A time-dependent Schr\"odinger equation for molecular core-hole dynamics

TL;DR

This paper develops a time-dependent Schrödinger equation framework to model the ultrafast electron and nuclear dynamics involved in core-hole decay processes induced by femtosecond x-ray pulses.

Contribution

It introduces a novel theoretical approach that captures the real-time evolution of core-hole dynamics during x-ray interactions.

Findings

Provides a comprehensive time-dependent model for core-hole decay.

Enables simulation of electron and nuclear relaxation processes.

Facilitates understanding of ultrafast x-ray spectroscopy phenomena.

Abstract

X-ray spectroscopy is an important tool for the investigation of matter. X rays primarily interact with inner-shell electrons creating core (inner-shell) holes that will decay on the time scale of attoseconds to few femtoseconds through electron relaxations involving the emission of a photon or an electron. The advent of femtosecond x-ray pulses expands x-ray spectroscopy to the time domain and will eventually allow the control of core-hole population on timescales comparable to core-vacancy lifetimes. For both cases, a theoretical approach that accounts for the x-ray interaction while the electron relaxations occur is required. Here we describe a time-dependent framework, based on solving the time-dependent Schr\"odinger equation, that is suitable for describing the induced electron and nuclear dynamics.