Preparation and control of electronic wave packets in neutral molecules via attosecond x-ray processes
Abstract
We present a perturbative framework for computing the dynamics of an electronic wave packet launched by an attosecond x-ray pulse in a neutral molecule. The x-ray pulse excites the molecule via both x-ray absorption and Impulsive Stimulated X-ray Raman Scattering (ISXRS), coherently populating both the core-excited states and valence-excited states. We describe the electronic structure within the Equation-of-Motion Coupled-Cluster framework, adopting a compact representation of the sum over states expression characterizing the second-order perturbative description of ISXRS. We study the coherent electronic dynamics in OCS and oxazole utilizing the time-dependent difference electron density, decomposing it in terms of its perturbative components. While the core-excited components dominate the initial stages of the dynamics, the valence-excited components dominate the electronic dynamics on a longer time scale. The pulse polarization controls the symmetry of the states included in the wave packet. We show how the spatial symmetry of the states plays a role in shaping the spatial properties of charge migration. The atom-specificity of the ISXRS process translates directly into the initial localization of the wave packet. This determines the starting point of charge migration, shaping its subsequent evolution.
Versions
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BibTeX
@misc{rossi2026preparation,
title = {{Preparation and control of electronic wave packets in neutral molecules via attosecond x-ray processes}},
author = {Emanuele Rossi and Stasis Chuchurka and Kaushik D. Nanda and Anna I. Krylov and Nina Rohringer and Robin Santra},
howpublished = {arXiv},
year = {2026},
month = jun,
doi = {10.48550/arxiv.2606.22102},
eprint = {2606.22102},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2606.22102},
note = {CC BY-SA 4.0},
}
RIS
TY - UNPB
TI - Preparation and control of electronic wave packets in neutral molecules via attosecond x-ray processes
AU - Emanuele Rossi
AU - Stasis Chuchurka
AU - Kaushik D. Nanda
AU - Anna I. Krylov
AU - Nina Rohringer
AU - Robin Santra
PY - 2026
DA - 2026/06/20
PB - arXiv
DO - 10.48550/arxiv.2606.22102
UR - https://arxiv.org/abs/2606.22102
AB - We present a perturbative framework for computing the dynamics of an electronic wave packet launched by an attosecond x-ray pulse in a neutral molecule. The x-ray pulse excites the molecule via both x-ray absorption and Impulsive Stimulated X-ray Raman Scattering (ISXRS), coherently populating both the core-excited states and valence-excited states. We describe the electronic structure within the Equation-of-Motion Coupled-Cluster framework, adopting a compact representation of the sum over states expression characterizing the second-order perturbative description of ISXRS. We study the coherent electronic dynamics in OCS and oxazole utilizing the time-dependent difference electron density, decomposing it in terms of its perturbative components. While the core-excited components dominate the initial stages of the dynamics, the valence-excited components dominate the electronic dynamics on a longer time scale. The pulse polarization controls the symmetry of the states included in the wave packet. We show how the spatial symmetry of the states plays a role in shaping the spatial properties of charge migration. The atom-specificity of the ISXRS process translates directly into the initial localization of the wave packet. This determines the starting point of charge migration, shaping its subsequent evolution.
ER -