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Title: X-ray Raman optical activity of chiral molecules

Journal Article · · Chemical Science
DOI:https://doi.org/10.1039/C8SC04120B· OSTI ID:1481432
ORCiD logo [1]; ORCiD logo [2];  [3]
  1. Ecole Polytechnique Fédérale de Lausanne, Laboratoire de Spectroscopie Ultrarapide, Faculté des Sciences de Base, ISIC-BSP, CH-1015 Lausanne
  2. PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, USA
  3. Department of Chemistry, University of California, Irvine, USA, Department of Physics and Astronomy

Resonant and off-resonant Raman Optical Activity signals in the X-ray regime (XROA) are predicted. XROA is a chiral-sensitive variant of the spontaneous Resonant Inelastic Scattering (RIXS) signal. Thanks to the highly localized nature of core excitations, these signals provide a direct probe of local chirality with high sensitivity to the molecular structure. We derive sum-over-states expressions for frequency domain XROA signals and apply them to tyrosine at the nitrogen and oxygen K-edges. Time-resolved extensions of ROA made possible by using additional pulses are briefly outlined.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-04ER15571; AC02-76SF00515; CHE-1663822
OSTI ID:
1481432
Alternate ID(s):
OSTI ID: 1503547
Journal Information:
Chemical Science, Journal Name: Chemical Science Vol. 10 Journal Issue: 3; ISSN 2041-6520
Publisher:
Royal Society of Chemistry (RSC)Copyright Statement
Country of Publication:
United Kingdom
Language:
English
Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

References (52)

Understanding glycoprotein behaviours using Raman and Raman optical activity spectroscopies: Characterising the entanglement induced conformational changes in oligosaccharide chains of mucin journal November 2013
X-Ray Natural Circular Dichroism journal May 1998
Theoretical CD spectrum calculations of the crown-ether aralkyl-ammonium salt complex: Theoretical CD of a Host-Guest Complex journal January 2002
Linear-Response and Real-Time Time-Dependent Density Functional Theory Studies of Core-Level Near-Edge X-Ray Absorption journal August 2012
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Two-dimensional stimulated resonance Raman spectroscopy of molecules with broadband x-ray pulses journal May 2012
COSMO: a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient journal January 1993
Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions journal May 1992
Non-Adiabatic Meson Theory of Nuclear Forces journal May 1950
Time-Dependent Density Functional Theory Study of the X-ray Absorption Spectroscopy of Acetylene, Ethylene, and Benzene on Si(100) journal January 2007
Time dependent density functional theory of core electrons excitations journal May 2003
Is the Tamm-Dancoff Approximation Reliable for the Calculation of Absorption and Fluorescence Band Shapes? journal September 2013
Core and valence excitations in resonant X-ray spectroscopy using restricted excitation window time-dependent density functional theory journal November 2012
NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations journal September 2010
X-ray circular dichroism signals: a unique probe of local molecular chirality journal January 2017
Approximate evaluations of the electrostatic free energy and internal energy changes in solution processes journal March 1982
Time-Dependent Density Functional Theory for Calculating Origin-Independent Optical Rotation and Rotatory Strength Tensors journal September 2011
Calculation of origin-independent optical rotation tensor components in approximate time-dependent density functional theory journal July 2006
The development of biomolecular Raman optical activity spectroscopy journal June 2015
The generation, characterization and applications of broadband isolated attosecond pulses journal February 2014
Generation of attosecond x-ray pulses with a multicycle two-color enhanced self-amplified spontaneous emission scheme journal June 2009
Molecular Light Scattering and Optical Activity book August 2009
Raman scattering of circularly polarized light by optically active molecules journal January 1973
Time-resolved circular dichroism in carbonmonoxy-myoglobin: The central role of the proximal histidine journal January 2006
Determination of multiwavelength anomalous diffraction coefficients at high x-ray intensity journal August 2013
Density‐functional thermochemistry. III. The role of exact exchange journal April 1993
A novel Raman optical activity instrument operating in the deep ultraviolet spectral region: Raman optical activity instrument operating in DUV spectral region journal March 2015
Time-dependent density functional calculations of ligand K-edge X-ray absorption spectra journal March 2008
Raman optical activity spectra of chiral transition metal complexes journal May 2008
Progress in Time-Dependent Density-Functional Theory journal May 2012
Rayleigh and Raman scattering from optically active molecules journal January 1971
Understanding excitation energy transfer in metalloporphyrin heterodimers with different linkers, bonding structures, and geometries through stimulated X-ray Raman spectroscopy journal March 2014
INFRARED AND RAMAN VIBRATIONAL OPTICAL ACTIVITY: Theoretical and Experimental Aspects journal October 1997
Nonlinear optical activity in chiral molecules: surface second harmonic generation and nonlinear circular dichroism journal January 2002
X-ray two-photon absorption competing against single and sequential multiphoton processes journal February 2014
Electrostatic interaction of a solute with a continuum. A direct utilizaion of AB initio molecular potentials for the prevision of solvent effects journal February 1981
Optical Chirality and Its Interaction with Matter journal April 2010
Giant circular dichroism of a molecule in a region of strong plasmon resonances between two neighboring gold nanocrystals journal February 2013
Calculating molecular electric and magnetic properties from time-dependent density functional response theory journal January 2002
Time-dependent density functional theory within the Tamm–Dancoff approximation journal December 1999
Energy-Specific Linear Response TDHF/TDDFT for Calculating High-Energy Excited States journal October 2011
Vibrational Raman optical activity calculations using London atomic orbitals journal January 1994
Coherent Multidimensional Optical Spectroscopy of Excitons in Molecular Aggregates; Quasiparticle versus Supermolecule Perspectives journal June 2009
Performance of Tamm-Dancoff approximation on nonadiabatic couplings by time-dependent density functional theory journal February 2014
Influence of Triplet Instabilities in TDDFT journal October 2011
Non-local real-space analysis of chiral optical signals journal January 2016
Théorie quantique des courants interatomiques dans les combinaisons aromatiques journal January 1937
Chiroptical properties from time-dependent density functional theory. I. Circular dichroism spectra of organic molecules journal April 2002
Circular Dichroism at the Edge:  Large X-ray Natural CD in the 1s → 3d Pre-Edge Feature of 2[Co(en) 3 Cl 3 ]·NaCl·6H 2 O journal November 1999
Ab Initio Calculation of Vibrational Absorption and Circular Dichroism Spectra Using Density Functional Force Fields journal November 1994
GEPOL: An improved description of molecular surfaces. III. A new algorithm for the computation of a solvent-excluding surface: GEPOL journal October 1994
Calibration of Scalar Relativistic Density Functional Theory for the Calculation of Sulfur K-Edge X-ray Absorption Spectra journal February 2010

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