Capturing electron-driven chiral dynamics in UV-excited molecules

Vincent Wanie (), Etienne Bloch, Erik P. Månsson, Lorenzo Colaizzi, Sergey Ryabchuk, Krishna Saraswathula, Andres F. Ordonez, David Ayuso, Olga Smirnova, Andrea Trabattoni, Valérie Blanchet, Nadia Amor, Marie-Catherine Heitz, Yann Mairesse, Bernard Pons () and Francesca Calegari ()
Additional contact information
Vincent Wanie: Deutsches Elektronen-Synchrotron DESY
Etienne Bloch: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107
Erik P. Månsson: Deutsches Elektronen-Synchrotron DESY
Lorenzo Colaizzi: Deutsches Elektronen-Synchrotron DESY
Sergey Ryabchuk: Universität Hamburg
Krishna Saraswathula: Deutsches Elektronen-Synchrotron DESY
Andres F. Ordonez: Imperial College London
David Ayuso: Imperial College London
Olga Smirnova: Max-Born-Institut
Andrea Trabattoni: Deutsches Elektronen-Synchrotron DESY
Valérie Blanchet: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107
Nadia Amor: CNRS, UPS, LCPQ (Laboratoire de Chimie et Physique Quantiques), FeRMI
Marie-Catherine Heitz: CNRS, UPS, LCPQ (Laboratoire de Chimie et Physique Quantiques), FeRMI
Yann Mairesse: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107
Bernard Pons: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107
Francesca Calegari: Deutsches Elektronen-Synchrotron DESY

Nature, 2024, vol. 630, issue 8015, 109-115

Abstract: Abstract Chiral molecules, used in applications such as enantioselective photocatalysis1, circularly polarized light detection2 and emission3 and molecular switches4,5, exist in two geometrical configurations that are non-superimposable mirror images of each other. These so-called (R) and (S) enantiomers exhibit different physical and chemical properties when interacting with other chiral entities. Attosecond technology might enable influence over such interactions, given that it can probe and even direct electron motion within molecules on the intrinsic electronic timescale6 and thereby control reactivity7–9. Electron currents in photoexcited chiral molecules have indeed been predicted to enable enantiosensitive molecular orientation10, but electron-driven chiral dynamics in neutral molecules have not yet been demonstrated owing to the lack of ultrashort, non-ionizing and perturbative light pulses. Here we use time-resolved photoelectron circular dichroism (TR-PECD)11–15 with an unprecedented temporal resolution of 2.9 fs to map the coherent electronic motion initiated by ultraviolet (UV) excitation of neutral chiral molecules. We find that electronic beatings between Rydberg states lead to periodic modulations of the chiroptical response on the few-femtosecond timescale, showing a sign inversion in less than 10 fs. Calculations validate this and also confirm that the combination of the photoinduced chiral current with a circularly polarized probe pulse realizes an enantioselective filter of molecular orientations following photoionization. We anticipate that our approach will enable further investigations of ultrafast electron dynamics in chiral systems and reveal a route towards enantiosensitive charge-directed reactivity.

Date: 2024
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DOI: 10.1038/s41586-024-07415-y

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