Direct Monitoring of Conical Intersection Passage via Electronic Coherences in Twisted X-Ray Diffraction

Haiwang Yong (1) , Jérémy Rouxel (2) , Daniel Keefer (1) , Shaul Mukamel (1)

1 UC Irvine - University of California [Irvine]
2 LHC - Laboratoire Hubert Curien

Quantum coherences in electronic motions play a critical role in determining the pathways and outcomes of virtually all photophysical and photochemical molecular processes. However, the direct observation of electronic coherences in the vicinity of conical intersections remains a formidable challenge. We propose a novel time-resolved twisted x-ray diffraction technique that can directly monitor the electronic coherences created as the molecule passes through a conical intersection. We show that the contribution of electronic populations to this signal is canceled out when using twisted x-ray beams that carry a light orbital angular momentum, providing a direct measurement of transient electronic coherences in gas-phase molecul

Domaines: Physique [physics]

Haiwang Yong, Jérémy Rouxel, Daniel Keefer, Shaul Mukamel. Direct Monitoring of Conical Intersection Passage via Electronic Coherences in Twisted X-Ray Diffraction. Physical Review Letters, 2022, 129 (10), pp.103001. ⟨10.1103/PhysRevLett.129.103001⟩. ⟨hal-03947350⟩