Light-matter interactions in two-dimensional layered WSe2 for gauging evolution of phonon dynamics

Abstract

Phonon dynamics is explored in mechanically exfoliated two-dimensional WSe2 using temperature-dependent and laser-power-dependent Raman and photoluminescence (PL) spectroscopy. From this analysis, phonon lifetime in the Raman active modes and phonon concentration, as correlated to the energy parameter E0, were calculated as a function of the laser power, P, and substrate temperature, T. For monolayer WSe2, from the power dependence it was determined that the phonon lifetime for the in-plane vibrational mode was twice that of the out-of-plane vibrational mode for P in the range from 0.308 mW up to 3.35 mW. On the other hand, the corresponding relationship for the temperature analysis showed that the phonon lifetime for the in-plane vibrational mode lies within 1.42x to 1.90x that of the out-of-plane vibrational mode over T = 79 K up to 523 K. To provide energy from external stimuli, as T and P were increased, peak broadening in the PL spectra of the A-exciton was observed. From this, a phonon concentration was tabulated using the Urbach formulism, which increased with increasing T and P; consequently, the phonon lifetime was found to decrease. Although phonon lifetime decreased with increasing temperature for all thicknesses, the decay rate in the phonon lifetime in the monolayer (1L) material was found to be 2x lower compared to the bulk. We invoke a harmonic oscillator model to explain the damping mechanism in WSe2. From this it was determined that the damping coefficient increases with the number of layers. The work reported here sheds fundamental insights into the evolution of phonon dynamics in WSe2 and should help pave the way for designing high-performance electronic, optoelectronic and thermoelectric devices in the future.