Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population decay and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond. At present, however, a consensus on the microscopic mechanisms governing exciton radiative and non-radiative recombination is lacking. The strong exciton oscillator strength resulting in up to 20% absorption for a single monolayer points to ultrafast radiative recombination. However, the low quantum yield and large variance in the reported lifetimes suggest that non-radiative Auger-type processes obscure the intrinsic exciton radiative lifetime. In either case, the electron-hole exchange interaction plays an important role in the exciton spin and valley dynamics. In this article, we review the experiments and theory that have led to these conclusions and comment on future experiments that could complement our current understanding.
We examine the excitonic properties of layered configurations of low dimensional transition metal dichalcogenides (LTMDCs) using the fractional dimensional space approach. The binding energies of the exciton, trion and biexciton in LTMDCs of varying layers are analyzed, and linked to the dimensionality parameter $α$, which provides insight into critical electro-optical properties (relative oscillator strength, absorption spectrum, exciton-exciton interaction) of the material systems. The usefulness of $α$ is highlighted by its independence of the physical mechanisms underlying the confinement …
Optical properties of transition metal dichalcogenides monolayers are controlled by the Wannier-Mott excitons forming a series of $1s$, $2s$, $2p$,... hydrogen-like states. We develop the theory of the excited excitonic states energy spectrum fine structure. We predict that $p$- and $s$-shell excitons are mixed due to the specific $D_{3h}$ point symmetry of the transition metal dichalcogenide monolayers. Hence, both $s$- and $p$-shell excitons are active in both single- and two-photon processes providing an efficient mechanism of second harmonic generation. The corresponding contribution to th…
We report a photoluminescence (PL) and transient reflection spectroscopy study of exciton dynamics in monolayer transition transition-metal dichalcogenides (TMDs). PL saturation in monolayer MoSe2 occurs an excitation intensity more than two orders of magnitude lower than in monolayer MoS2. Transient reflection shows that the nonlinear exciton-exciton annihilation is the dominant exciton decay process in monolayer MoSe2 in contrast to the previously reported linear exciton decay in monolayer MoS2. In addition, the exciton lifetime in MoSe2, > 125 ps, is more than an order of magnitude longer t…
It is shown that the strong Coulomb coupling in intrinsic suspended semiconducting transition metal dichalcogenides can exceed the critical value needed for an excitonic ground state. The dipole-allowed optical excitations then correspond to intra-excitonic transitions such that the optically bright excitonic transitions near the Dirac points have a $p$-like symmetry whereas the $s$-like states are dipole forbidden. The large intrinsic coupling strength seems to be a generic property of the semiconducting transition metal dichalcogenides and strong Coulomb-coupling signatures in the form of th…
We present results on the radiative lifetimes of excitons and trions in a monolayer of metal dichalcogenide MoS2. The small exciton radius and the large exciton optical oscillator strength result in radiative lifetimes in the 0.18-0.30 ps range for excitons that have small in-plane momenta and couple to radiation. Average lifetimes of thermally distributed excitons depend linearly on the exciton temperature and can be in the few picoseconds range at small temperatures and more than a nanosecond near room temperature. Localized excitons exhibit lifetimes in the same range and the lifetime incre…
Due to a strong Coulomb interaction, excitons dominate the excitation kinetics in 2D materials. While Coulomb-scattering between electrons has been well studied, the interaction of excitons is more challenging and remains to be explored. As neutral composite bosons consisting of electrons and holes, excitons show a non-trivial scattering dynamics. Here, we study on microscopic footing exciton-exciton interaction in transition-metal dichalcogenides and related van der Waals heterostructures. We demonstrate that the crucial criterion for efficient scattering is a large electron/hole mass asymmet…
The magneto-optical response of monolayer transition metal dichalcogenides (TMDs), including excitonic effects, is studied using a nanoribbon geometry. We compute the diagonal optical conductivity and the Hall conductivity. Comparing the excitonic optical Hall conductivity to results obtained in the independent particle approximation, we find an increase in the amplitude corresponding to one order of magnitude when excitonic effects are included. The Hall conductivities are used to calculate Faraday rotation spectra for MoS2 and WSe2. Finally, we have also calculated the diamagnetic shift of t…
Monolayer transition metal dichalcogenides (TMDs) have been in focus of current research, among others due to their remarkable exciton landscape consisting of bright and dark excitonic states. Although dark excitons are not directly visible in optical spectra, they have a large impact on exciton dynamics and hence their understanding is crucial for potential TMD-based applications. Here, we study brightening mechanisms of dark excitons via interaction with phonons and in-plane magnetic fields. We show clear signatures of momentum- and spin-dark excitons in WS$_2$, WSe$_2$ and MoS$_2$, while th…
We examine a mechanism by which excitons undergo ultrafast relaxation in common monolayer transition metal dichalcogenides. It is shown that at densities $\approx$ 1$\times$ 10$^{11}$ cm$^{-2}$ and temperatures $ \le 60$ K, excitons in well known monolayers (MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$) exist as point-like structureless electron-hole quasi-particles. We evaluate the average rate of exciton energy relaxation due to acoustic phonons via the deformation potential and the piezoelectric coupling mechanisms and examine the effect of spreading of the excitonic wavefunction into the region p…
Odd-angular momentum exciton states are dark to light in monolayers of transition-metal dichalcogenides and can be addressed only by two-photon probes. Besides, $2p$ excitons states are expected to show a fine splitting that arises from the peculiar electronic band structure of the material, characterized by a finite Berry curvature around each valley. In this work we study in detail the coupling of photons to $p$ exciton states and we find that the Rashba spin-orbit interaction or a Skyrmion in the transition-metal dichalcogenide substrate can be exploited to engineer finite optical selection…
The multivalley band structure of monolayer transition metal dichalcogenides (TMDs) gives rise to intravalley and intervalley excitons. Much knowledge of these excitons has been gained, but fundamental questions remain, such as how to describe them all in a unified picture with their correlations, how are those from different valleys coupled to form the intervalley biexciton? To address the issues, we derive an exciton Hamiltonian from interpair correlations between the constituent carriers-fermions of two excitons. Identifying excitons by irreducible representations of their point symmetry gr…
We investigate the spin-nonconserving relaxation channel of excitons by their couplings with phonons in two-dimensional transition metal dichalcogenides using $\textit{ab initio}$ approaches. Combining $\text{GW}$-Bethe-Salpeter equation method and density functional perturbation theory, we calculate the electron-phonon and exciton-phonon coupling matrix elements for the spin-flip scattering in monolayer WSe$_{\text{2}}$, and further analyze the microscopic mechanisms influencing these scattering strengths. We find that phonons could produce effective in-plane magnetic fields which flip spin o…
The intricate interplay between optically dark and bright excitons governs the light-matter interaction in transition metal dichalcogenide monolayers. We have performed a detailed investigation of the "spin-forbidden" dark excitons in WSe2 monolayers by optical spectroscopy in an out-of-plane magnetic field Bz. In agreement with the theoretical predictions deduced from group theory analysis, magneto-photoluminescence experiments reveal a zero field splitting $δ=0.6 \pm 0.1$ meV between two dark exciton states. The low energy state being strictly dipole forbidden (perfectly dark) at Bz=0 while …
In this paper, starting from a quantum master equation, we discuss the interaction between two negatively charged Nitrogen-vacancy color centers in diamond via exciton-polaritons propagating in a two-dimensional transition metal dichalcogenide layer in close proximity to a diamond crystal. We focus on the optical 1.945 eV transition and model the Nitrogen-vacancy color centers as two-level (artificial) atoms. We find that the interaction parameters and the energy levels renormalization constants are extremely sensitive to the distance of the Nitrogen-vacancy centers to the transition metal dic…
The photoluminescence (PL) spectrum of transition metal dichalcogenides (TMDs) shows a multitude of emission peaks below the bright exciton line and not all of them have been explained yet. Here, we study the emission traces of phonon-assisted recombinations of momentum-dark excitons. To this end, we develop a microscopic theory describing simultaneous exciton, phonon and photon interaction and including consistent many-particle dephasing. We explain the drastically different PL below the bright exciton in tungsten- and molybdenum-based materials as result of different configurations of bright…
In bilayers of semiconducting transition metal dichalcogenides, the twist angle between layers can be used to introduce a highly regular periodic potential modulation on a length scale that is large compared to the unit cell. In such structures, correlated states can emerge, in which excitons in the heterostructure are strongly localized to the potential minima due to exciton-exciton interactions. We explore the transition between Mott and extended exciton phases in terms of a moiré-Bose-Hubbard Hamiltonian. Hopping and on-site interaction parameters are obtained from a Wannier representation …
Electron valleys in transition-metal dichalcogenide monolayers drive novel physics and allow designing multifunctional architectures for applications. We propose to manipulate the electron valleys in these systems for spin/valley filter and valve devices through band engineering. Instead of the magnetic proximity effect that has been extensively used in previous studies, in our strategy, the electron valleys are directly coupled to the spin-polarized states of the two-dimensional ferromagnets. We find that this coupling results in a valley-selective gap opening due to the spin-momentum locking…
The optical properties of transition metal dichalcogenide monolayers such as the two-dimensional semiconductors MoS$_2$ and WSe$_2$ are dominated by excitons, Coulomb bound electron-hole pairs. The light emission yield depends on whether the electron-hole transitions are optically allowed (bright) or forbidden (dark). By solving the Bethe Salpeter Equation on top of $GW$ wave functions in density functional theory calculations, we determine the sign and amplitude of the splitting between bright and dark exciton states. We evaluate the influence of the spin-orbit coupling on the optical spectra…
Strain in two-dimensional (2D) transition metal dichalcogenide (TMD) has led to localized states with exciting optical properties, in particular in view of designing one photon sources. The naturally formed of the MoS2 monolayer deposed on hBN substrate leads to a reduction of the bandgap in the strained region creating a nanobubble. The photogenerated particles are thus confined in the strain-induced potential. Using numerical diagonalization, we simulate the spectra of the confined exciton states, their oscillator strengths and radiative lifetimes. We show that a single state of the confined…
We present a theory that elucidates the major momentum and spin relaxation processes for electrons, holes and hot excitons in monolayer transition-metal dichalcogenides. We expand on spin flips induced by flexural phonons and show that the spin relaxation is ultrafast for electrons in free-standing membranes while being mitigated in supported membranes. This behavior due to interaction with flexural phonons is universal in two-dimensional membranes that respect mirror symmetry and it leads to a counterintuitive inverse relation between mobility and spin relaxation.
Excitons, composite electron-hole quasiparticles, are known to play an important role in optoelectronic phenomena in many semiconducting materials. Recent experiments and theory indicate that the band-gap optics of the newly discovered monolayer transition-metal dichalcogenides (TMDs) is dominated by tightly bound valley excitons. The strong interaction of excitons with long-range electromagnetic fields in these 2D systems can significantly affect their intrinsic properties. Here, we develop a semi-classical framework for intrinsic exciton-polaritons in monolayer TMDs that treats their dispers…
We measure the optical absorption spectra and optical conductivities of excitons and trions in monolayers of metal dichalcogenide MoS$_{2}$ and compare the results with theoretical models. Our results show that the Wannier-Mott model for excitons, with modifications to account for small exciton radii and large exciton relative wavefunction spread in momentum space, phase space blocking due to Pauli exclusion in doped materials, and wavevector dependent dielectric constant, gives results that agree well with experiments. The measured exciton optical absorption spectra are used to obtain experim…
Second-harmonic generation (SHG) is a well-known nonlinear spectroscopy method to probe electronic structure, specifically, in transition metal dichalcogenide (TMDC) monolayers. This work investigates the nonlinear dynamics of a strongly excited TMDC monolayer by solving the time evolution equations for the density matrix. It is shown that the presence of excitons qualitatively changes the nonlinear dynamics leading, in particular, to a huge enhancement of the nonlinear signal as a function of the dielectric environment. It is also shown that the SHG polarization angular diagram and its depend…
Generation of photocurrents in semiconducting materials requires dissociation of excitons into free charge carriers. While thermal agitation is sufficient to induce dissociation in most bulk materials, an additional push is required to induce efficient dissociation of the strongly bound excitons in monolayer transition-metal dichalcogenides (TMDs). Recently, static in-plane electric fields have proven to be a promising candidate. In the present paper, we introduce a numerical procedure, based on exterior complex scaling, capable of computing field-induced exciton dissociation rates for a wider…
We analyze the dielectric-function spectra of low dimensional transition metal dichalcogenides (TMDCs) using a fully analytical model of the complex dielectric function that is applicable in fractional dimensional space. We extract the dimensionalities of the $A$ and $B$ excitons as well as their Lorentzian broadening widths by fitting the model to experimental data in the spectral range of photon energies (1.5 - 3 eV). Our results show the significant contribution of the lowest ground exciton state to the dielectric properties of exemplary monolayer materials (MoS$_2$, MoSe$_2$ and WSe$_2$). …
In this paper we develop a fully microscopic theory of the polarizability of excitons in transition metal dichalcogenides. We apply our method to the description of the excitation $2$p dark states. These states are not observable in absorption experiments but can be excited in a pump-probe experiment. As an example we consider $2$p dark states in WSe\textsubscript{2}. We find a good agreement between recent experimental measurements and our theoretical calculations.
It is shown that the three-fold rotational symmetry in transition metal dichalcogenides leads to a Coulomb induced renormalization of the effective electron and hole masses near the $K$-points of the Brillouin zone. The magnitude of the renormalization depends on the dielectric configuration. The effective exciton mass $m=0.4 m_0$ of a freely suspended MoS$_2$ monolayer changes to $m= 0.35 m_0$ with hBN encapsulation. The mass renormalization increases the excitonic binding energy and reduces the exciton diamagnetic shift and cyclotron frequency. Detailed comparisons with high field measuremen…
Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such d…
The polarization analysis of optical transitions in monolayer and bilayer transition-metal dichalcogenides provides invaluable information on the spin and valley (pseudospin) degrees of freedom. To explain optical properties of a given monolayer transition-metal dichalcogenide, one should consider (i) the order of its spin-split conduction bands, (ii) whether intervalley scattering is prone to phonon bottleneck, (iii) and whether valley mixing by electron-hole exchange can take place. Using these principles, we present a consistent physical picture that elucidates a variety of features in the …
The valley degree of freedom is a sought-after quantum number in monolayer transition-metal dichalcogenides. Similar to optical spin orientation in semiconductors, the helicity of absorbed photons can be relayed to the valley (pseudospin) quantum number of photoexcited electrons and holes. Also similar to the quantum-mechanical spin, the valley quantum number is not a conserved quantity. Valley depolarization of excitons in monolayer transition-metal dichalcogenides due to long-range electron-hole exchange typically takes a few ps at low temperatures. Exceptions to this behavior are monolayers…
Recently, the celebrated Keldysh potential has been widely used to describe the Coulomb interaction of few-body complexes in monolayer transition-metal dichalcogenides. Using this potential to model charged excitons (trions), one finds a strong dependence of the binding energy on whether the monolayer is suspended in air, supported on SiO$_2$, or encapsulated in hexagonal boron-nitride. However, empirical values of the trion binding energies show weak dependence on the monolayer configuration. This deficiency indicates that the description of the Coulomb potential is still lacking in this impo…
Just as photons are the quanta of light, plasmons are the quanta of orchestrated charge-density oscillations in conducting media. Plasmon phenomena in normal metals, superconductors and doped semiconductors are often driven by long-wavelength Coulomb interactions. However, in crystals whose Fermi surface is comprised of disconnected pockets in the Brillouin zone, collective electron excitations can also attain a shortwave component when electrons transition between these pockets. Here, we show that the band structure of monolayer transition-metal dichalcogenides gives rise to an intriguing mec…
We describe recent experimental efforts to perform polarization-resolved optical spectroscopy of monolayer transition-metal dichalcogenide semiconductors in very large pulsed magnetic fields to 65 tesla. The experimental setup and technical challenges are discussed in detail, and temperature-dependent magneto-reflection spectra from atomically thin tungsten disulphide (WS$_2$) are presented. The data clearly reveal not only the valley Zeeman effect in these 2D semiconductors, but also the small quadratic exciton diamagnetic shift from which the very small exciton size can be directly inferred.…
We study theoretically effects of an anisotropic elastic strain on the exciton energy spectrum fine structure and optical selection rules in atom-thin crystals based on transition-metal dichalcogenides. The presence of strain breaks the chiral selection rules at the $\bm K$-points of the Brillouin zone and makes optical transitions linearly polarized. The orientation of the induced linear polarization is related to the main axes of the strain tensor. Elastic strain provides an additive contribution to the exciton fine structure splitting in agreement with experimental evidence obtained from un…
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…
Using an equation of motion (EOM) approach, we calculate excitonic properties of monolayer transition metal dichalcogenides (TMDs) perturbed by an external magnetic field. We compare our findings to the widely used Wannier model for excitons in two-dimensional materials and to recent experimental results. We find good agreement between the calculated excitonic transition energies and the experimental results. In addition, we find that the exciton energies calculated using the EOM approach are slightly lower than the ones calculated using the Wannier model. Finally, we also show that the effect…
We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a …
We theoretically predict that vanadium-based Janus dichalcogenide monolayers constitute an ideal platform for spin-orbit-torque memories. Using first principles calculations, we demonstrate that magnetic exchange and magnetic anisotropy energies are higher for heavier chalcogen atoms, while the broken inversion symmetry in the Janus form leads to the emergence of Rashba-like spin-orbit coupling. The spin-orbit torque efficiency is evaluated using optimized quantum transport methodology and found to be comparable to heavy nonmagnetic metals. The coexistence of magnetism and spin-orbit coupling …
A self-consistent scheme for the calculations of the interacting groundstate and the near bandgap optical spectra of mono- and multilayer transition-metal-dichalcogenide systems is presented. The approach combines a dielectric model for the Coulomb interaction potential in a multilayer environment, gap equations for the renormalized groundstate, and the Dirac-Wannier-equation to determine the excitonic properties. To account for the extension of the individual monolayers perpendicular to their basic plane, an effective thickness parameter in the Coulomb interaction potential is introduced. Num…
Tunneling light-emitting devices (LEDs) based on transition metal dichalcogenides (TMDs) and other 2D materials are a new platform for on-chip optoelectronic integration. Some of the physical processes underlying this LED architecture are not fully understood, especially the emission at photon energies higher than the applied electrostatic potential, so-called overbias emission. Here we report overbias emission for potentials that are near half of the optical bandgap energy in TMD-based tunneling LEDs. We show that this emission is not thermal in nature, but consistent with exciton generation …
The weakly screened electron-hole interactions in an atomically thin semiconductor not only downshift its excitation spectrum from a quasiparticle one, but also redistribute excitation energies and wavefunction characters with profound effects on diverse modes of material response, including the exciton-phonon scattering processes accessible to resonant Raman measurements. Here we develop a first-principles framework to calculate frequency-dependent resonant Raman intensities that includes excitonic effects and goes beyond the Placzek approximation. We show how excitonic effects in MoS2 strong…
We develop an analytically solvable model able to qualitatively explain nonhydrogenic exciton spectra observed recently in two-dimensional (2d) semiconducting transition metal dichalcogenides. Our exciton Hamiltonian explicitly includes additional angular momentum associated with the pseudospin degree of freedom unavoidable in 2d semiconducting materials with honeycomb structure. We claim that this is the key ingredient for understanding the nonhydrogenic exciton spectra that was missing so far.
The performance limits of monolayer transition metal dichalcogenide transistors are examined with a ballistic MOSFET model. Using ab-initio theory, we calculate the band structures of two-dimensional (2D) transition metal dichalco-genide (MX2). We find the lattice structures of monolayer MX2 remain the same as the bulk MX2. Within the ballistic regime, the performances of monolayer MX2 transistors are better compared to the silicon transistors if thin high-κ gate insulator is used. This makes monolayer MX2 promising 2D materials for future nanoelectronic device applications.
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…
We investigate the correction of interlayer exciton binding energy in transition metal dichalcogenides double layers arising from the exciton-optical phonon coupling using the method of Lee-Low-Pines unitary transformation. We find that the binding energy varies in several tens of meV, depending on the polarizability of materials and interlayer distance between double layers. Moreover, the correction of binding energy results in the remarkable increasing of the critical temperature for the condensation of dilute excitonic gas basing on the Berezinskii-Kosterlitz-Thouless model. These results n…
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…
Semiconducting transition metal dichalcogenides (STMDC) are two-dimensional (2D) crystals characterized by electron volt size band gaps, spin-orbit coupling (SOC), and d-orbital character of its valence and conduction bands. We show that these materials carry unique exciton quasiparticles (electron-hole bound states) with energy within the gap but which can ``collapse'' in the strong coupling regime by merging into the band structure continuum. The exciton collapse seems to be a generic effect in these 2D crystals.
While exciton relaxation in transition metal dichalcogenides (TMDs) has been intensively studied, spatial exciton propagation has received only little attention - in spite of being a key process for optoelectronics and having already shown interesting unconventional behaviours (e.g. spatial halos). Here, we study the spatiotemporal dynamics in TMDs and track the way of optically excited excitons in time, momentum, and space. In particular, we investigate the temperature-dependent exciton diffusion including the remarkable exciton landscape constituted by bright and dark states. Based on a full…
A monolayer of transition metal dichalcogenide (TMDC) is shown to be capable of supporting a guided optical mode below the exciton resonance, a two-dimensional exciton polariton. This visible or near IR mode is confined roughly within a micrometer from the monolayer and has propagation length exceeding 100 micrometers. The light guiding ability makes TMDC monolayers more versatile and potentially attractive photonic platform.
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 have developed an ab-initio-based fully-quantum numerically-accurate methodology for the simulation of the exciton dynamics and time- and frequency-resolved fluorescence spectra of the cavity-controlled two-dimensional materials at finite temperature and applied this methodology to the single-layer WSe2 system. This allowed us to establish dynamical and spectroscopic signatures of the polaronic and polaritonic effects as well as uncover their characteristic timescales in the relevant range of temperatures.
Using the quasiclassical concept of Berry curvature we demonstrate that a Dirac exciton - a pair of Dirac quasiparticles bound by Coulomb interactions - inevitably possesses an intrinsic angular momentum making the exciton effectively self-rotating. The model is applied to excitons in two-dimensional transition metal dichalcogenides, in which the charge carriers are known to be described by a Dirac-like Hamiltonian. We show that the topological self-rotation strongly modifies the exciton spectrum and, as a consequence, resolves the puzzle of the overestimated two-dimensional polarizability emp…
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…
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…
When transition-metal dichalcogenide monolayers lack inversion symmetry, their low-energy single particle spectrum can described by tilted massive Dirac Hamiltonians. The so-called Janus materials fall into that category. Inversion symmetry can also be broken by the application of out-of-plane electric fields, or by the mere presence of a substrate. Here we explore the properties of excitons in TMDC monolayers lacking inversion symmetry. We find that exciton binding energies can be larger than the electronic band gap, making such materials promising candidates to host the elusive exciton insul…
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…
