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Title: Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

Abstract

Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. Here, we present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O) provide different local windows onto the parity breaking geometry change thus revealing the enantiomer asymmetry.

Authors:
 [1];  [1];  [1]
  1. Univ. of California, Irvine, CA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1374552
Grant/Contract Number:  
FG02-04ER15571; CHE-1361516
Resource Type:
Accepted Manuscript
Journal Name:
Structural Dynamics
Additional Journal Information:
Journal Volume: 4; Journal Issue: 4; Journal ID: ISSN 2329-7778
Publisher:
American Crystallographic Association/AIP
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chiral symmetries; Excited states; Optical signal processing; Ground states; X-ray lasers

Citation Formats

Rouxel, Jérémy R., Kowalewski, Markus, and Mukamel, Shaul. Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy. United States: N. p., 2017. Web. doi:10.1063/1.4974260.
Rouxel, Jérémy R., Kowalewski, Markus, & Mukamel, Shaul. Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy. United States. doi:10.1063/1.4974260.
Rouxel, Jérémy R., Kowalewski, Markus, and Mukamel, Shaul. Sat . "Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy". United States. doi:10.1063/1.4974260. https://www.osti.gov/servlets/purl/1374552.
@article{osti_1374552,
title = {Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy},
author = {Rouxel, Jérémy R. and Kowalewski, Markus and Mukamel, Shaul},
abstractNote = {Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. Here, we present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O) provide different local windows onto the parity breaking geometry change thus revealing the enantiomer asymmetry.},
doi = {10.1063/1.4974260},
journal = {Structural Dynamics},
number = 4,
volume = 4,
place = {United States},
year = {2017},
month = {7}
}

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Cited by: 7 works
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Works referenced in this record:

Generation of bright phase-matched circularly-polarized extreme ultraviolet high harmonics
journal, December 2014


Antennas for light
journal, February 2011


Circular dichroism measurements at an x-ray free-electron laser with polarization control
journal, August 2016

  • Hartmann, G.; Lindahl, A. O.; Knie, A.
  • Review of Scientific Instruments, Vol. 87, Issue 8
  • DOI: 10.1063/1.4961470

Single Shot Polarization Characterization of XUV FEL Pulses from Crossed Polarized Undulators
journal, August 2015

  • Ferrari, E.; Allaria, E.; Buck, J.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep13531

Opportunities for chiral discrimination using high harmonic generation in tailored laser fields
journal, October 2015

  • Smirnova, Olga; Mairesse, Yann; Patchkovskii, Serguei
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 23
  • DOI: 10.1088/0953-4075/48/23/234005

An accurate and efficient scheme for propagating the time dependent Schrödinger equation
journal, November 1984

  • Tal‐Ezer, H.; Kosloff, R.
  • The Journal of Chemical Physics, Vol. 81, Issue 9
  • DOI: 10.1063/1.448136

X-ray magnetic circular dichroism—A versatile tool to study magnetism
journal, October 2014


Recent advances in ultrafast time-resolved chirality measurements: perspective and outlook: Ultrafast transient molecular chirality
journal, January 2013

  • Meyer-Ilse, Julia; Akimov, Denis; Dietzek, Benjamin
  • Laser & Photonics Reviews, Vol. 7, Issue 4
  • DOI: 10.1002/lpor.201200065

First observation of undulator radiation from APPLE-1
journal, August 1994

  • Sasaki, Shigemi; Shimada, Taihei; Yanagida, Ken-ichi
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 347, Issue 1-3
  • DOI: 10.1016/0168-9002(94)91860-0

Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses
journal, March 2016


Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives
journal, June 2009

  • Abramavicius, Darius; Palmieri, Benoit; Voronine, Dmitri V.
  • Chemical Reviews, Vol. 109, Issue 6
  • DOI: 10.1021/cr800268n

Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond
journal, June 2000

  • Zewail, Ahmed H.
  • The Journal of Physical Chemistry A, Vol. 104, Issue 24
  • DOI: 10.1021/jp001460h

Generation of various polarization states from insertion devices: A review
journal, July 1989

  • Elleaume, Pascal
  • Review of Scientific Instruments, Vol. 60, Issue 7
  • DOI: 10.1063/1.1140915

Obtaining high degree of circular polarization at x-ray free electron lasers via a reverse undulator taper
journal, November 2013

  • Schneidmiller, E. A.; Yurkov, M. V.
  • Physical Review Special Topics - Accelerators and Beams, Vol. 16, Issue 11
  • DOI: 10.1103/PhysRevSTAB.16.110702

Probing molecular chirality on a sub-femtosecond timescale
journal, June 2015

  • Cireasa, R.; Boguslavskiy, A. E.; Pons, B.
  • Nature Physics, Vol. 11, Issue 8
  • DOI: 10.1038/nphys3369

Nonlinear optical spectroscopy of chiral molecules
journal, January 2005


Femtosecond X-ray magnetic circular dichroism absorption spectroscopy at an X-ray free electron laser
journal, March 2016

  • Higley, Daniel J.; Hirsch, Konstantin; Dakovski, Georgi L.
  • Review of Scientific Instruments, Vol. 87, Issue 3
  • DOI: 10.1063/1.4944410

Generation of attosecond x-ray pulses with a multicycle two-color enhanced self-amplified spontaneous emission scheme
journal, June 2009