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Hyper-Rayleigh scattering from correlated molecules
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10.1063/1.4799262
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Affiliations:
1 Department of Physics and Astronomy, University of Nevada, Las Vegas, Nevada 89154-4002, USA
a) Electronic mail: shelton@physics.unlv.edu
J. Chem. Phys. 138, 154502 (2013)
/content/aip/journal/jcp/138/15/10.1063/1.4799262
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/15/10.1063/1.4799262
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## Figures

FIG. 1.

Spherical domains containing 250 molecules at random positions are shown. The arrows denote the polar axis for each molecule, and the molecules exhibit perfect (a) radial ( ), (b) polar ( ), or (c) azimuthal ( ) orientational order about the Y symmetry axis. Domains in liquid water with R = 20 nm would contain 106 molecules.

FIG. 2.

Polarization ratios (a) I VV /I HV , (b) I HV /I VH , and (c) I HH /I VH for spherical domains with azimuthal molecular orientation correlations. The solid curves show results from Eqs. for perfectly ordered C v molecules with Kleinman symmetry (u = v = β zxx zzz = β xxz zzz ) plotted as functions of u. The dashed curves show results from Eqs. for molecules with statistical correlations and arbitrary symmetry plotted as functions of u 1, where for effective β is given by Eqs. . In this case, deviations from u 1 = 1/3 indicate deviations from Kleinman symmetry. Results for the perfectly ordered and statistical distributions agree only for u = u 1 = 1/3, shown by the dotted lines.

FIG. 3.

Polarization ratios (a) I VV /I HV and (b) I HV /I VH measured with 0.3 or 60 cm−1 spectral bandwidth for solutions of p-nitroaniline (PNA) in acetone-d6 for PNA concentrations up to 1.7 mol/l are shown by the open circles. The solid curves are fits as described in Ref. , with the incoherent contribution to the HRS signal determined from the zero concentration limit for the data, and I VV /I HV = 7.53 and I HV /I VH = 2.00 for the coherent contribution.

/content/aip/journal/jcp/138/15/10.1063/1.4799262
2013-04-15
2014-04-16

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