Nonthermal Dynamics of Dielectric Functions in a Resonantly Bonded Photoexcited Material

A fundamental question of whether it is thermal or nonthermal has often been argued, when the system undergoes an ultrafast phase change by femtosecond laser photoexcitation. One of the difficulties therein is how to consider the thermalization of a photoexcited system, in which the “lattice” and “electron” systems are decoupled from an equilibrium state just after photoexcitation. This work shows a methodology to identify a thermalization‐time domain of a photoexcited semiconductor, where it can be detected by monitoring the time‐resolved photoabsorption broadband spectrum and comparing that to thermally induced spectrum changes, by which the electron–lattice thermalization time is evaluated to be 12 ps for PbTe. Further analyzing the dynamic dielectric functions substantiates that thermalization time is related to the recovery time of the resonant bonding. Such a crucial determination of thermalization time would eliminate an uncertainty of “thermal or nonthermal” in ultrafast phase change of the resonantly bonded materials. It has been recently known that femtosecond‐laser‐induced ultrafast amorphization of “phase change materials” such as GeSbTe or AgInSbTe occurs in several picoseconds, and it remains unknown whether such an ultrafast phase change is thermal or nonthermal. In this work, by using a resonant bonding PbTe thin film, a new experimental methodology is provided to identify the nonthermal time domain after photoexcitation.