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Time-resolved chiral x-ray photoelectron spectroscopy with enhanced atomic site-selectivity: a Free Electron Laser investigation of electronically excited fenchome enantiomers

Facciala, D.; Devetta, M.; Beauvarlet, S.; Besley, N.; Calegari, F.; Callegari, C.; Catone, D.; Cinquanta, E.; Ciriolo, A.G.; Colaizzi, L.; Coreno, M.; Crippa, G.; De Ninno, G.; Di Fraia, M.; Galli, M.; Garcia, G.A.; Mairesse, Y.; Negro, M.; Plekan, O.; Prasannan Geetha, P.; Prince, K.C.; Pusala, A.; Stagira, S.; Turchini, S.; Ueda, K.; You, D.; Zema, N.; Blanchet, V.; Nahon, L.; Powis, I.; Vozzi, C.

Time-resolved chiral x-ray photoelectron spectroscopy with enhanced atomic site-selectivity: a Free Electron Laser investigation of electronically excited fenchome enantiomers Thumbnail


Authors

D. Facciala

M. Devetta

S. Beauvarlet

N. Besley

F. Calegari

C. Callegari

D. Catone

E. Cinquanta

A.G. Ciriolo

L. Colaizzi

M. Coreno

G. Crippa

G. De Ninno

M. Di Fraia

M. Galli

G.A. Garcia

Y. Mairesse

M. Negro

O. Plekan

P. Prasannan Geetha

K.C. Prince

A. Pusala

S. Stagira

S. Turchini

K. Ueda

D. You

N. Zema

V. Blanchet

L. Nahon

I. Powis

C. Vozzi



Abstract

Chirality is widespread in nature, playing a fundamental role in biochemical processes and in the origin of life itself. The observation of dynamics in chiral molecules is crucial for the understanding and control of the chiral activity of photoexcited states. One of the most promising techniques for the study of photoexcited chiral systems is time-resolved photoelectron circular dichroism (TR-PECD), which offers an intense and sensitive probe for vibronic and geometric molecular structure as well as electronic structures, and their evolution on a femtosecond timescale. However, the nonlocal character of the PECD effect, which is imprinted during the electron scattering off the molecule, makes the interpretation of TR-PECD experiments challenging. In this respect, core photoionization is known to allow site and chemical sensitivity to photelectron spectroscopy. Here we demonstrate that TR-PECD utilizing core-level photoemission enables probing the chiral electronic structure and its relaxation dynamics with atomic site sensitivity. Following UV pumped excitation to a 3s Rydberg state, fenchone enantiomers (C10H16O) were probed on a femtosecond scale using circularly polarized soft x-ray light pulses provided by the free-electron laser FERMI. C 1s binding energy shifts caused by the redistribution of valence electron density in this 3s-valence-Rydberg excitation allowed us to measure transient PECD chiral responses with an enhanced C atom site selectivity compared to that achievable in the ground state molecule. This chemical-specific, site-specific, and enantiosensitive observation of the electronic structure of a transiently photoexcited chiral molecule is expected to pave the way toward chiral femtochemistry probed by core-level photoemission.

Citation

Facciala, D., Devetta, M., Beauvarlet, S., Besley, N., Calegari, F., Callegari, C., …Vozzi, C. (2023). Time-resolved chiral x-ray photoelectron spectroscopy with enhanced atomic site-selectivity: a Free Electron Laser investigation of electronically excited fenchome enantiomers. Physical Review X, 13(1), Article 011044. https://doi.org/10.1103/PhysRevX.13.011044

Journal Article Type Article
Acceptance Date Feb 2, 2023
Online Publication Date Mar 23, 2023
Publication Date 2023-01
Deposit Date Feb 7, 2023
Publicly Available Date Feb 1, 2024
Journal Physical Review X
Publisher American Physical Society
Peer Reviewed Peer Reviewed
Volume 13
Issue 1
Article Number 011044
DOI https://doi.org/10.1103/PhysRevX.13.011044
Public URL https://nottingham-repository.worktribe.com/output/17075310
Publisher URL https://journals.aps.org/prx/abstract/10.1103/PhysRevX.13.011044

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