The interplay of the non-equivalent corners in the Brillouin zone of transition metal dichalcogenides have been investigated extensively. While experimental and theoretical works contributed to a detailed understanding of the relaxation of selective optical excitations and the related relaxation rates, only limited microscopic descriptions of stationary experiments are available so far. In this manuscript we present microscopic calculations for the non-equilibrium steady state properties of excitons during continuous wave pumping. We find sharp features in photoluminescence excitation spectra and degree of polarization which result from phonon assisted excitonic transitions dominating over exciton recombination and intervalley exchange coupling.
The p-n diodes represent the most fundamental device building block for diverse optoelectronic functions, but are difficult to achieve in atomically thin transition metal dichalcogenides (TMDs) due to the inability to selectively dope them into p- or n-type semiconductors. Here we report the first demonstration of an atomically thin and atomically sharp heterojunction p-n diode by vertically stacking p-type monolayer tungsten diselenide (WSe2) and n-type few-layer molybdenum disulfide (MoS2). Electrical measurement demonstrates excellent diode characteristics with well-defined current rectific…
The spectral and dispersive emission properties are analytically determined for the two-dimensional system of exciton-polaritons in microcavities excited by a resonant and coherent optical pump. New collective excitations result from the anomalous coupling between one generic polariton state and its idler, created by the scattering of two pumped polaritons. The corresponding parametric correlation is stimulated by the emitter and idler populations and drives very efficiently the luminescence. The intrinsic properties of the collective excitations determine a peculiar emission pattern.
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…
Recent developments in fabrication of van der Waals heterostructures enable new type of devices assembled by stacking atomically thin layers of two-dimensional materials. Using this approach, we fabricate light-emitting devices based on a monolayer WSe$_2$, and also comprising boron nitride tunnelling barriers and graphene electrodes, and observe sharp luminescence spectra from individual defects in WSe$_2$ under both optical and electrical excitation. This paves the way towards the realization of electrically-pumped quantum emitters in atomically thin semiconductors. In addition we demonstrat…
We report an experimental study of temperature-dependent spectral lineshapes of phonon side-band emission stemming from dark excitons in monolayer and bilayer WSe$_{2}$. Using photoluminescence spectroscopy in the range from 4 to 100K, we observe a pronounced asymmetry in the phonon-assisted luminescence from momentum-indirect exciton reservoirs. We demonstrate that the corresponding spectral profiles are distinct from those of bright excitons with direct radiative decay pathways. The lineshape asymmetry reflects thermal distribution of exciton states with finite center-of-mass momenta, charac…
The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N = 1, 2, ... 6 S-Mo-S monolayers have been investigated by optical spectroscopy. Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure. With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 0.6 eV. This leads to a crossover to a direct-gap material in the limit of the single monolayer. Unlike the bulk…
High energy resolution spectroscopic studies of quantum magnets have proven to be extremely valuable in directly accessing magnetodynamics quantities, such as energy barriers, magnetic interactions, lifetime of excited states and fluctuations at the most fundamental level. Here, we explore the existence of a new flavor of low-energy spin-excitations for quantum spins coupled to an electron bath. In sharp contrast to the usual tunneling signature of two steps symmetrically centered around the Fermi level, we find a single step in the conductance. Combining time-dependent and many-body perturbat…
We have studied on optical second harmonic generations (SHGs) from atomically thin MoTe2 flakes with 2H and 1T' phases. From 2H-MoTe2 samples with odd (even) numbers of layers, strong (negligible) SHGs are observed due to the layer-dependent broken inversion symmetry. When pumped by a telecom-band laser, SHG from a monolayer 2H-MoTe2 is about one order of magnitude stronger than that from a monolayer WS2; an extremely high second-order nonlinear susceptibility of 2.5 nm/V is estimated, presenting the highest value among those reported in two-dimensional materials. SHG measurements in MoTe2 are…
The emergence of two-dimensional crystals has revolutionized modern solid-state physics. From a fundamental point of view, the enhancement of charge carrier correlations has sparked enormous research activities in the transport- and quantum optics communities. One of the most intriguing effects, in this regard, is the bosonic condensation and spontaneous coherence of many-particle complexes. Here, we find compelling evidence of bosonic condensation of exciton-polaritons emerging from an atomically thin crystal of MoSe2 embedded in a dielectric microcavity under optical pumping. The formation o…
Nonlinear optical effects such as four-wave mixing and generation of squeezed light are ubiquitous in optical devices and light sources. For new devices operating at low optical power, the resonant nonlinearity arising from the two-photon sensitive bound biexciton in a semiconductor microcavity is an interesting prospective platform. Due to the particularly strong Coulomb interaction in atomically thin semiconductors, these materials have strongly bound biexcitons and operate in the visible frequency range of the electromagnetic spectrum. To remove the strong pump laser from the generated ligh…
Atomically thin transition metal dichalcogenides (TMDs) have distinct opto-electronic properties including enhanced luminescence and high on-off current ratios, which can be further modulated by making more complex TMD heterostructures. However, resolution limits of conventional optical methods do not allow for direct optical-structural correlation measurements in these materials, particularly of buried interfaces in TMD heterostructures. Here we use, for the first time, electron beam induced cathodoluminescence in a scanning transmission electron microscope (CL-STEM) to measure optical proper…
The defect states in atomically thin layers of transition metal dichalcogenides are promising candidates for single photon emission. However, the brightness of such quantum emission is often weak, and is accompanied with undesirable effects like spectral diffusion and strong background emission. By placing a monolayer WSe$_2$ directly on a rough gold substrate, here we show a selective enhancement of sharp defect-bound exciton peaks, coupled with a suppressed spectral diffusion and strong quenching of background luminescence. By combining the experimental data with detailed electromagnetic sim…
Above cryogenic temperatures, random laser (RL) emission under continuous wave (CW) optical pumping is often challenging for materials having plenty of lattice defects. Thus, intensive care is required while fabricating the RL device. Synthesis of 2D materials having unique functionality at the atomic limit is necessary for use in such devices. In this work, defects-free 2D yellow pearl (2D-YP) has been synthesized from bulk south sea pearl using liquid-phase exfoliation (LPE) technique. Thereafter, 2D-YP has been employed as passive scatterer to achieve CW pumped RL emission from a convention…
