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

• 成果类型: Article
• 署名作者: Rouxel, Jeremy R.; Nam, Yeonsig; Chernyak, Vladimir Y.; Mukamel, Shaul
• 署名单位: United States Department of Energy (DOE); Argonne National Laboratory; Wayne State University; University of California System; University of California Irvine; University of California System; University of California Irvine
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-13472
• DOI: 10.1073/pnas.2402660121
• 发表日期: 2024-06-04
• 关键词: sum-frequency generation; x-ray; broad-band; spectroscopy; specificity

摘要

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. Evenorder nonlinear signals in chiral molecules have gained attention thanks to their existence in the electric dipole approximation, without relying on the weaker higherorder 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.