Unraveling intra-pulse dynamics and fast energy transfer in silica glass: A pathway for smart processing using ultrafast lasers

• Applicant: Dr. Tamas Nagy
• Subject Area: Experimental Condensed Matter Physics ; Optics, Quantum Optics and Physics of Atoms, Molecules and Plasmas ; Theoretical Condensed Matter Physics
• Term: from 2019 to 2025
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 431657459

• Final Report Year: 2025

Final Report Abstract

Unraveling intra-pulse dynamics in silica glass for smart ultrafast laser processing. The INTRALAS project aimed to revolutionize material processing tools by leveraging ultrafast laser structuring. This technique is essential for advancing nanoscale 3D glass processing. By optimizing yield and scale, smart processing concepts have emerged using spatiotemporal beam design tuned to material responses. Understanding primary electronic processes for energy deposition and relaxation paths for structural modifications is crucial. Controlling the sequence of processes during irradiation (intrapulse) is vital. Our goal was to define intra-pulse electronic processes and electron-matrix dynamics during the excitation phase, coupling timeresolved spectral interferometry and vibrational spectroscopy with time-dependent ab initio (DFT) simulations. Innovative VUV near-edge fs-resolved probing and calculations of electron screening effects, alongside IR spectroscopy of matrix markers, enabled access to band-gap dynamics and energy coupling to the matrix. These are key elements for smart processing strategies, paving the way for significant advancements in manufacturing and novel material properties. Innovative Techniques in Laser-Material Interaction Studies. To achieve the project's objectives, a combination of advanced methods and technologies was employed. The research utilized time-resolved spectral interferometry and vibrational spectroscopy, coupled with time-dependent ab initio (DFT) simulations. These techniques allowed for detailed analysis of intra-pulse electronic processes and electron-matrix dynamics. Additionally, innovative VUV near-edge femtosecond-resolved probing and calculations of electron screening effects were conducted alongside IR spectroscopy of matrix markers. These methodologies provided critical insights into band-gap dynamics and energy coupling within the matrix, enabling the development of smart processing strategies tailored to specific material responses. Project Main Results: The INTRALAS project yielded several significant outcomes, including novel insights into ultrafast laser-material interactions and the development of advanced processing techniques for glass at the nanoscale. The research facilitated new applications in precision manufacturing and material science. International partnerships were established, leading to collaborative research opportunities and the potential for new contracts and start-ups. The project's findings have set the stage for future innovations in smart material processing, enhancing competitiveness in related industries. INTRALAS research has yielded multiple high-impact publications detailing breakthroughs in ultrafast laser structuring and nanoscale processing, furthering scientific knowledge and practical applications in material science.

Publications

• Full Explicit Numerical Modeling in Time-Domain for Nonlinear Electromagnetics Simulations in Ultrafast Laser Nanostructuring. Applied Sciences, 11(16), 7429.
  Moreno, Enrique; Nguyen, Huu Dat; Stoian, Razvan & Colombier, Jean-Philippe
  
• French Photonics Days, Saint-Etienne, France Octobre (2022). Structuration des surfaces par laser à des échelles extrêmes
  J.P. Colombier
  
• Laser’AP, Laser et Applications, Semur-en-Auxois, France Octobre (2022). Modélisation de l’interaction laser ultrabref-matière
  J.P. Colombier
  
• Laser’AP, Laser et Applications, Semur-en-Auxois, France Octobre (2022). Structuration de surface par laser de l’excitation à son auto-organisation
  J.P. Colombier
  
• Ultrafast bandgap narrowing and cohesion loss of photoexcited fused silica. The Journal of Chemical Physics, 156(22).
  Tsaturyan, Arshak; Kachan, Elena; Stoian, Razvan & Colombier, Jean-Philippe
  
• 44th PIERS (PhotonIcs and Electromagnetics Research Symposium) July (2023), Prague, Czech Republic, Polarization and complexity effects on ultrafast laser-induced nanoscale surface structuring. [Invited]
  J.P.Colombier, E. Moreno, A. Rudenko & V. Fedorov
  
• First-principles study of ultrafast bandgap dynamics in laser-excited α-quartz. The European Physical Journal Special Topics, 232(13), 2241-2245.
  Kachan, Elena; Tsaturyan, Arshak; Stoian, Razvan & Colombier, Jean-Philippe
  
• Journée Thématique Micro/Nano-structuration par laser, Rennes, France Septembre, (2023). Organisation spontanée à l’échelle nanométrique induite par impulsions laser ultrabrèves
  J.P. Colombier
  
• Micromachining of Transparent Solids with Few-Cycle Laser Pulses. 2023 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC), 1-1. IEEE.
  Andrade, José R.C.; Sneftrup, Peter; de Michele, Vincenzo; Rammelt, Laura; Jürgens, Peter; Vrakking, Marc; Nagy, Tamas & Mermillod-Blondin, Alexandre
  
• Procédés Laser pour l’Industrie, Rennes, France Septembre (2023). Spontaneous surface organization induced by ultra-short laser pulses
  J.P. Colombier
  
• High-energy, few-cycle light pulses tunable across the vacuum ultraviolet
  Andrade J. R. C., Kretschmar, M., Danylo, R., Carlström, S., Witting, T., Mermillod-Blondin, A., Patchkovskii, S., Ivanov, M.Y., Vrakking, J.J.M., Rouzée, A. & Nagy, T.
  
• Probing nonlinear excitation conditions: photoluminescence and nonlinear absorption studies in laser-irradiated dielectrics. Applied Physics A, 130(3).
  Sneftrup, Peter S.; Juergens, Peter; Michele, Vincenzo De; Andrade, José R. C.; Vrakking, Marc J. J.; Balling, Peter & Mermillod-Blondin, Alexandre
  
• Quantitative Mapping of Transient Thermodynamic States in Ultrafast Laser Nanostructuring of Quartz. Ultrafast Science, 6.
  Nguyen, H. D.; Tsaturyan, A.; Joao, S. Sao; Dwivedi, R.; Yedigaryan, A.; D.’Amico, C.; Kachan, E.; Colombier, J. P.; Kermouche, G. & Stoian, R.
  
• The quest for resolution: a dynamic view on ultrafast laser extreme volume nanostructuring. High-Power Laser Ablation VIII, PC129390G (2024) [Invited]
  R. Stoian
  
• «Amnesia of previous nonlinear plasma formation in fused silica excited by few-cycle pulses», in ultrafast phenomena conference (2024)
  Andrade, J. R. C., Fedorov, V., De Michele, V., Sneftrup, P., Jürgens, P., Rammelt, L., Vrakking, M. J. J., Razvan, S., Colombier, J.-P., Nagy, T. & Mermillod-Blondin, A.
  
• «Excited-state bandgap dynamics in silica from first principles», High-Power Laser Ablation VIII, PC129391B (2024) [Invited]
  E. Kachan, A. Tsaturyan, R. Stoian & J.P. Colombier
  
• «Ultrafast laser-irradiated silica: from excited-state dynamics to nanostructuring», Spie Laser Damage (2024) [Invited]
  J.P. Colombier, A. Tsaturyan, A.. Rudenko, E. Kachan & R. Stoian