Lee Jong-Won, Kim Minju, Kang Gyeongbo, Vinko Sam M, Bae Leejin, Cho Min Sang, Chung Hyun-Kyung, Kim Minseok, Kwon Soonnam, Lee Gyusang, Nam Chang Hee, Park Sang Han, Sohn Jang Hyeob, Yang Seong Hyeok, Zastrau Ulf, Cho Byoung Ick
Center for Relativistic Laser Science, Institute for Basic Science, Gwangju 61005, Republic of Korea.
Department of Physics and Photon Science, Gwangju Institute of Science and Technology, Gwangju 61005, Republic of Korea.
Phys Rev Lett. 2021 Oct 22;127(17):175003. doi: 10.1103/PhysRevLett.127.175003.
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.
物质的超快光学激发会导致远离平衡的高激发态。在本研究中,飞秒X射线吸收光谱被用于可视化光激发热密铜中的超快动力学。在飞秒时间尺度上观察到了与d空位相关的丰富动力学特征。尽管在皮秒时间范围内解释X射线吸收数据取得了成功,但基于快速热化概念和高温金属静态电子结构的传统双温模型对新的飞秒数据理解不佳。通过纳入非热电子的复合动力学以及激发d块的屏蔽变化,可以实现更好的理解。4sp和3d能带之间的布居平衡主要由非热电子的复合率决定,而布居不足的3d块最初会强烈下移,并在几百飞秒内恢复。