通过x射线光电子能谱的时间相关性揭示的实时界面电子动力学。

IF 2.3 2区 物理与天体物理 Q3 CHEMISTRY, PHYSICAL
Structural Dynamics-Us Pub Date : 2021-07-08 eCollection Date: 2021-07-01 DOI:10.1063/4.0000099
Felix Brausse, Mario Borgwardt, Johannes Mahl, Matthew Fraund, Friedrich Roth, Monika Blum, Wolfgang Eberhardt, Oliver Gessner
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引用次数: 1

摘要

我们提出了一种通过x射线光电子能谱(XPS)信号的时间相关性来监测界面系统动力学的新技术。迄今为止,绝大多数时间分辨x射线光谱技术都依赖于泵浦-探针方案,在这种方案中,样品被泵浦脉冲激发出平衡状态,随后的动力学由探测脉冲监测,探测脉冲到达一系列明确定义的相对于激发的延迟。根据定义,这种方法仅限于可以直接或间接由光启动的过程。它不能进入自发动力学或微观波动的系综在化学或热平衡。启用此功能需要在实时(实验室)时间内以高时间分辨率执行测量,并且最终不需要定义良好的触发事件。本文介绍的时间相关XPS技术是实现这一目标的第一步。基于相关的技术是通过扩展现有的光激光泵浦/多重x射线探针装置来实现的,该装置能够记录每个被探测光电子的动能和绝对到达时间。利用传统的泵浦探针数据采集和基于实验室时间的新技术,在一个典型的时间分辨XPS实验中,通过监测能量依赖的周期性信号调制来对该方法进行基准测试。这两次测量得出了相同的结果。这一发现为通过基于时间相关的XPS测量研究表面和界面的平衡动力学提供了一个关键的里程碑。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy.

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy.

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy.

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy.

We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump-probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump-probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.

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来源期刊
Structural Dynamics-Us
Structural Dynamics-Us CHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
CiteScore
5.50
自引率
3.60%
发文量
24
审稿时长
16 weeks
期刊介绍: Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods. The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as: Time-resolved X-ray and electron diffraction and scattering, Coherent diffractive imaging, Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.), Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy, Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.), Multidimensional spectroscopies in the infrared, the visible and the ultraviolet, Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains, Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals. These new methods are enabled by new instrumentation, such as: X-ray free electron lasers, which provide flux, coherence, and time resolution, New sources of ultrashort electron pulses, New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources, New sources of ultrashort infrared and terahertz (THz) radiation, New detectors for X-rays and electrons, New sample handling and delivery schemes, New computational capabilities.
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