Laser Control of Electronic Exchange Interaction within a Molecule

• Main Authors: Amberg, S. (Author), Aufleger, L. (Author), Ding, T. (Author), Haverkort, M.W (Author), Heinze, S. (Author), Henrich, F. (Author), Magunia, A. (Author), Mollov, N. (Author), Ott, C. (Author), Pfeifer, T. (Author), Rebholz, M. (Author), Rupprecht, P. (Author)
• Format: Article
• Language: English
• Published: American Physical Society 2022
• Subjects: Core hole; Electronic interactions; Exchange energy; Exchange interactions; Excited-states; Infrared intensity; Infrared-laser; Intense laser field; Laser control; Molecules; Proof of principles; Soft-X-ray lasers
• Online Access: View Fulltext in Publisher
• ISBN: 00319007 (ISSN)
• DOI: 10.1103/PhysRevLett.128.153001

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. © 2022 authors. Published by the American Physical Society.