 10.1103/PhysRevMateri- [157] Daniel Erkensten, Samuel Brem, and Ermin
als.6.124002. Malic, “Exciton-exciton interaction in transition metal
[149] Junho Choi, Wei-Ting Hsu, Li-Syuan Lu, Liuyang Sun, dichalcogenide monolayers and van der Waals het-
Hui-Yu Cheng, Ming-Hao Lee, Jiamin Quan, Kha Tran, erostructures,” Physical Review B 103, 045426 (2021).
Chun-Yuan Wang, Matthew Staab, Kayleigh Jones, [158] Jue Wang, Qianhui Shi, En-Min Shih, Lin Zhou, Wen-
Takashi Taniguchi, Kenji Watanabe, Ming-Wen Chu, jing Wu, Yusong Bai, Daniel Rhodes, Katayun Bar-
Shangjr Gwo, Suenne Kim, Chih-Kang Shih, Xiaoqin mak, James Hone, Cory R Dean, et al., “Diffusivity
Li, and Wen-Hao Chang, “Moiré potential impedes reveals three distinct phases of interlayer excitons in
interlayer exciton diffusion in van der waals het- MoSe2 /WSe2 heterobilayers,” Physical Review Letters
erostructures,” Science Advances 6, eaba8866 (2020), 126, 106804 (2021).
https://www.science.org/doi/pdf/10.1126/sciadv.aba8866. [159] Niclas Götting, Frederik Lohof, and Christopher Gies,
[150] Long Yuan, Biyuan Zheng, Jens Kunstmann, Thomas “Moiré-bose-hubbard model for interlayer excitons in
Brumme, Agnieszka Beata Kuc, Chao Ma, Shibin Deng, twisted transition metal dichalcogenide heterostruc-
Daria Blach, Anlian Pan, and Libai Huang, “Twist- tures,” Physical Review B 105, 165419 (2022).
angle-dependent interlayer exciton diffusion in ws2-wse2 [160] M. Kögl, P. Soubelet, M. Brotons-Gisbert, A. V. Stier,
heterobilayers,” Nature materials 19, 617–623 (2020). B. D. Gerardot, and J. J. Finley, “Moiré straintronics:
[151] Zidong Li, Xiaobo Lu, Darwin F. Cordovilla Leon, a universal platform for reconfigurable quantum ma-
Zhengyang Lyu, Hongchao Xie, Jize Hou, Yanzhao Lu, terials,” npj 2D Materials and Applications 7 (2023),
Xiaoyu Guo, Austin Kaczmarek, Takashi Taniguchi, 10.1038/s41699-023-00382-4.
Kenji Watanabe, Liuyan Zhao, Li Yang, and Parag B. [161] A. Inbar, J. Birkbeck, J. Xiao, T. Taniguchi, K. Watan-
Deotare, “Interlayer exciton transport in mose2/wse2 abe, B. Yan, Y. Oreg, Ady Stern, E. Berg, and S. Ilani,
heterostructures,” ACS nano 15, 1539–1547 (2021). “The quantum twisting microscope,” Nature 614, 682–
687 (2023).