Coherent Control of Ion-Photoelectron Dynamics through Rabi Oscillations: An ab initio study

TL;DR

This paper uses first-principles simulations to demonstrate how bichromatic EUV pulses can coherently control ion-photoelectron dynamics in neon by inducing Rabi oscillations between subshells, validating analytical models.

Contribution

It provides an ab initio demonstration of Rabi-driven coherence in photoionization, confirming analytical predictions and suggesting experimental feasibility with free electron lasers.

Findings

Rabi oscillations induce coherence between photoelectron wave packets

Validation of analytical models through ab initio simulations

Potential for experimental observation with FELs

Abstract

We present first-principles numerical simulations of photoionization in neon induced by bichromatic extreme ultraviolet pulses with frequencies $\omega$ and $2\omega$, specially chosen to make $\omega$ equal to the energy difference between the $2s$ and $2p$ subshells. This allows for the production of photoelectrons from the $2s$ shell by $2\omega$ pulse and from the $2p$ shell by $\omega$ pulse with the same energy. Using the multi-configurational time-dependent Hartree-Fock method, we explore how Rabi coupling between subshells generates coherence between the corresponding photoelectron wave packets. Our \textit{ab initio} calculations confirm the analytical results derived from the essential-states approach in [K. L. Ishikawa, K. C. Prince, and K. Ueda, J. Phys. Chem. A 127, 10638 (2023)], validating the theoretical predictions. Although we focus on the Ne $2p$ and $2s$ subshells, our approach is applicable to a broad range of systems exhibiting photoionization from multiple subshells. The laser parameters employed in our simulations are available in modern Free Electron Lasers (FELs), and we anticipate that this work could stimulate experimental investigations using FELs to study ion-photoelectron coherence and entanglement.