Voltage-controlled quantum light from an atomically thin semiconductor

Chakraborty, Chitraleema; Kinnischtzke, Laura; Goodfellow, Kenneth M.; Beams, Ryan; Vamivakas, A. Nick

doi:10.1038/nnano.2015.79

Cited by 569 publications

(762 citation statements)

References 34 publications

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“…Hence, the energy of defect excitons is only slightly lower than that of free excitons, which is consistent with the low temperature photoluminescence spectra. The energy of defect excitons also matches well with that from SQEs observed in the WSe 2 monolayer, suggesting the tungsten vacancy defect to be a candidate of such emitters [20][21][22][23]. According to previous studies, the SQEs are subject to the circularly polarized optical selection rule, especially under high magnetic field.…”

Section: Prl 119 046101 (2017) P H Y S I C a L R E V I E W L E T T Esupporting

confidence: 72%

“…Moreover, in conjunction with giant spin-orbit splitting and spin-valley locking at the valence band, p-type doping facilitates the manipulation of valley coherence for a more extended time to 1-10 ns [17,18], in comparison to ∼10 ps with n-type doping [19]. More interestingly, when the WSe 2 monolayer is cooled below ∼10 K, the defectrelated localized exciton emissions behave as single quantum emitters (SQEs) [20][21][22][23], which are essential for quantum information processing [9]. Nevertheless, very little is known about the atomic and electronic structures of the defects in the WSe 2 monolayer.…”

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confidence: 99%

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Defect Structure of Localized Excitons in a WSe2 Monolayer

et al. 2017

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Section: Prl 119 046101 (2017) P H Y S I C a L R E V I E W L E T T Esupporting

confidence: 72%

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confidence: 99%

Defect Structure of Localized Excitons in a WSe2 Monolayer

et al. 2017

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“…Our scheme for valley pseudospin manipulation should also extend to the recently discovered quantum-confined states of excitons in TMDC layers [29][30][31][32][33] . For these localized excitonic states, the valley pseudospin degree of freedom is expected to be well preserved 34 , but their lifetimes are far longer than for the free excitons examined in this work.…”

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confidence: 97%

Optical manipulation of valley pseudospin

Ye¹,

Sun²,

Heinz³

2016

Nature Phys

227

223

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The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including quantum communication and quantum computation 1,2 . Valley polarization, associated with the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum electronics 3,4 . Valley exciton polarization has been created in the transition metal dichalcogenide monolayers using excitation by circularly polarized light and has been detected both optically 5-7 and electrically 8 . In addition, the existence of coherence in the valley pseudospin has been identified experimentally 9 . The manipulation of such valley coherence has, however, remained out of reach. Here we demonstrate all-optical control of the valley coherence by means of the pseudomagnetic field associated with the optical Stark e ect. Using below-bandgap circularly polarized light, we rotate the valley exciton pseudospin in monolayer WSe 2 on the femtosecond timescale. Both the direction and speed of the rotation can be manipulated optically by tuning the dynamic phase of excitons in opposite valleys. This study unveils the possibility of generation, manipulation, and detection of the valley pseudospin by coupling to photons.The broken inversion symmetry in monolayer transition metal dichalcogenide (TMDC) crystals in the semiconducting MX 2 (M = Mo, W; X = S, Se) family gives rise to a nontrivial Berry phase at the K and K valleys in momentum space 10 , where the optically accessible direct bandgap occurs in these materials 11,12 . This Berry phase, together with the angular momentum of the atomic orbitals, leads to different optical selection rules for the two valleys: excitons in the K valley couple to left-circularly polarized photons, while excitons in the K valley couple to right-circularly polarized photons, thus permitting the optical generation of valley polarization through control of the helicity of light [5][6][7] . Moreover, when a TMDC monolayer is excited with linearly polarized light, a coherent superposition state is established between the K and K valley excitons 9 . Such a coherent state can, in principle, be manipulated by lifting the energy degeneracy between valleys through the breaking of time-reversal symmetry in the material. In this regard, d.c. magnetic fields have been applied to achieve a valley splitting of a few meV [13][14][15][16] . Circularly polarized light also breaks time-reversal symmetry, and researchers have used it to create larger valley splittings, corresponding to pseudomagnetic fields up to 60 T (refs 17,18). In addition, this optical approach permits us to access the ultrafast timescale: in this work, we demonstrate the coherent manipulation of the valley pseudospin on the femtosecond timescale.The optical Stark effect has been applied to manipulate the spin/pseudospin in quantum systems, such as atomic quantum gases 19 , quantum dots 20,21 , and III-V quantum wells 22 . H...

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“…[6][7][8][9] In particular, defect-derived excitonic states have recently received much attention for their applications in single-photon emitters. To date, several groups have reported that atomic-layer TMDCs show photoluminescence (PL) from optically active defects at low temperature (4 ∼ 90 K).…”

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Growth and optical properties of Nb-doped WS₂ monolayers

Sasaki

Kobayashi

Liu³

et al. 2016

Appl. Phys. Express

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We report the chemical vapor deposition growth of Nb-doped WS 2 monolayers and their characterization. Electron microscopy observations reveal that the Nb atom was substituted at the W site at a rate of approximately 0.5%. Unlike Mo doping, Nb-doped samples have photoluminescence (PL) peaks at 1.4-1.6 eV at room temperature. The peak energies are lower than the optical bandgap of 1.8 eV, and a saturation behavior of PL intensity is observed with the increase in excitation power. These results indicate that the observed PL peaks are assignable to the emission from impurity states generated by the substitution of Nb. © 2016 The Japan Society of Applied Physics T he optical properties of atomic-layer transition metal dichalcogenides (TMDCs) have recently attracted much attention owing to their wide-range bandgap energies from visible to infrared, 1-3) unique phenomena related to spin-valley physics, 4,5) and single-photon emission. [6][7][8][9] In particular, defect-derived excitonic states have recently received much attention for their applications in single-photon emitters. To date, several groups have reported that atomic-layer TMDCs show photoluminescence (PL) from optically active defects at low temperature (4 ∼ 90 K). 6-11) Such a two-dimensional (2D) single-quantum emission has practical advantages in efficient photon extraction and high integration capability. However, the details of such defect sites are still unclear, and PL can generally be observed only at low temperature. These issues may be resolved by the controlled fabrication of defect states, which is an important challenge in understanding and using TMDC atomic layers as quantum light sources.In general, defect states in low-dimensional materials are created through several mechanisms, including atomic vacancy formation, 12) impurity doping, [13][14][15][16] and chemical functionalization. 17) In this study, we have investigated impuritydoped WS 2 monolayers as a model system. Monolayer WS 2 is a semiconductor with a relatively wide direct bandgap and high air stability, and there have been many reports on its growth process and characterization. 10,[18][19][20][21][22] To implant impurities in WS 2 , we employed halide-assisted chemical vapor deposition (CVD), which was recently developed by Li et al. 21) This method can produce large-area monolayer WS 2 at relatively low temperatures (700°C) and under atmospheric pressure. Importantly, the use of halides can effectively transport precursors of transition metals, which usually have very low vapor pressure. As an impurity, Mo atoms are well studied and cause bandgap narrowing through the substitution of W sites in monolayer WS 2 . 14,15,23,24) However, there are very few studies on the doping of other transition metals for monolayer TMDCs. In the present study, Nb is selected because its atomic size is comparable to that of Mo and it is reported to generate acceptor states for some TMDCs. 16,25) Here, we report the synthesis and characterization of monolayer impurity-doped WS 2 using halide-ass...

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Voltage-controlled quantum light from an atomically thin semiconductor

Cited by 569 publications

References 34 publications

Defect Structure of Localized Excitons in a WSe2 Monolayer

Defect Structure of Localized Excitons in a WSe2 Monolayer

Optical manipulation of valley pseudospin

Growth and optical properties of Nb-doped WS₂ monolayers

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Voltage-controlled quantum light from an atomically thin semiconductor

Cited by 569 publications

References 34 publications

Defect Structure of Localized Excitons in a WSe2 Monolayer

Defect Structure of Localized Excitons in a WSe2 Monolayer

Optical manipulation of valley pseudospin

Growth and optical properties of Nb-doped WS2 monolayers

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Growth and optical properties of Nb-doped WS₂ monolayers