Bulletin of the American Physical Society
54th Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics
Volume 68, Number 7
Monday–Friday, June 5–9, 2023; Spokane, Washington
Session S11: V: Ultrafast Phenomena
10:30 AM–12:30 PM,
Thursday, June 8, 2023
Room: Virtual Platform
Chair: Carlos Marante Valdes, University of Central Florida
Abstract: S11.00001 : Experimentally resolving and decomposing the transfer of charge through a molecule on a single-femtosecond timescale*
10:30 AM–10:42 AM
Presenter:
Danylo T Matselyukh
(ETH Zurich)
Authors:
Danylo T Matselyukh
(ETH Zurich)
Florian Rott
(LMU Munich)
Thomas Schnappinger
(Stockholm University)
Pengju Zhang
(ETH Zurich)
Zheng Li
(Peking University)
Regina de Vivie-Riedle
(LMU Munich)
Hans Jakob Wörner
(ETH Zurich)
Thanks to the extremely short, σ = 1 fs, experimental cross correlation afforded by ATAS, the rise of the E state absorption is measured to be σ = 2.34 ± 0.36 fs. Furthermore, the sigmoid rise of the absorption is found to be significantly asymmetric, exhibiting a negative skew. The origin of this skew is understood through a Landau-Zener-like model, and found to originate from the modulation of the non-adiabatic coupling as the nuclear wavepacket passes through the vicinity of the CoIn. Finally, a 1.46 ± 0.41 fs delay is observed between the fall in the B state and the rise in the E state transient absorption – a yet unobserved signature of the non-adiabatic effects driving electron motion.
Along with establishing a purely experimental method for transiently probing the non-adiabatic coupling, these observations allow us to propose three separate timescales that are involved in electronic CT modulated by conical intersections; the “non-adiabatic CT time” - the time taken for the electron to travel through the molecule, the “adiabatic CT time” - the time taken for the diabatic population of a single state to rise/fall, and the “CT rearrangement time” the time taken for the vibrational wavepacket of the system to reach the CoIn.
*We acknowledge the computational resources provided by the Leibniz Supercomputing Centre and funding from the ERC Consolidator Grant (project no. 772797-ATTOLIQ), the Swiss National Science Foundation through projects 200021_172946, the NCCR-MUST and the DFG Normalverfahre.
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