Excited-State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation

被引:1
|
作者
Tsaturyan, Arshak A. [1 ]
Kachan, Elena [1 ]
Stoian, Razvan [1 ]
Colombier, Jean-Philippe [1 ]
机构
[1] Univ Jean Monnet St Etienne, CNRS, UMR 5516, Inst Opt Grad Sch,Lab Hubert Curien, F-42023 St Etienne, France
来源
ADVANCED PHYSICS RESEARCH | 2025年 / 4卷 / 02期
关键词
ab initio molecular dynamics; BSE; GW; laser excitation; optical properties; silica; ELECTRONIC-STRUCTURE;
D O I
10.1002/apxr.202400106
中图分类号
O59 [应用物理学];
学科分类号
摘要
Excited by intense infrared ultrafast light pulses, a wide bandgap material undergoes nonlinear ionization, generating a high density of free electrons in conduction states. As a result, the electronic band structure is critically modified and the bandgap shrinks. This induces rapid changes in optical properties, dramatically affecting the absorption spectrum during light coupling to the dielectric surface or during nonlinear propagation inside the bulk. This study analyzes the structural behavior and the modification of the optical properties of laser-excited silica glass at the molecular cluster level through first-principles simulations. Employing density functional theory and the GW approximations for band structure under nonequilibrium conditions, alongside the Bethe-Salpeter equation, the dynamics of the optical properties of fused silica are comprehensively explored. The behavior of excited fused silica in a wide photon energy range (from a few to 20 eV) is thus predicted. Laser-induced electron excitation triggers a redistribution of charges between oxygen and silicon atoms, accompanied by a significant increase in electronic pressure, local atomic structure rearrangement, and material expansion. Molecular dynamics simulations offer a temporal perspective on the excited state dynamics, unveiling the intricate interplay between electronic and atomic effects on bandgap evolution. The analysis sheds light on excitonic resonances, intraband and interband transitions in fused silica under ultrafast laser irradiation, providing valuable insights into its excited state behavior and optical properties.
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页数:7
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