We investigate Landau-quantized excitonic absorption and luminescence of monolayer WSe$_2$ under magnetic field. We observe gate-dependent quantum oscillations in the bright exciton and trions (or exciton-polarons) as well as the dark trions and their phonon replicas. Our results reveal spin- and valley-polarized Landau levels (LLs) with filling factors $n = +0, +1$ in the bottom conduction band and $n = -0$ to $-6$ in the top valence band, including the Berry-curvature-induced $n = \pm0$ LLs of massive Dirac fermions. The LL filling produces periodic plateaus in the exciton energy shift accompanied by sharp oscillations in the exciton absorption width and magnitude. This peculiar exciton behavior can be simulated by semi-empirical calculations. The experimentally deduced g-factors of the conduction band (g ~ 2.5) and valence band (g ~ 15) exceed those predicted in a single-particle model (g = 1.5, 5.5, respectively). Such g-factor enhancement implies strong many-body interactions in gated monolayer WSe$_2$. The complex interplay between Landau quantization, excitonic effects, and many-body interactions makes monolayer WSe$_2$ a promising platform to explore novel correlated quantum phenomena.
Photoluminescence from bulk HfS$_2$ grown by the chemical vapor transport method is reported. A series of emission lines is apparent at low temperature in the energy range of 1.4 - 1.5 eV. Two groups of the observed excitonic transitions followed by their replicas involving acoustic and optical phonons are distinguished using classical intensity correlation analysis. The emission is attributed to the recombination of excitons bound to iodine (I$_2$) molecules intercalated between layers of HfS$_2$. The I$_2$ molecules are introduced to the crystal during the growth as halogen transport agents …
A fully microscopic theory for the spontaneous emission from semiconductors is discussed. The theory is evaluated for a quantum-well system and the role of excitonic and unbound electron-hole-pair contributions to the emission is analyzed. Simplifying aproximations to the full theory and their range of validity are discussed. Numerical solutions are presented for experimentally relevant situations and it is shown that a detailed analysis of measured spectra requires the knowledge of both absorption and emission under identical conditions.
In twisted homobilayer transition metal dichalcogenides, intra- and inter-layer valley excitons hybridize with the layer configurations spatially varying in the moiré. The ground state valley excitons are trapped at two high-symmetry points with opposite electric dipoles in a moiré supercell, forming a honeycomb superlattice of nearest-neighbor dipolar attraction. We find that the spatial texture of layer configuration results in a luminescence anomaly of the moiré trapped excitons, where a tiny displacement by interactions dramatically increases the brightness and changes polarization from ci…
Atomically thin semiconductors have dimensions that are commensurate with critical feature sizes of future optoelectronic devices defined using electron/ion beam lithography. Robustness of their emergent optical and valleytronic properties is essential for typical exposure doses used during fabrication. Here, we explore how focused helium ion bombardment affects the intrinsic vibrational, luminescence and valleytronic properties of atomically thin MoS$_{2}$. By probing the disorder dependent vibrational response we deduce the interdefect distance by applying a phonon confinement model. We show…
Due to degeneracies arising from crystal symmetries, it is possible for electron states at band edges ("valleys") to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that routinely implemented using true spin, in the quest for quantum technologies. Here we show for the first time that SU(2) valley coherence can indeed be generated and detected. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley e…
Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yield…
The results of investigation of bulk GaAs photoluminescence are presented taken from near-surface layers of different thicknesses using for excitation the light with the wavelengths which are close but some greater than the excitonic absorption resonances (so-called "bulk" photoexcitation). Only the excitonic and band-edge luminescence is seen under the interband excitation, while under the "bulk" excitation, the spectra are much more informative. The interband excited spectra of all the samples investigated in the present work are practically identical, whereas the bulk excited PL spectra are…
With the both spin and valley degrees of freedom, the low-lying excitonic spectra of photo-excited transition-metal dichalcogenide monolayers (TMDC-MLs) are featured by rich fine structures, comprising the intra-valley bright exciton states as well as various intra- and inter-valley dark ones. The latter states can be classified as those of the spin- and momentum-forbidden dark excitons according to the violated optical selection rules. Because of the optical invisibility, the two types of the dark states are in general hardly observed and even distinguished in conventional spectroscopies alth…
Excitons in monolayer semiconductors have large optical transition dipole for strong coupling with light field. Interlayer excitons in heterobilayers, with layer separation of electron and hole components, feature large electric dipole that enables strong coupling with electric field and exciton-exciton interaction, at the cost that the optical dipole is substantially quenched (by several orders of magnitude). In this letter, we demonstrate the ability to create a new class of excitons in transition metal dichalcogenide (TMD) hetero- and homo-bilayers that combines the advantages of monolayer-…
We show room temperature valley coherence with in MoS2, MoSe2, WS2 and WSe2 monolayers using linear polarization resolved hot photoluminescence (PL), at energies close to the excitation - demonstrating preservation of valley coherence before sufficient scattering events. The features of the co-polarized hot luminescence allow us to extract the lower bound of the binding energy of the A exciton in monolayer MoS2 as 0.42 (+/- 0.02) eV. The broadening of the PL peak is found to be dominated by Boltzmann-type hot luminescence tail, and using the slope of the exponential decay, the carrier temperat…
The results of investigation of bulk GaAs photoluminescence are presented taken from near-surface layers of different thicknesses using for excitation the light with the wavelengths which are close but some greater than the excitonic absorption resonances (so-called bulk photoexcitation). Only the excitonic and band-edge luminescence is seen under the interband excitation, while under the bulk excitation, the spectra are much more informative. The interband excited spectra of all the samples investigated in the present work are practically identical, whereas the bulk excited PL spectra are dif…
Transition-metal dichalcogenides can be easily produced as atomically thin sheets, exhibiting the possibility to optically polarize and read out the valley pseudospin of extremely stable excitonic quasiparticles present in these 2D semiconductors. Here, we investigate a monolayer of tungsten disulphide in high magnetic fields up to 30\,T via photoluminescence spectroscopy at low temperatures. The valley degeneracy is lifted for all optical features, particularly for excitons, singlet and triplet trions, for which we determine the g factor separately. While the observation of a diamagnetic shif…
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 show that band topology can dramatically change the photophysics of two-dimensional (2D) semiconductors. For systems in which states near the band extrema are of multiple orbitals character and the spinors describing the orbital components (pseudospins) pick up nonzero winding numbers (topological invariants) around the extremal k-point, the optical strength and nature (i.e., helicity) of the excitonic states are dictated by the optical matrix element winding number, a unique and heretofore unrecognized characteristic. We illustrate these findings in three gapped graphene systems - monolaye…
This paper applies analytical approximations for the luminescence of short period semiconductor superlattices and analyses the low density regime, demonstrating that the theory clearly connects with low density absorption with ratios of oscillator strengths of bound and continuum states as expected from the Elliott formula. A numerical study illustrates in detail the bleaching of higher order bound state. The analytical expressions have potential for systematic studies of controlled excitonic pathways characterized by THz responses.
Monolayer transition metal dichalcogenides feature tightly bound bright excitons at the degenerate valleys, where electron-hole Coulomb exchange interaction strongly couples the valley pseudospin to the momentum of exciton. Placed on periodically structured dielectric substrate, the spatial modulation of the Coulomb interaction leads to the formation of exciton Bloch states with real-space valley pseudospin texture displayed in a mesoscopic supercell. We find this spatial valley texture in the exciton Bloch function is pattern-locked to the propagation direction, enabling nano-optical excitati…
A microscopic approach is developed to compute the excitonic properties and the corresponding terahertz response for semiconductors characterized by anisotropic effective masses. The approach is illustrated for the example of germanium where it is shown that the anisotropic electron mass in the L-valley leads to two distinct terahertz absorption resonances separated by 0.8 meV.
Using polarization-resolved photoluminescence spectroscopy, we investigate valley degeneracy breaking by out-of-plane magnetic field in back-gated monolayer MoSe$_2$ devices. We observe a linear splitting of $-0.22 \frac{\text{meV}}{\text{T}}$ between luminescence peak energies in $σ_{+}$ and $σ_{-}$ emission for both neutral and charged excitons. The optical selection rules of monolayer MoSe$_2$ couple photon handedness to the exciton valley degree of freedom, so this splitting demonstrates valley degeneracy breaking. In addition, we find that the luminescence handedness can be controlled wit…
Preserving a high degree of valley polarization of excitons in photo-excited transition-metal dichalcogenide monolayers (TMD-MLs) is desirable for the valley-based photonic applications, but widely recognized as a hard task hindered by the intrinsic electron-hole exchange interaction. In this study, we present a comprehensive investigation of valley-polarized finite-momentum excitons in WSe$_2$-MLs over the entire Brillouin zone by solving the density-functional-theory(DFT)-based Bethe-Salpeter equation (BSE) under the guidance of symmetry analysis. We reveal that finite-momentum excitons are …
Heterobilayers consisting of MoSe$_2$ and WSe$_2$ monolayers can host optically bright interlayer excitons with intriguing properties such as ultralong lifetimes and pronounced circular polarization of their photoluminescence due to valley polarization, which can be induced by circularly polarized excitation or applied magnetic fields. Here, we report on the observation of an intrinsic valley-magnetophonon resonance for localized interlayer excitons promoted by invervalley hole scattering. It leads to a resonant increase of the photoluminescence polarization degree at the same field of 24.2 Te…
Indirect excitons (IX) in semiconductor heterostructures are bosons, which can cool below the temperature of quantum degeneracy and can be effectively controlled by voltage and light. IX quantum Bose gases and IX devices were explored in GaAs heterostructures where an IX range of existence is limited to low temperatures due to low IX binding energies. IXs in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by large binding energies giving the opportunity for exploring excitonic quantum gases and for creating excitonic devices at high temperatures. TMD hete…
We investigate with polarized microphotoluminescence the optical pumping of the valley degree of freedom in charge-tunable MoS2 monolayers encapsulated with hexagonal boron nitride at cryogenic temperatures. We report a large steady state valley polarization of the different excitonic complexes following circularly-polarized laser excitation 25 meV above the neutral exciton transition. For the first time in this material we reveal efficient valley pumping of positively-charged trions, which were so far elusive in non-encapsulated monolayers due to defect and laser-induced large electron doping…
Indirect excitons (IXs), also known as interlayer excitons, can form the medium for excitonic devices whose operation is based on controlled propagation of excitons. A proof of principle for excitonic devices was demonstrated in GaAs heterostructures where the operation of excitonic devices is limited to low temperatures. IXs in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by high binding energies making IXs robust at room temperature and offering an opportunity to create excitonic devices operating at high temperatures suitable for applications. Howev…
We investigate polarization properties of neutral exciton emission in single self-assembled InAs/GaAs quantum dots. The in-plane shape and strain anisotropy strongly couple the heavy and light hole states and lead to large optical anisotropy with non-orthogonal linearly polarized states misaligned with respect to the crystallographic axes. Owing to a waveguiding experimental configuration, luminescence polarization along the growth axis has been observed revealing the presence of shear components of the deformation tensor out of the growth plane. Resonant luminescence experiments allowed deter…
We report experimental evidences on selective occupation of the degenerate valleys in MoS2 monolayers by circularly polarized optical pumping. Over 30% valley polarization has been observed at K and K' valley via the polarization resolved luminescence spectra on pristine MoS2 monolayers. It demonstrates one viable way to generate and detect valley polarization towards the conceptual valleytronics applications with information carried by the valley index.
We observe a set of three replica luminescent peaks at ~21.4 meV below the dark exciton, negative and positive dark trions (or exciton-polarons) in monolayer WSe2. The replica redshift energy matches the energy of the zone-center E"-mode optical phonons. The phonon replicas exhibit parallel gate dependence and same g-factors as the dark excitonic states, but follow the valley selection rules of the bright excitonic states. While the dark states exhibit out-of-plane transition dipole and valley-independent linearly polarized emission in the in-plane directions, their phonon replicas exhibit in-…
The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects because they possess unique spin-valley locking physics for hosting rich excitonic species and the reduced screening for strong Coulomb interactions. Here, we report the observation of multiple valley phonons, phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone, and the resulting exciton complexes…
Monolayer transition metal dichalcogenides, known for exhibiting strong excitonic resonances, constitute a very interesting and versatile platform for investigation of light-matter interactions. In this work we report on a strong coupling regime between excitons in monolayer WSe2 and photons confined in an open, voltage-tunable dielectric microcavity. The tunability of our system allows us to extend the exciton-polariton state over a wide energy range and, in particular, to bring the excitonic component of the lower polariton mode into resonance with other excitonic transitions in monolayer WS…
Hexagonal boron nitride (hBN) is a wide band gap material with both strong excitonic light emission in the ultraviolet and strong exciton-phonon coupling. Luminescence experiments performed on the recently synthesized monolayer form (m-hBN) present emission spectra that differ from one another, with some suggesting a coexistence between phonon-assisted and direct emission channels. Motivated by these results, we investigated the optical response of (m-hBN) using a new \textit{ab initio} approach that takes into account the effects of atomic vibrations on the luminescence spectra. We construct …
High degree of valley polarization of optically active excitons in transition-metal dichalcogenide monolayers (TMD-MLs) is vital in valley-based photonic applications but known to be likely spoiled by the intrinsic electron-hole exchange interactions. In this study, we present a theoretical investigation of the valley and optical properties of finite-momentum dark excitons in WSe$_2$-MLs by solving the density-functional-theory(DFT)-based Bethe-Salpeter equation (BSE) under the guidance of symmetry analysis. %We reveal that, in general, finite-momentum excitons are actually well immune from th…
The optical properties of monolayer transition metal dichalcogenides are dominated by tightly-bound excitons. They form at distinct valleys in reciprocal space, and can interact via the valley-exchange coupling, modifying their dispersion considerably. Here, we predict that angle-resolved photoluminescence can be used to probe the changes of the excitonic dispersion. The exchange-coupling leads to a unique angle dependence of the emission intensity for both circularly and linearly-polarised light. We show that these emission characteristics can be strongly tuned by an external magnetic field d…
Optical selection rule fundamentally determines the optical transition between energy states in a variety of physical systems from hydrogen atoms to bulk crystals such as GaAs. It is important for optoelectronic applications such as lasers, energy-dispersive X-ray spectroscopy and quantum computation. Recently, single layer transition metal dichalcogenide (TMDC) exhibits valleys in momentum space with nontrivial Berry curvature and excitons with large binding energy. However, it is unclear how the unique valley degree of freedom combined with the strong excitonic effect influences the optical …
Local energy extrema of the bands in momentum space, or valleys, can endow electrons in solids with pseudo-spin in addition to real spin. In transition metal dichalcogenides this valley pseudo-spin, like real spin, is associated with a magnetic moment which underlies the valley-dependent circular dichroism that allows optical generation of valley polarization, intervalley quantum coherence, and the valley Hall effect. However, magnetic manipulation of valley pseudospin via this magnetic moment, analogous to what is possible with real spin, has not been shown before. Here we report observation …
The strong light-matter interaction in monolayer transition metal dichalcogenides (TMDs) is promising for nanoscale optoelectronics with their direct band gap nature and the ultra-fast radiative decay of the strongly bound excitons these materials host. However, the impeded amount of light absorption imposed by the ultra-thin nature of the monolayers impairs their viability in photonic applications. Using a layered heterostructure of a monolayer TMD stacked on top of strongly absorbing, non-luminescent, multi-layer SnSe2, we show that both single-photon and two-photon luminescence from the TMD…
We show that, because of the inevitable twist and lattice mismatch in heterobilayers of transition metal dichalcogenides, interlayer excitons have six-fold degenerate light cones anomalously located at finite velocities on the parabolic energy dispersion. The photon emissions at each light cone are elliptically polarized, with major axis locked to the direction of exciton velocity, and helicity specified by the valley indices of the electron and the hole. These finite-velocity light cones allow unprecedented possibilities to optically inject valley polarization and valley current, and the obse…
Single-photon emitters play a key role in present and emerging quantum technologies. Several recent measurements have established monolayer WSe$_2$ as a promising candidate for a reliable single photon source. The origin and underlying microscopic processes have remained, however, largely elusive. We present a multi-scale tight-binding simulation for the optical spectra of WSe$_2$ under non-uniform strain and in the presence of point defects employing the Bethe-Salpeter equation. Strain locally shifts excitonic energy levels into the band gap where they overlap with localized intra-gap defect …
Excitons and trions (or exciton-polarons) in transition metal dichalcogenides (TMDs) are known to decay predominantly through intravalley transitions. Electron-hole recombination across different valleys can also play a significant role in the excitonic dynamics, but intervalley transitions are rarely observed in monolayer TMDs, because they violate the conservation of momentum. Here we reveal the intervalley recombination of dark excitons and trions through more than one path in monolayer WSe$_2$. We observe the intervalley dark excitons, which can recombine by the assistance of defect scatte…
We report experimental observation of 2s exciton radiative emission from monolayer tungsten diselenide, enabled by hexagonal boron nitride protected high-quality samples. The 2s luminescence is highly robust and persists up to 150K, offering a new quantum entity for manipulating the valley degree of freedom. Remarkably, the 2s exciton displays superior valley polarization and coherence than 1s under similar experimental conditions. This observation provides evidence that the Coulomb-exchange-interaction-driven valley-depolarization process, the Maialle-Silva-Sham mechanism, plays an important …
Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. While WS2 and WSe2 are known for their excellent valley polarization due to the strong spin-orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS2xSe2(1-x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN en…
We examine the full static non-linear optical response of uniaxially strained transition metal dichalcogenide monolayers doped with a finite carrier density in the conduction band, in the presence of disorder. We find that the customary shift current is suppressed, yet we identify a strong, valley-dependent non-reciprocal response, which we term a \textit{unidirectional valley-contrasting photo-current} (UVCP). This DC current originates from the combined effect of strain and Kramers symmetry breaking by trigonal warping, while the contributions due to individual valleys can be separated by in…
The effect of 30 keV Ga^+ ion beam irradiation on the low-temperature photoluminescence from a single crystal of the hybrid organic-inorganic perovskite MAPbBr3 is presented for the first time. The irradiation leads to the suppression of the crystal's excitonic luminescence starting from the dose of 10^14/cm2. However, its integral luminescence does not drop up to the doses of two orders of magnitude higher. Further increase of the irradiation dose starts to affect the integral luminescence and causes the crystal to sputter. The spatial resolution of modification by the ion beam found in the e…
Two graphene monolayers that are oppositely charged and placed close to each other are considered. Taking into account valley and spin degeneracy of electrons we analyze the symmetry of the excitonic insulator states in such a system and build a phase diagram that takes into account the effect of the symmetry breaking due to the external in-plane magnetic field and the carrier density imbalance between the layers.
The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (> 6 $μ$s) and…
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
