Work

Catching Conical Intersections in the Act: Monitoring Transient Electronic Coherences by Attosecond Stimulated X-Ray Raman Signals

Year: 2015

Type: article

Abstract: Conical intersections (CIs) dominate the pathways and outcomes of virtually all photophysical and photochemical molecular processes. Despite extensive experimental and theoretical effort, CIs have not been directly observed yet and the experimental evidence is being inferred from fast reaction rates and some vibrational signatures. We show that short x-ray (rather than optical) pulses can directly detect the passage through a CI with the adequate temporal and spectral sensitivity. The technique is based on a coherent Raman process that employs a composite femtosecond or attosecond x-ray pulse to detect the electronic coherences (rather than populations) that are generated as the system passes through the CI.

Source: Physical Review Letters

DOI: 10.1103/physrevlett.115.193003

Authors: Markus Kowalewski, Kochise Bennett, Konstantin E. Dorfman, Shaul Mukamel

Institution: University of California, Irvine

Language: English

Topic: Laser-Matter Interactions and Applications

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: green

Funders: National Science Foundation, U.S. Department of Energy, Alexander von Humboldt-Stiftung

Awards: TAS::89 0222::TAS - THEORY AND SIMULATION OF NONLINEAR X-RAY SPECTROSCOPY OF MOLECULES, Molecular Radiative and Relaxation Processes