Laser Control of Electronic Exchange Interaction within a Molecule

Abstract

Electronic interactions play a fundamental role in atoms, molecular structure and reactivity. We introduce a general concept to control the effective electronic exchange interaction with intense laser fields via coupling to excited states. As an experimental proof of principle, we study the SF6 molecule using a combination of soft x-ray and infrared (IR) laser pulses. Increasing the IR intensity increases the effective exchange energy of the core hole with the excited electron by 50%, as observed by a characteristic spin-orbit branching ratio change. This work demonstrates altering electronic interactions by targeting many-particle quantum properties.