Direct Monitoring of Conical Intersection Passage via Electronic Coherences in Twisted X-Ray Diffraction - Archive ouverte HAL Access content directly
Journal Articles Physical Review Letters Year : 2022

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

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Haiwang Yong
Daniel Keefer
Shaul Mukamel

Abstract

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
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Dates and versions

hal-03947350 , version 1 (19-01-2023)

Identifiers

Cite

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⟩
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