氧化铈光激发引起的电子和结构修饰的超快动力学

IF 5.3 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Samuele Pelatti, Eleonora Spurio, Daniele Catone, Patrick O'Keeffe, Stefano Turchini, Giuseppe Ammirati, Fulvio Paleari, Daniele Varsano, Stefania Benedetti, Alessandro di Bona, Sergio D'Addato, Yifeng Jiang, Peter Zalden, Yohei Uemura, Hao Wang, Doriana Vinci, Xinchao Huang, Frederico Lima, Mykola Biednov, Dmitry Khakhulin, Christopher Jackson Milne, Federico Boscherini, Paola Luches
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引用次数: 0

摘要

利用x射线自由电子激光器的泵浦探针光谱为光催化剂在光激发后发生的过程提供了特定元素的见解,这对于合理优化这些材料的效率至关重要。本研究利用x射线自由电子激光器,在cel3边缘的近边缘和扩展能量范围内,利用超快泵浦探针x射线吸收光谱(XAS)研究了化学计量氧化铈薄膜在光激发后的电子和原子结构的动态演变。结果显示,在最初的几百飞秒内出现了一个快速的弛豫途径,随后形成了一个寿命约为几百皮秒的激发态。在扩展能量范围内对泵浦探针XAS的分析发现了与光致小极化子态形成一致的结构畸变。观察到的光致电子和结构变化之间的时间相关性进一步加强了光致极化子形成的假设。约束密度泛函理论模拟提供了对光激发材料中的电子修饰和结构扭曲的见解。讨论了观察到的过程对材料功能的影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Ultrafast Dynamics of Electronic and Structural Modifications Induced by Photoexcitation in Cerium Oxide

Ultrafast Dynamics of Electronic and Structural Modifications Induced by Photoexcitation in Cerium Oxide
Pump-probe spectroscopies utilizing X-ray free-electron lasers offer element-specific insights into the processes occurring in photocatalysts following photoexcitation, which are essential for the rational optimization of the efficiency of these materials. This study examines the dynamic evolution of the electronic and atomic structure in stoichiometric cerium oxide films following photoexcitation, employing ultrafast pump-probe X-ray absorption spectroscopy (XAS) at the Ce L3 edge in both the near-edge and extended energy ranges using an X-ray free electron laser. The results reveal a rapid relaxation pathway occurring within the first few hundred femtoseconds, followed by the formation of an excited state with a lifetime on the order of hundreds of picoseconds. The analysis of pump-probe XAS in the extended energy range identifies a structural distortion consistent with the formation of a photoinduced small polaron state. The observed time correlation between the photoinduced electronic and structural changes further reinforces the hypothesis of photoinduced polaron formation. Constrained density functional theory simulations offer insights into the electronic modifications and structural distortions in the photoexcited material. The consequences of the observed processes on material functionality are discussed.
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来源期刊
Advanced Electronic Materials
Advanced Electronic Materials NANOSCIENCE & NANOTECHNOLOGYMATERIALS SCIE-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
11.00
自引率
3.20%
发文量
433
期刊介绍: Advanced Electronic Materials is an interdisciplinary forum for peer-reviewed, high-quality, high-impact research in the fields of materials science, physics, and engineering of electronic and magnetic materials. It includes research on physics and physical properties of electronic and magnetic materials, spintronics, electronics, device physics and engineering, micro- and nano-electromechanical systems, and organic electronics, in addition to fundamental research.
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