All-electron molecular tunnel ionization based on the weak-field asymptotic theory in the integral representation

Wahyutama, Imam S.; Jayasinghe, Denawakage D.; Mauger, François; Lopata, Kenneth; Schafer, Kenneth J.

doi:10.1103/physreva.111.013117

Title: All-electron molecular tunnel ionization based on the weak-field asymptotic theory in the integral representation

Journal Article · 26 January 2025 · Physical Review A

DOI: https://doi.org/10.1103/physreva.111.013117 · OSTI ID:2510981

^[1]; Jayasinghe, Denawakage D. ^[2];

^[2]; Lopata, Kenneth ^[2];

^[2]

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

Tunnel ionization (TI) underlies many important ultrafast processes, such as high-harmonic generation andstrong-field ionization. Among the existing theories for TI, many-electron weak-field asymptotic theory (ME-WFAT) is by design capable of accurately treating many-electron effects in TI. An earlier version of ME-WFATrelied on an accurate representation of the asymptotic tail of the orbitals, which hindered its implementation inGaussian-basis-set-based quantum chemistry programs. In this work, we reformulate ME-WFAT in the integralrepresentation, which makes the quality of the asymptotic tail much less critical, hence greatly facilitating itsimplementation in standard quantum chemistry packages. The integral reformulation introduced here is thereforemuch more robust when applied to molecules with arbitrary geometry. Here, we present several case studies, amongwhich is the CO molecule where some earlier theories disagree with experiments. Here we find that ME-WFATproduces the largest ionization probability when the field points from C to O, as experiments suggest. Anattractive feature of ME-WFAT is that it can be used with various types of multielectron methods whether ofdensity functional or multiconfiguration types, this inturn facilitates tunnel ionization calculation in systems exhibiting a strong multireference character.

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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:: SC0012462

OSTI ID:: 2510981

Journal Information:: Physical Review A, Journal Name: Physical Review A Journal Issue: 1 Vol. 111; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: All-electron molecular tunnel ionization based on the weak-field asymptotic theory in the integral representation

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