Abstract
Energy relaxation of photo-excited charge carriers is of significant fundamental interest and crucial for the performance of monolayer transition metal dichalcogenides in optoelectronics. The primary stages of carrier relaxation affect a plethora of subsequent physical mechanisms. Here we measure light scattering and emission in tungsten diselenide monolayers close to the laser excitation energy (down to ~0.6 meV). We reveal a series of periodic maxima in the hot photoluminescence intensity, stemming from energy states higher than the A-exciton state. We find a period ~15 meV for 7 peaks below (Stokes) and 5 peaks above (anti-Stokes) the laser excitation energy, with a strong temperature dependence. These are assigned to phonon cascades, whereby carriers undergo phonon-induced transitions between real states above the free-carrier gap with a probability of radiative recombination at each step. We infer that intermediate states in the conduction band at the Λ-valley of the Brillouin zone participate in the cascade process of tungsten diselenide monolayers. This provides a fundamental understanding of the first stages of carrier–phonon interaction, useful for optoelectronic applications of layered semiconductors.
Highlights
Energy relaxation of photo-excited charge carriers is of significant fundamental interest and crucial for the performance of monolayer transition metal dichalcogenides in optoelectronics
The optical properties of group VI transition metal dichalcogenide monolayer (1L-TMD) semiconductors are dominated by excitons with binding energies of hundreds of meV1, with spin and valley properties highly beneficial for optoelectronics[2], valleytronics[3] and spintronics[3,4,5,6,7,8,9,10,11,12]
Understanding the relaxation pathways in tungsten diselenide monolayers (1L-WSe2) is important for optoelectronic applications, such as photodetectors[34] and lasers[35], because it determines the recovery rate and, as a result, the devices’ speed and efficiency
Summary
Energy relaxation of photo-excited charge carriers is of significant fundamental interest and crucial for the performance of monolayer transition metal dichalcogenides in optoelectronics. We find a period ~15 meV for 7 peaks below (Stokes) and 5 peaks above (anti-Stokes) the laser excitation energy, with a strong temperature dependence These are assigned to phonon cascades, whereby carriers undergo phonon-induced transitions between real states above the free-carrier gap with a probability of radiative recombination at each step. We infer that intermediate states in the conduction band at the Λ-valley of the Brillouin zone participate in the cascade process of tungsten diselenide monolayers. This provides a fundamental understanding of the first stages of carrier–phonon interaction, useful for optoelectronic applications of layered semiconductors. Our approach can be extended to all layered materials (LMs) and their heterostructures (LMHs), as well as to other materials systems, such as perovskites[37,38]
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