Selection rules and symmetry relations for four-wave mixing measurements of uniaxial assemblies

The Journal of Physical Chemistry. B
Ryan P DavisGarth J Simpson

Abstract

Uniaxial systems represent the next lowest symmetry below isotropic and are ubiquitous. The objective of the present work is to present a systematic foundation for interpreting polarization-dependent four-wave mixing measurements of oriented and aligned assemblies. Orientational averages connecting the molecular frame to the macroscopic frame in uniaxial assemblies were derived for several common molecular symmetry groups for coherent anti-Stokes Raman spectroscopy (CARS) measurements, coherent anti-Stokes two-photon spectroscopy (CATS) probing electronic transitions, resonant two-photon absorption (2PA), and traditional Raman measurements. First, the complete set of orientational averages connecting the molecular and macroscopic frames was compiled for the most general case of C1 molecular symmetry. Then, the orientational averages of a select few commonly occurring molecular symmetry groups (Cs, C2, C2v, and C3v) were explored in greater detail to illustrate the approach and to facilitate the interpretation of routine experimental measurements. One outcome of this analysis is the prediction of efficient electric dipole-allowed chiral-specific four-wave mixing in uniaxially oriented media.

References

Oct 27, 2004·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Garth J Simpson
Apr 26, 2005·The Journal of Chemical Physics·Darius Abramavicius, Shaul Mukamel
Aug 6, 2005·Chirality·Peer Fischer, François Hache
Jul 13, 2006·The Journal of Physical Chemistry. a·Andrew J Moad, Garth J Simpson
Jul 21, 2006·The Journal of Physical Chemistry. B·John M PerryGarth J Simpson
Apr 24, 2007·Journal of Computational Chemistry·Andrew J MoadGarth J Simpson

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Citations

Dec 3, 2008·Annual Review of Physical Chemistry·Levi M Haupert, Garth J Simpson
Dec 19, 2012·Annual Review of Physical Chemistry·Chao-Yu Chung, Eric O Potma
May 17, 2014·The Journal of Physical Chemistry. a·Gregory R SnyderGarth J Simpson
Jun 30, 2018·Topics in Catalysis·Patrik K JohanssonDavid G Castner
Sep 2, 2013·Chemistry : a European Journal·Sapun H Parekh, Katrin F Domke
Aug 6, 2009·Optics Express·Jorge Alejandro Reyes-EsquedaAlicia Oliver
Apr 8, 2020·The Journal of Physical Chemistry. a·Megan K PettiMartin T Zanni

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