Abstract

Coherent quantum control and resonance fluorescence of few-level quantum systems is integral for quantum technologies. Here we perform resonance and near-resonance excitation of three-dimensionally confined excitons in monolayer WSe2 to reveal near-ideal single-photon fluorescence with count rates up to 3 MHz. Using high-resolution photoluminescence excitation spectroscopy of the localized excitons, we uncover a weakly fluorescent exciton state 5  meV blue shifted from the ground-state exciton, providing important information to unravel the precise nature of quantum states. Successful demonstration of resonance fluorescence paves the way to probe the localized exciton coherence in two-dimensional semiconductors.

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    [Crossref]
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  36. A. Castellanos-Gomez, M. Buscema, R. Molenaar, V. Singh, L. Janssen, H. S. J. van der Zant, and G. A. Steele, “Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping,” 2D Mater. 1, 011002 (2014).
    [Crossref]

2016 (3)

T. T. Tran, K. Bray, M. J. Ford, M. Toth, and I. Aharonovich, “Quantum emission from hexagonal boron nitride monolayers,” Nat. Nanotechnol. 11, 37–41 (2016).
[Crossref]

A. Branny, G. Wang, C. Kumar, S. Robert, B. Lassagne, X. Marie, B. D. Gerardot, and B. Urbaszek, “Discrete quantum dot like emitters in monolayer MoSe2: spatial mapping, magneto-optics and charge tuning,” Appl. Phys. Lett. 108, 142101 (2016).
[Crossref]

Y. Wu, Q. Tong, G.-B. Liu, H. Yu, and W. Yao, “Spin-valley qubit in nanostructures of monolayer semiconductors: optical control and hyperfine interaction,” Physica Rev. B 93, 045313 (2016).
[Crossref]

2015 (14)

X. Zhang, X.-F. Qiao, W. Shi, J.-B. Wu, D.-S. Jiang, and P.-H. Tan, “Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material,” Chem. Soc. Rev. 44, 2757–2785 (2015).
[Crossref]

X.-X. Zhang, Y. You, S. Y. F. Zhao, and T. F. Heinz, “Experimental evidence for dark excitons in monolayer WSe2,” Phys. Rev. Lett. 115, 257403 (2015).
[Crossref]

G. Wang, L. Bouet, M. M. Glazov, T. Amand, E. L. Ivchenko, E. Palleau, X. Marie, and B. Urbaszek, “Magneto-optics in transition metal diselenide monolayers,” 2D Mater. 2, 034002 (2015).

A. Srivastava, M. Sidler, A. V. Allain, D. S. Lembke, A. Kis, and A. Imamoglu, “Optically active quantum dots in monolayer WSe2,” Nat. Nanotechnol. 10, 491–496 (2015).
[Crossref]

Y.-M. He, G. Clark, J. R. Schaibley, Y. He, M.-C. Chen, Y.-J. Wei, X. Ding, Q. Zhang, W. Yao, C.-Y. Xu, X. Lu, and J.-W. Pan, “Single quantum emitters in monolayer semiconductors,” Nat. Nanotechnol. 10, 497–502 (2015).
[Crossref]

M. Koperski, K. Nogajewski, A. Arora, J. Marcus, P. Kossacki, and M. Potemski, “Single photon emitters in exfoliated WSe2 structures,” Nat. Nanotechnol. 10, 503–506 (2015).
[Crossref]

C. Chakraborty, L. Kinnischtzke, K. M. Goodfellow, R. Beams, and A. N. Vamivakas, “Voltage-controlled quantum light from an atomically thin semiconductor,” Nat. Nanotechnol. 10, 507–511 (2015).
[Crossref]

P. Tonndorf, R. Schmidt, R. Schneider, J. Kern, M. Buscema, G. A. Steele, A. Castellanos-Gomez, H. S. van der Zant, S. M. de Vasconcellos, and R. Bratschitsch, “Single-photon emission from localized excitons in an atomically thin semiconductor,” Optica 2, 347–352 (2015).
[Crossref]

S. Kumar, A. Kaczmarczyk, and B. D. Gerardot, “Strain-induced spatial and spectral isolation of quantum emitters in mono- and bilayer WSe2,” Nano Lett. 15, 7567–7573 (2015).
[Crossref]

K. Xia, R. Kolesov, Y. Wang, P. Siyushev, R. Reuter, T. Kornher, N. Kukharchyk, A. D. Wieck, B. Villa, S. Yang, and J. Wrachtrup, “All-optical preparation of coherent dark states of a single rare earth ion spin in a crystal,” Phys. Rev. Lett. 115, 093602 (2015).
[Crossref]

R. Proux, M. Maragkou, E. Baudin, C. Voisin, P. Roussignol, and C. Diederichs, “Measuring the photon coalescence time window in the continuous-wave regime for resonantly driven semiconductor quantum dots,” Phys. Rev. Lett. 114, 067401 (2015).
[Crossref]

W. B. Gao, A. Imamoglu, H. Bernien, and R. Hanson, “Coherent manipulation, measurement and entanglement of individual solid-state spins using optical fields,” Nat. Photonics 9, 363–373 (2015).
[Crossref]

G.-B. Liu, D. Xiao, Y. Yao, X. Xu, and W. Yao, “Electronic structures and theoretical modelling of two-dimensional group-vib transition metal dichalcogenides,” Chem. Soc. Rev. 44, 2643–2663 (2015).
[Crossref]

M. M. Glazov, E. L. Ivchenko, G. Wang, T. Amand, X. Marie, B. Urbaszek, and B. L. Liu, “Spin and valley dynamics of excitons in transition metal dichalcogenide monolayers,” Phys. Status Solidi B 252, 2349–2362 (2015).
[Crossref]

2014 (7)

X. Xu, W. Yao, D. Xiao, and T. F. Heinz, “Spin and pseudospins in layered transition metal dichalcogenides,” Nat. Phys. 10, 343–350 (2014).
[Crossref]

G.-B. Liu, H. Pang, Y. Yao, and W. Yao, “Intervalley coupling by quantum dot confinement potentials in monolayer transition metal dichalcogenides,” New J. Phys. 16, 105011 (2014).
[Crossref]

G. Wang, L. Bouet, D. Lagarde, M. Vidal, A. Balocchi, T. Amand, X. Marie, and B. Urbaszek, “Valley dynamics probed through charged and neutral exciton emission in monolayer WSe2,” Phys. Rev. B 90, 075413 (2014).
[Crossref]

K. He, N. Kumar, L. Zhao, Z. Wang, K. F. Mak, H. Zhao, and J. Shan, “Tightly bound excitons in monolayer WSe2,” Phys. Rev. Lett. 113, 026803 (2014).
[Crossref]

A. Chernikov, T. C. Berkelbach, H. M. Hill, A. Rigosi, Y. Li, O. B. Aslan, D. R. Reichman, M. S. Hybertsen, and T. F. Heinz, “Exciton binding energy and nonhydrogenic Rydberg series in monolayer WS2,” Phys. Rev. Lett. 113, 076802 (2014).
[Crossref]

A. Castellanos-Gomez, M. Buscema, R. Molenaar, V. Singh, L. Janssen, H. S. J. van der Zant, and G. A. Steele, “Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping,” 2D Mater. 1, 011002 (2014).
[Crossref]

A. Sipahigil, K. D. Jahnke, L. J. Rogers, T. Teraji, J. Isoya, A. S. Zibrov, F. Jelezko, and M. D. Lukin, “Indistinguishable photons from separated silicon-vacancy centers in diamond,” Phys. Rev. Lett. 113, 113602 (2014).
[Crossref]

2013 (3)

A. M. Jones, H. Yu, N. J. Ghimire, S. Wu, G. Aivazian, J. S. Ross, B. Zhao, J. Yan, D. G. Mandrus, D. Xiao, W. Yao, and X. Xu, “Optical generation of excitonic valley coherence in monolayer WSe2,” Nat. Nanotechnol. 8, 634–638 (2013).
[Crossref]

Y.-M. He, Y. He, Y.-J. Wei, D. Wu, M. Atatuere, C. Schneider, S. Hoefling, M. Kamp, C.-Y. Lu, and J.-W. Pan, “On-demand semiconductor single-photon source with near-unity indistinguishability,” Nat. Nanotechnol. 8, 213–217 (2013).
[Crossref]

C. G. Yale, B. B. Buckley, D. J. Christle, G. Burkard, F. J. Heremans, L. C. Bassett, and D. D. Awschalom, “All-optical control of a solid-state spin using coherent dark states,” Proc. Natl. Acad. Sci. USA 110, 7595 (2013).
[Crossref]

2012 (1)

J. Houel, A. V. Kuhlmann, L. Greuter, F. Xue, M. Poggio, B. D. Gerardot, P. A. Dalgarno, A. Badolato, P. M. Petroff, A. Ludwig, D. Reuter, A. D. Wieck, and R. J. Warburton, “Probing single-charge fluctuations at a GaAs/AlAs interface using laser spectroscopy on a nearby InGaAs quantum dot,” Phys. Rev. Lett. 108, 107401 (2012).
[Crossref]

2011 (2)

D. Kim, S. G. Carter, A. Greilich, A. S. Bracker, and D. Gammon, “Ultrafast optical control of entanglement between two quantum-dot spins,” Nat. Phys. 7, 223–229 (2011).
[Crossref]

E. Poem, O. Kenneth, Y. Kodriano, Y. Benny, S. Khatsevich, J. E. Avron, and D. Gershoni, “Optically induced rotation of an exciton spin in a semiconductor quantum dot,” Phys. Rev. Lett. 107, 087401 (2011).
[Crossref]

2010 (1)

R. Lettow, Y. L. A. Rezus, A. Renn, G. Zumofen, E. Ikonen, S. Goetzinger, and V. Sandoghdar, “Quantum interference of tunably indistinguishable photons from remote organic molecules,” Phys. Rev. Lett. 104, 123605 (2010).
[Crossref]

2008 (3)

D. Press, T. D. Ladd, B. Zhang, and Y. Yamamoto, “Complete quantum control of a single quantum dot spin using ultrafast optical pulses,” Nature 456, 218–221 (2008).
[Crossref]

A. J. Ramsay, S. J. Boyle, R. S. Kolodka, J. B. B. Oliveira, J. Skiba-Szymanska, H. Y. Liu, M. Hopkinson, A. M. Fox, and M. S. Skolnick, “Fast optical preparation, control, and readout of a single quantum dot spin,” Phys. Rev. Lett. 100, 197401 (2008).
[Crossref]

G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, “Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence,” Nat. Phys. 4, 60–66 (2008).
[Crossref]

2007 (1)

A. Muller, E. B. Flagg, P. Bianucci, X. Y. Wang, D. G. Deppe, W. Ma, J. Zhang, G. J. Salamo, M. Xiao, and C. K. Shih, “Resonance fluorescence from a coherently driven semiconductor quantum dot in a cavity,” Phys. Rev. Lett. 99, 187402 (2007).
[Crossref]

1991 (1)

C. Dekker, A. J. Scholten, F. Liefrink, R. Eppenga, H. van Houten, and C. T. Foxon, “Spontaneous resistance switching and low-frequency noise in quantum point contacts,” Phys. Rev. Lett. 66, 2148 (1991).
[Crossref]

Aharonovich, I.

T. T. Tran, K. Bray, M. J. Ford, M. Toth, and I. Aharonovich, “Quantum emission from hexagonal boron nitride monolayers,” Nat. Nanotechnol. 11, 37–41 (2016).
[Crossref]

Aivazian, G.

A. M. Jones, H. Yu, N. J. Ghimire, S. Wu, G. Aivazian, J. S. Ross, B. Zhao, J. Yan, D. G. Mandrus, D. Xiao, W. Yao, and X. Xu, “Optical generation of excitonic valley coherence in monolayer WSe2,” Nat. Nanotechnol. 8, 634–638 (2013).
[Crossref]

Allain, A. V.

A. Srivastava, M. Sidler, A. V. Allain, D. S. Lembke, A. Kis, and A. Imamoglu, “Optically active quantum dots in monolayer WSe2,” Nat. Nanotechnol. 10, 491–496 (2015).
[Crossref]

Amand, T.

G. Wang, L. Bouet, M. M. Glazov, T. Amand, E. L. Ivchenko, E. Palleau, X. Marie, and B. Urbaszek, “Magneto-optics in transition metal diselenide monolayers,” 2D Mater. 2, 034002 (2015).

M. M. Glazov, E. L. Ivchenko, G. Wang, T. Amand, X. Marie, B. Urbaszek, and B. L. Liu, “Spin and valley dynamics of excitons in transition metal dichalcogenide monolayers,” Phys. Status Solidi B 252, 2349–2362 (2015).
[Crossref]

G. Wang, L. Bouet, D. Lagarde, M. Vidal, A. Balocchi, T. Amand, X. Marie, and B. Urbaszek, “Valley dynamics probed through charged and neutral exciton emission in monolayer WSe2,” Phys. Rev. B 90, 075413 (2014).
[Crossref]

Arora, A.

M. Koperski, K. Nogajewski, A. Arora, J. Marcus, P. Kossacki, and M. Potemski, “Single photon emitters in exfoliated WSe2 structures,” Nat. Nanotechnol. 10, 503–506 (2015).
[Crossref]

Aslan, O. B.

A. Chernikov, T. C. Berkelbach, H. M. Hill, A. Rigosi, Y. Li, O. B. Aslan, D. R. Reichman, M. S. Hybertsen, and T. F. Heinz, “Exciton binding energy and nonhydrogenic Rydberg series in monolayer WS2,” Phys. Rev. Lett. 113, 076802 (2014).
[Crossref]

Atatuere, M.

Y.-M. He, Y. He, Y.-J. Wei, D. Wu, M. Atatuere, C. Schneider, S. Hoefling, M. Kamp, C.-Y. Lu, and J.-W. Pan, “On-demand semiconductor single-photon source with near-unity indistinguishability,” Nat. Nanotechnol. 8, 213–217 (2013).
[Crossref]

Avron, J. E.

E. Poem, O. Kenneth, Y. Kodriano, Y. Benny, S. Khatsevich, J. E. Avron, and D. Gershoni, “Optically induced rotation of an exciton spin in a semiconductor quantum dot,” Phys. Rev. Lett. 107, 087401 (2011).
[Crossref]

Awschalom, D. D.

C. G. Yale, B. B. Buckley, D. J. Christle, G. Burkard, F. J. Heremans, L. C. Bassett, and D. D. Awschalom, “All-optical control of a solid-state spin using coherent dark states,” Proc. Natl. Acad. Sci. USA 110, 7595 (2013).
[Crossref]

Badolato, A.

J. Houel, A. V. Kuhlmann, L. Greuter, F. Xue, M. Poggio, B. D. Gerardot, P. A. Dalgarno, A. Badolato, P. M. Petroff, A. Ludwig, D. Reuter, A. D. Wieck, and R. J. Warburton, “Probing single-charge fluctuations at a GaAs/AlAs interface using laser spectroscopy on a nearby InGaAs quantum dot,” Phys. Rev. Lett. 108, 107401 (2012).
[Crossref]

Balocchi, A.

G. Wang, L. Bouet, D. Lagarde, M. Vidal, A. Balocchi, T. Amand, X. Marie, and B. Urbaszek, “Valley dynamics probed through charged and neutral exciton emission in monolayer WSe2,” Phys. Rev. B 90, 075413 (2014).
[Crossref]

Bassett, L. C.

C. G. Yale, B. B. Buckley, D. J. Christle, G. Burkard, F. J. Heremans, L. C. Bassett, and D. D. Awschalom, “All-optical control of a solid-state spin using coherent dark states,” Proc. Natl. Acad. Sci. USA 110, 7595 (2013).
[Crossref]

Baudin, E.

R. Proux, M. Maragkou, E. Baudin, C. Voisin, P. Roussignol, and C. Diederichs, “Measuring the photon coalescence time window in the continuous-wave regime for resonantly driven semiconductor quantum dots,” Phys. Rev. Lett. 114, 067401 (2015).
[Crossref]

Beams, R.

C. Chakraborty, L. Kinnischtzke, K. M. Goodfellow, R. Beams, and A. N. Vamivakas, “Voltage-controlled quantum light from an atomically thin semiconductor,” Nat. Nanotechnol. 10, 507–511 (2015).
[Crossref]

Benny, Y.

E. Poem, O. Kenneth, Y. Kodriano, Y. Benny, S. Khatsevich, J. E. Avron, and D. Gershoni, “Optically induced rotation of an exciton spin in a semiconductor quantum dot,” Phys. Rev. Lett. 107, 087401 (2011).
[Crossref]

Berkelbach, T. C.

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Nat. Photonics (1)

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Optica (1)

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Phys. Rev. Lett. (12)

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X.-X. Zhang, Y. You, S. Y. F. Zhao, and T. F. Heinz, “Experimental evidence for dark excitons in monolayer WSe2,” Phys. Rev. Lett. 115, 257403 (2015).
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J. Houel, A. V. Kuhlmann, L. Greuter, F. Xue, M. Poggio, B. D. Gerardot, P. A. Dalgarno, A. Badolato, P. M. Petroff, A. Ludwig, D. Reuter, A. D. Wieck, and R. J. Warburton, “Probing single-charge fluctuations at a GaAs/AlAs interface using laser spectroscopy on a nearby InGaAs quantum dot,” Phys. Rev. Lett. 108, 107401 (2012).
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Phys. Status Solidi B (1)

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Physica Rev. B (1)

Y. Wu, Q. Tong, G.-B. Liu, H. Yu, and W. Yao, “Spin-valley qubit in nanostructures of monolayer semiconductors: optical control and hyperfine interaction,” Physica Rev. B 93, 045313 (2016).
[Crossref]

Proc. Natl. Acad. Sci. USA (1)

C. G. Yale, B. B. Buckley, D. J. Christle, G. Burkard, F. J. Heremans, L. C. Bassett, and D. D. Awschalom, “All-optical control of a solid-state spin using coherent dark states,” Proc. Natl. Acad. Sci. USA 110, 7595 (2013).
[Crossref]

Supplementary Material (1)

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Figures (4)

Fig. 1.
Fig. 1. (a) A low-resolution emission spectrum from location A on the WSe2 monolayer showing a single emission line from a single localized emitter. Inset left: a high-resolution spectrum showing the ZPL and a low-energy phonon sideband (PSB). Inset right: color-coded normalized peak intensities map of emitter A and a neighboring emitter B with strong spatial localization of both emitters. (b) Normalized second-order correlation function g(2)(τ) of the emission line of emitter A exhibiting nearly perfect antibunching. The solid red line is a 95% confidence band for fitting of the measured data. The thin cyan line is the calculated deconvolved g(2)(τ). Time bin=128  ps. Nonresonant CW excitation at λ=532  nm with powers of 4 nW for (a) and 2 nW for (b). Inset left: power dependence of integrated intensity and photon counting rate for emitter A. Inset right: the probability density of g(2)(0) calculated using the probabilistic values of the fitted parameters.
Fig. 2.
Fig. 2. Simultaneous time traces of the fluorescence from emitter B under resonant CW excitation at λ=784.69460  nm with a power of 1 μW as recorded on (a) an APD and (b) a high-resolution spectrometer with 70 ms and 5 s integration, respectively. The background level of 0.4 MHz shown by a horizontal dashed line in (a) and the line at 1580.03  meV in (b) is due to the scattered excitation laser. (c) The time trace of emitter detuning δ=ElaserEp1 of the dominant emission line p1 of emitter B. The gray area is the fitting errors of δ. (d) g(2)(τ) for a time interval when δ0. The solid thick line is a 95% confidence band for fitting of the measured data. The dashed line shows the experimental limitation for g(2)(0) due to the scattered laser background. (e) The fluorescence spectra of emitter B at two different time instances marked by black (blue) dashed lines in (a)–(c) corresponding to time t=12.8 (16.2) min for δ=10 (190) μeV. The black (blue) closed circles are measured data and solid lines are fits.
Fig. 3.
Fig. 3. (a) Polarization-resolved single fluorescence spectrum (top) and color-coded intensity map (bottom) of emitter B under nonresonant excitation showing three emission lines. (b) The PLE spectrum of emitter B shows two bright-exciton peaks p0 and p1 and a BS-X resonance. Closed blue circles are integrated intensities of the line p1 obtained by scanning the laser wavelengths. The open red circles are PLE resonances for peaks p1 and p0 obtained using high-resolution PLE spectroscopy. Peak p2 is not visible in this experiment due to its lower emission energy.
Fig. 4.
Fig. 4. (a) PLE spectrum of emitter C identifying the “BS-X” exciton at an energy 5  meV higher than the ground-state exciton. The closed blue circles are data points, while the solid red curve is a guide for the eye composed of three Gaussian functions. (b) The fluorescence spectrum of emitter C under nonresonant excitation at a power of 4 μW. The spectrum matches the energy range for which PLE is performed in (a). Insets: the full fluorescence spectrum of emitter C acquired on the high-resolution grating under nonresonant excitation. (c) The fluorescence spectrum of emitter C under resonant excitation of the BS-X. The excitation power for (a) and (c) was 80 nW. Inset: schematic of resonant excitation to the BS-X and emission via the ground-state exciton. (d) g(2)(τ) under resonant CW excitation of the BS-X.

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