Calibrating Out-of-Equilibrium Electron–Phonon Couplings in Photoexcited MoS2

• Published in: Nano letters 2022-06, Vol.22 (12), p.4800-4806
• Main Authors: Liu, Xin-Bao, Hu, Shi-Qi, Chen, Daqiang, Guan, Mengxue, Chen, Qing, Meng, Sheng
• Format: Article
• Language: English
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/acs.nanolett.2c01105

Nonequilibrium electron–phonon coupling (EPC) serves as a dominant interaction in a multitude of transient processes, including photoinduced phase transitions, coherent phonon generation, and possible light-induced superconductivity. Here we use monolayer MoS2 as a prototype to investigate the variation in electron–phonon couplings under laser excitation, on the basis of real-time time-dependent density functional theory simulations. Phonon softening, anisotropic modification of the deformation potential, and enhancement of EPC are observed, which are attributed to the reduced electronic screening and modulated potential energy surfaces by photoexcitation. Furthermore, by tracking the transient deformation potential and nonthermal electronic population, we can monitor the ultrafast time evolution of the energy exchange rate between electrons and phonons upon laser excitation. This work provides an effective strategy to investigate the nonequilibrium EPC and constructs a scaffold for understanding nonequilibrium states beyond the multitemperature models.