论文标题

非线性高弹性X射线吸收的电子种群的速率模型近边光谱

A Rate Model of Electron Populations for Non-linear High-Fluence X-ray Absorption Near-Edge Spectra

论文作者

Engel, Robin Y., Scholz, Markus, Schunck, Jan O., Beye, Martin

论文摘要

从自由电子激光器(FEL)吸收聚焦的飞秒X射线脉冲可以导致固体中极端的电子激发。这种激发在脉冲持续时间内驱动电子系统的变化,并且脉冲的总体吸收变为通量依赖性。因此,在边缘光谱(XANES)附近的Vuly依赖性非线性X射线吸收对在几年的时间表上费米水平周围的价激发动力学敏感。在这里,我们基于建立的物理机制提出了一个简化的速率模型,以描述电子系统的演变。我们构建了时间和空间差异,以进行共振吸收,刺激的发射,非谐波吸收,螺旋螺旋腐烂,价带热化和自由电子的散射级联反应。现象学速率模型方法提供了直接理解每个物理过程如何有助于在XANES测量中观察到的通量依赖性变化。如果不考虑其对状态密度的依赖性变化,该模型与金属镍在超过三个数量级上的实验结果表现出良好的一致性,从而确立了电子重新分布,这是高流动率在高流量下非线性吸收变化的主要驱动因素。尽管在共振的最接近的附近,必须采用更复杂的方法来描述其依赖性依赖性变化的剩余差异,但所证明的能力描述了光谱变化到极端流动性的能力,可以在激烈的核心激发后对复杂动态进行基本的见解,并为未来的feel实验的设计和评估提供了一个重要的工具,以实现未来的x-Rean x-riNear x-riNear x-rien x-ray x-ray x-ray x-ray x-ray x-ray x-ray x-ray x-ray x-ray x-ray x-ray x-ray。

Absorbing a focused, femtosecond X-ray pulse from a Free-Electron Laser (FEL) can lead to extreme electronic excitations in solids. This excitation drives changes of the electronic system over the course of the pulse duration and the overall absorption of the pulse becomes fluence-dependent. Thus, fluence-dependent non-linear X-ray Absorption Near Edge Spectroscopy (XANES) is sensitive to the valence excitation dynamics around the Fermi level on the few-femtosecond timescale. Here we present a simplified rate model based on well-established physical mechanisms to describe the evolution of the electronic system. We construct temporal and spatial differentials for the processes of resonant absorption, stimulated emission, non-resonant absorption, Auger decay, valence band thermalization and scattering cascades of free electrons. The phenomenological rate model approach provides a direct understanding how each physical process contributes to the fluence-dependent changes observed in XANES measurements. Without accounting for fluence-dependent changes to the density of states, the model shows good agreement with experimental results on metallic nickel over more than three orders of magnitude in fluence, establishing electron redistribution as the main driver of non-linear absorption changes at high fluences. Although in the closest vicinity of the resonance, more complex approaches are necessary to describe remaining discrepancies of the fluence-dependence changes, the demonstrated capability to describe spectral changes up to extreme fluences yields fundamental insights into the complex dynamics after intense core excitation and provides an important tool for the design and evaluation of future FEL experiments, in particular for the development of non-linear X-ray spectroscopy.

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