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

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 E ₀, 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 1.42× to 1.90× 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 2× 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.