Continuum-electron interferometry for enhancement of photoelectron circular dichroism and measurement of bound, free, and mixed contributions to chiral response

TL;DR

This paper introduces a novel photoelectron interferometry technique using XUV and IR pulses to control and analyze chiral responses in molecules, enabling time-resolved insights into bound and continuum state contributions to PECD.

Contribution

It presents a new method for controlling and dissecting chiral photoelectron signals using laser-assisted interferometry with simple delay adjustments.

Findings

The chiral signal magnitude is controlled by the delay between XUV and IR pulses.

Polarization configurations allow separation of bound and continuum state contributions.

The method is robust, versatile, and suitable for time-resolved chiral studies.

Abstract

We develop photoelectron interferometry based on laser-assisted extreme ultraviolet ionization for flexible and robust control of photoelectron circular dichroism in randomly oriented chiral molecules. A comb of XUV photons ionizes a sample of chiral molecules in the presence of a time-delayed infrared or visible laser pulse promoting interferences between components of the XUV-ionized photoelectron wave packet. In striking contrast to multicolor phase control schemes relying on pulse shaping techniques, the magnitude of the resulting chiral signal is here controlled by the time delay between the XUV and laser pulses. Furthermore, we show that the relative polarization configurations of the XUV and IR fields allows for disentangling the contributions of bound and continuum states to the chiral response. Our proposal provides a simple, robust and versatile tool for the control of photoelectron circular dichroism and experimentally feasible protocol for probing the individual contributions of bound and continuum states to the PECD in a time-resolved manner.