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Gas phase hyper-Rayleigh scattering measurements
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10.1063/1.4738897
/content/aip/journal/jcp/137/4/10.1063/1.4738897
http://aip.metastore.ingenta.com/content/aip/journal/jcp/137/4/10.1063/1.4738897

Figures

Image of FIG. 1.
FIG. 1.

HRS polarization ratio measurements for CF2Cl2 are shown by the open circles with error bars representing photon counting statistics, and the solid curves show the functions fit to the data as described in Appendix B. The fit parameters P 2, Q 2, and R 2 are the NA = 0 intercepts for the functions in (a), (b), and (c), respectively. The curve through the I HV /I VH data in (d) has no additional adjustable parameters and serves as a check.

Image of FIG. 2.
FIG. 2.

Measurements of the normalized HRS signal S VV are shown by the open circles with error bars representing photon counting statistics. The data for each molecule is adequately fit by a horizontal line.

Tables

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Table I.

HRS intensity factors in Eqs. (12)–(17) expressed in terms of molecule-frame β tensor components, obtained using Eqs. (34)–(44) and Table I of Ref. 4. For C ∞v molecules β yyy = 0. The last line gives results for β|| measured by ESHG.

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Table II.

Experimental measurements of HRS polarization ratios.

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Table III.

Experimental measurements of normalized HRS signal and first hyperpolarizability.

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Table IV.

Ratios of β tensor component consistent with the observed HRS polarization ratios. A unique solution is obtained for N2O. For the other molecules, the first line gives a typical solution, and the second line in brackets gives the range of values obtained.

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Table V.

Comparison of calculated (MP2) (Ref. 18) and experimental βxyz(a.u.) for CX4 molecules.

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Table VI.

Comparison of calculated β e (a.u.) [static, CCSD(T), 162 CGTF basis] (Ref. 20) and experimental β(a.u.) for N2O.

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Table VII.

Comparison of calculated β e (a.u.) [static, CCSD(T), 168 CGTF basis] (Ref. 21) and experimental β(a.u.) for SO2.

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Table VIII.

Ab initio electronic hyperpolarizabilities β e (a.u.) for H2O.

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Table IX.

Ab initio vibrational hyperpolarizabilities (a.u.) and βv(a.u.) for H2O. Results for D2O are in parentheses.

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Table X.

Comparison of calculated and experimental β (a.u.) for D2O at ω = 0.04282 a.u.

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Table XI.

Ab initio electronic hyperpolarizabilities β e (a.u.) for NH3.

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Table XII.

Ab initio vibrational hyperpolarizabilities (a.u.) and βv (a.u.) for NH3.

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Table XIII.

Comparison of calculated and experimental β(a.u.) for NH3 at ω = 0.04282 a.u.

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/content/aip/journal/jcp/137/4/10.1063/1.4738897
2012-07-30
2014-04-17
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Gas phase hyper-Rayleigh scattering measurements
http://aip.metastore.ingenta.com/content/aip/journal/jcp/137/4/10.1063/1.4738897
10.1063/1.4738897
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