期刊
PHYSICAL REVIEW B
卷 94, 期 7, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.94.075120
关键词
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资金
- Office of Science of the U.S. Department of Energy [DE-SC0004993, DE-AC02-05CH11231]
- NG NEXT
- National Science Foundation Graduate Research Fellowship
- Resnick Sustainability Institute
- Link Foundation Energy Fellowship
- DOE Light-Material Interactions in Energy Conversion Energy Frontier Research Center [DE-SC0001293]
Ultrafast laser measurements probe the nonequilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. We present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial differences from free-electron and semiempirical estimates, especially in noble metals above transient electron temperatures of 2000 K, because of the previously neglected strong dependence of electron-phonon matrix elements on electron energy. We also present first-principles calculations of the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions, facilitating complete theoretical predictions of the time-resolved optical probe signatures in ultrafast laser experiments.
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