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Transient optics of gold during laser irradiation: From first principles to experiment

DOI:10.1103/PhysRevB.101.165140 期刊:Physical Review B 出版年份:2020 更新时间:2025-09-23 15:19:57
摘要: Intense femtosecond laser pulses can induce dramatic changes on different properties of materials. Laser induced changes of the optical properties are particularly relevant, since they can lead to a modi?cation of the amount of energy that the material absorbs from the laser pulse. In noble metals, changes of re?ectivity upon femtosecond laser illumination are expected to be strong due to the excitation of d electrons. In this work we perform measurements of the re?ectivity of laser excited gold in the infrared and in the ultraviolet range, respectively. We ?nd a remarkable dependence of the re?ectivity on laser ?uence, which is in turn different in both ranges of photon energy. In order to understand the behavior of the re?ectivity in laser excited solids and to explain our measured re?ectivity curves we develop a theoretical scheme in the framework of the two-temperature model with the electronic temperature as the key parameter. Our approach is based on all-electron calculations of the interband contribution to the re?ectivity and a careful determination of the intraband, Drude-like terms and a realistic model for the space and time resolved energy transfer from a Gaussian laser pulse into the electronic system. We obtain very good agreement between experiment and theory and identify the main mechanisms for re?ectivity changes as a function of laser ?uence.
作者: A. Blumenstein,E. S. Zijlstra,D. S. Ivanov,S. T. Weber,T. Zier,F. Kleinwort,B. Rethfeld,J. Ihlemann,P. Simon,M. E. Garcia
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Investigating the transient changes of the optical properties, specifically re?ectivity, of gold under intense femtosecond laser irradiation, and understanding the mechanisms behind these changes.

The study provides a comprehensive understanding of the transient changes of collision frequencies and their dependence on temperature for the description of energy absorption in laser-excited gold. The approach represents a powerful tool for describing the most general case of laser self-re?ectivity and its precise absorbed energy at a certain time and location for elevated electronic temperatures.

The study does not account for effects like two photon absorption, fluorescence, or an onset of a plasma state at very high peak fluences. It also neglects effects of a non-Fermi distribution of the excited electrons.

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