Stimulated X-ray Raman scattering for selective preparation of dark states bypassing optical selection rules

TL;DR

This paper introduces an X-ray stimulated Raman technique that enables selective preparation of optically dark states in molecules, bypassing traditional optical selection rules by exploiting core-level excitations.

Contribution

The work presents a novel X-ray based method to access optically forbidden states, expanding control over molecular electronic states beyond conventional optical methods.

Findings

Demonstrates feasibility of accessing dark states via X-ray stimulated Raman.

Shows potential for controlling electronic states in molecular systems.

Discusses experimental implementation and challenges.

Abstract

We present an X-ray based stimulated Raman approach to control the preparation of optically dark electronic states in generic molecular systems. Leveraging on the unique properties of core-level excited states, we demonstrate that optically forbidden transitions between singlet states, or between singlet and triplet states are made accessible. Two molecular systems are studied as a test-bed of the proposed approach, and its experimental feasibility is eventually discussed.