We report a study of the quantum Hall states (QHSs) sequence of holes in mono- and bilayer WSe$_2$. The QHSs sequence transitions between predominantly even and predominantly odd filling factors as the hole density is tuned in the range $1.6 - 12\times10^{12}$ cm$^{-2}$. The QHSs sequence is insensitive to the transverse electric field, and tilted magnetic field measurements reveal an insensitivity of the QHSs sequence to the in-plane magnetic field, evincing that the hole spin is locked perpendicular to the WSe$_2$ plane. These observations imply that the QHSs sequence is controlled by the Zeeman-to-cyclotron energy ratio, which remains constant as a function of perpendicular magnetic field at a fixed carrier density, but changes as a function of density due to strong electron-electron interaction.
We study the magnetotransport properties of high mobility holes in monolayer and bilayer WSe$_2$, which display well defined Shubnikov-de Haas (SdH) oscillations, and quantum Hall states (QHSs) in high magnetic fields. In both mono and bilayer WSe$_2$, the SdH oscillations and the QHSs occur predominantly at even filling factors, evincing a two-fold Landau level degeneracy. The Fourier transform analysis of the SdH oscillations in bilayer WSe$_2$ reveal the presence of two subbands localized in the top or the bottom layer, as well as negative compressibility. From the temperature dependence of…
The phenomenon originating from spin-orbit coupling (SOC) provides energy-efficient strategies for spin manipulation and device applications. The broken inversion symmetry interface and resulting electric field induce a Rashba-type spin-orbit field (SOF), which has been demonstrated to generate spin-orbit torque for data storage applications. In this study, we found that spin flipping can be achieved by the valley-Zeeman SOF in monolayer WSe2 at room temperature, which manifests as a negative magnetoresistance in the vertical spin valve. Quantum transmission calculations based on an effective …
Moiré superlattices in van der Waals heterostructures have emerged as a powerful tool for engineering novel quantum phenomena. Here we report the observation of a correlated interlayer exciton insulator in a double-layer heterostructure composed of a WSe2 monolayer and a WS2/WSe2 moiré bilayer that are separated by an ultrathin hexagonal boron nitride (hBN). The moiré WS2/WSe2 bilayer features a Mott insulator state at hole density p/p0 = 1, where p0 corresponds to one hole per moiré lattice site. When electrons are added to the Mott insulator in the WS2/WSe2 moiré bilayer and an equal number …
Monolayer transition metal dichalcogenides (TMDs) hold great promise for future information processing applications utilizing a combination of electron spin and valley pseudospin. This unique spin system has led to observation of the valley Zeeman effect in neutral and charged excitonic resonances under applied magnetic fields. However, reported values of the trion valley Zeeman splitting remain highly inconsistent across studies. Here, we utilize high quality hBN encapsulated monolayer WSe$_2$ to enable simultaneous measurement of both intervalley and intravalley trion photoluminescence. We f…
The newly developed two-dimensional layered materials provide perfect platform for valley-spintronics exploration. To determine the prospect of utilizing the valley degree of freedom, it is of great importance to directly detect and understand the valley dynamics in these materials. Here, the exciton valley dynamics in monolayer WSe$_2$ is investigated by the two-color pump-probe magneto-optical Kerr technique. By tuning the probe photon energy in resonance with the free excitons and trions, the valley relaxation time of different excitonic states in monolayer WSe$_2$ is determined. Valley rel…
Monolayers and multilayers of semiconducting transition metal dichalcogenides (TMDCs) offer an ideal platform to explore valley-selective physics with promising applications in valleytronics and information processing. Here we manipulate the energetic degeneracy of the $\mathrm{K}^+$ and $\mathrm{K}^-$ valleys in few-layer TMDCs. We perform high-field magneto-reflectance spectroscopy on WSe$_2$, MoSe$_2$, and MoTe$_2$ crystals of thickness from monolayer to the bulk limit under magnetic fields up to 30 T applied perpendicular to the sample plane. Because of a strong spin-layer locking, the gro…
We present a comprehensive optical study of the excitonic Zeeman effects in transition metal dichalcogenide monolayers, which are discussed comparatively for selected materials: MoSe$_2$, WSe$_2$ and WS$_2$. We introduce a simple semi-phenomenological description of the magnetic field evolution of individual electronic states in fundamental sub-bands by considering three additive components: valley, spin and orbital terms. We corroborate the validity of the proposed description by inspecting the Zeeman-like splitting of neutral and charged excitonic resonances in absorption-type spectra. The v…
We have systematically examined the circular polarization of monolayer WSe2 at different temperature, excitation energy and exciton density. The valley depolarization in WSe2 is experimentally confirmed to be governed by the intervalley electron-hole exchange interaction. More importantly, a non-monotonic dependence of valley circular polarization on the excitation power density has been observed, providing the experimental evidence for the non-monotonic dependence of exciton intervalley scattering rate on the excited exciton density. The physical origination of our experimental observations h…
Acquisition and analysis is described for scanning tunneling spectroscopy data acquired from a monolayer of WSe$_2$ grown on epitaxial graphene on SiC. Curve fitting of the data is performed, in order to deduce band-edge energies. In addition to describing the details of the theoretical curves used for the fitting, the acquisition and analysis methods are also discussed within the larger context of the historical development of scanning tunneling spectroscopy techniques.
A monolayer of a transition metal dichalcogenide (TMD) such as WSe$_2$ is a two-dimensional (2D) direct band-gap valley-semiconductor having an effective Honeycomb lattice structure with broken inversion symmetry. The inequivalent valleys in the Brillouin zone could be selectively addressed using circularly-polarized light fields, suggesting the possibility for magneto-optical measurement and manipulation of the valley pseudospin degree of freedom. Here we report such experiments that demonstrate the valley Zeeman effect -- strongly anisotropic lifting of the degeneracy of the valley pseudospi…
WSe$_2$ monolayers with variable doping are an ideal system to study two-dimensional excitonic complexes. Here, we find that the strongest photoluminescence from bright neutral excitons occurs at moderate $p$-doping levels, owing to a rapid decrease of signal from positive dark trions and a slow increase of signal from positive bright trions with growing $p$-concentrations. We explain our observations with a qualitative model, in which the scattering rate of bright excitons into dark complexes is enhanced by exciton localization, while the scattering rate into positive bright trions increases …
We report a first principles theoretical investigation of quantum transport in monolayer WSe2 field effect transistor (FET). Due to a strong spin-orbit interaction (SOI) and the atomic structure of the two-dimensional (2D) lattice, monolayer WSe2 has an interesting electronic structure that exhibits Zeeman-like up-down spin texture near the K and K' points of the Brillouin zone. In a FET, the gate electric field induces an extra, externally tunable SOI that re-orients the spins into a Rashba-like texture thereby realizing electric control of the spin. Quantum transport is modulated by the spin…
Optical spectroscopy in high magnetic fields $B\leq65$ T is used to reveal the very different nature of carriers in monolayer and bulk transition metal dichalcogenides. In monolayer WSe$_{2}$, the exciton emission shifts linearly with the magnetic field and exhibits a splitting which originates from the magnetic field induced valley splitting. The monolayer data can be described using a single particle picture with a Dirac-like Hamiltonian for massive Dirac fermions, with an additional term to phenomenologically include the valley splitting. In contrast, in bulk WSe$_{2}$ where the inversion s…
We report the strong dependence of resistance on uniaxial strain in monolayer WSe2 at various temperatures, where the gauge factor can reach as large as 2400. The observation of strain-dependent resistance and giant gauge factor is attributed to the emergence of nonzero Berry curvature dipole. Upon increasing strain, Berry curvature dipole can generate net orbital magnetization, which would introduce additional magnetic scattering, decreasing the mobility and thus conductivity. Our work demonstrates the strain engineering of Berry curvature and thus the transport properties, making monolayer W…
We report the fabrication and characterization of gate-defined hole quantum dots in monolayer and bilayer WSe$_2$. The devices were operated with gates above and below the WSe$_2$ layer to accumulate a hole gas, which for some devices was then selectively depleted to define the dot. Temperature dependence of conductance in the Coulomb blockade regime is consistent with transport through a single level, and excited state transport through the dots was observed at temperatures up to 10 K. For adjacent charge states of a bilayer WSe$_2$ dot, magnetic field dependence of excited state energies was…
We report the first observation of gate-controlled field emission current from a tungsten diselenide (WSe2) monolayer, synthesized by chemical-vapour deposition on SiO2/Si substrate. Ni contacted WSe2 monolayer back-gated transistors, under high vacuum, exhibit n-type conduction and drain-bias dependent transfer characteristics, which are attributed to oxygen/water desorption and drain induced Schottky barrier lowering, respectively. The gate-tuned n-type conduction enables field emission, i.e. the extraction of electrons by quantum tunnelling, even from the flat part of the WSe2 monolayers. E…
The optical properties of monolayer and bilayer transition metal dichalcogenide semiconductors are governed by excitons in different spin and valley configurations, providing versatile aspects for van der Waals heterostructures and devices. We present experimental and theoretical studies of exciton energy splittings in external magnetic field in neutral and charged WSe$_2$ monolayer and bilayer crystals embedded in a field effect device for active doping control. We develop theoretical methods to calculate the exciton $g$-factors from first principles and tight-binding for all possible spin-va…
Atomic monolayers of transition metal dichalcogenides represent an emerging material platform for the implementation of ultra compact quantum light emitters via strain engineering. In this framework, we discuss experimental results on creation of strain induced single photon sources using a WSe2 monolayer on a silver substrate, coated with a very thin dielectric layer. We identify quantum emitters which are formed at various locations in the sample. The emission is highly linearly polarized, stable in linewidth and decay times down to 300 ps are observed. We provide numerical calculations of o…
Quantum confinenement and manipulation of charge carriers are critical for achieving devices practical for quantum technologies. The interplay between electron spin and valley, as well as the possibility to address their quantum states electrically and optically, make two-dimensional (2D) transition metal dichalcogenides an emerging platform for the development of quantum devices. In this work, we fabricate devices based on heterostructures of layered 2D materials, in which we realize gate-controlled tungsten diselenide (WSe2) hole quantum dots. We discuss the observed mesoscopic transport fea…
Proximity orbital and spin-orbit effects of bilayer graphene on monolayer WSe$_2$ are investigated from first-principles. We find that the built-in electric field induces an orbital band gap of about 10 meV in bilayer graphene. Remarkably, the proximity spin-orbit splitting for holes is two orders of magnitude---the spin-orbit splitting of the valence band at K is about 2 meV---more than for electrons. Effectively, holes experience spin-valley locking due to the strong proximity of the lower graphene layer to WSe$_2$. However, applying an external transverse electric field of some 1 V/nm, coun…
We study Shubnikov-de Haas oscillations in a p-type WSe$_2$ monolayer under very high magnetic field. The oscillation pattern is complex due to a large spin and valley splitting, in the non-fully-resolved Landau level regime. Our experimental data can be reproduced with a model in which the main parameter is the ratio between the Zeeman energy and the cyclotron energy. The model takes into account the Landau levels from both valleys with the same Gaussian broadening, which allows to predict the relative amplitude of the resistance oscillation originating from each valley. The Zeeman energy is …
We propose a novel phonon assisted Auger process unique to the electronic band structure of monolayer transition metal dichalcogenides (TMDCs), which dominates the radiative recombination of ground state excitons in Tungsten based TMDCs. Using experimental and DFT computed values for the exciton energies, spin-orbit splittings, optical matrix element, and the Auger matrix elements, we find that the Auger process begins to dominate at carrier densities as low as $10^{9-10}~{\rm cm^{-2}}$, thus providing a plausible explanation for the low quantum efficiencies reported for these materials.
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and tripl…
Strong Coulomb interactions in atomically thin semiconductors like monolayer WSe$_2$ induce not only tightly bound excitons, but also make their optical properties very sensible to doping. By utilizing a microscopic theory based on the excitonic Heisenberg equations of motion, we systematically determine the influence of doping on the excitonic linewidth, lineshift, and oscillator strength. We calculate trion resonances and demonstrate that the Coulomb coupling of excitons to the trionic continuum generates a non-Markovian interference, which, due to a time retardation, builds up a phase respo…
In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe2 reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime app…
Monolayer WSe$_2$ hosts a series of exciton Rydberg states denoted by the principal quantum number n = 1, 2, 3, etc. While most research focuses on their absorption properties, their optical emission is also important but much less studied. Here we measure the photoluminescence from the 1s - 5s exciton Rydberg states in ultraclean monolayer WSe$_2$ encapsulated by boron nitride under magnetic fields from -31 T to 31 T. The exciton Rydberg states exhibit similar Zeeman shifts but distinct diamagnetic shifts from each other. From their luminescence spectra, Zeeman and diamagnetic shifts, we dedu…
The monolayer WSe2 is interesting and important for future application in nanoelectronics, spintronics and valleytronics devices, because it has the largest spin splitting and longest valley coherence time among all the known monolayer transition-metal dichalcogenides (TMDs). To obtain the large-area monolayer TMDs' crystal is the first step to manufacture scalable and high-performance electronic devices. In this letter, we have successfully fabricated millimeter-sized monolayer WSe2 single crystals with very high quality, based on our improved mechanical exfoliation method. With such superior…
Monolayer semiconductors are atomically thin quantum wells with strong confinement of electrons in two-dimensional (2D) plane. Here, we experimentally study the out-of-plane polarizability of excitons in hBN-encapsulated monolayer WSe$_{2}$ in strong electric fields of up to 1.6 V/nm (16 MV/cm). We monitor free and bound exciton photoluminescence peaks with increasing electric fields at a constant carrier density, carefully compensating for unintentional photodoping in our double-gated device at 4K. We show that the Stark shift is < 0.4 meV despite the large electric fields applied, yielding a…
Monolayers of semiconducting transition metal dichalcogenides are two-dimensional direct-gap systems which host tightly-bound excitons with an internal degree of freedom corresponding to the valley of the constituting carriers. Strong spin-orbit interaction and the resulting ordering of the spin-split subbands in the valence and conduction bands makes the lowest-lying excitons in WX$_2$ (X~being S or Se) spin-forbidden and optically dark. With polarization-resolved photoluminescence experiments performed on a WSe$_2$ monolayer encapsulated in a hexagonal boron nitride, we show how the intrinsi…
Coulomb interaction between electrons lies at the heart of magnetism in solids. In contrast to conventional two-dimensional (2D) systems, electrons in monolayer transition metal dichalcogenides (TMDs) possess coupled spin and valley degrees of freedom by the spin-orbit interaction. The electrons are also strongly interacting even in the high-density regime because of the weak dielectric screening in two dimensions and a large band mass. The combination of these properties presents a unique platform for exploring spin and valley magnetism in 2D electron liquids. Here we report an observation by…
We discuss coupling of site-selectively induced quantum emitters in exfoliated monolayers of WSe$_2$ to plasmonic nanostructures. Squared and rectangular gold nanopillars, which are arranged in pitches of \SI{4}{\micro\meter} on the surface, have sizes of tens of nanometers, and act as seeds for the formation of quantum emitters in the atomically thin materials. We observe chraracteristic narrow-band emission signals from the monolayers, which correspond well with the positions of the metallic nanopillars with and without thin dielectric coating. Single photon emission from the emitters is con…
Using time-resolved Kerr rotation, we measure the spin/valley dynamics of resident electrons and holes in single charge-tunable monolayers of the archetypal transition-metal dichalcogenide (TMD) semiconductor WSe2. In the n-type regime, we observe long (70 ns) polarization relaxation of electrons that is sensitive to in-plane magnetic fields $B_y$, indicating spin relaxation. In marked contrast, extraordinarily long (2 microsecond) polarization relaxation of holes is revealed in the p-type regime, that is unaffected by $B_y$, directly confirming long-standing expectations of strong spin-valley…
Strong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction and possible new optoelectronic applications are at the heart of studies of the rich physics of excitons in semiconductor structures made of monolayers of transition metal dichalcogenides (TMD). In intrinsic TMD monolayers the basic, intravalley excitons are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is "dark", although possibly …
In monolayer transition-metal dichalcogenide semiconductors, many-body correlations can manifest in optical spectra when photoexcited electron-hole pairs (excitons) are introduced into a 2D Fermi sea of mobile carriers. At low carrier densities, the formation of positively and negatively charged excitons ($X^\pm$) is well documented. However, in WSe$_2$ monolayers, an additional absorption resonance, often called $X^{-\prime}$, emerges at high electron density. Its origin is not understood. Here we investigate the $X^{-\prime}$ state via polarized absorption spectroscopy of electrostatically-g…
The variety of excitonic states in tungsten-based dichalcogenide monolayers stems from unique interplay between the spin and valley degrees of freedom. One of the exciton species is the indirect exciton (momentum or valley dark), which is responsible to a series of resonances when the monolayer is charge neutral. We investigate the short-range electron-hole exchange interaction of the indirect exciton, as well as its recombination mechanism mediated by impurities. The analysis provides thorough understanding of the energy and polarization of the zero-phonon indirect exciton resonance in the em…
Two-dimensional materials and their heterostructures have opened up new possibilities for magnetism at the nanoscale. In this study, we utilize first-principles simulations to investigate the structural, electronic, and magnetic properties of $\textrm{Fe}/\textrm{WSe}_2/\textrm{Pt}$ systems containing pristine, defective, or doped $\textrm{WSe}_2$ monolayers. The proximity effects of the ferromagnetic Fe layer are studied by considering defective and vanadium-doped $\textrm{WSe}_2$ monolayers. All heterostructures are found to be ferromagnetic, and the insertion of the transition-metal dichalc…
Monolayers of transition metal dichalcogenides (TMDs) have recently emerged as a promising optoelectronic platform. To leverage their full potential, however, it is important to understand and engineer the properties of the different exciton species that exist in these monolayers, as well as to control their transport through the material. A promising approach relies on engineering strain landscapes in atomically thin semiconductors that excitons navigate. In WSe$_2$ monolayers, for example, localized strain has been used to control the emission wavelength of excitons, induce exciton funneling…
We report the experimental observation of radiative recombination from Rydberg excitons in a two-dimensional semiconductor, monolayer WSe2, encapsulated in hexagonal boron nitride. Excitonic emission up to the 4s excited state is directly observed in photoluminescence spectroscopy in an out-of-plane magnetic field up to 31 Tesla. We confirm the progressively larger exciton size for higher energy excited states through diamagnetic shift measurements. This also enables us to estimate the 1s exciton binding energy to be about 170 meV, which is significantly smaller than most previous reports. The…
Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition metal dichalcogenide (TMDC) with broken inversion symmetry possesses two degenerate yet inequivalent valleys, offering unique opportunities for valley control through helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest, (~ 0.2 meV/T). Here we show greatly enhanced valley spitting in monolayer WSe2, …
We report the observation and gate manipulation of intrinsic dark trions in monolayer WSe$_2$. By using ultraclean WSe$_2$ devices encapsulated by boron nitride, we directly resolve the weak photoluminescence of dark trions. The dark trions can be tuned continuously between negative and positive charged trions with electrostatic gating. We also reveal their spin triplet configuration and distinct valley optical emission by their characteristic Zeeman splitting under magnetic field. The dark trions exhibit large binding energy (14-16 meV). Their lifetime (~1.3 ns) is two orders of magnitude lon…
The rich optical properties of transition metal dichalcogenide monolayers (TMD-MLs) render these materials promising candidates for the design of new optoelectronic devices. Despite the large number of excitonic complexes in TMD-MLs, the main focus has been put on optically bright neutral excitons. Spin-forbidden dark excitonic complexes have been addressed for basic science purposes, but not for applications. We report on spin-forbidden dark excitonic complexes in ML WSe$_2$ as an ideal system for the facile generation of radially polarized light beams. Furthermore, the spatially resolved pol…
Monolayers (MLs) of transition metal dichalcogenides (TMDs) exhibit unusual electrical behavior under magnetic fields due to their intrinsic spin-orbit coupling and lack of inversion symmetry. While recent experiments have also identified the critical role of carrier interactions within these materials, a complete mapping of the ambipolar Landau level (LL) sequence has remained elusive. Here, we use single-electron transistors to perform LL spectroscopy in ML WSe$_2$, for the first time providing a comprehensive picture of the electronic structure of a ML TMD for both electrons and holes. We f…
Tailoring pure valley-Zeeman spin-orbit coupling in WSe$_2$-encapsulated monolayer graphene
National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, School of Physics, Nanjing University（南京大学固体微结构物理国家重点实验室、先进微结构协同创新中心、物理学院）；Center for Quantum Matter, School of Physics, Zhejiang University（浙江大学量子物质科学研究中心、物理学院）
The defect states in atomically thin layers of transition metal dichalcogenides are promising candidates for single photon emission. However, the brightness of such quantum emission is often weak, and is accompanied with undesirable effects like spectral diffusion and strong background emission. By placing a monolayer WSe$_2$ directly on a rough gold substrate, here we show a selective enhancement of sharp defect-bound exciton peaks, coupled with a suppressed spectral diffusion and strong quenching of background luminescence. By combining the experimental data with detailed electromagnetic sim…
We report an experimental study of temperature-dependent spectral lineshapes of phonon side-band emission stemming from dark excitons in monolayer and bilayer WSe$_{2}$. Using photoluminescence spectroscopy in the range from 4 to 100K, we observe a pronounced asymmetry in the phonon-assisted luminescence from momentum-indirect exciton reservoirs. We demonstrate that the corresponding spectral profiles are distinct from those of bright excitons with direct radiative decay pathways. The lineshape asymmetry reflects thermal distribution of exciton states with finite center-of-mass momenta, charac…
Low-temperature photoluminescence (PL) of hBN-encapsulated monolayer tungsten diselenide (WSe$_2$) shows a multitude of sharp emission peaks below the bright exciton. Some of them have been recently identified as phonon sidebands of momentum-dark states. However, the exciton dynamics behind the emergence of these sidebands has not been revealed yet. In this joint theory-experiment study, we theoretically predict and experimentally observe time-resolved PL providing microscopic insights into thermalization of hot excitons formed after optical excitation. In good agreement between theory and exp…
Optical probing of Wigner crystallization in monolayer WSe$_2$ via diffraction of longitudinal excitons
ITMO University（ITMO大学）；Moscow Institute of Physics and Technology (National Research University)（莫斯科物理科学与技术学院（国立研究大学））；Russian Quantum Center（俄罗斯量子中心）；Laboratory of Programmable Functional Materials, Center for Neurophysics and Neuromorphic Technologies（可编程功能材料实验室，神经物理与类脑技术中心）；Moscow Center for Advanced Studies（莫斯科高级研究中心）；Queen’s University（女王大学）
We demonstrate a deterministic Purcell-enhanced single-photon source realized by integrating an atomically thin WSe$_{2}$ layer with a circular Bragg grating cavity. The cavity significantly enhances the photoluminescence from the atomically thin layer, and supports single-photon generation with $g^{(2)}(0)<0.25$. We observe a consistent increase of the spontaneous emission rate for WSe$_{2}$ emitters located in the center of the Bragg grating cavity. These WSe$_{2}$ emitters are self-aligned and deterministically coupled to such a broadband cavity, configuring a new generation of deterministi…
We report on nanosecond long, gate-dependent valley lifetimes of free charge carriers in monolayer WSe$_2$, unambiguously identified by the combination of time-resolved Kerr rotation and electrical transport measurements. While the valley polarization increases when tuning the Fermi level into the conduction or valence band, there is a strong decrease of the respective valley lifetime consistent with both electron-phonon and spin-orbit scattering. The longest lifetimes are seen for spin-polarized bound excitons in the band gap region. We explain our findings via two distinct, Fermi level-depen…
We present a high-resolution resonance Raman study of hBN encapsulated MoSe$_2$ and WSe$_2$ monolayers at 4 K using excitation energies from 1.6 eV to 2.25 eV. We report resonances with the WSe$_2$ A2s and MoSe$_2$ A2s and B2s excited Rydberg states despite their low oscillator strength. When resonant with the 2s states we identify new Raman peaks which are associated with intravalley scattering between different Rydberg states via optical phonons. By calibrating the Raman scattering efficiency and separately constraining the electric dipole matrix elements, we reveal that the scattering rates…
We report scanning tunneling microscopy (STM) and spectroscopy (STS) measurements of monolayer and bilayer WSe$_2$. We measure a band gap of 2.21 $\pm$ 0.08 eV in monolayer WSe$_2$, which is much larger than the energy of the photoluminescence peak indicating a large excitonic binding energy. We additionally observe significant electronic scattering arising from atomic-scale defects. Using Fourier transform STS (FT-STS), we map the energy versus momentum dispersion relations for monolayer and bilayer WSe$_2$. Further, by tracking allowed and forbidden scattering channels as a function of energ…
In crystals, energy band extrema in momentum space can be identified by their valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides. However, the valley coherence time, a key quantity for manipulating the valley pseudospin, has never been measured in any material. In this work, we use a sequence of laser pulses …
Using time-resolved optical Kerr rotation, we measure the low temperature valley dynamics of resident electrons and holes in exfoliated WSe$_2$ monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically-gated WSe$_2$ monolayers having different dielectric environments. In a fully-encapsulated structure (hBN/WSe$_2$/hBN, where hBN is hexagonal boron nitride), valley relaxation is found to…
