Excitation-dependent photoluminescence intensity of monolayer MoS2: Role of heat-dissipating area and phonon-assisted exciton scattering

Abstract

We studied the excitation-dependent photoluminescence (PL) quantum yield (QY) of monolayer MoS2 (1L-MoS2) with various flake areas grown on SiO2/Si substrates. The PL measurements were carried out by 532, 488, and 325 nm excitations which fulfill the conditions of quasi-resonant excitation of A-exciton, above bandgap, and far above the bandgap excitations, respectively. The PL QY was found to be reduced by decreasing the excitation wavelength, and it is attributed to variation in the thermal energy dissipated to the lattice. PL emission from 1L-MoS2 was observed with 325 nm excitation in large-area flakes (≥532 μm2) because of efficient heat dissipation. In the literature, PL emission of 1L-MoS2 is hardly reported with 325 nm laser excitations. Under 325 nm laser irradiation, 50% of excitation energy is converted to heat, which substantially increases the local temperature. From the temperature-dependent Raman analysis, the rise in the local temperature is approximated to be ∼382 K in the case of a small-area flake, whereas such an effect is alleviated in large-area flakes. Moreover, inter-valley exciton scattering dominates as the excitation wavelength decreases because of a substantial rise in the phonon population for small-area flakes. As a consequence of inter-valley exciton scattering, dark excitons (K-Σ) dominate over the bright excitons (K-K) under the 325 nm excitation. Hence, total suppression of PL emission was observed for small-area flakes because of dark exciton recombination. The noticeable PL emission of large-area flakes is attributed to the improved bright exciton recombination.