Simulations of Attosecond Metallization in Quartz and Diamond Probed with Inner-Shell Transient Absorption Spectroscopy

Kurkowski, Lucas; Sissay, Adonay; Yang, Mengqi; Meyer, Alexander; Lopata, Kenneth

doi:10.1021/acs.jpca.4c05137

Title: Simulations of Attosecond Metallization in Quartz and Diamond Probed with Inner-Shell Transient Absorption Spectroscopy

Journal Article · 13 January 2025 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI: https://doi.org/10.1021/acs.jpca.4c05137 · OSTI ID:2506694

^[1]; Sissay, Adonay ^[1]; Yang, Mengqi ^[1]; Meyer, Alexander ^[1];

^[1]

Louisiana State University, Baton Rouge, LA (United States)

When dielectrics are hit with intense infrared (IR) laser pulses, transient metalization can occur. The initial attosecond dynamics behind this metallization are not entirely understood. Therefore, simulations are needed to understand this process and to help interpret experimental observations of it, such as with attosecond transient absorption (ATA). In this paper, we present first-principles simulations of ATA based on bulk-mimicking clusters and real-time time-dependent density functional theory (RT-TDDFT), with Koopmans-tuned range-separated hybrid functionals and Gaussian basis sets. Our method gives good agreement with the experiment for the breakdown threshold in silica and diamond. This breakdown voltage corresponds to a Keldysh parameter of approximately one and thus involves a transition to a regime where the dynamics are driven by tunneling. Pumping at an amplitude just below this value causes a mixture of multiphoton and tunneling excitations across the band gap to occur. The computed extreme ultraviolet and X-ray attosecond transient spectra also agree well with the experiment and show a decrease in optical density due to the transient population of the conduction band from the IR field. First-principles approaches such as this are valuable for interpreting the complicated modulations in a spectrum and for guiding future attosecond experiments on solids.

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Research Organization:: Louisiana State University, Baton Rouge, LA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0024484; SC0017868

OSTI ID:: 2506694

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 3 Vol. 129; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Simulations of Attosecond Metallization in Quartz and Diamond Probed with Inner-Shell Transient Absorption Spectroscopy

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