论文标题

建立泵探针电子 - 放松动力学中的非热机制

Establishing non-thermal regimes in pump-probe electron-relaxation dynamics

论文作者

Na, MengXing, Boschini, Fabio, Mills, Arthur K., Michiardi, Matteo, Day, Ryan P., Zwartsenberg, Berend, Levy, Giorgio, Zhdanovich, Sergey, Kemper, Alexander F., Jones, David J., Damascelli, Andrea

论文摘要

时间和角度分辨的光发射光谱(TR-ARPES)在光激发下访问固体的电子结构,并且是研究电子与集体模式之间耦合的强大技术。推断电子玻色子耦合的一种方法是通过光学兴奋的电子的松弛动力学以及能量重新分布的特征时间标准。电子弛豫动力学的共同描述是通过有效的电子温度。这样的描述要求热力学数量明确定义,这一假设通常在早期延迟时违反。另外,对非热窗口的精确估计(可能无法应用有效温度模型)是具有挑战性的。我们在石墨上执行TR-ARPES,并表明Boltzmann速率方程可用于计算时间依赖性的电子职业函数,并重现非热电子职业给出的实验特征。使用此模型,我们定义了非热电子占用的定量度量,并使用它来定义通量延迟空间中电子松弛的不同阶段。更一般而言,这种方法可用于在泵探针实验中通知非热到热的跨界。

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) accesses the electronic structure of solids under optical excitation, and is a powerful technique for studying the coupling between electrons and collective modes. One approach to infer electron-boson coupling is through the relaxation dynamics of optically-excited electrons, and the characteristic timescales of energy redistribution. A common description of electron relaxation dynamics is through the effective electronic temperature. Such a description requires that thermodynamic quantities are well-defined, an assumption that is generally violated at early delays. Additionally, precise estimation of the non-thermal window -- within which effective temperature models may not be applied -- is challenging. We perform TR-ARPES on graphite and show that Boltzmann rate equations can be used to calculate the time-dependent electronic occupation function, and reproduce experimental features given by non-thermal electron occupation. Using this model, we define a quantitative measure of non-thermal electron occupation and use it to define distinct phases of electron relaxation in the fluence-delay phase space. More generally, this approach can be used to inform the non-thermal-to-thermal crossover in pump-probe experiments.

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