Atomic and Molecular Systems Driven by Intense Chaotic Light

TL;DR

This paper explores how intense chaotic light can enhance photoionization in atomic and molecular systems, revealing optimal conditions and mechanisms for control using spectrally-shaped and high harmonic generated chaotic fields.

Contribution

It introduces a theoretical analysis of photoionization enhancement via shaped chaotic fields, including broadband and narrowband spectra, and demonstrates the effect with high harmonic synthesis.

Findings

Optimal photoionization enhancement with broadband chaotic fields.

Spectrally-shaped chaotic fields can control atomic level populations.

High harmonic generated chaotic fields also produce significant enhancement.

Abstract

We investigate dynamics of atomic and molecular systems exposed to intense, shaped chaotic fields and a weak femtosecond laser pulse theoretically. As a prototype example, the photoionization of a hydrogen atom is considered in detail. The net photoionization undergoes an optimal enhancement when a broadband chaotic field is added to the weak laser pulse. The enhanced ionization is analyzed using time-resolved wavepacket evolution and the population dynamics of the atomic levels. We elucidate the enhancement produced by spectrally-shaped chaotic fields of two different classes, one with a tunable bandwidth and another with a narrow bandwidth centered at the first atomic transition. Motivated by the large bandwidth provided in the high harmonic generation, we also demonstrate the enhancement effect exploiting chaotic fields synthesized from discrete, phase randomized, odd-order and all-order high harmonics of the driving pulse. These findings are generic and can have applications to other atomic and simple molecular systems.