Nonlinear dynamics of a two-level system of a single spin driven beyond the

rotating-wave approximation
K. Rama Koteswara Rao and Dieter Suter
Fakultät Physik, Technische Universität Dortmund, D-44221 Dortmund, Germany
(Dated: May 12, 2017)
Quantum systems driven by strong oscillating fields are the source of many interesting physical
phenomena. In this work, we experimentally study the dynamics of a two-level system of a single
spin driven in the strong-driving regime where the rotating-wave approximation is not valid. This
two-level system is a subsystem of a single Nitrogen-Vacancy center in diamond coupled to a first-
shell 13 C nuclear spin at a level anti-crossing point. This near-degeneracy occurs in the ms = ±1
manifold of the electron spin when the energy level splitting between the ms = −1 and +1 states due
to the static magnetic field is ≈ 127 MHz and thus equal to the splitting due to the 13 C hyperfine
arXiv:1610.04512v2 [quant-ph] 11 May 2017

interaction. The transition frequency of this electron spin two-level system in a static magnetic
field of 28.9 G is 1.7 MHz and it can be driven only by the component of the RF field along the
NV symmetry axis. Electron spin Rabi frequencies in this system can reach tens of MHz even for
moderate RF powers. The simple sinusoidal Rabi oscillations that occur when the amplitude of the
driving field is small compared to the transition frequency evolve into complex patterns when the
driving field amplitude is comparable to or greater than the energy level splitting. We observe that
the system oscillates faster than the amplitude of the driving field and the response of the system
shows multiple frequencies.

PACS numbers: [Link], [Link], 33.35.+r, 61.72.J-

I. INTRODUCTION but not chaotic [8, 9]. Recently, the strong-driving regime
has been of particular interest to quantum information
processing because of the ultra-fast quantum gates pos-
Two-level systems are the basis for many important
sible in this regime [10–15].
fundamental concepts in diverse areas of physics, includ-
ing various types of resonance phenomena [1, 2]. A quan- In this work, we experimentally observe the anhar-
tum bit or qubit, which is realized physically by a two monic and non-linear dynamics of a two-level system of a
level quantum system, is the fundamental building block single solid-state spin driven in the strong-driving regime.
of quantum computation and quantum information pro- The system of interest is a single Nitrogen-Vacancy (NV)
tocols [3]. center (electron spin S=1) in diamond coupled to a first-
A two-level system is equivalent to a spin-1/2 parti- shell 13 C nuclear spin (I=1/2) and the intrinsic 14 N nu-
cle precessing in a static magnetic field, where the spin clear spin (I=1) of the center, which together form an
precession frequency is equal to the frequency separa- 18-level system. A small static magnetic field is applied
tion between the two levels. Resonance occurs when an at an orientation such that the energy level splitting due
oscillating field with a frequency equal to the spin pre- to the Zeeman interaction of the electron spin is equal
cession frequency is applied in a direction perpendicular to the corresponding splitting due to the 13 C hyperfine
to the static field. In most experimental situations, the interaction, which is approximately 127 MHz. At this
driving field is a linearly oscillating one and it can be point, Level Anti-Crossings (LACs) occur between the
written as a sum of a co- and a counter-rotating field ms = −1 and +1 spin-sublevels due to the strong non-
with respect to the spin precession. Most of the funda- secular components of the Hamiltonian. Far away from
mental concepts in optical and magnetic resonance are the LAC, electron spin transitions between these spin-
derived in the so-called weak-driving regime, where the sublevels are forbidden. At the LAC point, the ms = +1
amplitude of the driving field is much smaller than the and −1 spin states are completely mixed and a transition
spin precession frequency. In this regime, the effect of the can be excited between these levels by the component
counter-rotating field component can be neglected, which of an applied radio-frequency (RF) field that is parallel
is known as the rotating-wave approximation [2]. The to the NV symmetry axis (z-axis). The transition fre-
co-rotating field component causes harmonic oscillations quency of this electron spin transition is 1.7 MHz in a
between the two levels, which are known as Rabi oscilla- static magnetic field of 28.9 G. In this system, the elec-
tions. In the strong-driving regime, where the amplitude tron spin Rabi frequencies can reach tens of MHz even
of the driving field is of the order or greater than the for moderate RF powers. Hence, this two-level system
spin precession frequency, the rotating-wave approxima- forms a very interesting platform for studying dynamics
tion breaks down and the counter-rotating field compo- in the strong-driving regime. In the weak-driving regime,
nent, which can not be neglected any more, leads to many we observe clear sinusoidal Rabi oscillations of this two-
interesting physical phenomena [4–7]. In this regime, the level system. In the strong-driving regime, the dynamics
system’s dynamics are highly anharmonic and nonlinear, become complex as the system oscillates with multiple
 2

(a) (c)
2875
H =DSz2 + γe B · S + γn1 B · I1 + γn2 B · I2
2
2870 + P I2z + S · A 1 · I1 + S · A 2 · I2 . (1)
Here, S, I1 , and I2 represent spin angular momenta
2865 of the electron, 13 C and 14 N nuclei respectively, and
γe , γn1 , and γn2 the corresponding gyromagnetic ra-
(b) tios. D = 2870.2 MHz is the zero-field splitting, and
13 30 35 40 45
C B = B(sin θ cos φ, sin θ sin φ, cos θ) is the magnetic field
Electron Energy (MHz)
vector, θ and φ represent its polar and azimuthal an-
0
gles. P = −4.95 MHz [16] is the quadrupolar split-
ting of the 14 N nucleus, and A1 and A2 represent hy-
−5 perfine tensors of the 13 C and 14 N nuclear spins respec-
deg2 tively with the electron spin. The values for the hyper-
fine tensor components have been taken from previous
−10
work. For the 13 C nuclear spin, these are A1zz = 128.9,
deg2
A1yy = 128.4, A1xx = 189.3, and A1xz = 24.1 MHz [17]
14
−15
30 35 40 45 q the N nuclear spin these are A2zz = −2.3 MHz
and for
θ (in degrees) and A22xx + A22yy = −2.6 MHz [18–20]. All the other
components of the hyperfine tensors are zero due to the
FIG. 1. (a) Structure of an NV center coupled to a first- symmetry of the system.
shell 13 C nuclear spin. (b) Simplified energy level diagram of Now, we analyze the LACs that occur between the
this system considering only the electron and the13 C nuclear ms = −1 and +1 spin states due to the strong non-
spins. (c) The energy levels marked by gray rectangles in (b) secular components of the Hamiltonian when the energy
are plotted as functions of θ of a magnetic field of strength, level splitting between them due to the Zeeman interac-
B=28.9 G, and φ=0◦ . Here, interactions due to the 14 N nu- tion of the electron spin is roughly equal to the energy
clear spin are also included. The energy levels labeled by
splitting due to the 13 C hyperfine interaction: 2γe B cos θ
deg2 are nearly doubly degenerate. The transitions marked
by thick red and thin green arrows are electron spin transi- is ≈ 127 MHz. Fig. 1(b) shows a simplified energy level
tions and the one marked by dashed violet arrow is a 13 C diagram, considering only the electron and 13 C nuclear
nuclear spin transition. spins. In this diagram, the energy levels relevant for the
present work are marked with gray rectangles. These spe-
cific energy levels, after including the interaction with the
14
N nuclear spin, have been plotted as a function of θ of a
frequencies and faster than the amplitude of the applied static magnetic field of strength, B=28.9 G, and φ=0◦ in
RF field. Fig. 1(c). For this magnetic field strength, the LAC con-
dition (2γe B cos θ ≈ 127 MHz) corresponds to θ = 38.4◦ .
All the experiments of this work have been performed
As can be seen from Fig. 1(c), there are several LAC
using a home-built confocal microscope for optical ex-
points near θ=38.4◦ . Out of these, the LACs relevant
citation and detection of single NV centers and RF
for the present work have been marked with gray ovals.
and microwave (MW) electronics for resonant excitation.
These three LACs differ mainly with respect to the state
The diamond crystal used has natural abundance of 13 C
of the 14 N nuclear spin. Here, we discuss specifically the
atoms and a nitrogen impurity concentration of < 5 ppb.
LAC at θ=38.4◦ , which is marked with the solid gray
oval and corresponds to mI2 = 0. The two energy levels
shown in this gray oval represent the two-level system of
which we study the strong-driving dynamics. Away from
the LAC, the electron spin states of these two levels are
II. SYSTEM AND HAMILTONIAN ms = +1 and −1, and the transition between them is
forbidden. At the LAC point, there is a strong mixing
The structure of an NV center coupled to a first-shell between the electron spin states and the energy eigen-
13
C nuclear spin is illustrated in Fig. 1(a) along with it’s states become
coordinate system, which is defined as follows: The NV

|−1i ± |+1i 1
symmetry axis is defined as the z-axis, the x-axis is per- |ψ1,2 i ≈ √ ,− ,0 ,
2 2
pendicular to this axis and lies in the plane containing the
nitrogen, the vacancy and the 13 C atom, and the y-axis where − 21 and 0 represent spin states of the 13 C and 14 N
is perpendicular to this plane. The total Hamiltonian of nuclei respectively. Consequently, a transition can be ex-
the system including the intrinsic 14 N nuclear spin of the cited between these two levels by the z-component (par-
center in this coordinate system can be written as allel to the NV axis) of the RF field as | hψ1 | Sz |ψ2 i | ≈ 1.
 3

The Hamiltonian of this two-level system can be writ- = 0.10 MHz = 2.35 MHz
ten as x
1
HTLS (t) =
2
ω0 σx + ω1 cos(2πωt)σz , (2) z
where, ω0 = 1.7 MHz is the transition frequency, and
ω1 and ω are the amplitude and frequency of the driving
field respectively. σx and σz are the Pauli spin matrices.
In this system, ω1 can have values that are more than an y
order of magnitude larger than ω0 even for moderate RF
powers and hence it forms a very interesting system for
experimental studies of strong-driving dynamics. = 0.70 MHz = 3.62 MHz
As discussed in Section I, the linearly oscillating driv-
ing field, cos(2πωt)σz can be written as a sum of
co- ( 21 cos(2πωt)σz − 21 sin(2πωt)σy ) and counter-rotating
( 12 cos(2πωt)σz + 12 sin(2πωt)σy ) field components. In the
weak driving regime i.e., ω1  ω0 , the rotating-wave ap-
proximation is valid and the counter-rotating field com-
ponent can be neglected while the co-rotating field com-
ponent drives Rabi oscillations of the system. These os-
cillations, damped by relaxation processes, were first ob-
served in nuclear spins by Torrey [21]. The neglected
counter-rotating field component was shown to shift the FIG. 2. Bloch sphere representation of the simulated on-
resonance frequency of the system by ω12 /4ω0 , which is resonance (ω = ω0 = 1.7 MHz) rotating-frame dynamics of
known as Bloch-Siegert shift [22, 23]. This shift, how- the system of Eq. 2 for different values of ω1 .
ever, is very small when ω1  ω0 , and when ω1 is of
the order or greater than ω0 (strong-driving regime), the
approximations that are used to derive the shift them-
selves are not valid. In this strong-driving regime, the (a)
Laser

rotating-wave approximation breaks down and both the Init. Read

(c)
l
co- and counter-rotating field components drive the sys-
MW
k
tem dynamics in a non-trivial way. ij
The Bloch sphere representation of the simulated on-
de ij
(b) l
gh
k
l

resonance (ω = ω0 ) dynamics of the above two-level sys- gh

ab gh

ab ij
f
f

10

c l
de
f
k

tem for different values of ω1 , in a frame rotating with c k

5
c

the same frequency (ω) and direction of the co-rotating

field component, are shown in Fig. 2. The system is ini- 0
Amplitude (arb. units)

10
tialized into the |+xi eigenstate of σx . When ω1 = 0.10
MHz ( ω0 = 1.7 MHz), where the rotating-wave ap- 5
f
proximation is valid, the system rotates on the surface of 0

the sphere in the xy-plane with a frequency ω1 . When 60 de

40 c
ω1 = 0.70 MHz (comparable to ω0 ), the system’s dynam- 20
ics deviate from the xy-plane due to the counter-rotating 0 ab
0 5 10 15 20 25 30
field component. When ω1 = 2.35 MHz (> ω0 ), where Frequency (MHz)
the rotating-wave approximation is no longer valid, the
spin trajectory occupies a large fraction of the surface of
FIG. 3. (a) Pulse sequence used to measure Ramsey fringes.
the sphere and when ω1 = 3.62 MHz, the system doesn’t
(b) Fourier transforms of Ramsey fringes, recorded at the
flip to the |−xi state completely for any finite time t. LAC point θ=38.4◦ and φ=0◦ . For the top and middle traces,
the flip angle of the MW pulses was π/2 and the frequency de-
tuning (νd ) was 20 and 15 MHz respectively. For the bottom
III. EXPERIMENTS trace, the flip angle was π. The spectral lines marked by thick
red, thin green, and dotted violet arrows represent electron
An experimental study of this two-level system re- spin transitions of frequency 1.7 and 2873.9 MHz, and a 13 C
quires precise orientation of the magnetic field with re- nuclear spin transition of frequency 6.4 MHz respectively. (c)
Corresponding energy level diagram at the LAC point. En-
spect to the NV coordinate system. In this work, this
ergy levels labeled by two letters (e.g., ab) are nearly doubly
was achieved by a permanent magnet placed at a fixed degenerate.
distance from the NV center and rotated around two
orthogonal axes crossing at the NV center [17]. The
 4

magnetic field B was 28.9 G, oriented at θ = 38.4◦ and (a) 1 (b) FFT of (a)
φ = 0◦ , which corresponds to a LAC point (Fig. 1(c)). = 0.23 MHz
1
The experimental electron spin resonance (ESR) spectra
between the energy levels marked by gray rectangles in 0.95 0.5
Fig. 1(b) at this magnetic field orientation are shown in
0
Fig. 3(b). These were recorded as Fourier transforms 0 2 4 6 8 10 12 0 1 2 3 4 5 6
1
of Ramsey fringes by using the pulse sequence shown in = 0.70 MHz
Fig. 3(a). All the spectral lines are labeled in comparison 1
with the corresponding energy level diagram illustrated
0.95 0.5
in Fig. 3(c). The frequency of the MW pulses was 2876.6
MHz. The phase of the second MW pulse (-2πνd τ ) was 0 0 1 2 3 4 5 6

Normalized photons
0 1 2 3 4 5 6 7 8
varied with respect to that of the first pulse as a lin- 1
= 1.60 MHz
ear function of τ (delay between the pulses) such that

Probability
1
an artificial detuning (νd ) is introduced in the spectra.
The top trace of these spectra was recorded with a fre- 0.95 0.5
quency detuning (νd ) of 20 MHz. In this spectrum, along 0 0 1 2 3 4 5
0 0.5 1 1.5 2 2.5 3 3.5 4
with the electron spin transitions between the ms = 0 1
and ms = ±1 spin states (transitions in the range 15- = 2.35 MHz
30 MHz), two other transitions also appear. Of these, 1
0.98 1.5 2

the transition that appears at 1.7 MHz (marked by the 0.5

thick red arrow) is an electron spin transition between 0.96
0
two levels of the ms = ±1 manifolds. These two levels, 0 0.5 1 1.5 2 2.5 3 3.5 4 0 1 2 3 4 5
which are shown inside the solid gray oval in Fig. 1(c), 1
= 3.62 MHz
are the levels that we use to study the strong-driving dy- 1
namics. The other transition, which appears at 6.4 MHz
0.5
(marked by the violet dashed arrow) is a 13 C nuclear spin 0.95

transition of the ms = 0 state. 0

0 1 2 3 4 5
0 0.5 1 1.5 2
These two transitions appear in the ESR spectrum in- Pulse width (µs) Frequency/
directly as zero-quantum transitions [17]. For example,
the transition between the two levels of the ms = ±1
manifold can be excited by simultaneously driving the FIG. 5. Dynamics of the two-level system for increasing am-
plitudes, ω1 of the driving field. (a) Dynamics as a function
two transitions that connect these two levels with the
of the duration of the RF pulse. The upper blue dots con-
same ms = 0 spin sub-level (Raman excitation scheme). nected by solid lines are the experimental data and the lower
The zero-quantum nature of these transitions is clear by red solid curves are the corresponding simulated dynamics.
comparing the top trace of Fig. 3(b) with the middle (b) Fourier transforms of (a).
trace of the same, which was recorded with a frequency
detuning (νd ) of 15 MHz. The transitions between the
ms = 0 and ms = ±1 manifolds shift correspondingly
ms = 0 spin state. The first MW π pulse applied at a
by 5 MHz whereas positions of the zero-quantum tran-
frequency of 2873.9 MHz selectively inverts the transition
sitions do not change. The lower trace of Fig. 3(b) was
marked by solid green arrow in Figs. 1(c) and 3(b), which
recorded with the same pulse sequence of Fig. 3(a) but
is a transition between the ms = 0 and ms = ±1 man-
the flip angle of the MW pulses is π instead of π/2, which
ifolds. This creates a population difference between the
optimizes the signal from the zero-quantum transitions.
two levels of interest. Then an RF pulse of variable dura-
Now, we study the dynamics of the two-level system at tion is applied on resonance (ω = ω0 = 1.7 MHz) to drive
the LAC (marked by solid gray oval in Fig. 1(c)). These the transition between the two levels. The correspond-
dynamics can be observed by using the pulse sequence ing dynamics are observed by applying another selective
shown in Fig. 4. Here, the first laser pulse polarizes the MW π pulse followed by the read-out laser pulse, which
reads the total population of the ms = 0 state. The ob-
served dynamics for different amplitudes (ω1 ) of the RF
Laser

Init. Read pulse are shown in Fig. 5(a) (upper blue curves). The
values of ω1 in the strong-driving regime are obtained by
scaling the values measured in the weak-driving regime
MW with the square root of the RF power. The correspond-
RF ing dynamics simulated numerically using Eq. 2 are also
shown in Fig. 5(a) (lower red curves). The correspond-
ing Fourier transforms are shown in Fig. 5(b). When
FIG. 4. Pulse sequence for observing the dynamics of the the amplitude, ω1 of the driving field is 0.23 MHz, which
two-level system. is small compared to the transition frequency, ω0 of the
 5

system, the Rabi oscillations of the system are clearly si- the frequencies of the identifiable peaks of the experimen-
nusoidal. As we increase ω1 to 1.6 MHz, which is close tal spectrum should match the frequencies of the peaks
to ω0 =1.7 MHz, the effects due to the counter-rotating in the simulated one for any phase but their amplitudes
field component become significant and the oscillations can be different. This can be observed in Fig. 5. When
of the system deviate significantly from the simple sinu- ω1 = 3.62 MHz, there is a strong peak in the experimen-
soidal behavior. When ω1 > ω0 , the oscillations become tal spectrum, roughly at frequency/ω1 = 1.2. At this
strongly anharmonic as the effects due to the counter- position, there is also a peak in the simulated spectrum,
rotating field component become more prominent. In but it is of very low intensity for the phase (0◦ ) used in
this strong-driving regime, the system’s dynamics con- the simulation. This experimental spectrum has a bet-
tain frequency components that are significantly higher ter match with the simulated one averaged over many
than the amplitude ω1 of the field. This anharmonic and different phases of the driving field (data shown in the
non-linear behavior of the system can be seen from Fig. 5 Appendix).
when ω1 =2.35 and 3.62 MHz: the system dynamics now
includes multiple frequencies, some of which are higher
than ω1 . The results of the numerical simulations, which IV. CONCLUSION
are also shown in Fig. 5 are in good agreement with the
experimental observations. However, there is some devia- We studied, theoretically and experimentally, the an-
tion between the experimental results and the simulated harmonic and non-linear dynamics of a two-level system
ones, in particular when ω1 = 3.62 MHz. This can be of a single spin driven in the strong-driving regime, where
explained as follows. the rotating-wave approximation is not valid. Study-
ing spin dynamics in this regime is interesting not only
In the strong-driving regime, the dynamics are very from the fundamental physics perspective but also to the
sensitive to the amplitude, phase and shape of the RF quantum information processing because of the ultra-
pulse. In the present case, the deviations between the fast quantum gates possible in this regime. The two-
experiment and the simulation are mainly due to the ef- level system explored here will be useful to experimen-
fect of the phase of the RF pulse. Each data point of the tally study strong-driving dynamics for very high ratios
experimental time-domain data was obtained by taking of driving field’s amplitude to the transition frequency
the average value over 200,000 repetitions of the pulse of the system. This system will also be useful as a
sequence shown in Fig. 4. The RF pulse of this pulse good test bed to explore time-optimal pulse shapes in
sequence was applied by chopping a continuous RF sig- the strong-driving regime by using optimal control the-
nal with an RF switch. This implies that the phase of ory techniques [12, 24–27].
this pulse is not the same in all the repetitions. This has
no significant effect on the dynamics in the weak-driving
regime. However, in the strong-driving regime, in par- V. ACKNOWLEDGMENTS
ticular when ω1 > ω0 , this has significant effects. How-
ever, the phase of the RF pulse only alters the intensity We acknowledge experimental assistance from Fabian
pattern of the spectral peaks in the Fourier-transformed Lehmann for the construction of the magnetic field rota-
dynamics not their positions (frequencies). This is ex- tion setup. We thank Jingfu Zhang for useful discussions.
plained in detail by using numerical simulations, in Ap- This work was supported by the DFG through grant no.
pendix for the case ω1 = 3.62 MHz. This implies that Su 192/31-1.

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 6

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same. Fig. 6(b) shows the Fourier transform of the av-
APPENDIX erage time-domain dynamics for 100 random values of ϕ
between 0 and 180◦ in comparison with the experimental
Effect of the phase of the driving field on the one for ω1 = 3.62 MHz. The match between the experi-
dynamics of the two-level system: We write the ment and the simulation is better here than in Fig. 5.
 7

0 1 2 3 4 5
(a)
400
200
0
0 0.5 1 1.5 2 2.5 3 3.5 4 4.5 5
600
400
200
0
0 1 2 3 4 5
(b)
0 0.5 1 1.5
0.1
0.08
0.06
0.04
0.02
0
0 1 2 3 4 5
Frequency (MHz)

FIG. 6. (a) Fourier transforms of numerically simulated time-

domain dynamics for three different values of ϕ when ω0 =
ω = 1.7 and ω1 = 3.62 MHz. (b) Fourier transform of these
dynamics averaged over 100 random values of ϕ between 0 and
180◦ (lower spectrum) in comparison with the experimental
one (upper spectrum).