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Hyper-Rayleigh scattering from correlated molecules
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View: Figures


Image of FIG. 1.
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.

Image of FIG. 2.
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. (19a)–(19d) 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. (29a)–(29c) for molecules with statistical correlations and arbitrary symmetry plotted as functions of u 1, where for effective β is given by Eqs. (24a)–(24c) . 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.

Image of FIG. 3.
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. 12 The solid curves are fits as described in Ref. 12 , 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.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Hyper-Rayleigh scattering from correlated molecules