LETTERS
PUBLISHED ONLINE: 4 MAY 2015 | DOI: 10.1038/NNANO.2015.79
Voltage-controlled quantum light from
an atomically thin semiconductor
Chitraleema Chakraborty1, Laura Kinnischtzke2,3, Kenneth M. Goodfellow3,4, Ryan Beams5
and A. Nick Vamivakas1,3,4*
Although semiconductor defects can often be detrimental to
device performance, they are also responsible for the breadth
of functionality exhibited by modern optoelectronic devices1.
Artificially engineered defects (so-called quantum dots) or
naturally occurring defects in solids are currently being investi-
gated for applications ranging from quantum information
science2,3 and optoelectronics4 to high-resolution metrology5.
In parallel, the quantum confinement exhibited by atomically
thin materials (semi-metals, semiconductors and insulators)
has ushered in an era of flatland optoelectronics whose full
potential is still being articulated6–18. In this Letter we demon-
strate the possibility of leveraging the atomically thin semicon-
ductor tungsten diselenide (WSe2) as a host for quantum
dot-like defects. We report that this previously unexplored
solid-state quantum emitter in WSe2 generates single
photons with emission properties that can be controlled via
the application of external d.c. electric and magnetic fields.
These new optically active quantum dots exhibit excited-state
lifetimes on the order of 1 ns and remarkably large excitonic
g-factors of 10. It is anticipated that WSe2 quantum dots will
provide a novel platform for integrated solid-state quantum
photonics2,3 and quantum information processing19, as well as
a rich condensed-matter physics playground with which
to explore the coupling of quantum dots and atomically
thin semiconductors.
Groundbreaking work on the electronic and optical properties of
monolayer graphene5–8 flakes has recently stimulated the search for
other atomically thin material systems with appealing physical prop-
erties. Of particular interest are monolayer materials that exhibit
semiconducting and insulating behaviour. Remarkably, it has been
discovered that a large class of transition-metal dichalcogenides,
when reduced to a single layer, exhibit emergent photoluminescence
as a result of quantum well-like quantum confinement19–21. The
two-dimensional nature of the materials, the availability of semicon-
ductors, metals and insulators, and the possibility to assemble van
der Waals heterostructures has resulted in numerous fundamental
physics investigations as well as the demonstration of advanced
optoelectronic and nanophotonic devices9–15. In addition to the
conventional physical characteristics of these materials, the elec-
tronic excitations also exhibit a robust valley degree of freedom
that coherently interfaces with photon polarization and can poten-
tially provide the physical basis of next-generation information
processing applications16–18.
A natural question that arises when studying any material is the
role that defects play in mediating the observed properties1.
Although the label ‘defect’ sounds pejorative, it is no stretch of
1
Materials Science, University of Rochester, Rochester, New York 14627, USA. 2 Department of Physics, University of Rochester, Rochester, New York
14627, USA. 3 Center for Coherence and Quantum Optics, University of Rochester, Rochester, New York 14627, USA. 4 Institute of Optics, University of
Rochester, Rochester, New York 14627, USA. 5 Material Measurement Lab, National Institute of Standards and Technology Gaithersburg, Maryland 20899,
USA. * e-mail: nick.vamivakas@rochester.edu
NATURE NANOTECHNOLOGY | VOL 10 | JUNE 2015 | www.nature.com/naturenanotechnology
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the truth to say that the controlled introduction of defects is a
driving force behind the myriad functionalities available with
modern optoelectronic and nanophotonic devices. From the per-
spective of quantum technology, the potential for defects to localize
excitons can enable novel sources of quantum light as well as
provide a physical implementation of a stationary qubit. Along
these lines, the last decade has witnessed intense quantum optical
investigations of optically active defects in both GaAs and nitrogen
vacancies (NVs) in diamond, as well as artificial defects such as InAs
quantum dots2,3. In this Letter the quantum optical properties of
light emission from quantum dots in electrically gated WSe2 are
investigated22,23.
The inset of Fig. 1a shows an optical microscope image of our
gated device (Supplementary Fig. 1), in which the dashed box ident-
ifies the single-layer flake. The sample was prepared by mechanical
exfoliation of single layers from a WSe2 bulk crystal onto a poly-
dimethylsiloxane (PDMS) viscoelastic stamp (see Methods).
Photoluminescence was used to identify the number of WSe2
layers (see Supplementary Fig. 2 for photoluminescence data). A
dry transfer technique was applied to position the desired flake
onto a doped silicon substrate, with 270 nm of SiO2 as a dielectric
layer, into which electrode arrays were patterned for electrical
gating (see Methods). The device was loaded into a magneto-
optical cryostat with x–y–z positioners for sample positioning
and the temperature was maintained at ∼4 K. The microscope
objective had a numerical aperture of 0.8 and enabled diffraction-
limited excitation and collection. Light emitted from the material
following optical excitation at 532 nm was directed to a
spectrometer that sent the dispersed light to a charge-coupled
device (CCD) array for spectral measurements or through an exit
slit to filter the emission before measuring the second-order
intensity autocorrelation.
An exemplary spectrum of a WSe2 monolayer, taken near the
centre of the flake under 0 V gate bias, is presented in Fig. 1a. A
characteristic emission spectrum composed of excitons and trions
is observed22,23. This was confirmed by gate voltage-dependent
photoluminescence measurements (Supplementary Fig. 3). More
interesting results were obtained when the sample was positioned
at an interface between the WSe2 monolayer and the WSe2 multi-
layer, where the spectrum in Fig. 1b was recorded. In stark contrast
to Fig. 1a, the spectrum now consists of a number of narrow emis-
sion lines that are bright when compared to the extended two-
dimensional WSe2 excitons, even at an excitation power ∼20
times less than the excitation power used for the spectrum in
Fig. 1a. For clarity, in the remainder of this Letter we will refer to
these bright lines as quantum dots and adopt the labelling QD1
507
LETTERS NATURE NANOTECHNOLOGY DOI: 10.1038/NNANO.2015.79

a 30 b
QD2
QD1
Au

Intensity (×103 counts)

900
pad

Intensity (c.p.s.)
20
600
1.700 1.701 1.702
Energy (eV)
10
X0 300 QD2

0 0

1.60 1.65 1.70 1.75 1.80 1.60 1.65 1.70 1.75 1.80
Energy (eV) Energy (eV)

Figure 1 | Device and emission spectra. a, Fluorescence spectra from the single-layer region of the WSe2 flake at 4.2 K, integrated for 10 s. The peak at
1.75 eV is from neutral excitons in the WSe2 flake. Inset: Optical microscope image of the WSe2 device. The white dashed line outlines the single-layer
region of the flake. b, Narrow emission lines identified as QD1 (1.65 eV) and QD2 (1.70 eV) in the photoluminescence spectrum around the interface of the
single- and multilayer regions in the flake.

a b 2.5
1.60
2.0

Counts (a.u.)
Energy (eV)

1.65
1.5
0 μm 4 μm 1.668 eV
1.70 1.0

0.5
1.75 1.716 eV
0.0
0 1 2 3 4 0 1 2 3 4
Position (μm) Position (μm)

c 0.1 d
30 3 2 1 1.00
−0.2
T (K)

coincidence counts

20
In(1 − (IPL/I4.2))

−0.4 1.0 0.75

Normalized

10
Data
−0.6 1.64 1.67 1.70 0.50 Fit
Energy (eV)
EA = 0.96 meV
−0.8 0.25
EB = 0.30 meV

−1.0 0.00
0.05 0.10 0.15 −20 −10 0 10 20
1/T (K−1) Time delay (ns)

Figure 2 | Quantum dot light emission. a, One-dimensional hyperspectral image of WSe2 quantum dot emission exhibiting spatial localization. Inset: Zoom-in
of the black dashed box in the main image. b, One-dimensional line cuts of two different quantum dots. Inset: Optical microscope image of the flake. The
start and finish locations of the line cut are identified by two arrows. Total line cut, 4 μm. c, Arrhenius plot for QD2, showing two different slopes. Inset:
Temperature (T) dependence of multiple quantum dots. The bottom of the panel corresponds to 4.2 K and the top to 34 K. The colour bar is normalized
such that the maximum number of photocounts is set to 1. d, Intensity autocorrelation measured on QD3. The horizontal dashed line corresponds to the
zero delay value of 0.36. The zero delay value is corrected according to d.

(1.65 eV) and QD2 (1.70 eV). The inset of Fig. 1b shows the localization observed from many of the narrow emission features
emission spectrum for QD2. Data from a third quantum dot, investigated and is the first piece of evidence that these lines are
QD3 (emission energy 1.68 eV), are also presented in Fig. 3. We defect-related. Another clue to the nature of these features is their
note that spectral wandering was observed on many of the emitters temperature stability. In the inset of Fig. 2c, temperature-dependent
(see Supplementary Fig. 4 for a discussion). photoluminescence is recorded for a number of quantum dots. As
To explore the origin of these narrow emission lines, a expected for defects24, above a certain temperature, in this case
one-dimensional hyperspectral image was acquired (Fig. 2a). ∼35 K, light emission is nearly suppressed. Figure 2c presents the
One-dimensional line cuts for two distinct spectral lines (1.668 eV line cut for QD2 fit to the Arrhenius equation IPL = I4.2 (1 − e−Ea /kT ),
and 1.716 eV) are shown in Fig. 2b. The inset in Fig. 2b identifies where I4.2 is the low-temperature photoluminescence strength and
the path for the hyperpectral line cuts. The start and stop positions Ea is the defect ionization energy. As is apparent in the data, there
are indicated by arrows. Interestingly, we observe these features is a change in slope at ∼18 K. From the fit below 18 K we estimate
along the interface of the single and multilayer flakes (data shown a thermal ionization energy of 0.3 meV and from the fit above 18 K,
in Fig. 2a) and along the edges of flakes. The diffraction-limited 0.96 meV. We further find that the photoluminescence is restored
resolution observed in the spatial line cut is typical of the spatial when the temperature is lowered back to 4 K, and is robust

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NATURE NANOTECHNOLOGY DOI: 10.1038/NNANO.2015.79 LETTERS
Intensity (×103 cps)
a 4 8 12 b c

60

40
X Y
Gate voltage (V)

20

−20
X Y
−40

−60
1.67 1.70 1.73 1.76 Normalized counts Normalized counts
Energy (eV)

d e f
1.0 50 V 1.0 0V 1.0 1.0 −50 V 1.0
Counts (a.u.)

Counts (a.u.)

Counts (a.u.)
0.5 0.5
Y X
0.0 0.0
0.5 0.5 −20 0 20 0.5 −20 0 20
Time (ns) Time (ns)

0.0 0.0 0.0

1.67 1.70 1.73 1.67 1.70 1.73 1.67 1.70 1.73
Energy (eV) Energy (eV) Energy (eV)

Figure 3 | Voltage-controlled quantum light generation. a, WSe2 quantum dot emission spectra as a function of applied gate voltage (X = QD3 and
Y = QD2). b,c, Voltage-dependent photoluminescence for QD3 and QD2. A bandwidth of 5 meV is used to generate each data set. d–f, Recorded spectra for
QD3 and QD2 at the gate voltage values indicated in the panel. Insets: Intensity autocorrelation function for indicated gate voltages.

against temperature cycling (see Supplementary Fig. 5 for additional defect stability is modified by changes to the local potential energy
temperature-dependent data). landscape induced by the applied voltage. Line cuts at specific gate
After investigating the spatial and thermal character of the loca- voltage values from the data in Fig. 3a are presented in Fig. 3d–f.
lized emitters, the photophysical properties were further examined. Each of these voltage-controlled emitters is a quantum dot, as demon-
As is well known, generic two-level systems exhibit saturation as strated by the intensity autocorrelation measurements in the insets of
their excitation rate increases. Such behaviour has been observed Fig. 3e,f. The lifetimes of these two transitions differ by a factor of 4.
in atomic systems, semiconductor quantum dots and defects in Whether the decay time of an isolated WSe2 quantum dot is voltage-
solids. The defect-related light emission in WSe2 is no different, controllable will be the subject of a future study.
and we observe a saturation of photoluminescence emission at Finally, examination of many quantum dot emission spectra
50 nW from power-dependent spectra (Supplementary Fig. 6). A revealed a characteristic doublet structure, as shown in the bottom
natural consequence of these previous observations is that the loca- spectra at 0 T in Fig. 4a (QD2). The doublet is highlighted by grey
lized emitter is, in fact, emitting a stream of non-classical light, in shading. The doublets exhibit correlated spectral wandering, suggesting
this case single photons. Figure 2d presents the second-order inten- they originate from the same localized state. To test if this doublet is
sity autocorrelation function measured on the defect line QD3. related to the spin structure of emission, magneto-optical spectroscopy
From the pronounced anti-bunching dip, the excited-state lifetime was performed in the Faraday configuration (magnetic field applied
is determined to be 1.8 ns. We observed single photon statistics perpendicular to the sample plane and parallel to the optical
on approximately half of the 20 localized emission sites measured, axis). Figure 4a shows the emission spectra recorded for increasing
with lifetimes in the range 0.5–1.8 ns. Compared to extended magnetic fields. The doublet separation increases with field, as
WSe2 excitons, which have lifetimes on the order of ∼30 ps expected for spin-correlated optical transitions.
(ref. 25), the marked increase in excited-state lifetime is characteristic In Fig. 4b, the peak spectral location is plotted as a function of
of three-dimensional quantum confinement26. field. The spectral wandering in the emission appears as a correlated
We next investigated whether external d.c. electric and magnetic jitter in the absolute emission energy of the doublet. This further
fields can control the spectral and/or emission properties of the confirms that the emission does indeed originate from the same
WSe2 quantum dots. WSe2 is well known to support gate-voltage- quantum emitter. The relative separation of the magnetic field
controlled exciton emission22 (Supplementary Fig. 3). Figure 3a split transitions is plotted in Fig. 4c. The data are fit with the
presents the gate-voltage-dependent photoluminescence from two equation
spectrally distinct quantum dots (QD2 and QD3). It is evident that 
















the local electrical environment determines the activity of the Δ = (( gμB B)2 + Δ2o )
observed emission. Figure 3b,c present the spectrally integrated
voltage-dependent emission profiles for the lines labelled X and Y where g is the exciton g-factor, μB is the Bohr magneton, and Δo is
in Fig. 3a (this mitigates the impact of spectral wandering on the the zero-field splitting27. This equation is expected for electron–
photoluminescence). Feature X exhibits a reproducible voltage- hole exchange-dominated magnetic field-dependent optical tran-
dependent maximum in its photoluminescence. It is likely that the sitions in quantum dots of symmetry <D2d. This is a physical

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LETTERS NATURE NANOTECHNOLOGY DOI: 10.1038/NNANO.2015.79

a b 1.703
B field
4 1.702

Energy (eV)
4.2 T

1.701
3.8 T

Normalized intensity (a.u.)

3 1.700
3.0 T

2.6 T 0 1 2 3 4
2 B (T)
2.0 T
c 2.4
1.6 T

1 1.6
0.4 T

Δ (meV)
0.0 T
0.8 g = 9.8 ± 0.1
0 Δo = 730 ± 29 μeV
0.0
1.700 1.703 1.706
Energy (eV) 0 1 2 3 4
B (T)

Figure 4 | Magneto-optical spectroscopy. a, Magnetic field dependence of QD2 emission spectra in the Faraday configuration. The grey shading identifies
QD2. b, Spectral location of two emission peaks associated with QD2. c, Spectral separation of QD2 emission peaks (blue circles) as a function of magnetic
field fitted with a hyperbolic function (red curve). All data were taken at 4 K with a 532 nm excitation laser.

manifestation of the anisotropic potential energy landscape
presented to the localized exciton. The zero-field splitting Δo is
dictated by the electron–hole exchange interaction and is measured
to be 730 ± 29 μeV. From the fit we also determine a g-factor of
9.8 ± 0.1. Remarkably, this g-factor is nearly an order of magnitude
larger than measured for III–V-based InAs quantum dot
excitons27,28.
In conclusion, we have demonstrated that atomically thin semi-
conductors can host optically active quantum dot-like defects. The
localized emitters serve as a source of single photons that are corre-
lated with the internal spin structure, much like semiconductor
quantum dots and NV centres in diamond. We envisage a number
of future directions enabled by this demonstration. Van der Waals
heterostructures will provide a novel platform for the natural exten-
sion of the demonstrated gate voltage control and make WSe2 electri-
cally controlled quantum dots a viable physical implementation for
quantum information processing19. In the context of metrology, the
sensitivity of WSe2 quantum dots to their environment makes these
systems natural candidates for the sensing of nanoscale electromag-
netic fields29, phonon dynamics in WSe2-based membranes, as well
as the Casimir force30. Finally, understanding the interplay between
the WSe2 quantum dots and the WSe2 excitons will enable new
perspectives on valleytronic devices.
Note added in proof: During the preparation of this Letter we
became aware of three similar studies31–33.
Methods
Methods and any associated references are available in the online
version of the paper.
Received 23 December 2014; accepted 17 March 2015;
published online 4 May 2015
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LETTERS
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Acknowledgements
A.N.V. acknowledges support from the Institute of Optics and National Science
Foundation DMR award no. 1309734.
Author contributions
R.B. and A.N.V. conceived the research. C.C. and K.G. fabricated the samples. C.C., L.K.
and A.N.V. conducted the measurements. All authors discussed the data and wrote
the manuscript.
Additional information
Supplementary information is available in the online version of the paper. Reprints and
permissions information is available online at www.nature.com/reprints. Correspondence and
requests for materials should be addressed to A.N.V.
Competing financial interests
The authors declare no competing financial interests.
511
LETTERS NATURE NANOTECHNOLOGY DOI: 10.1038/NNANO.2015.79

Methods
Single-layer WSe2 was mechanically exfoliated onto PDMS-based viscoelastic
stamps. Monolayer flakes were identified under an optical microscope and
verified using optical contrast and photoluminescence spectra. The flakes were
then transferred onto Cr/Au electrodes pre-patterned onto a Si/SiO2 substrate
using an all-dry transfer, as described in the Supplementary Fig. 1. The doped Si
under the substrate was used as the backgate for electrical modulation. The sample
was electrically connected and mounted into an Attodry-1000 cryostat integrated
with a microscope head to perform low-temperature optical studies under applied
magnetic and electric fields. A Keithley 2400 sourcemeter was used as the supply for
the backgate voltage. For anti-bunching measurements, light from the collection
port of the Attodry CFM-1 was fibre-coupled to the entrance port of an Acton
SP2750 spectrometer. The collimated light was diffracted from the grating and
directed to either a nitrogen-cooled CCD for spectral measurements or to the exit slit
of the spectrometer. The width of the exit slit was adjusted to spatially select a narrow
wavelength band centred at the quantum dot emission frequency. The light from the
exit slit of the spectrometer was collimated and directed to a Hanbury-Brown and
Twiss set-up for intensity autocorrelation measurements.

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