Temperature Dependence of Electron–Phonon Interactions in Gold Films Rationalized by Time-Domain Ab Initio Analysis
Temperature Dependence of Electron–Phonon Interactions in Gold Films Rationalized by Time-Domain Ab Initio Analysis
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DOI：
10.1021/acs.jpcc.7b05211
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发表时间：
2017-08
影响因子：
3.7
通讯作者：
Xin Zhou;Linqiu Li;Hao. Dong;A. Giri;P. Hopkins;O. Prezhdo
中科院分区：
文献类型：
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作者：
Xin Zhou;Linqiu Li;Hao. Dong;A. Giri;P. Hopkins;O. Prezhdo
用超快激光测量方法研究了金属中受激电子的非平衡动力学。使用实时Kohn-Sham含时密度泛函理论和非绝热分子动力学，我们报告直接建模这样的实验，合理化所观察到的温度依赖性。聚焦于薄的金膜，我们分析了温度对膜结构，电子态密度，非绝热电子-声子耦合，弹性电子-声子散射时间，和电子-声子弛豫速率的影响。计算得到的不同温度下的有效电子-声子耦合常数与实验值和另一种理论值符合得很好。温度的升高加速了非弹性和弹性电子-声子散射，并允许大量的高频声子模式耦合到电子子系统。非弹性电子-声子耦合是最大的最近的状态之间，表明载流子弛豫涉及…
The nonequilibrium dynamics of excited electrons in metals is probed by ultrafast laser measurements. Using a real-time Kohn–Sham time-dependent density functional theory and nonadiabatic molecular dynamics, we report direct modeling of such experiments, rationalizing the observed temperature dependence. Focusing on thin gold films, we analyze the effect of temperature on film structure, electronic state densities, nonadiabatic electron–phonon coupling, elastic electron–phonon scattering times, and electron–phonon relaxation rates. The effective electron–phonon coupling constants calculated at different temperatures are in good agreement with the values deduced from experiments and an alternative theory. A temperature increase accelerates both inelastic and elastic electron–phonon scattering and allows a larger number of higher-frequency phonon modes to couple to the electronic subsystem. The inelastic electron–phonon coupling is largest between nearest states, indicating that carrier relaxation involves ...