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Optically dark states play an important role in the electronic and optical properties of monolayers (MLs) of semiconducting transition metal dichalcogenides. The effect of temperature on the in-plane-field activation of the neutral and charged dark excitons is investigated in a WSe2 ML encapsulated in hexagonal BN flakes. The brightening rates of the neutral dark (X D) and grey (X G) excitons and the negative dark trion (T D) differ substantially at particular temperature. More importantly, they weaken considerably by about 3–4 orders of magnitude with temperature increased from 4.2 K to 100 K. The quenching of the dark-related emissions is accompanied by the two-order-of-magnitude increase in the emissions of their neutral bright counterparts, i.e. neutral bright exciton (X B) and spin-singlet (T S) and spin-triplet (T T) negative trions, due to the thermal activations of dark states. Furthermore, the energy splittings between the dark X D and T D complexes and the corresponding bright X B, T S, and T T ones vary with temperature rises from 4.2 K to 100 K. This is explained in terms of the different exciton–phonon coupling for the bright and dark excitons stemming from their distinct symmetry properties.

We present femtosecond pump-probe measurements of neutral and charged exciton optical response in monolayer MoSe2 to resonant photoexcitation of a given exciton state in the presence of 2D electron gas. We show that creation of charged exciton (X−) population in a given K+, K− valley requires the capture of available free carriers in the opposite valley and reduces the interaction of neutral exciton (X) with the electron Fermi sea. We also observe spectral broadening of the X transition line with the increasing X− population caused by efficient scattering and excitation induced dephasing. From the valley-resolved analysis of the observed effects we are able to extract the spin-valley relaxation times of free carriers as a function of carrier density. Moreover, we analyze the oscillator strength and energy shift of X in the regime of interaction with electron Fermi sea under resonant excitation. From this we can observe the process of X decay by radiative recombination paired with trion formation. We demonstrate an increase of neutral exciton relaxation rate with the introduction of Fermi sea of electrons. We ascribe the observed effect to the increased efficiency of the trion formation, as well as the radiative decay caused by the screening of disorder by the free carriers.

Excitonic physics dominates the optical response of semiconductor monolayers but single particle band structure parameters are hard to probe experimentally. Here, spin-orbit splitting in the conduction band of monolayer WSe2 is revealed by the identification of the Rydberg series of dark excitons.

Using ultrafast resonant pump-probe spectroscopy in an unconventional experimental setup we investigate the spectral shape and dynamics of absorption features related to the A exciton in an hexagonal boron nitride (hBN)/MoSe2/hBN van der Waals heterostructure. While in a pure two-level system a pump-probe experiment measures the occupation or the polarization dynamics, depending on the time ordering of the pulse pair, in the transition metal dichalcogenide (TMD) system both quantities get thoroughly mixed by strong exciton–exciton interaction. We find that for short positive delays the spectral lines experience pronounced changes in their shape and energy and they relax to the original situation on a picosecond time scale. For negative delays, distinctive spectral oscillations appear indicating the first-time observation of perturbed free induction decay for a TMD system. The comparison between co-circular and cross-circular excitation schemes further allows us to investigate the rapid inter-valley scattering. By considering a three-level system as a minimal model including the local field effect, excitation-induced dephasing (EID), and scattering between the excited states we explain all phenomena observed in the experiment with excellent consistency. Our handy model can be even further reduced to two levels in the case of a co-circular excitation, for which we derive analytic expressions to describe the detected signals. This allows us to trace back the spectral shapes and shifts to the impact of local field effect and EID thus fully reproducing the complex behavior of the observed effects.

We report magneto-optical spectroscopy of gated monolayer MoS_{2} in high magnetic fields up to 28T and obtain new insights on the many-body interaction of neutral and charged excitons with the resident charges of distinct spin and valley texture. For neutral excitons at low electron doping, we observe a nonlinear valley Zeeman shift due to dipolar spin-interactions that depends sensitively on the local carrier concentration. As the Fermi energy increases to dominate over the other relevant energy scales in the system, the magneto-optical response depends on the occupation of the fully spin-polarized Landau levels (LL) in both K/K^{′} valleys. This manifests itself in a many-body state. Our experiments demonstrate that the exciton in monolayer semiconductors is only a single particle boson close to charge neutrality. We find that away from charge neutrality it smoothly transitions into polaronic states with a distinct spin-valley flavor that is defined by the LL quantized spin and valley texture.

Recent results on the optical properties of monolayer and few layers of semiconducting transition metal dichalcogenides are reviewed. Experimental observations are presented and discussed in the frame of existing models, highlighting the limits of our understanding in this emerging field of research. We first introduce the representative band structure of these systems and their interband optical transitions. The effect of an external magnetic field is then considered to discuss Zeeman spectroscopy and optical pumping experiments, both revealing phenomena related to the valley degree of freedom. Finally, we discuss the observation of single photon emitters in different types of layered materials, including wide band gap hexagonal boron nitride. While going through these topics, we try to focus on open questions and on experimental observations, which do not yet have a clear explanation.

Since their theoretical prediction by Peierls in the 1930s, charge density waves (CDWs have been one of the most commonly encountered electronic phases in low-dimensional metallic systems. The instability mechanism originally proposed combines Fermi surface nesting and electron-phonon coupling but is, strictly speaking, only valid in one dimension. In higher dimensions, its relevance is questionable as sharp maxima in the static electronic susceptibility χ(q) are smeared out, and is, in many cases, unable to account for the periodicity of the observed charge modulations. Here, we investigate the quasi-two-dimensional LaAgSb_{2}, which exhibits two CDW transitions, by a combination of diffuse x-ray scattering, inelastic x-ray scattering, and ab initio calculations. We demonstrate that the CDW formation is driven by phonon softening. The corresponding Kohn anomalies are visualized in three dimensions through the momentum distribution of the x-ray diffuse scattering intensity. We show that they can be quantitatively accounted for by considering the electronic susceptibility calculated from a Dirac-like band, weighted by anisotropic electron-phonon coupling. This remarkable agreement sheds new light on the importance of Fermi surface nesting in CDW formation.

Temperature-dependent (5 K–300 K) Raman scattering study of A1g/A′1 phonon modes in mono-layer (1L), bilayer (2L), trilayer (3L), and tetralayer (4L) MoTe2 is reported. The temperature evolution of the modes’ intensity critically depends on the flake thickness. In particular with λ=632.8-nm light excitation, a strongly non-monotonic dependence of the A1g mode intensity is observed in 2L MoTe2. The intensity decreases with decreasing temperature down to 220 K, and the A1g mode almost completely vanishes from the Stokes scattering spectrum in the temperature range between 160 K and 220 K. The peak recovers at lower temperatures, and at T=5 K, it becomes three times more intense that at room temperature. Similar non-monotonic intensity evolution is observed for the out-of-plane mode in 3L MoTe2 in which tellurium atoms in all three layers vibrate in-phase. The intensity of the other out-of-plane Raman-active mode (with vibrations of tellurium atoms in the central layer shifted by 180° with respect to the vibrations in outer layers) only weakly depends on temperature. The observed quenching of the Raman scattering in 2L and 3L MoTe2 is attributed to a destructive interference between the resonant and non-resonant contributions to the Raman scattering amplitude. The observed “antiresonance” is related to the electronic excitation at the M point of the Brillouin zone in few-layer MoTe2.

Recent experimental and theoretical work on hydrogen-like absorption spectra of excitons in external magnetic fields revealed new effects when the Coulomb interaction becomes comparable to the magnetic perturbation. We present a theoretical approach that allows for calculation of absorption spectra for any value of magnetic field. This approach opens the possibility to compute the optical functions i.e. reflectivity, transmission and absorption including the excitonic effects for various strength of external magnetic field.

In monolayers of semiconducting transition metal dichalcogenides, the light helicity (σ^{+} or σ^{-}) is locked to the valley degree of freedom, leading to the possibility of optical initialization of distinct valley populations. However, an extremely rapid valley pseudospin relaxation (at the time scale of picoseconds) occurring for optically bright (electric-dipole active) excitons imposes some limitations on the development of opto-valleytronics. Here, we show that valley pseudospin relaxation of excitons can be significantly suppressed in a WSe_{2} monolayer, a direct-gap two-dimensional semiconductor with the exciton ground state being optically dark. We demonstrate that the already inefficient relaxation of the exciton pseudospin in such a system can be suppressed even further by the application of a tiny magnetic field of about 100 mT. Time-resolved spectroscopy reveals the pseudospin dynamics to be a two-step relaxation process. An initial decay of the pseudospin occurs at the level of dark excitons on a time scale of 100 ps, which is tunable with a magnetic field. This decay is followed by even longer decay (>1 ns), once the dark excitons form more complex pseudo-particles allowing for their radiative recombination. Our findings of slow valley pseudospin relaxation easily manipulated by the magnetic field open new prospects for engineering the dynamics of the valley pseudospin in transition metal dichalcogenides.

We investigate the low-energy carrier dynamics in Landau quantized multilayer epitaxial graphene on $(000\bar{1})$ SiC, using 14 meV photons. The THz absorption is dominated by Landau-level transitions within the conduction bands of several graphene layers with different doping. Varying the magnetic field allows us to tune the THz-induced response from induced transmission around B = 0 to induced absorption at intermediate fields (1.5 T–3.3 T) and back to induced transmission at higher fields (3.3 T–7 T). The main features of this complex response are explained by a strong dependence of the absorption on the electron temperature. Furthermore a prolonged relaxation at high fields, which is attributed to reduced scattering via optical phonons, is observed.

We report on absolute magneto-transmission experiments on highly doped quasi-free-standing epitaxial graphene targeting the classical-to-quantum crossover of the cyclotron resonance. This study allows us to directly extract the carrier density and also other relevant quantities such as the quasiparticle velocity and the Drude weight, which is precisely measured from the strength of the cyclotron resonance. We find that the Drude weight is renormalized with respect to its non-interacting (or random phase approximation) value and that the renormalization is tied to the quasiparticle velocity enhancement. This finding is in agreement with recent theoretical predictions, which attribute the renormalization of the Drude weight in graphene to the interplay between broken Galilean invariance and electron–electron interactions.

We show how the magneto-phonon resonance, particularly pronounced in sp ^2 carbon allotropes, can be used as a tool to probe the band structure of multilayer graphene specimens. Even when electronic excitations cannot be directly observed, their coupling to the E _2g phonon leads to pronounced oscillations of the phonon feature observed through Raman scattering experiments with multiple periods and amplitudes determined by the electronic excitation spectrum. Such experiment and analysis has been performed up to 28 T on an exfoliated four-layer graphene specimen deposited on SiO _2 , and the observed oscillations correspond to the specific AB stacked four-layer graphene electronic excitation spectrum.