Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation
Abstract 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...
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| Language: | English |
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Wiley-VCH
2025-02-01
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| Series: | Advanced Physics Research |
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| Online Access: | https://doi.org/10.1002/apxr.202400106 |
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| author | Arshak A. Tsaturyan Elena Kachan Razvan Stoian Jean‐Philippe Colombier |
| author_facet | Arshak A. Tsaturyan Elena Kachan Razvan Stoian Jean‐Philippe Colombier |
| author_sort | Arshak A. Tsaturyan |
| collection | DOAJ |
| description | Abstract 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. |
| format | Article |
| id | doaj-art-549c3b96367e4e1b8ecafd122c6e73c8 |
| institution | DOAJ |
| issn | 2751-1200 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Advanced Physics Research |
| spelling | doaj-art-549c3b96367e4e1b8ecafd122c6e73c82025-08-20T03:05:39ZengWiley-VCHAdvanced Physics Research2751-12002025-02-0142n/an/a10.1002/apxr.202400106Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser IrradiationArshak A. Tsaturyan0Elena Kachan1Razvan Stoian2Jean‐Philippe Colombier3Université Jean Monnet Saint‐Etienne, CNRS Institut d'Optique Graduate School Laboratoire Hubert Curien UMR 5516 Saint‐Etienne F‐42023 FranceUniversité Jean Monnet Saint‐Etienne, CNRS Institut d'Optique Graduate School Laboratoire Hubert Curien UMR 5516 Saint‐Etienne F‐42023 FranceUniversité Jean Monnet Saint‐Etienne, CNRS Institut d'Optique Graduate School Laboratoire Hubert Curien UMR 5516 Saint‐Etienne F‐42023 FranceUniversité Jean Monnet Saint‐Etienne, CNRS Institut d'Optique Graduate School Laboratoire Hubert Curien UMR 5516 Saint‐Etienne F‐42023 FranceAbstract 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.https://doi.org/10.1002/apxr.202400106ab initio molecular dynamicsBSEGWlaser excitationoptical propertiessilica |
| spellingShingle | Arshak A. Tsaturyan Elena Kachan Razvan Stoian Jean‐Philippe Colombier Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation Advanced Physics Research ab initio molecular dynamics BSE GW laser excitation optical properties silica |
| title | Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation |
| title_full | Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation |
| title_fullStr | Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation |
| title_full_unstemmed | Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation |
| title_short | Excited‐State Dynamics and Optical Properties of Silica Under Ultrafast Laser Irradiation |
| title_sort | excited state dynamics and optical properties of silica under ultrafast laser irradiation |
| topic | ab initio molecular dynamics BSE GW laser excitation optical properties silica |
| url | https://doi.org/10.1002/apxr.202400106 |
| work_keys_str_mv | AT arshakatsaturyan excitedstatedynamicsandopticalpropertiesofsilicaunderultrafastlaserirradiation AT elenakachan excitedstatedynamicsandopticalpropertiesofsilicaunderultrafastlaserirradiation AT razvanstoian excitedstatedynamicsandopticalpropertiesofsilicaunderultrafastlaserirradiation AT jeanphilippecolombier excitedstatedynamicsandopticalpropertiesofsilicaunderultrafastlaserirradiation |