| Autor: |
Woźniak, Aleksander P., Adamowicz, Ludwik, Pedersen, Thomas Bondo, Kvaal, Simen |
| Rok vydání: |
2024 |
| Předmět: |
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| Druh dokumentu: |
Working Paper |
| DOI: |
10.1021/acs.jpca.4c00364 |
| Popis: |
The assumptions underpinning the adiabatic Born-Oppenheimer (BO) approximation are broken for molecules interacting with attosecond laser pulses, which generate complicated coupled electronic-nuclear wavepackets that generally will have components of electronic and dissociation continua as well as bound-state contributions. The conceptually most straightforward way to overcome this challenge is to treat the electronic and nuclear degrees of freedom on equal quantum-mechanical footing by not invoking the BO approximation at all. Explicitly correlated Gaussian (ECG) basis functions have proved successful for non-BO calculations of stationary molecular states and energies, reproducing rovibrational absorption spectra with very high accuracy. In this paper, we present a proof-of-principle study of the ability of fully flexible ECGs (FFECGs) to capture the intricate electronic and rovibrational dynamics generated by short, high-intensity laser pulses. By fitting linear combinations of FFECGs to accurate wave function histories obtained on a large real-space grid for a regularized 2D model of the hydrogen atom and for the 2D Morse potential we demonstrate that FFECGs provide a very compact description of laser-driven electronic and rovibrational dynamics. |
| Databáze: |
arXiv |
| Externí odkaz: |
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