No Arabic abstract
Unidirectional in-plane structural anisotropy in Rhenium-based transition metal dichalcogenides (TMDs) introduces a new class of 2-D materials, exhibiting anisotropic optical properties. In this work, we perform temperature dependent, polarization-resolved photoluminescence and reflectance measurements on several-layer ReS$_{2}$. We discover two additional excitonic resonances (X$_{3}$ and X$_{4}$), which can be attributed to splitting of spin degenerate states. Strong in-plane oscillator strength of exciton species X$_{1}$ and X$_{2}$ are accompanied by weaker counterparts X$_{3}$ and X$_{4}$ with similar polarization orientations. The in-plane anisotropic dielectric function has been obtained for ReS$_{2}$ which is essential for engineering light matter coupling for polarization sensitive optoelectronic devices. Furthermore, our temperature dependent study revealed the existence of low-lying momentum-forbidden dark states causing an anomalous PL intensity variation at 30 K, which has been elucidated using a rate equation model involving phonon scattering from these states. Our findings of the additional excitonic features and the momentum-dark states can shed light on the true nature of the electronic band structure of ReS$_{2}$.
We show that new low-energy photoluminescence (PL) bands can be created in semiconducting single-walled carbon nanotubes by intense pulsed excitation. The new bands are attributed to PL from different nominally dark excitons that are brightened due to defect-induced mixing of states with different parity and/or spin. Time-resolved PL studies on single nanotubes reveal a significant reduction of the bright exciton lifetime upon brightening of the dark excitons. The lowest energy dark state has longer lifetimes and is not in thermal equilibrium with the bright state.
Twist-engineering of the electronic structure of van-der-Waals layered materials relies predominantly on band hybridization between layers. Band-edge states in transition-metal-dichalcogenide semiconductors are localized around the metal atoms at the center of the three-atom layer and are therefore not particularly susceptible to twisting. Here, we report that high-lying excitons in bilayer WSe2 can be tuned over 235 meV by twisting, with a twist-angle susceptibility of 8.1 meV/{deg}, an order of magnitude larger than that of the band-edge A-exciton. This tunability arises because the electronic states associated with upper conduction bands delocalize into the chalcogenide atoms. The effect gives control over excitonic quantum interference, revealed in selective activation and deactivation of electromagnetically induced transparency (EIT) in second-harmonic generation. Such a degree of freedom does not exist in conventional dilute atomic-gas systems, where EIT was originally established, and allows us to shape the frequency dependence, i.e. the dispersion, of the optical nonlinearity.
The reduced dielectric screening in atomically thin transition metal dichalcogenides allows to study the hydrogen-like series of higher exciton states in optical spectra even at room temperature. The width of excitonic peaks provides information about the radiative decay and phonon-assisted scattering channels limiting the lifetime of these quasi-particles. While linewidth studies so far have been limited to the exciton ground state, encapsulation with hBN has recently enabled quantitative measurements of the broadening of excited exciton resonances. Here, we present a joint experiment-theory study combining microscopic calculations with spectroscopic measurements on the intrinsic linewidth and lifetime of higher exciton states in hBN-encapsulated WSe$_2$ monolayers. Surprisingly, despite the increased number of scattering channels, we find both in theory and experiment that the linewidth of higher excitonic states is similar or even smaller compared to the ground state. Our microscopic calculations ascribe this behavior to a reduced exciton-phonon scattering efficiency for higher excitons due to spatially extended orbital functions.
ReS$_2$ has recently emerged as a new member in the rapidly growing family of two-dimensional materials. Unlike MoS$_2$ or WSe$_2$, the optical and electrical properties of ReS$_2$ are not isotropic due to the reduced symmetry of the crystal. Here, we present layer-dependent Raman measurements of ReS$_2$ samples ranging from monolayers to ten layers in the ultralow frequency regime. We observe layer breathing and shear modes which allow for easy assignment of the number of layers. Polarization-dependent measurements give further insight into the crystal structure and reveal an energetic shift of the shear mode which stems from the in-plane anisotropy of the shear modulus in this material.
Two-dimensional quantum spin Hall (QSH) insulators are a promising material class for spintronic applications based on dissipationless topologically-protected spin currents in their edges. Yet, they have not lived up to their technological potential, as experimental realizations are scarce and limited to cryogenic temperatures. These constraints have also severely restricted the characterization of their dynamical properties, imperative for the design of QSH devices operating under nonequilibrium conditions. Here, we report on the electron dynamics of the novel room-temperature QSH candidate bismuthene after photoexcitation using time- and angle-resolved photoemission spectroscopy. We map the transiently occupied conduction band and observe a metallic dispersive feature within the bulk band gap - a signature of topological edge states. Our analysis of hot photocarrier lifetimes provides insight into the microscopic scattering processes and the key role of edge states. The demonstration of the large bulk band gap and stability of edge states at room temperature marks a critical step towards QSH applications.