Element- and enantiomer-selective visualization of molecular motion in real-time

Year: 2023

Authors: Mincigrucci R., Rouxel JR., Rossi B., Principi E., Bottari C., Catalini S., Pelli-Cresi JS., Fainozzi D., Foglia L., Simoncig A., Matruglio A., Kurdi G., Capotondi F., Pedersoli E., Perucchi A., Piccirilli F., Gessini A., Giarola M., Mariotto G., Oppermann M., Mukamel S., Bencivenga F., Chergui M., Masciovecchio C.

Autors Affiliation: Elettra Sincrotrone Trieste SCpA, Str Statale 14,Km 163,5 AREA Sci Pk, I-34149 Trieste, Italy; Ecole Polytech Fed Lausanne, Lausanne Ctr Ultrafast Spect LACUS, CH-1015 Lausanne, Switzerland; Univ Lyon, UJM St Etienne, Lab Hubert Curien UMR 5516, CNRS,IOGS, F-42023 St Etienne, France; Univ Trento, Dept Phys, Via Sommar 14, I-38123 Povo, Trento, Italy; Univ Trieste, Dept Phys, Trieste, Italy; Univ Firenze, European Lab Nonlinear Spect LENS, I-50121 Florence, Italy; Univ Perugia, Dept Phys & Geol, I-06123 Perugia, Italy; CNR, CNR INO, Ist Nazl Ottica, Largo Fermi 6, I-50125 Florence, Italy; CERIC ERIC, Str Statale 14,Km 1635 AREA Sci Pk, I-34149 Trieste, Italy; Univ Verona, Policlin GB Rossi, Ctr Piattaforme Tecnol, Ple LA Scuro 10, I-37134 Verona, Italy; Univ Verona, Dept Comp Sci, Str Grazie 15, I-37134 Verona, Italy; Univ Basel, Dept Chem, Klingelbergstr 80, CH-4056 Basel, Switzerland; Univ Calif Irvine, Dept Chem & Phys & astron, Irvine, CA 92697 USA.

Abstract: Ultrafast optical-domain spectroscopies allow to monitor in real time the motion of nuclei in molecules. Achieving element-selectivity had to await the advent of time resolved X-ray spectroscopy, which is now commonly carried at X-ray free electron lasers. However, detecting light element that are commonly encountered in organic molecules, remained elusive due to the need to work under vacuum. Here, we present an impulsive stimulated Raman scattering (ISRS) pump/carbon K-edge absorption probe investigation, which allowed observation of the low-frequency vibrational modes involving specific selected carbon atoms in the Ibuprofen RS dimer. Remarkably, by controlling the probe light polarization we can preferentially access the enantiomer of the dimer to which the carbon atoms belong.

Journal/Review: NATURE COMMUNICATIONS

Volume: 14 (1)      Pages from: 386-1  to: 386-8

More Information: M.C. acknowledges support by the Swiss NSF via the NCCR:MUST and by the European Research Council Advanced H2020 Grant ERCEA 695197 DYNAMOX. S.M gratefully acknowledges the support of National Science Foundation (Grant CHE-1953045) and computational support of the Department of Energy (DE-FG02-04ER15571). J.R.R. was supported by the LABEX MANUTECH-SISE (ANR-10-LABX-0075) of Universite de Lyon and by the Federation de Recherche Andre Marie Ampere (FRAMA). S.C. also thanks the research project FSE-REACT EU financed by National Social Fund-National Operative Research Program and Innovation 2014-2020 (D.M. 1062/2021), personal Grant number 23-G-15445-3. We acknowledge Prof. S. Lupi and CNR-IOM for the use of the FTIR interferometer Thanks to A. Ajdarzadeh, K. Oberhofer, J. Hugues and R. Versteeg for their help with the deep-UV transient absorption measurements of the IBP powders.
KeyWords: X-ray-absorption; Photoinduced Structural Dynamics; Sum-frequency Generation; Circular-dichroism; Polarization Control; Racemic Ibuprofen; Raman-scattering; Spectroscopy; Spectra; Phase
DOI: 10.1038/s41467-023-36047-5

Citations: 7
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