Investigation of Nonequilibrium Electronic Dynamics of Warm Dense Copper with Femtosecond X-Ray Absorption Spectroscopy

Ultrafast optical excitation of matter leads to highly excited states that are far from equilibrium. In this study, femtosecond x-ray absorption spectroscopy was used to visualize the ultrafast dynamics in photoexcited warm dense Cu. The rich dynamical features related to d vacancies are observed on femtosecond timescales. Despite the success in explaining x-ray absorption data in the picosecond regime, the new femtosecond data are poorly understood through the traditional two-temperature model based on the fast thermalization concept and the static electronic structure for high-temperature metals. An improved understanding can be achieved by including the recombination dynamics of nonthermal electrons and changes in the screening of the excited d block. The population balance between the 4sp and 3d bands is mainly determined by the recombination rate of nonthermal electrons, and the underpopulated 3d block is initially strongly downshifted and recovered in several hundreds of femtoseconds.

Automated summary

Ultrafast dynamics in photoexcited warm dense Cu were visualized using femtosecond x-ray absorption spectroscopy, revealing rich dynamical features related to d vacancies. Improved understanding can be achieved by including recombination dynamics of nonthermal electrons and changes in screening of the excited d block. The population balance between the 4sp and 3d bands is mainly determined by the recombination rate of nonthermal electrons, showing recovery of the underpopulated 3d block on picosecond timescales.