Manipulating ultrafast even-order nonlinear chiral responses of L-tryptophan by polarization pulse shaping

Rouxel, Jérémy R.; Nam, Yeonsig; Chernyak, Vladimir Y.; Mukamel, Shaul

doi:10.1073/pnas.2402660121

Manipulating ultrafast even-order nonlinear chiral responses of L-tryptophan by polarization pulse shaping

Journal Article · Fri May 31 00:00:00 EDT 2024 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.2402660121· OSTI ID:2369024

^[1]; Nam, Yeonsig ^[1]; Chernyak, Vladimir Y. ^[2]; ^[3]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Wayne State Univ., Detroit, MI (United States)
InfraDerm, LLC, Irvine, CA (United States)

Molecular chirality has long been monitored in the frequency domain in the ultraviolet, visible, and infrared regimes. Recently developed time-domain approaches can detect time-dependent chiral dynamics by enhancing intrinsically weak chiral signals. Even-order nonlinear signals in chiral molecules have gained attention thanks to their existence in the electric dipole approximation, without relying on the weaker higher-order multipole interactions. We illustrate the optimization of temporal polarization pulse-shaping in various frequency ranges (infrared/optical and optical/X ray) to enhance chiral nonlinear signals. These signals can be recast as an overlap integral of matter and field pseudoscalars which contain the relevant chiral information. Simulations are carried out for second- and fourth-order nonlinear spectroscopies in L-tryptophan.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-06CH11357; SC0022134

OSTI ID:: 2369024

Alternate ID(s):: OSTI ID: 2569697

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 23 Vol. 121; ISSN 1091-6490; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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