RESEARCH ARTICLE | MAY 31 2024

A scanning probe microscope compatible with quantum

sensing at ambient conditions 
Ke Bian  ; Wentian Zheng ; Xiakun Chen ; Shichen Zhang; Rainer Stöhr ; Andrej Denisenko ;
Sen Yang ; Jörg Wrachtrup; Ying Jiang 

Rev. Sci. Instrum. 95, 053707 (2024)

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A scanning probe microscope compatible

with quantum sensing at ambient conditions
Cite as: Rev. Sci. Instrum. 95, 053707 (2024); doi: 10.1063/5.0202756
Submitted: 6 February 2024 • Accepted: 8 May 2024 •
Published Online: 31 May 2024

Ke Bian,1,a) Wentian Zheng,1 Xiakun Chen,1 Shichen Zhang,1 Rainer Stöhr,2,3 Andrej Denisenko,2,3
Sen Yang,4 2,3
Jörg Wrachtrup, and Ying Jiang 1,5,6,7,a)

AFFILIATIONS
1
International Center for Quantum Materials, School of Physics, Peking University, Beijing 100871, China
2
Third Institute of Physics, University of Stuttgart and Institute for Quantum Science and Technology (IQST),
Stuttgart 70569, Germany
3
Max Planck Institute for Solid State Research, Stuttgart 70569, Germany
4
Department of Physics, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon,
Hong Kong 999077, China
5
Collaborative Innovation Center of Quantum Matter, Beijing 100871, China
6
Interdisciplinary Institute of Light-Element Quantum Materials and Research Center for Light-Element Advanced Materials,
Peking University, Beijing 100871, China
7
New Cornerstone Science Laboratory, Peking University, Beijing 100871, China

23 April 2025 [Link]

a)
Authors to whom correspondence should be addressed: bian.k@[Link] and yjiang@[Link]

ABSTRACT
We designed and built up a new type of ambient scanning probe microscope (SPM), which is fully compatible with state-of-the-art quantum
sensing technology based on the nitrogen-vacancy (NV) centers in diamond. We chose a qPlus-type tuning fork (Q up to ∼4400) as the
current/force sensor of SPM for its high stiffness and stability under various environments, which yields atomic resolution under scanning
tunneling microscopy mode and 1.2-nm resolution under atomic force microscopy mode. The tip of SPM can be used to directly image the
topography of nanoscale targets on diamond surfaces for quantum sensing and to manipulate the electrostatic environment of NV centers
to enhance their sensitivity up to a single proton spin. In addition, we also demonstrated scanning magnetometry and electrometry with a
spatial resolution of ∼20 nm. Our new system not only paves the way for integrating atomic/molecular-scale color-center qubits onto SPM
tips to produce quantum tips but also provides the possibility of fabricating color-center qubits with nanoscale or atomic precision.
Published under an exclusive license by AIP Publishing. [Link]

I. INTRODUCTION spin8,9 and single elementary charge,10 which makes it a power-

ful tool for chemical identification11,12 and structural analysis.13,14
Quantum sensing1 harnesses fundamental quantum properties In addition, the NV center has an atomic size, which makes it
such as quantum coherence to realize measurements with a sensitiv- promising for achieving nanoscale spatial resolution for quantum
ity surpassing that of classical methods. Although many advanced sensing.
quantum sensors such as superconducting quantum interference Although NV has been proven to be an ultrasensitive sensor,
devices,2 single-electron transistors,3 and single atoms/molecules4,5 there are still two critical problems for NV-based quantum sensing.
have been used to detect subtle signals at mesoscopic and micro- First, because of the magnetic/electric noise on/near the diamond
scopic scales, all of them can only work in low temperature and high surface produced during the NV growth,15,16 the coherence and sen-
vacuum environments. Recently, the nitrogen-vacancy (NV) center sitivity of shallow NVs are severely decreased, hence impeding their
in diamond1,6 (Fig. 1) has attracted broad attention because of its application for detecting subtle signals such as single proton spin.
long coherence time of up to milliseconds even at room temper- Second, due to the long-range dipolar interaction, the spatial resolu-
ature.7 The NV-based quantum sensor can resolve single nuclear tion of the NV center is greatly limited, such that the topography of

Rev. Sci. Instrum. 95, 053707 (2024); doi: 10.1063/5.0202756 95, 053707-1
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FIG. 1. (a) Energy levels of the NV center. Once excited, the ms = 0 state emits fluorescence within ∼10 ns. However, the ms = ±1 state can be shelved on a metastable
state for a much longer time (∼250 ns) and relax back to the ms = 0 state, which results in different fluorescence intensities dependent on its spin-state. (b) Schematic of
a qPlus-SPM compatible with NV-based quantum sensing. Inset: The NV center consists of one substitutional nitrogen atom and one adjacent carbon vacancy defect. To
apply quantum sensing, a biased magnetic field is used for tuning the spin levels of NV, while a laser beam and microwave are used for readout and coherent control of the
quantum states of NV.

nanoscale targets cannot be determined with high precision. There- ambient conditions. The SPM tip can be used to directly image the

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fore, it is ideal to develop a technique capable of directly imaging topography of nanoscale targets on diamond surfaces for quantum
and manipulating the local environment of NV centers as well as sensing and to manipulate the electrostatic environment of NV cen-
the sensing targets with a spatial resolution at the sub-nanometer ters to enhance their sensitivity up to a single proton spin. Finally, we
level. also demonstrated proof-of-principle scanning magnetometry and
The scanning probe microscope (SPM) is one of the greatest electrometry using the SPM tip at the nanoscale.
inventions in nanoscience.17 Typically based on short-range inter-
actions such as quantum tunneling18 or Pauli repulsion,19 SPM
II. SYSTEM DESCRIPTION
can characterize the surface topography and manipulate the sur-
face species with atomic resolution.20,21 By combining SPM with The NV center consists of one substitutional nitrogen atom
NV-based quantum sensing, it is promising to clearly visualize and and one adjacent carbon vacancy [Fig. 1(b), inset]. Two unpaired
precisely manipulate the electromagnetic environments and the tar- electrons are trapped in NV, leading to a spin-1 system that acts
get elements in the neighborhood of shallow NVs. In this way, as a magnetic sensor for external signals. Due to the intersystem
SPM may help to enhance the coherence and sensitivity of the crossing (ISC), the spin state of NV can be efficiently initialized
shallow NV and provide a more comprehensive understanding of and read out by measuring its fluorescence24 [Fig. 1(a)]. Combined
the structure–property relationship of the interested nanostructures. with microwaves, the external signals can be measured by monitor-
Here, we designed and built up a new type of SPM compatible ing the spin level or quantum phase of NV centers. In Fig. 1(b),
with NV centers (NV-SPM) under ambient conditions. For the SPM a diamond chip with high-quality shallow NV centers is used as a
part, we chose the qPlus22 force sensor for its high stability against substrate, and the sharp SPM tip on the qPlus sensor is used for
external dissipations in various environments. The homemade qPlus imaging and manipulating the local environment of single NV cen-
sensor was optimized with a high Q factor of up to 4400 under ters and the target elements25 for quantum sensing with high spatial
ambient conditions. To accommodate quantum sensing, we also resolution.
integrated a vector magnetic field apparatus, an objective with a Figure 2 shows the schematic of our experimental set-up. The
high numerical aperture, and a high-frequency coplanar waveguide scanner head is encompassed by both the electric and thermal
(CPW). Considering their compactness and rigidity, we chose the shields (now shown). The qPlus sensor, vector magnet driver, objec-
modified Pan-type23 nano-positioners for the accurate adjustments tive lens, and microwave waveguides are directly integrated inside
of the tip position, laser focus, and magnetic field. Due to the low the scanner head. A home-built confocal setup is applied to address
mechanical noise (<10 pm⋅Hz−1/2 ), this NV-SPM obtains atomic the single shallow NV. A 532-nm laser (MLL-III-532, Changchun
resolution under STM mode and 1.2-nm resolution under AFM New Industries Optoelectronics Tech.) is applied to excite the NV,
mode. Meanwhile, this system can apply nanoscale NMR measure- and the fluorescence is collected by an avalanche photodiode (APD,
ments on external spins such as protons with a spectral resolution Excelitas). The exciting laser beam is chopped by an acoustic-optic
of 18.4 kHz, limited by the diffusion rate of surface molecules under modulator (AOM, Gooch & Housego). The red fluorescence is

Rev. Sci. Instrum. 95, 053707 (2024); doi: 10.1063/5.0202756 95, 053707-2
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FIG. 2. Schematic showing the experimental setup. The SPM qPlus sensor, magnet, objective, and CPW were integrated into the scanner head with both the electric and
thermal shields (not shown). The synchronization of the laser beam (green lines), microwave pulse (blue lines), and photon counter (red lines) is realized through an AWG.
AWG is also used to tune the frequency and phase of the microwave through an IQ mixer.

separated from the green exciting laser through a dichroic mirror wave generator (DN2-662, AWG, Spectrum) with a sampling rate of
(Newport) and filtered through a 650-nm long-pass filter (Thor- 1.25 GS/s (corresponding to the minimum time bin of 0.8 ns).
labs) before being collected by the APD. The microwave from the
source (N5181B, Keysight) is chopped by an IQ mixer (Marki)
III. SPM SCANNER
through the single sideband mode, amplified by a power amplifier

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(Mini-Circuits), and fed through a home-designed CPW for manip- The scanner head is encompassed with two aluminum boxes
ulating the spin state of NVs. The synchronization of microwave [Fig. 3(a)] for electric shielding. An extra box made of foam (not
pulses, laser pulses, and photon counts is realized by an arbitrary shown) combined with four proportional–integral–differentiate

FIG. 3. (a) 3D model of the whole SPM scanner head. Only the Pan-type motor for the coarse motion of the SPM tip and the sample stage are hung by the springs. (b)
Explosion-view of the Pan-type motor for the coarse motion of the SPM tip; the CPW is directly deposited on the sample surface. (c) Photo of the scanner head. The AFM
pre-amplifier is fixed on the inner shield to reduce the length of wires from qPlus to the pre-amplifier, which can simultaneously reduce the electric noise of AFM signals.

Rev. Sci. Instrum. 95, 053707 (2024); doi: 10.1063/5.0202756 95, 053707-3
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(PID) modules is used to stabilize the temperature. The motor for are used to introduce the microwave pulses, which are detached
the coarse motion of the SPM tip and the sample stage are freely from the scanner to avoid the blocking of the spring during the
hung by the springs for vibration isolation, combined with the cop- atomic-resolution imaging in part V-A.
per damping pieces. The designed resonance of springs is around In previous studies, the scanner head of the NV-SPM
2.0 Hz. The objective and magnet, with their homemade drivers, was generally constructed through commercial slip-stick stacking
are directly fixed to the shielding box. The coaxes (Pasternack) motors.26,27 Such a configuration is not rigid enough to guarantee

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FIG. 4. (a) and (b) 3D model and photo of the homemade Pan-type nano-positioner for tuning the magnetic field in a 3D manner. (c) The schematic shows three identical
nano-positioners with magnets in an orthogonal manner above a (001) diamond surface where an NV pointed to the [111] direction. Magnet 1 is aligned with the axis of NV,
while Magnets 2 and 3 are used to reduce the off-axis magnetic field caused by the mechanical deviation of Magnet 1. (d) A series of ODMR under different positions of
Magnet 2. The black dashed line denotes the zero-field splitting of NV (2870 MHz), while the blue, green, and red ones denote the average value of two fitted resonance
peaks: 2877.7, 2874.2, and 2872.2 MHz, respectively. (e) and (f) A 3D model and photo of the homemade Pan-type nano-positioner stacks applied for the alignment of the
tip and single NV. Three Z actuators are used for finely adjusting the focal plane of the objective, while a commercial closed-loop XY scanner is used for confocal imaging.

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low mechanical noise. Here, we adopted the design of a Pan-type fork under frequency modulation,25,32,33 both of which rely on an
motor,23 which is compact, robust, and widely applied in SPM sys- oscillating tip with a large oscillation amplitude (typically larger than
tems with ultrahigh-resolution.28 The body of the scanner head is several nanometers). This will induce strong disturbances on the
mostly made from titanium, considering its low thermal expansion NV and the target elements, unavoidably raising magnetic/electric
against temperature variations. A piezo tube (EBL No. 2) with a noise and decreasing the sensitivity of the NV to subtle signals.34
length of 1 in. and a diameter of 1/4 in. is used for scanning the In addition, the large oscillation amplitude also decreases the spa-
tip, which is enclosed by a prism. For the tip’s coarse motion in the tial resolution because of the contribution of long-range forces. The
Z-direction, six homemade piezo stacks (shear mode, EBL No. 2) qPlus sensor is a modified quartz-based tuning fork with one prong
are used to drive the prism [Fig. 3(b)]. The designed walking range fixed on a solid base.22 With this asymmetric design and a mechan-
is ∼10 mm to provide the convenience of integrating magnets into ical driving scheme, the cross talk caused by the parasitic capacitive
the vicinity of the tip. Two leaf springs made of beryllium copper coupling in the conventional tuning forks is largely suppressed, lead-
are used for adjusting the pressure between the prism and actuators. ing to an enhanced Q-factor (>104 under 4.2 K) and, therefore, a
Besides, three extra homemade piezo stacks (shear mode, EBL No. 2) high signal-to-noise ratio. Due to the large stiffness of the quartz
are stuck at the bottom of the Z-slider for the coarse motion of the tuning fork (1800 N/m), the qPlus tip can work at very small oscilla-
tip in the XY-direction, with a designed walking range of ∼±3 mm. tion amplitudes (<50 pm) and working distances (<1 nm), leading to
Another beryllium-copper leaf spring is applied to press the Z-slider high sensitivity to short-range forces, which is the key to achieving
on top of the scanner holder through a screw-like XY pusher with high spatial resolution.28 The qPlus sensor has been proven not only
thread. as a powerful tool for investigating the chemical reaction21,35 and
To align the laser focus with the SPM tip, we applied homemade hydrogen-bonding structure36,37 at the sub-molecular level under
nano-positioners to move the qPlus sensor and objective while the ultra-high vacuum and low temperature (UHV & LT) but also to
sample was unmovable. Another set of homemade nano-positioners be able to obtain atomic spatial resolution under ambient and even
is used to finely adjust the magnetic field. Typically, any misalign- liquid environments.38
ment between the external bias magnetic field and NV’s axis will To be compatible with both STM and AFM working modes,
decrease the spin contrast of NV. Therefore, it is necessary to adjust a qPlus sensor has three electrodes, as shown in Fig. 5(a), one
the direction of the bias field with high accuracy in a vector man- for the STM signal and the other two for the AFM signal. A pre-
ner. As shown in Figs. 4(a) and 4(b), we used a compact Pan-type amplifier (Createc) for AFM is integrated inside the inner shield,
nano-positioner with a similar design as the Z-slider in Fig. 3(b). The while the amplifier (Femto DLPCA-200) for STM is fixed outside

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prism is made from iron with an RbFeB magnet at the termination. the outer shield. To make the qPlus sensor more stable and robust
Three identical nano-positioners are fixed on the inner shield in an against disturbances from ambient conditions, a special design is
orthogonal configuration [Fig. 4(c)]. Since it is challenging to ide- applied for the accommodation of the qPlus sensor inside the scan-
ally assemble the magnets with their axes perfectly aligning with the ner head.38 Without the need for in situ tip exchange as used in UHV
NV, we applied a strategy to adjust the magnets with three degrees & LT systems, two screws are used to directly fix the qPlus sensor
of freedom.29,30 onto the tip holder [Fig. 5(b)], which is glued at the bottom of the
As shown in Fig. 4(c), we usually use the diamond sample with scanning tube shown in Fig. 3(b). The maximum Q-factor obtained
a (001) surface and shallow NV centers pointed in the [111] direc- was around 4400, nearly three times larger than the commercial
tion. The axis of Magnet 1 was aligned to [111] with unavoidable design.
mechanical deviations, leading to a decreased spin contrast in the To assemble an electric tip, we first put a tungsten fila-
optically detectable magnetic resonance (ODMR)24 [blue curve in ment with a length of ∼5 mm and a diameter of 25 μm on a
Fig. 4(d)]. After adjusting the positions of Magnets 2 and 3, the mis- clean substrate (such as polished sapphire), then we used a set
alignment was alleviated and the spin contrast recovered. Here, the of translation stages to carefully align the tip to the end of the
error of the magnetic field direction is limited by the measurement qPlus tuning fork [Fig. 5(d)]. The assembly process was oper-
precision of the resonance peaks.31 In Fig. 4(d), the fitted resonance ated with the assistance of an optical microscope with a long
peaks of the red curve are 1805.1 ± 0.25 and 3939.2 ± 0.16 MHz, working distance (BA310Met-H, Motic). The tungsten filament
corresponding to an alignment error of ±0.11○ for the magnetic was stuck onto the qPlus through the silver epoxy (H20E, Epoxy
field after a measurement time of 200 s. The maximum magnetic Technology). Finally, the tip was chemically etched by the NaOH
field realized in this scanner is 544 G. Similarly, to navigate the laser solution and further sharpened by the focused ion beam (FIB)
focus on the interested NV and align it to the tip apex, we applied [Fig. 5(e)].
another set of 3D nano-positioners. In this motor, three modified Besides, to assemble a magnetic tip, since the magnetic field
Pan-type sliders are stacked successively [Figs. 4(e) and 4(f)]. The from an entire nickel tip is very high, it will severely decrease the
designed range for XYZ coarse motion is 10 × 10 × 15 mm3 . Three spin contrast of the NV center if the magnetic field from the tip does
stretch-mode piezo actuators are integrated to finely adjust the laser not align perfectly with the axis of NV. Therefore, we chose to graft
focus with a designed range of 0–30 μm. A commercial closed-loop the commercially available magnetic tip made of Co/Cr film (MFM-
XY scanner is adopted for scanning the laser focus during confocal LM, TipsNano) with weak field strength onto the qPlus sensor. The
imaging. process is illustrated in Fig. 5(f). First, a holding bar of ∼5-μm width
on the cantilever of the commercial magnetic tip was fabricated by
IV. QPLUS SENSOR FIB. Meanwhile, a tungsten filament with a length of ∼2 mm and
At present, the existing NV-based AFM system always works a diameter of 25 μm was assembled on the qPlus without further
with a silicon cantilever under tapping mode31 or a quartz tuning etching process. Next, a droplet of UV (ultraviolet) curable glue

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FIG. 5. (a) The photo of the qPlus sensor fixed on a solid base with glue, where the three electrodes are applied for STM and AFM signals, respectively. (b) The 3D model
shows the accommodation of qPlus onto the tip holder with two screws. (c) Measured frequency sweep of our homemade qPlus sensor. The blue and red curves represent
the amplitude and phase responses, respectively. The gray curve shows the frequency sweep of the qPlus mounted with a commercial design. (d) Schematics showing the
process of assembling the electric tip to the qPlus sensor. (e) FIB image of the sharpened tungsten tip apex. (f) Schematics showing the process of transferring the magnetic
tip to the top of a tungsten filament. (g) The optical microscope photograph shows a magnetic tip fixed on the top of the tungsten filament.

(NOA81, Norland) was applied on the top side of the tungsten fil- conditions. The spectrum shows that the electronic noise floor is
ament. After curing the glue, the magnetic tip was transferred onto around 5 fA/Hz1/2 , with the highest peak around ∼20 fA/Hz1/2 ,
the end of the tungsten filament by mechanically breaking down the which is comparable with the noise level of STM systems under
holding bar [Fig. 5(g)]. UHV & LT.28 To evaluate the mechanical noise level of our sys-
tem, we also measured the z PSD under the constant-frequency
V. PERFORMANCE shift mode on the surface of mica. Figure 6(b) shows the tip
height in the frequency domain, where the noise floor is lower
A. SPM performance than 10 pm/Hz1/2 , which is good enough for AFM imaging with
In Fig. 6(a), we measured the current power spectral den- nanoscale spatial resolution. The resonant peak around 2 Hz caused
sity (PSD) spectrum when the tip was retracted under ambient by the springs for vibration isolation is not resolved in our system,

Rev. Sci. Instrum. 95, 053707 (2024); doi: 10.1063/5.0202756 95, 053707-6
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high-temperature annealing.15 The diamond sample is a membrane

with a thickness of 30 μm. Figure 8(a) shows a typical confocal
image obtained through an oil-immersed objective (N. A. = 1.3).
The saturated photon count of single NVs under a 532 nm laser is
around ∼100 kcts/s. The rings around single NVs are caused by the
mismatch between the perfect size of the pinhole (with a diameter
of 62.5 μm) and the 100 μm-fiber used for photon collection. The
microwave is fed through our homemade CPW with a broad band-
width (1–4 GHz) and high efficiency. Figure 8(b) is the ODMR24
of a single NV, which shows a fluorescence minimum when the
microwave is resonant with the transition of two sublevels of NV.
The resonant peak indicates the approachable magnetic field is up to
544 G in our system. Figure 8(c) demonstrates the coherent control
when sweeping the duration of a microwave pulse. The rate of Rabi
oscillation realized in our system is 20–30 MHz, which is large
enough for multi-pulse microwave sequences such as dynamical
decoupling40 and correlation.41 The coherence time T 2 measured by
the spin echo of a shallow NV is up to tens of μs [Fig. 8(d)], which
is influenced by its depth and immediate electrostatic environment.
The oscillation that appeared in the spin-echo curve is induced by
FIG. 6. (a) Measured current PSD when the tip was retracted, showing the noise the coupling between NV and its surrounding 13 C nuclear spin
level lower than 20 fA/Hz1/2 . (b) Measured tip height PSD when the tip was bath.42
on the mica surface, showing a noise floor lower than 10 pm/Hz1/2 . Set point:
Δf = +90 Hz, amplitude = 70 pm. Under ambient conditions, there are inevitably hydration lay-
ers adsorbed on a hydrophilic diamond surface after acid-boiling.
To demonstrate the high magnetic-field sensitivity of our system, we
measured the proton spins of the hydration layers through nanoscale
probably due to disturbances from molecules (such as water and nuclear magnetic resonance (NMR) based on the shallow NV cen-
oxygen) in the atmosphere.

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ters, where the spatial resolution is determined by the depth of NVs
To demonstrate the spatial resolution of our homemade SPM [Fig. 9(a)]. Under the external magnetic field of hundreds of Gauss,
system, we performed both STM and AFM imaging under ambi- it is difficult to realize a finite polarization of protons at room tem-
ent conditions. In Fig. 7(a), due to the high mechanical stability, we perature. However, due to the high sensitivity of the NV center, the
obtained atomic resolution on the surface of cleaved HOPG (Highly magnetic variance of several hundred protons is detectable through
Oriented Pyrolytic Graphite) through STM mode using a chemically dynamical decoupling sequences.12 Figure 9(b) shows the nanoscale
etched tungsten tip. The hexagonal lattice of graphite is resolved, NMR measurement based on an XY8-16 sequence (corresponding
which enabled us to calibrate the actual displacement of the piezo to 128 π-pulses in total). When the delay time between two π pulses
tube for scanning. Meanwhile, we performed AFM imaging on the matches the precession period of protons, the fluctuating magnetic
surface of cleaved KBr (100) [Fig. 7(b)]. We transferred a commer- noise from protons leads to decoherence and a concomitant fluo-
cial silicon tip (CSG10_SS) with a nominal tip apex of 2 nm onto the rescence change of the NV center. The fitted strength of magnetic
qPlus sensor and observed hydration layers39 under the atmosphere. variance is ∼(780 nT),2 contributed by hundreds of proton spins
The sharp edge of the hydration layer shows a spatial resolution of distributed in a volume of only several nanometers.12 To enhance
1.2 nm. the spectral resolution, Fig. 9(c) demonstrates the correlation mea-
Besides, we also characterized the topography of the diamond surement consisting of two dynamical decoupling sequences.41 In
surface by AFM. The stripe-like features produced during the pol- this condition, the π–π delay was fixed at 385 ns, as determined
ishing process are shown in Fig. 7(c). After growing the shallow NV in Fig. 9(b). The periodic oscillation corresponds to the preces-
centers with the boron-doped method,15 the stripe-like features dis- sion frequency of protons, where a decayed envelope indicates the
appear due to the etching of a few-layer diamond lattice. Instead, dwelling time of water molecules within the detection volume of
many nanoscale protrusions are left on the surface [Fig. 7(d)], NV marked in Fig. 9(a). Fast Fourier Transformation (FFT) yields
which are considered to be the nano-diamonds or other kinds of a spectral resolution of 18.4 kHz, nearly 370 times higher than
by-products formed during the procedures of NV growth and subse- ODMR in Fig. 8(b) (6.83 MHz). It is worth noting that the spectral
quent surface treatments such as acid boiling. Figure 7(d) also shows resolution of our system reported here is just limited by the diffu-
regions covered by a hexagonal boron nitride (hBN) film of ∼58 lay- sion rate of surface molecules under ambient conditions,43 which
ers, which demonstrates the ability for topographic characterization should be up to several kHz, ultimately determined by the T 1 time
of nano-devices or nano-structures near the interested NV centers of NV.
in future applications.
C. Coherence enhancement by local manipulation
B. Nanoscale nuclear magnetic resonance of electron spin bath
The shallow NV centers used in our system were grown Based on the high spatial resolution of our NV-SPM system,
through low-energy nitrogen implantation and subsequent the SPM tip can be used to locally manipulate the charges near the

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FIG. 7. (a) Upper panel: STM image on a HOPG surface under the ambient condition with atomic resolution. Lower panel: the line profile showing the atomic corrugations. Set
point: I = 3 nA, bias = 100 mV. (b) Upper panel: AFM image on a KBr (100) surface under the ambient condition showing the adsorbed hydration layer under the atmosphere.
Lower panel: the line profile showing the resolution of 1.2 nm fitted by the step function. Set point: +25 Hz. Amplitude: 70 pm. (c) AFM image on the surface of a commercially
purchased diamond chip from Element Six under the ambient condition, showing the polished features. Sep point: +1 Hz. Amplitude: 4.3 nm. (d) Topography of the diamond
surface after the etching process demonstrates the residual nanoscale protrusions without polished features. Meanwhile, the regions covered by an hBN film of ∼58 layers
show a flat surface compared to the diamond surface. Sep point: +5 Hz. Amplitude: 800 pm.

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FIG. 8. (a) Confocal image of a diamond chip showing the individual shallow NV centers. (b) ODMR of a single NV shows that the maximum magnetic field approached in our
system is up to 544 G. (c) Rabi oscillation is realized by sweeping the duration of the microwave pulse. The first minimum is defined as π-pulse. (d) Spin-echo measurement
for single shallow NV, showing the long T 2 time up to several tens of μs. Upper panel: the pulse sequence for spin-echo, including two π/2 pulses and one π pulse at the
mid-time.

FIG. 9. (a) Schematic showing the principle of NV-based nanoscale NMR. The magnetic variance, with a characteristic frequency corresponding to the precession of protons’
nuclear spins, is sensed by a single shallow NV center through the dynamical decoupling sequence. The detectable volume is determined by the dipolar interaction and
depth of NV. (b) Upper panel: the sequence of XY8-k, with equidistant π pulses of alternating phases. Lower panel: the measured XY8-16 under a magnetic field of 305 G.
(c) Correlation spectrum of single NV showing the oscillation results from the precession of proton nuclear spins. (d) FFT of the correlation spectrum in (c) shows the spectral
resolution of the NV center, limited by the diffusion of adsorbed water molecules under ambient conditions.

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diamond surface, leading to the control and optimization of shal- step are pushed away from the NV center [Fig. 10(b)], leading to a
low NV properties. One promising route is to use the tip-induced decreased density of spin noise and improved coherence of the NV.
band-bending effect,44 which changes the concentration of charges With this method, the maximum coherence enhancement was up to
near the NV center. With this NV-SPM, we have demonstrated the 20-fold [from 1.3 to 26 μs in Fig. 10(c)].45 After calibrating the depth
ability to control the charge state of shallow NVs with nanome- of NV in Fig. 10(c) using double electron–electron resonance,46
ter resolution32 and enhance the coherence time of shallow NVs we calculated its sensitivity for external proton nuclear spins after
up to 20 fold.45 Figure 10 gives a schematic demonstration of the the charge manipulation [Fig. 10(d)]. The results show that our
charge manipulation scheme, where we developed a “pull-and-push” NV-SPM can be used to manipulate the electrostatic environment
method consisting of two successive steps. First, a positively biased of shallow NV and enhance its sensitivity up to a single proton
tip is approached in the vicinity of a single shallow NV center. At spin.45
the same time, a 532 nm laser focuses on the NV and ionizes its
neighboring unpaired electrons, which are then pulled from subsur-
face to surface through the local electric field [Fig. 10(a)]. Second, D. Scanning field-gradient imaging
the tip is moved a distance of hundreds of nanometers to the NV To demonstrate proof-of-principle scanning magnetometry
center and applied with a large negative bias voltage. Due to the through our NV-SPM system, we used a commercial magnetized
electrostatic interaction, the pulled unpaired electrons in the first AFM tip to scan around a single selected NV center.31,47 Figure 11

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FIG. 10. (a) Schematic showing the process of pulling the unpaired electrons from subsurface to surface. A positively biased tungsten tip is approached close to the single
NV center. Unpaired electrons (blue balls) are ionized through a strong 532 nm laser and then pulled upward to the diamond surface by the local electric field. (b) Schematic
showing the process of pushing the unpaired electrons on the diamond surface away from the NV center. In this case, the tip is negatively biased and located hundreds
of nanometers away from the NV. (c) Spin echo measurements showing a 20-fold coherence time enhancement from 1.3 ± 0.1 to 26 ± 3 μs using the “pull-and-push”
method. The envelope of the decayed curves is fitted by C = exp(−(τ/T 2 )n ). (d) Calculated sensitivity for detecting protons vs the depth and T 2 of a single shallow. Using
the “pull-and-push” method, the sensitivity of NV (marked by an orange star) is close to the single proton nuclear spin (dashed gray line). Reproduced with permission from
Zheng et al., Nat. Phys. 18, 1317 (2022). Copyright Springer Nature Limited.

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FIG. 11. (a) ODMR of the NV when the magnetic tip was far away. The red arrow indicates the frequency setpoint for scanning magnetic field-gradient imaging. (b) The
iso-magnetic rings obtained by scanning a magnetic tip around a single NV demonstrate a spatial resolution of 18.8 nm. (c) Pulsed-ODMR of the NV when the bias of the
conductive tip was 0 V. The red arrow indicates the frequency setpoint for scanning electric field-gradient imaging. (d) The iso-electric rings obtained by scanning a conductive

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tip around a single NV demonstrate a spatial resolution of 24.2 nm.

demonstrates the scanning field-gradient imaging. Since the objec- resolution of 24.2 nm. In this case, the spatial resolution and sen-
tive and its driver are not hung by springs together with the tip sitivity are also influenced by the finite signal-to-noise ratio under
and sample during the scanning field-gradient imaging, we have to the mapping of pulsed-ODMR, which can be further improved
clamp the tip motor and the sample stage to avoid jittering between by using optical nanostructures or AC-based measurement
NV and laser focus when collecting the photons from NV. Without strategies.49
vibration isolation, our system is still rigid enough for nanoscale We also demonstrate the feasibility of imaging a weak mag-
imaging due to the compact design of the Pan-type motor. During netic field in an AC mode (Fig. 12). We used a commercial silicon
the scanning magnetic field-gradient imaging, the frequency of the tip coated with 1/5 nm Cr/Ni film through electron-beam evapo-
microwave was fixed several tens of MHz away from the resonant ration. In this case, such a tip is weakly magnetized, and we used
peak f0 of NV in the absence of the magnetized tip [Fig. 11(a)], an NV center to detect the magnetic noise with a basic frequency
leading to a resonant ring with decreased fluorescence intensity, of around 44.8 kHz, induced by the oscillating tip on a qPlus sen-
representing the iso-magnetic field strength. In Fig. 11(b), we sor (type: S0.8) [Fig. 12(a)]. The tip was scanned around a single
observed two iso-magnetic rings resulting from the spin-1 system NV with its photon number continuously monitored [Fig. 12(b)].
of NV with two resonance peaks near 2870 MHz under the external An area with a quenched fluorescence caused by the tip apex
magnetic field. The line profile indicates a spatial resolution of roughly indicates the position of NV near the diamond surface.50
18.8 nm, which is determined by the magnetic field gradient of the We applied pulsed-ODMR at two tip positions marked in Fig. 12(b)
tip and the spectral resolution of the ODMR in Fig. 11(a). The full and found no measurable energy shift of NV’s spin level [Fig. 12(c)].
width at half maximum in Fig. 11(a) corresponds to a minimum To enhance the magnetic sensitivity, we applied spin-echo mea-
detectable field strength of 770 μT with a total measurement surement and found a decoherence induced by the weak magnetic
time of 5 s. Similar to the magnetic imaging, we also performed noise during spin-echo. The minimum of fluorescence is around
the scanning electric field-gradient imaging using a sharp biased 22 μs [Fig. 12(d)], which is consistent with the center frequency of
tungsten tip.34 Since the coupling strength of the electric field with qPlus (44.8 kHz). It is worth noting that the coherence of NV is
NV is weaker than the magnetic field, we used pulsed-ODMR48 nearly unaffected under an oscillating amplitude of only 0.5 nm,
to measure the field strength [Fig. 11(c)]. The spectra resolution indicating the importance of using small oscillating amplitudes
gives out a minimum detectable field strength of 1.98 mV/nm to protect quantum sensors when mapping weak signals such as
with a total measurement time of 80 s. In Fig. 11(d), we obtained nuclear spin noise or electric field.34 The mapping of magnetic noise
the iso-electric rings of the tungsten tip, which show a spatial is demonstrated in Fig. 12(e), where a resolution of 62.6 nm for

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FIG. 12. (a) Schematic showing the principle of detecting magnetic noise from an oscillating tip attached to the cantilever of qPlus. (b) The fluorescence mapping was obtained
by scanning a Si tip with Cr/Ni films around a single NV. The feature of decreased fluorescence results from the quenching effect of metal films, roughly indicating the position
of NV beneath the surface. (c) Pulsed-ODMR of the NV under two tip positions marked in (b). AFM amplitude: 2 nm. (d) Spin-echo of the NV when the tip was located in
position 1 in (b). A feature of decoherence around 22 μs appears when increasing the amplitude of qPlus. The dashed lines are used for guiding the eyes. (e) Mapping of spin
noise from the tip with Cr/Ni films, showing the accuracy of 62.6 nm for locating the NV center. The delay time of spin echo is 25.616 μs and the AFM amplitude is 1.7 nm.

positioning the NV is marked in the line profile. Further improve- apply nanoscale NMR measurements on external spins such as pro-
ment of spatial resolution can be realized by applying synchronized tons with a spectral resolution of 18.4 kHz, limited by the diffusion
modulation of NV and the qPlus tip, as reported in scanning rate of surface molecules under ambient conditions. The SPM tip can
gradiometry.51 be used to image the topography of nanoscale targets on diamond
surfaces for quantum sensing and to manipulate the electrostatic
environment of NV centers to enhance their sensitivity up to single
VI. CONCLUSION proton spin. Finally, we also demonstrated proof-of-principle scan-
In summary, we designed and built up a new type of qPlus- ning magnetometry/electrometry using sharp SPM tips, both with a
based scanning probe microscope compatible with NV-based quan- spatial resolution of about 20 nm.
tum sensing under ambient conditions. In this system, homemade Our homemade NV-SPM paves the way for diagnosing the
compact Pan-type positioners were integrated to finely adjust the decoherence and charge instability of shallow color centers from a
laser focus and the magnetic field. The qPlus sensor was optimized microscopic view and offers a powerful toolkit for structural analyses
to achieve a high Q factor of up to 4400 under ambient conditions. and chemical identification of complex nanostructures. For exam-
The mechanical noise of our system is lower than 10 pm⋅Hz−1/2 , ple, in this system, one can not only detect the internal radicals,
which guarantees the atomic resolution under STM mode and the ions, and even nuclear spins inside the large biomolecules, con-
1.2-nm resolution under AFM mode. Meanwhile, this system can fined liquids,52,53 and solid electrolyte interphase films54 but also

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obtain the topographic information of them with high spatial res- Y.J. supervised the project. K.B., S.Y., J.W., and Y.J. designed the
olution under both ambient and liquid phases. In this way, our whole system. K.B., W.Z., and X.C. constructed the system. K.B.,
system can help provide a comprehensive understanding of the W.Z., X.C., and S.Z. performed the data acquisition. R.S. and A.D.
structure–property relationship of complex nanostructures. fabricated the shallow NVs. K.B., W.Z., and Y.J. wrote the paper with
Furthermore, benefiting from the strong local electric field of input from all other authors. All the authors commented on the final
the sharp metal tip and the ability to position the tip with atomic paper.
accuracy, this NV-SPM is also promising to produce qubits in a
more controllable manner55,56 while avoiding producing large quan- Ke Bian: Conceptualization (equal); Data curation (equal); Formal
tities of dark spins as in ion implantations.15 In this method, the analysis (equal); Funding acquisition (supporting); Investigation
advanced multi-qubit quantum gates made of color-center qubits (equal); Methodology (equal); Software (equal); Validation (equal);
can also be constructed with sub-nanoscale resolution.57 Besides, Visualization (equal); Writing – original draft (equal); Writing –
in previous studies, the spatial resolution of the diamond tip-based review & editing (equal). Wentian Zheng: Data curation (equal);
scanning magnetometry/electrometry is always limited by the depth Formal analysis (equal); Funding acquisition (supporting); Inves-
of the NV and the uncontrollable shape of the tip apex.49,50,58 Our tigation (equal); Validation (equal); Visualization (equal); Writing
system provides opportunities to address this problem by produc- – original draft (supporting); Writing – review & editing (equal).
ing quantum tips with both nanoscale tip apex and high-quality Xiakun Chen: Data curation (equal); Formal analysis (equal); Inves-
quantum sensors through color centers in 2D materials59,60 or tigation (equal); Methodology (equal); Validation (equal); Visual-
molecules.61,62 For example, one can transfer few-layer 2D materi- ization (equal); Writing – review & editing (supporting). Shichen
als on top of a nanoscale photonics structure as the tip, where a Zhang: Data curation (supporting); Formal analysis (supporting);
color center can be placed close to the tip’s apex with high pre- Investigation (supporting); Software (equal); Validation (support-
cision using our system. This will open the door for atomic-scale ing); Writing – review & editing (supporting). Rainer Stöhr:
magnetic/electric imaging, thus finding broad applications in var- Resources (equal); Writing – review & editing (supporting). Andrej
ious novel quantum materials such as searching for the hidden Deniseko: Resources (equal); Writing – review & editing (sup-
quantum phase in Kagome lattices,63 revealing the spin orders in porting). Sen Yang: Conceptualization (equal); Funding acquisi-
complex glassy systems,64 or disentangling the intertwined orders in tion (equal); Project administration (supporting); Resources (equal);
high-temperature superconductors.65 Supervision (equal); Writing – review & editing (supporting). Jörg
Wrachtrup: Conceptualization (equal); Funding acquisition (equal);

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Project administration (supporting); Resources (equal); Supervision
ACKNOWLEDGMENTS (equal); Writing – review & editing (supporting). Ying Jiang: Con-
The authors acknowledge Bowei Cheng for useful discussions ceptualization (equal); Funding acquisition (lead); Project admin-
on the SPM design, Franz J. Giessibl for his valuable help on istration (lead); Resources (lead); Supervision (lead); Writing –
qPlus-based AFM under ambient conditions, and Xinyu Pan for his original draft (equal); Writing – review & editing (equal).
generous help on NV instrumentations. This work was supported by
the National Key R&D Program under Grant No. 2021YFA1400500,
DATA AVAILABILITY
the National Natural Science Foundation of China under Grant
Nos. 11888101, 21725302, U22A20260, and 12250001, the Strate- The data that support the findings of this study are available
gic Priority Research Program of the Chinese Academy of Sciences from the corresponding author upon reasonable request.
under Grant No. XDB28000000, and the Beijing Municipal Science
& Technology Commission under Grant No. Z231100006623009.
W.Z. acknowledges the China Postdoctoral Science Foundation REFERENCES
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Rev. Sci. Instrum. 95, 053707 (2024); doi: 10.1063/5.0202756 95, 053707-14
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