Transition metal dichalcogenides (TMDs) are layered materials that have a semiconducting phase with many advantageous optoelectronic properties, including tightly bound excitons and spin-valley locking. In Tungsten-based TMDs, spin and momentum forbidden transitions give rise to dark excitons that typically are optically inaccessible but represent the lowest excitonic states of the system. Dark excitons can deeply affect transport, dynamics and coherence of bright excitons, hampering device performance. Therefore, it is crucial to create conditions in which these excitonic states can be visualized and controlled. Here, we show that compressive strain in WS2 enables phonon scattering of photoexcited electrons between momentum valleys, enhancing the formation of dark intervalley excitons. We show that the emission and spectral properties of momentum-forbidden excitons are accessible and strongly depend on the local strain environment that modifies the band alignment. This mechanism is further exploited for strain sensing in two-dimensional semiconductors revealing a gauge factor exceeding 10^4.
The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observ…
We study theoretically the exciton Bose-Einstein condensation and exciton vortices in a two-dimensional (2D) perovskite (PEA)2PbI4 monolayer. Combining the first-principles calculations and the Keldysh model, the exciton binding energy of (PEA)2PbI4 in a monolayer can approach hundreds meV, which make it possible to observe the excitonic effect at room temperature. Due to the large exciton binding energy, and hence the high density of excitons, we find that the critical temperature of the exciton condensation could approach the liquid nitrogen regime. In presence of perpendicular electric fiel…
We present low temperature magneto-photoluminescence experiments which demonstrate the brightening of dark excitons by an in-plane magnetic field $B$ applied to monolayers of different semiconducting transition metal dichalcogenides. For both WSe$_2$ and WS$_2$ monolayers, the dark exciton emission is observed at $\sim$50 meV below the bright exciton peak and displays a characteristic doublet structure which intensity is growing with $B^2$, while no magnetic field induced emission peaks appear for MoSe$_2$ monolayer. Our experiments also show that the MoS$_2$ monolayer has a dark exciton groun…
The optical properties of monolayer transition metal dichalcogenides (TMDC) feature prominent excitonic natures. Here we report an experimental approach toward measuring the exciton binding energy of monolayer WS2 with linear differential transmission spectroscopy and two-photon photoluminescence excitation spectroscopy (TP-PLE). TP-PLE measurements show the exciton binding energy of 0.71eV around K valley in the Brillouin zone. The trion binding energy of 34meV, two-photon absorption cross section 4X10^{4}cm^{2}W^{-2}S^{-1} at 780nm and exciton-exciton annihilation rate around 0.5cm^{2}/s are…
We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the non-monotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula whic…
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…
The valley pseudospin in monolayer transition metal dichalcogenides (TMDs) has been proposed as a new way to manipulate information in various optoelectronic devices. This relies on a large valley polarization that remains stable over long timescales (hundreds of ns). However, time resolved measurements report valley lifetimes of only a few ps. This has been attributed to mechanisms such as phonon-mediated inter-valley scattering and a precession of the valley psedospin through electron-hole exchange. Here we use transient spin grating to directly measure the valley depolarization lifetime in …
The ultrathin transition metal dichalcogenides (TMDs) have emerged as promising materials for various applications using two dimensional (2D) semiconductors. They have attracted increasing attention due to their unique optical properties originate from neutral and charged excitons. Here, we report negatively charged exciton formation in monolayer TMDs, notably tungsten disulfide WS2. Our theory is based on an effective mass model of neutral and charged excitons, parameterized by ab-initio calculations. Taking into the account the strong correlation between the monolayer WS2 and the surrounding…
In heterostructures consisting of different transition-metal dichalcogenide monolayers, a staggered band alignment can occur, leading to rapid charge separation of optically generated electron-hole pairs into opposite monolayers. These spatially separated electron-hole pairs are Coulomb-coupled and form interlayer excitons. Here, we study these interlayer excitons in a heterostructure consisting of MoSe$_2$ and WSe$_2$ monolayers using photoluminescence spectroscopy. We observe a non-trivial temperature dependence of the linewidth and the peak energy of the interlayer exciton, including an unu…
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 …
We study the interface exciton at lateral type II heterojunctions of monolayer transition metal dichalcogenides (TMDs), where the electron and hole prefer to stay at complementary sides of the junction. We find that the 1D interface exciton has giant binding energy in the same order as 2D excitons in pristine monolayer TMDs although the effective radius (electron-hole seperation) of interface exciton is much larger than that of 2D excitons. The binding energy, exciton radius and optical dipole strongly depends on the band offset at the junction. The inter-valley coupling induced by the electro…
By pumping nonresonantly a MoS$_2$ monolayer at $13$ K under a circularly polarized cw laser, we observe exciton energy redshifts that break the degeneracy between B excitons with opposite spin. The energy splitting increases monotonically with the laser power reaching as much as $18$ meV, while it diminishes with the temperature. The phenomenon can be explained theoretically by considering simultaneously the bandgap renormalization which gives rise to the redshift and exciton-exciton Coulomb exchange interaction which is responsible for the spin-dependent splitting. Our results offer a simple…
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…
Exciton spectra of monolayer transition metal dichalcogenides (TMDs) in various dielectric environments are studied. The screened hydrogen model (SHM) [Phys. Rev. Lett. 116, 056401 (2016)] is examined by comparing its exciton spectra with the radial equation (RE) solutions. While the SHM is found to describe the nonhydrogenic exciton Rydberg series reasonably well, it fails to account for the linear decrease of the exciton energy with the orbital quantum number $m$. The exciton Bohr orbit shrinks as $\lvert m\rvert$ becomes larger resulting in increased strength of the electron-hole interactio…
We address the problem of free carrier screening of exciton states in two-dimensional monolayer semiconductors. Basic theoretical considerations are presented concerning the applicability of the commonly used static approximation of the screening effect and the implications are discussed. We show that the low-frequency models lead to a major overestimation of the free carrier response and are inadequate to describe the screening of strongly bound excitons in monolayer materials. The presented arguments are consistent with existing high-level many-body theories and transparently illustrate the …
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…
The optical spectra of transition metal dichalcogenide (TMDC) monolayers are dominated by excitons and trions. Here we establish the dependences of these optical transitions on disorder from hyperspectral imaging of h-BN encapsulated monolayer MoSe2. While both exciton and trion energies vary spatially, these two quantities are almost perfectly correlated, with spatial variation in the trion binding energy of only ~0.18 meV. In contrast, variation in the energy splitting between the two lowest energy exciton states is one order of magnitude larger at ~1.7 meV. Statistical analysis and theoreti…
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…
We predict a phase transition in freestanding monolayer Xenes from the semiconducting phase to the excitonic insulating (EI) phase can be induced by reducing an external electric field below some critical value which is unique to each material. The splitting of the conduction and valence bands due to spin-orbit coupling at non-zero electric fields leads to the formation of $A$ and $B$ excitons in the larger or smaller band gap, with correspondingly larger or smaller binding energies. Our calculations show the coexistence of the semiconducting phase of $A$ excitons with the EI phase of $B$ exci…
The strong Coulomb forces in monolayer transition metal dichalcogenides ensure that optical excitation of band electrons gives rise to Wannier-Mott excitonic states, each of which can be conceptualized as a composite of a Gaussian wavepacket corresponding to center-of-mass motion and an orbital state corresponding to the motion of the electron and hole about the center-of-mass. Here, we show that at low temperature in monolayer MoS2, given quasi-localized excitons and consequently a significant inter-exciton spacing, the excitons undergo dipole-dipole interaction and annihilate one another in …
We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to inter-par…
We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number =2. The dependences of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength are numerically revealed. The chiral topological valley excitons are no…
We demonstrate robust power- and wavelength-dependent optical bistability in fully suspended monolayers of WSe2 near the exciton resonance. Bistability has been achieved under continuous-wave optical excitation at an intensity level of 10^3 W/cm^2. The observed bistability is originated from a photo-thermal mechanism, which provides both optical nonlinearity and passive feedback, two essential elements for optical bistability. Under a finite magnetic field, the exciton bistability becomes helicity dependent, which enables repeatable switching of light purely by its polarization.
We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of mono- layer MoS2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second harmonic generation in monolayer MoS2, and find that the third- harmonic process is efficient only for linearly polarized input light while the third-order two photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton…
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…
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 …
Monolayer transition-metal dichalcogenides (TMDCs) have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. In these semiconducting materials, optically excited electron-hole pairs form tightly Coulomb-bound excitons with large binding energies. The selection rules for excitonic transitions allow for direct optical generation of a valley-polarized exciton population using resonant excitation. Here, we investigate the exciton valley dynamics in monolayers of three different TMDCs …
Excitons, quasi particles composed of an electron and a hole, play an important role in optical responses in low-dimensional nanostructures. In this work, we have investigated exciton diffusion in a monolayer MoSe2 encapsulated between flakes of hexagonal boron nitrides (hBN/MoSe2/hBN). Through PL imaging and numerical solving the 2D diffusion equation, we revealed that temperature dependence of exciton mobility in the hBN/MoSe2/hBN shows non-saturating increase at low temperature, which is qualitatively different from those of quantum wells composed of compound semiconductors. Ultraflat struc…
We address the properties of excitons in monolayer MoS$_2$ from a theoretical point of view, showing that low-energy excitonic states occur both at the Brillouin zone center and at the Brillouin-zone corners, that binding energies at the Brillouin-zone center deviate strongly from the $(n-1/2)^{-2}$ pattern of the two-dimensional hydrogenic model, and that the valley-degenerate exciton doublet at the Brillouin-zone center splits at finite momentum into an upper mode with non-analytic linear dispersion and a lower mode with quadratic dispersion. Although monolayer MoS$_2$ is a direct-gap semico…
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 …
Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quantifying the fundamental properties of the exciton. A key parameter is the intrinsic exciton homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath…
We show that excitons and free carriers in K and K' valleys of transition metal dichalcogenide monolayers can be entangled with respect to their valley degree of freedom by absorbing linearly polarized single photons. This effect does not require any interaction between K and K' excitons in contrast to conventional mechanisms of entanglement that are mediated by coupling between quantum systems (e.g.~entanglement of photons in nonlinear optical interactions). The valley entanglement of excitons and free carriers can be verified by measuring the polarization of their photoluminescence or fluctu…
Monolayers of semiconducting transition metal dichalcogenides (TMDCs) with unique spin-valley contrasting properties and remarkably strong excitonic effects continue to be a subject of intense research interests. These model 2D semiconductors feature two fundamental intravalley excitons species - optically accessible ' bright' excitons with anti-parallel spins and optically inactive 'dark' excitons with parallel spins. For applications exploiting radiative recombination of bright excitons or long lifetime dark excitons, it is essential to understand the radiative character of the exciton groun…
We directly monitor exciton propagation in freestanding and SiO2-supported WS2 monolayers through spatially- and time-resolved micro-photoluminescence under ambient conditions. We find highly nonlinear behavior with characteristic, qualitative changes in the spatial profiles of the exciton emission and an effective diffusion coefficient increasing from 0.3 to more than 30 cm2/s, depending on the injected exciton density. Solving the diffusion equation while accounting for Auger recombination allows us to identify and quantitatively understand the main origin of the increase in the observed dif…
We theoretically investigate the corrections of exciton binding energy in monolayer transition metal dichalcogenides (TMDs) due to the exciton-optical phonon coupling in the Fr$\ddot{o}$hlich interaction model by using the linear operator combined Lee-Low-Pines variational method. We not only consider the excitons couple with the intrinsic longitudinal optical (LO) phonon modes, but also the surface optical phonon modes that induced by the polar substrates underneath the TMDs. We find that exciton binding energies are corrected in a large scale due to these exciton-optical phonon couplings. We…
Transition metal dichalcogenide (TMD) monolayers are two-dimensional semiconductors with two valleys in their band structure that can be selectively addressed using circularly polarized light. Their photoluminescence spectrum is characterized by neutral and charged excitons (trions) that form a chemical equilibrium governed by the net charge density. Here, we use chemical doping to drive the conversion of excitons into trions in $\text{WS}_{2}$ monolayers at room temperature, and study the resulting valley polarization via photoluminescence measurements under valley-selective optical excitatio…
We have experimentally studied the pump-probe Kerr rotation dynamics in WSe$_2$ monolayers. This yields a direct measurement of the exciton valley depolarization time $τ_v$. At T=4K, we find $τ_v\approx 6$ps, a fast relaxation time resulting from the strong electron-hole Coulomb exchange interaction in bright excitons. The exciton valley depolarization time decreases significantly when the lattice temperature increases with $τ_v$ being as short as 1.5ps at 125K. The temperature dependence is well explained by the developed theory taking into account the exchange interaction and a fast exciton …
The excitonic spectra of single layer GeS and GeSe are predicted by ab initio GW-Bethe Salpeter equation calculations. G 0 W 0 calculations for the band structures find a fundamental band gap of 2.85 eV for GeS and 1.70 eV for GeSe monolayer. However, excitons are tightly bound, specially in GeS at the Γ point, where the quasi-particle interactions are so strong that they shift the Γ exciton peak energy into the visible range and below the off-Γ exciton peak. The lowest energy excitons in both materials are excited by light along the zigzag direction and have exciton binding energies of 1.05 e…
Tungsten-based monolayer transition metal dichalcogenides host a long-lived dark exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located be…
We study spatial photoluminescence characteristics of neutral and charged excitons across extended monolayer MoS$_2$ synthesized by chemical vapor deposition. Using two-dimensional hyperspectral photoluminescence mapping at cryogenic temperatures we identify regions with increased emission from charged excitons associated with both spin-orbit split valence subbands. Such regions are attributed to unintentional doping at defect sites with excess charge that bind neutral excitons to form defect-pinned trions. Our findings imply comparable timescales for the formation, relaxation, and radiative d…
We study the neutral exciton energy spectrum fine structure and its spin dephasing in transition metal dichalcogenides such as MoS$_2$. The interaction of the mechanical exciton with its macroscopic longitudinal electric field is taken into account. The splitting between the longitudinal and transverse excitons is calculated by means of the both electrodynamical approach and $\mathbf k \cdot \mathbf p$ perturbation theory. This long-range exciton exchange interaction can induce valley polarization decay. The estimated exciton spin dephasing time is in the picosecond range, in agreement with av…
Scientific curiosity to uncover original optical properties and functionalities of atomically thin semiconductors, stemming from unusual Coulomb interactions in the two-dimensional geometry and multi-valley band structure, drives the research on monolayers of transition metal dichalcogenides (TMDs). While recent works ascertained the exotic energetic schemes of exciton complexes in TMDs, we here employ four-wave mixing microscopy to indicate that their subpicosecond dynamics is determined by the surrounding disorder. Focusing on a monolayer WS$_2$, we observe that exciton coherence is lost pri…
The direct gap interband transitions in transition metal dichalcogenides monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the $K^+$ or $K^-$ valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here we demonstrate the control of the exciton valley coherence in monolayer WSe2 by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30 degrees in appli…
The effect of a magnetic field on the optical absorption in semiconductors has been measured experimentally and modeled theoretically for various systems in previous decades. We present a new first-principles approach to systematically determine the response of excitons to magnetic fields, i.e. exciton $g$ factors. By utilizing the $GW$-Bethe-Salpeter equation methodology we show that $g$ factors extracted from the Zeeman shift of electronic bands are strongly renormalized by many-body effects which we trace back to the extent of the excitons in reciprocal space. We apply our approach to monol…
The exceptionally strong Coulomb interaction in semiconducting transition-metal dichalcogenides (TMDs) gives rise to a rich exciton landscape consisting of bright and dark exciton states. At elevated densities, excitons can interact through exciton-exciton annihilation (EEA), an Auger-like recombination process limiting the efficiency of optoelectronic applications. Although EEA is a well-known and particularly important process in atomically thin semiconductors determining exciton lifetimes and affecting transport at elevated densities, its microscopic origin has remained elusive. In this joi…
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.
Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 μeV and <0.2 μeV at low-temperature. These linewidths are more than three orders of magnitude narrower than the p…
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…
In monolayers of the semiconducting transition metal dichalcogenides, the electron-hole exchange interaction splits the exciton dispersion into a massive transverse branch, and a longitudinal branch that has very light or even zero mass depending on the form of screened Coulomb interaction. The group velocity of the longitudinal branch is sensitive to the strength of electron-hole exchange, which can be engineered through the dielectric environment. Here we show that dielectric patterning of the substrate can be exploited to realize waveguide of the exciton in the longitudinal branch in a homo…
The interaction between off-resonant laser pulses and excitons in monolayer transition metal dichalcogenides is attracting increasing interest as a route for the valley-selective coherent control of the exciton properties. Here, we extend the classification of the known off-resonant phenomena by unveiling the impact of a strong THz field on the excitonic resonances of monolayer MoS$_2$. We observe that the THz pump pulse causes a selective modification of the coherence lifetime of the excitons, while keeping their oscillator strength and peak energy unchanged. We rationalize these results theo…
In monolayer transition metal dichalcogenides, tightly bound excitons have been discovered with a valley pseudospin that can be optically addressed through polarization selection rules. Here, we show that this valley pseudospin is strongly coupled to the exciton center-of-mass motion through electron-hole exchange. This coupling realizes a massless Dirac cone with chirality index I=2 for excitons inside the light cone, i.e. bright excitons. Under moderate strain, the I=2 Dirac cone splits into two degenerate I=1 Dirac cones, and saddle points with a linear Dirac spectrum emerge in the bright e…
We experimentally demonstrate time-resolved exciton propagation in a monolayer semiconductor at cryogenic temperatures. Monitoring phonon-assisted recombination of dark states, we find a highly unusual case of exciton diffusion. While at 5 K the diffusivity is intrinsically limited by acoustic phonon scattering, we observe a pronounced decrease of the diffusion coefficient with increasing temperature, far below the activation threshold of higher-energy phonon modes. This behavior corresponds neither to well-known regimes of semiclassical free-particle transport nor to the thermally activated h…
The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant timescales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons a…
The recent accessibility of high quality, charge neutral monolayer transition metal dichalcogenides with narrow exciton linewidths at the homogeneous limit provides an ideal platform to study excitonic many-body interactions. In particular, the possibility to manipulate coherent exciton-exciton interactions, which govern the ultrafast nonlinear optical response, by applying an external magnetic field has not been considered so far. We address this discrepancy by presenting a nonlinear microscopic theory in the coherent limit for optical excitations in the presence of out-of-plane, in-plane, an…
A four-band exciton Hamiltonian is constructed starting from the single-particle Dirac Hamiltonian for charge carriers in monolayer transition metal dichalcogenides (TMDs). The angular part of the exciton wave function can be separated from the radial part, in the case of zero center of mass momentum excitons, by exploiting the eigenstates of the total exciton angular momentum operator with which the Hamiltonian commutes. We explain why this approach fails for excitons with finite center of mass momentum or in the presence of a perpendicular magnetic field and present an approximation to resol…
The luminescence yield of transition metal dichalcogenide monolayers frequently suffers from the formation of long-lived dark states, which include excitons with intervalley charge carriers, spin-forbidden transitions, and a large center-of-mass momentum located outside the light cone of dispersion relations. Efficient relaxation from bright exciton states to dark states suppresses the quantum yield of photon emission. In addition, the radiative recombination of excitons is heavily influenced by Auger-type exciton-exciton scattering, which yields another nonradiative relaxation channel at room…
