Coherent two-dimensional electronic and infrared crystallography
File(s)2D-convert-2-20-references-B-correctedproof.pdf (1.08 MB)
Accepted version
Author(s)
van Thor, Jasper J
Type
Journal Article
Abstract
The two-dimensional electronic and infrared spectroscopy of oriented single crystals is sensitive to structure and point group symmetry. The third order response of crystals is generally different from measurements of isotropic solutions because each coherence path that contributes to the measured field scales to the ensemble average of the four-point correlation functions of the four field-dipole interactions involved in the respective Feynman paths. An analytical evaluation of 2D optical crystallography which depends on the crystal symmetry, laboratory orientation, and the orientation in the crystallographic frame is presented. Applying a symmetry operator in the basis of the allowed polarised radiation modes provides a method for evaluation of non-zero fourth rank tensor elements alternative to direct inspection methods. Uniaxial and biaxial systems are distinguished and the contributions to the rephasing and non-rephasing directions are evaluated for isolated and coupled oscillators. By exploiting coordinate analysis, the extension of non-linear electronic and infrared crystallography for coupled oscillators demonstrates the structural, directional, and symmetry dependent selection of coherences to the four-wave mixing signal.
Date Issued
2019-03-28
Date Acceptance
2019-02-16
Citation
The Journal of Chemical Physics, 2019, 150 (12)
ISSN
0021-9606
Publisher
AIP Publishing
Journal / Book Title
The Journal of Chemical Physics
Volume
150
Issue
12
Copyright Statement
© 2019 Author(s). Published under license by AIP Publishing. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The article appeared in the Journal of Chemical Physics and may be found at https://dx.doi.org/10.1063/1.5079319
Sponsor
The Leverhulme Trust
Engineering & Physical Science Research Council (EPSRC)
Grant Number
RPG-2014-126
EP/R020574/1
Subjects
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Chemical Physics
Publication Status
Published
Article Number
ARTN 124113
Date Publish Online
2019-03-29