Quantum control of photoelectron circular dichroism

TL;DR

This paper demonstrates a method to coherently control photoelectron circular dichroism in chiral molecules by exploiting quantum interference among multiple ionization pathways, significantly enhancing the chiral signal.

Contribution

It introduces a novel quantum interference scheme using a finite manifold of indistinguishable pathways to maximize dichroism, outperforming previous methods.

Findings

Maximized chiral signal through interference of multiple pathways.

Outperformed bichromatic and sequential ionization schemes.

Enhanced sensitivity in chiral molecule detection.

Abstract

We demonstrate coherent control over the photoelectron circular dichroism in randomly oriented chiral molecules, based on quantum interference between multiple photoionization pathways. To significantly enhance the chiral signature, we use a finite manifold of indistinguishable $(1+1^\prime)$ REMPI pathways interfering at a common photoelectron energy but probing different intermediate states. We show that this coherent control mechanism maximizes the number of molecular states that constructively contribute to the dichroism at an optimal photoelectron energy and thus outperforms other schemes, including interference between opposite-parity pathways driven by bichromatic $({\omega}, 2{\omega})$ fields as well as sequential pump-probe ionization.