We have developed a microspectroscopy technique for measuring gate-modulated reflectance to probe excitonic states in two-dimensional transition metal dichalcogenides. Successfully observing excited states of excitons from cryogenic to room temperature showed that this method is more sensitive to excitonic signals than traditional reflectance spectroscopy. Our results demonstrated the potential of this reflectance spectroscopy method in studying exciton physics in two-dimensional transition metal dichalcogenides and their heterostructures.
In this work the broadening of interband transitions in InGaN/GaN quantum wells (QWs) resulting from structural inhomogeneities is analyzed. The role of polarization-induced electric field in the mechanism behind the inhomogeneous broadening observed in photoluminescence (PL) and electromodulated reflectance (ER) spectra of InGaN QWs dedicated to green/blue lasers is explained. Spectra of both polar and non-polar QWs are simulated within the random QW model distinguishing contributions of individual transitions taking into account QW inhomogeneities (QW width and indium content fluctuations). …
Reflectance and magneto-reflectance experiments together with theoretical modelling based on the $\mathbf{k\cdot p}$ approach have been employed to study the evolution of direct bandgap excitons in MoS$_2$ layers with a thickness ranging from mono- to trilayer. The extra excitonic resonances observed in MoS$_2$ multilayers emerge as a result of the hybridization of Bloch states of each sub-layer due to the interlayer coupling. The properties of such excitons in bi- and trilayers are classified by the symmetry of corresponding crystals. The inter- and intralayer character of the reported excito…
Optical spectroscopy techniques such as differential reflectance and transmittance have proven to be very powerful techniques to study 2D materials. However, a thorough description of the experimental setups needed to carry out these measurements is lacking in the literature. We describe a versatile optical microscope setup to carry out differential reflectance and transmittance spectroscopy in 2D materials with a lateral resolution of ~1 micron in the visible and near-infrared part of the spectrum. We demonstrate the potential of the presented setup to determine the number of layers of 2D mat…
Transition metal dichalcogenides (TMDs) are known to support complex excitonic states. Revealing the differences in relaxation dynamics among different excitonic species and elucidating the transition dynamics between them may provide important guidelines for designing TMD-based excitonic devices. Combining photoluminescence (PL) and reflectance contrast measurements with ultrafast pump-probe spectroscopy under cryogenic temperatures, we herein study the relaxation dynamics of neutral and charged excitons in a back-gate-controlled monolayer device. Pump-probe results reveal quite different rel…
We present optical spectroscopy (photoluminescence and reflectance) studies of thin layers of the transition metal dichalcogenide WSe2, with thickness ranging from mono- to tetra-layer and in the bulk limit. The investigated spectra show the evolution of excitonic resonances as a function of layer thickness, due to changes in the band structure and, importantly, due to modifications of the strength of Coulomb interaction as well. The observed temperature-activated energy shift and broadening of the fundamental direct exciton are well accounted for by standard formalisms used for conventional s…
We consider a system consisting of a large individual quantum dot with excitonic resonance coupled to a single mode photonic cavity in the nonlinear regime when exciton- exciton interaction becomes important. We show that in the presence of time-modulated external coherent pumping the system demonstrates essentially non classical behavior reflected in sub-Poissonian statistics of exciton- and photon-modes and the Wigner functions with negative values in phase-space for time-intervals exceeding the characteristic time of dissipative processes, $t\ggγ^{-1}$. It is shown that these results are ca…
Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both refl…
We present the micro-photoluminescence ($μ$PL) and micro-reflectance contrast spectroscopy studies on thin films of MoSe2 with layer thicknesses ranging from a monolayer (1L) up to 5L. The thickness dependent evolution of the ground and excited state excitonic transitions taking place at various points of the Brillouin zone is determined. Temperature activated energy shifts and linewidth broadenings of the excitonic resonances in 1L, 2L and 3L flakes are accounted for by using standard formalisms previously developed for semiconductors. A peculiar shape of the optical response of the ground st…
Excitons in monolayer transition metal dichalcogenide (TMD) provide a paradigm of composite Boson in 2D system. This letter reports a photoluminescence and reflectance study of excitons in monolayer molybdenum diselenide (MoSe2) with electrostatic gating. We observe the repulsive and attractive Fermi polaron modes of the band edge exciton, its excited state and the spin-off excitons. Our data validate the polaronic behavior of excitonic states in the system quantitatively where the simple three-particle trion model is insufficient to explain.
Mott transition has been realized in atomically thin monolayer (ML) of two dimensional semiconductors (WS$_2$) via optically excited carriers above a critical carrier density through many body interactions. The above nonlinear optical transition occurs when excited electron hole pairs in ML WS2 continuum heavily interact with each other followed by transformation into a collective electron hole plasma phase (EHP), by losing their identity as individual quasiparticles. This is manifested by the alluring red-shift-blue-shift crossover (RBC) phenomena of the excitonic peaks in the emission spectr…
We calculate the near-field optical spectra of excitons and biexcitons in semiconductor quantum dots naturally occurring at interface fluctuations in GaAs-based quantum wells, using a non-local description of the response function to a spatially modulated electro-magnetic field. The relative intensity of the lowest, far-field forbidden excitonic states is predicted; the spatial extension of the ground biexciton state is found in agreement with recently published experiments.
Semiconductor microresonators embedding quantum wells can host tightly confined and mutually interacting excitonic, optical and mechanical modes at once. We theoretically investigate the case where the system operates in the strong exciton-photon coupling regime, while the optical and excitonic resonances are parametrically modulated by the interaction with a mechanical mode. Owing to the large exciton-phonon coupling at play in semiconductors, we predict an enhancement of polariton-phonon interactions by two orders of magnitude with respect to mere optomechanical coupling: a near-unity single…
Moiré patterns of transition metal dichalcogenide (TMD) heterobilayers have proven to be an ideal platform to host unusual correlated electronic phases, emerging magnetism, and correlated exciton physics. While the existence of novel moiré excitonic states is established through optical measurements, the microscopic nature of these states is still poorly understood, often relying on empirically fit models. Here, combining large-scale first-principles GW-BSE calculations and micro-reflection spectroscopy, we identify the nature of the exciton resonances in WSe$_2$/WS$_2$ moiré superlattices, di…
Theoretical investigation of two-dimensional semiconductor nanoribbons and nanoparticles for tailored light--matter interactions
University of Southern Denmark（南丹麦大学）；POLIMA—Center for Polariton-driven Light-Matter Interactions, University of Southern Denmark（POLIMA——极化子驱动光-物质相互作用中心，南丹麦大学）；D-IAS—Danish Institute for Advanced Study, University of Southern Denmark（D-IAS——丹麦高级研究院，南丹麦大学）
Structural Colours with Transition Metal Dichalcogenide Nanostructures
University of Southern Denmark（南丹麦大学）；POLIMA—Center for Polariton-driven Light–Matter Interactions, University of Southern Denmark（POLIMA——极化激元光-物质相互作用中心，南丹麦大学）；SCC — SDU Climate Cluster, University of Southern Denmark（SCC——SDU气候集群，南丹麦大学）
Low-dimensional multiferroic materials hold great promises in miniaturized device applications such as nanoscale transducers, actuators, sensors, photovoltaics, and nonvolatile memories. Here, using first-principles theory we predict that two-dimensional (2D) monolayer Group IV monochalcogenides including GeS, GeSe, SnS, and SnSe are a class of 2D semiconducting multiferroics with strongly coupled giant in-plane spontaneous ferroelectric polarization and spontaneous ferroelastic lattice strain that are thermodynamically stable at room temperature and beyond, and can be effectively modulated by…
Transition metal dichalcogenide monolayers are promising candidates for exploring new electronic and optical phenomena and for realizing atomically thin optoelectronic devices. They host tightly bound electron-hole pairs (excitons) that can be efficiently excited by resonant light fields. Here, we demonstrate that a single monolayer of molybdenum diselenide (MoSe2) can dramatically modify light transmission near the excitonic resonance, acting as an electrically switchable mirror that reflects up to 85% of incident light at cryogenic temperatures. This high reflectance is a direct consequence …
We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photo…
We investigate the phase diagram of a two-dimensional driven-dissipative system of polaritons coupled to the excitonic reservoir. We find that two critical points exists. The first corresponds to the quasi-condensation and the second to a first-order phase transition from the non-uniform state with spatially modulated density to a uniform state. The latter is related to the modulational instability of a homogeneous state due to the repulsive interactions with the non-condensed reservoir. The first-order character of the transition is evidenced by a discontinuity in the density and the correlat…
Integration of 2D Materials in Radial van der Waals Heterostructure Metasurfaces
Ludwig-Maximilians-Universität München（慕尼黑大学）；Politecnico di Milano（米兰理工大学）；Universidade Federal de Pernambuco（伯南布哥联邦大学）；IFN-CNR, Istituto di Fotonica e Nanotecnologie（意大利国家研究委员会光子学与纳米技术研究所）
Graphene covered metal nanoparticles constitute a novel type of hybrid materials, which provide a unique platform to study plasmonic effects, surface-enhanced Raman scattering (SERS), and metal-graphene interactions at the nanoscale. Such a hybrid material is fabricated by transferring graphene grown by chemical vapor deposition onto closely spaced gold nanoparticles produced on a silica wafer. The morphology and physical properties of nanoparticle-supported graphene is investigated by atomic force microscopy, optical reflectance spectroscopy, scanning tunneling microscopy and spectroscopy (ST…
