Journal Article

PUBDB-2022-04966

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Capturing electron-driven chiral dynamics in UV-excited molecules

Wanie, V. (Corresponding author)CFEL*DESY* ; Bloch, E. ; Maansson, E.DESY* ; Colaizzi, L.Extern* ; Riabchuk, S.Extern* ; Saraswathula, K.Extern* ; Trabattoni, A.DESY* ; Blanchet, V. ; Ben-Amor, N. ; Heitz, M.-C. ; Mairesse, Y. ; Pons, B. (Corresponding author) ; Calegari, F. (Corresponding author)DESY*

2024
Nature Publ. Group London [u.a.]

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Please use a persistent id in citations: doi:10.1038/s41586-024-07415-y  doi:10.3204/PUBDB-2022-04966

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 reactivity7,8,9. 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)11,12,13,14,15 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.

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Contributing Institute(s):

1. Attosecond Science and Technology (FS-ATTO)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. STARLIGHT - Steering attosecond electron dynamics in biomolecules with UV-XUV LIGHT pulses (637756) (637756)
3. AIM, DFG project G:(GEPRIS)390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)

Experiment(s):

1. No specific instrument

Appears in the scientific report 2024

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Linked articles:

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Journal Article Wanie, V. (Corresponding author)CFEL*DESY* ; Bloch, E. ; Månsson, E. P.DESY* ; Colaizzi, L.Extern* ; Ryabchuk, S. ; Saraswathula, K. ; Ordonez, A. F. ; Ayuso, D. ; Smirnova, O. ; Trabattoni, A.DESY* ; Blanchet, V. ; Ben Amor, N. ; Heitz, M.-C. ; Mairesse, Y. ; Pons, B. (Corresponding author) ; Calegari, F. (Corresponding author)DESY*
Author Correction: Capturing electron-driven chiral dynamics in UV-excited molecules
Nature 631(8019), E4-E4 (2024) [10.1038/s41586-024-07676-7]2024     Files BibTeX | EndNote: XML, Text | RIS

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Journal Article Wanie, V. (Corresponding author)CFEL*DESY* ; Calegari, F. (Corresponding author)DESY*
A window on molecular chirality at the timescale of electron motion
Nature 630, d41586-024-01633-0 (2024) [10.1038/d41586-024-01633-0]2024     Files BibTeX | EndNote: XML, Text | RIS

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