Photoelectron circular dichroism with two overlapping laser pulses of carrier frequencies $\omega$ and $2\omega$ linearly polarized in two mutually-orthogonal directions

TL;DR

This paper theoretically demonstrates a method to induce and control photoelectron circular dichroism (PECD) using two overlapping linearly polarized laser pulses of different frequencies and orthogonal polarization directions, revealing phase- and enantiomer-sensitive effects.

Contribution

It introduces a novel approach to access PECD with a single experiment using two orthogonally polarized pulses of different frequencies, providing new insights into controlling chiral photoelectron emission.

Findings

Strong forward/backward asymmetry in photoelectron emission predicted

PECD effect is phase- and enantiomer-sensitive

Optimization possible by varying pulse intensities

Abstract

Using a model methane-like chiral system, we theoretically demonstrate a possibility to access photoelectron circular dichroism (PECD) by a single experiment with two overlapping laser pulses of carrier frequencies $\omega$ and $2\omega$, which are linearly polarized in two mutually-orthogonal directions. Depending on the relative phase, the resulting electric field can be tailored to have two different rotational directions in the upper and lower hemispheres along the polarization of the $\omega$-pulse. We predict a strong forward/backward asymmetry in the emission of photoelectrons from randomly oriented samples, which has an opposite sign in the upper and lower hemispheres. The predicted PECD effect is phase- and enantiomer-sensitive, providing new insight in this fascinating fundamental phenomenon. The effect can be optimized by varying relative intensities of the pulses.