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Register a new userIncoherent phonon population and exciton-exciton annihilation in monolayer WS2 revealed by time-resolved spontaneous Raman scattering
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Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications in nano-electronics. In this work, we study the incoherent optical phonon and exciton population dynamics in monolayer WS2 by time-resolved spontaneous Raman scattering spectroscopy. Upon excitation of the exciton transition, both the Stokes and anti-Stokes optical phonon scattering strength exhibit a large reduction. Based on the detailed balance, the optical phonon population is retrieved, which shows an instant build-up and a relaxation lifetime of around 4 ps at an exciton density E12 cm-2. The corresponding optical phonon temperature rises by 25 K, eventually, after some 10s of picoseconds, leading to a lattice heating by only around 3 K. The exciton relaxation dynamics extracted from the transient vibrational Raman response shows a strong excitation density dependence, signaling an important bi-molecular contribution to the decay. The exciton relaxation rate is found to be (70 ps)-1 and exciton-exciton annihilation rate 0.1 cm2s-1. These results provide valuable insight into the thermal dynamics after optical excitation and enhance the understanding of the fundamental exciton dynamics in two-dimensional transition metal materials.
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In monolayer semiconductor transition metal dichalcogenides, the exciton-phonon interaction is expected to strongly affect the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M). Oscillatory behavior is also observed in the steady-state emission linewidth and in timeresolved photoluminescence excitation data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.
The dynamics of exciton formation in transition metal dichalcogenides is difficult to measure experimentally, since many momentum-indirect exciton states are not accessible to optical interband spectroscopy. Here, we combine a tuneable pump, high-harmonic probe laser source with a 3D momentum imaging technique to map photoemitted electrons from monolayer WS$_2$. This provides momentum-, energy- and time-resolved access to excited states on an ultrafast timescale. The high temporal resolution of the setup allows us to trace the early-stage exciton dynamics on its intrinsic timescale and observe the formation of a momentum-forbidden dark K$Sigma$ exciton a few tens of femtoseconds after optical excitation. By tuning the excitation energy we manipulate the temporal evolution of the coherent excitonic polarization and observe its influence on the dark exciton formation. The experimental results are in excellent agreement with a fully microscopic theory, resolving the temporal and spectral dynamics of bright and dark excitons in WS$_2$.
We discuss here the effect of band nesting and topology on the spectrum of excitons in a single layer of MoS$_2$, a prototype transition metal dichalcogenide material. We solve for the single particle states using the ab initio based tight-binding model containing metal $d$ and sulfur $p$ orbitals. The metal orbitals contribution evolving from $K$ to $Gamma$ points results in conduction-valence band nesting and a set of second minima at $Q$ points in the conduction band. There are three $Q$ minima for each $K$ valley. We accurately solve the Bethe-Salpeter equation including both $K$ and $Q$ points and obtain ground and excited exciton states. We determine the effects of the electron-hole single particle energies including band nesting, direct and exchange screened Coulomb electron-hole interactions and resulting topological magnetic moments on the exciton spectrum. The ability to control different contributions combined with accurate calculations of the ground and excited exciton states allows for the determination of the importance of different contributions and a comparison with effective mass and $kcdot p$ massive Dirac fermion models.
Monolayer transition metal dichalcogenides (TMDs) are direct gap semiconductors emerging promising applications in diverse optoelectronic devices. To improve performance, recent investigations have been systematically focused on the tuning of their optical properties. However, an all-optical approach with the reversible feature is still a challenge. Here we demonstrate the tunability of the photoluminescence (PL) properties of monolayer WS2 via laser irradiation. The modulation of PL intensity, as well as the conversion between neutral exciton and charged trion have been readily and reversibly achieved by using different laser power densities. We attribute the reversible manipulation to the laser-assisted adsorption and desorption of gas molecules, which will deplete or release free electrons from the surface of WS2 and thus modify its PL properties. This all-optical manipulation, with advantages of reversibility, quantitative control, and high spatial resolution, suggests promising applications of TMDs monolayers in optoelectronic and nanophotonic applications, such as optical data storage, micropatterning, and display.
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 joint theory-experiment study combining microscopic and material-specific theory with time- and temperature-resolved photoluminescence measurements, we demonstrate the key role of dark intervalley states that are found to dominate the EEA rate in monolayer WSe$_2$. We reveal an intriguing, characteristic temperature dependence of Auger scattering in this class of materials with an excellent agreement between theory and experiment. Our study provides microscopic insights into the efficiency of technologically relevant Auger scattering channels within the remarkable exciton landscape of atomically thin semiconductors.
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