Effect of coating few-layer WS2 on the Raman spectra and whispering gallery modes of a microbottle resonator
TL;DR: In this article, multi-layered tungsten disulfide (WS2) coated silicon/silica (Si/SiO2) substrate and SiO2 micro-bottle resonators (MBRs) have been prepared by van der Waals epitaxy method.
Abstract: Multi-layered tungsten disulfide (WS2) coated silicon/silica (Si/SiO2) substrate and SiO2 micro-bottle resonators (MBRs) have been prepared by van der Waals epitaxy method. Raman spectra of WS2-coated MBR show that the out-of-plane Raman mode is sensitive to the polarization of the excitation laser. The quality factor (Q) values of the whispering gallery modes (WGMs) in the transmission spectrum of an MBR decrease by 2 orders of magnitude on coating with WS2. On coating, a cleaner spectrum is obtained along with a concomitant effect of decrease in the number of lossy modes. Fano resonances as well as Autler-Townes splitting (ATS) was observed for the WGMs in the cleaned transmission spectrum. From the simulations it has been verified that the scattered electric field of the WS2 flakes contributes to the observation of the Fano resonances and ATS in the coated MBR spectra.
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TL;DR: The optical properties of transition metal dichalcogenide monolayers are widely dominated by excitons, Coulomb-bound electron-hole pairs as mentioned in this paper, which give rise to narrow-band, well-pronounced optical transitions, which can be brought into resonance with electromagnetic fields in microcavities and plasmonic nanostructures.
Abstract: The optical properties of transition metal dichalcogenide monolayers are widely dominated by excitons, Coulomb-bound electron-hole pairs. These quasi-particles exhibit giant oscillator strength and give rise to narrow-band, well-pronounced optical transitions, which can be brought into resonance with electromagnetic fields in microcavities and plasmonic nanostructures. Due to the atomic thinness and robustness of the monolayers, their integration in van der Waals heterostructures provides unique opportunities for engineering strong light-matter coupling. We review first results in this emerging field and outline future opportunities and challenges.
185 citations
Journal Article•
TL;DR: In this paper, the authors quantitatively reproduce existing experimental data and present evidence that the apparent discrepancy between intensity ratios observed experimentally can be explained by the high sensitivity of the Raman-active modes to laser polarization.
Abstract: Raman spectra of MoS2, WS2, and their heterostructures are studied by density functional theory. We quantitatively reproduce existing experimental data and present evidence that the apparent discrepancy between intensity ratios observed experimentally can be explained by the high sensitivity of the Raman-active modes to laser polarization. Furthermore, MoS2/WS2 heterostructures up to four layers are considered in every possible combination and stacking order. Each heterostructure configuration possesses a unique Raman spectrum in both frequency and intensity that can be explained by changes in dielectric screening and interlayer interaction. The results establish a set of guidelines for the practical experimental identification of heterostructure configurations.
13 citations
Journal Article•
TL;DR: This work demonstrates, for the first time, a precisely controlled hybrid composition with angular dependence and dispersion-correlated polariton emission by tuning the polariton dispersion in TMD over a broad temperature range of 110-230 K in a single cavity.
Abstract: Monolayer transition metal dichalcogenides (TMD) with confined 2D Wannier-Mott excitons are intriguing for the fundamental study of strong light-matter interactions and the exploration of exciton polaritons at high temperatures. However, the research of 2D exciton polaritons has been hindered because the polaritons in these atomically thin semiconductors discovered so far can hardly support strong nonlinear interactions and quantum coherence due to uncontrollable polariton dynamics and weakened coherent coupling. In this work, we demonstrate, for the first time, a precisely controlled hybrid composition with angular dependence and dispersion-correlated polariton emission by tuning the polariton dispersion in TMD over a broad temperature range of 110--230 K in a single cavity. This tamed polariton emission is achieved by the realization of robust coherent exciton-photon coupling in monolayer tungsten disulphide (${\mathrm{WS}}_{2}$) with large splitting-to-linewidth ratios ($g3.3$). The unprecedented ability to manipulate the dispersion and correlated properties of TMD exciton polaritons at will offers new possibilities to explore important quantum phenomena such as inversionless lasing, Bose-Einstein condensation, and superfluidity.
3 citations
TL;DR: In this paper , a few-layered tungsten disulfide (WS2) nanosheets were synthesized via a cost-effective, low-temperature hydrothermal route.
Abstract: Highly crystalline few-layered tungsten disulfide (WS2) nanosheets were synthesized via a cost-effective, low-temperature hydrothermal route. X-ray diffraction and HR-TEM analysis confirmed the formation of hexagonal nanosheets with thickness of ∼6-8 nm. Raman analysis and AFM results confirmed the few-layered 2H phase of WS2 nanosheets. The UV-vis study shows absorption peaks at 219 and 271 nm with large band gap value of ∼3.12 eV for WS2 nanosheets. Surprisingly, WS2 nanosheets show a dielectric constant of approximately ε' ≈ 5245, whereas bulk WS2 material exhibits a dielectric constant of 7482373. An almost 1426-fold decrease in the value of dielectric constant for the WS2 nanosheet is observed. Such an extreme reduction in dielectric constant and observance of large band gap in WS2 nanosheet were observed for the first time. The present study reveals the excellent and unusual optical and dielectric properties for their potential application in optoelectronic, dielectric, solar, phosphor, and various nanoelectronic devices.
3 citations
TL;DR: In this article, an extremely fast red and blue-shift crossover was observed in the temporal evolution of exciton resonances by resonant exciton A excitation, which is the net result of the competition among many-body effects in the hot-exciton cooling process.
Abstract: Femtosecond transient absorption spectroscopy has been employed to unravel separate initial nonequilibrium dynamic processes of photo-injected electrons and holes during the formation process of the lowest excitons at the K-valley in few-layer tungsten disulfide. Charge carrier thermalization and cooling, as well as concomitant many-body effects on the exciton resonances, are distinguished. The thermalization of holes is observed to be faster than that of electrons. Both of them proceed predominantly via carrier–carrier scattering, as evidenced by the observed dependence of the thermalization time on pump fluences. The fluence dependent time constants also suggest that the subsequent cooling for electrons is probably dominated by acoustic phonons, whereas for holes it is mostly controlled by LO phonons. An extremely fast red- and blue-shift crossover followed by a slow blue-shift of exciton resonance was observed in the temporal evolution of exciton resonances by resonant exciton A excitation. The rapid red-shift could be due to the strong screening of the Coulomb interaction between quasi-free charge carriers in electron–hole plasma. The subsequent slow blue-shift is the net result of the competition among many-body effects in the hot-exciton cooling process. Our findings elucidate the carrier-selective ultrafast dynamics and their many-body effects, underpinning new possibilities for developing optoelectronic devices based on transport properties of a single type of carrier.
References
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TL;DR: Monocrystalline graphitic films are found to be a two-dimensional semimetal with a tiny overlap between valence and conductance bands and they exhibit a strong ambipolar electric field effect.
Abstract: We describe monocrystalline graphitic films, which are a few atoms thick but are nonetheless stable under ambient conditions, metallic, and of remarkably high quality. The films are found to be a two-dimensional semimetal with a tiny overlap between valence and conductance bands, and they exhibit a strong ambipolar electric field effect such that electrons and holes in concentrations up to 10 13 per square centimeter and with room-temperature mobilities of ∼10,000 square centimeters per volt-second can be induced by applying gate voltage.
55,532 citations
TL;DR: The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N=1,2,…,6 S-Mo-S monolayers have been investigated by optical spectroscopy and the effect of quantum confinement on the material's electronic structure is traced.
Abstract: The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N=1,2,…,6 S-Mo-S monolayers have been investigated by optical spectroscopy Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 06 eV This leads to a crossover to a direct-gap material in the limit of the single monolayer Unlike the bulk material, the MoS₂ monolayer emits light strongly The freestanding monolayer exhibits an increase in luminescence quantum efficiency by more than a factor of 10⁴ compared with the bulk material
12,822 citations
"Effect of coating few-layer WS2 on ..." refers background in this paper
...These materials exhibit phenomena such as indirect to direct band-gap transitions [3], strong photo- and electro-luminescence [3, 4] and are promising materials for...
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TL;DR: In this paper, a theoretical analysis of the shape of the 2s2p^{1}P resonance of He observed in the inelastic scattering of electrons is presented. But the analysis is restricted to the case of one discrete level with two or more continua and of a set of discrete levels with one continuum.
Abstract: The interference of a discrete autoionized state with a continuum gives rise to characteristically asymmetric peaks in excitation spectra. The earlier qualitative interpretation of this phenomenon is extended and revised. A theoretical formula is fitted to the shape of the $2s2p^{1}P$ resonance of He observed in the inelastic scattering of electrons. The fitting determines the parameters of the $2s2p^{1}P$ resonance as follows: $E=60.1$ ev, $\ensuremath{\Gamma}\ensuremath{\sim}0.04$ ev, $f\ensuremath{\sim}2 \mathrm{to} 4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}$. The theory is extended to the interaction of one discrete level with two or more continua and of a set of discrete levels with one continuum. The theory can also give the position and intensity shifts produced in a Rydberg series of discrete levels by interaction with a level of another configuration. The connection with the nuclear theory of resonance scattering is indicated.
8,210 citations
TL;DR: Experimental evidence is presented that the threshold pressure of ~120 GPa induces in molecular ammonia the process of autoionization to yet experimentally unknown ionic compound--ammonium amide, opening new possibilities for studying molecular interactions in hydrogen-bonded systems.
Abstract: Ionization of highly compressed ammonia has previously been predicted by computation. Here, the authors provide experimental evidence for this autoionization process at high pressures, showing the transformation of molecular ammonia into ammonium amide.
3,638 citations
TL;DR: In this article, the optical properties and applications of various two-dimensional materials including transition metal dichalcogenides are reviewed with an emphasis on nanophotonic applications, and two different approaches for enhancing their interactions with light: through their integration with external photonic structures, and through intrinsic polaritonic resonances.
Abstract: The optical properties of graphene and emerging two-dimensional materials including transition metal dichalcogenides are reviewed with an emphasis on nanophotonic applications. Two-dimensional materials exhibit diverse electronic properties, ranging from insulating hexagonal boron nitride and semiconducting transition metal dichalcogenides such as molybdenum disulphide, to semimetallic graphene. In this Review, we first discuss the optical properties and applications of various two-dimensional materials, and then cover two different approaches for enhancing their interactions with light: through their integration with external photonic structures, and through intrinsic polaritonic resonances. Finally, we present a narrow-bandgap layered material — black phosphorus — that serendipitously bridges the energy gap between the zero-bandgap graphene and the relatively large-bandgap transition metal dichalcogenides. The plethora of two-dimensional materials and their heterostructures, together with the array of available approaches for enhancing the light–matter interaction, offers the promise of scientific discoveries and nanophotonics technologies across a wide range of the electromagnetic spectrum.
2,414 citations