Vibration Overtone Hyperpolarizability Measured for H2
Journal of Chemical Physics
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The second hyperpolarizability (γ) of the H2 molecule was measured by gas-phase electric field induced second harmonic generation at the frequencies of the one-photon resonance for the 3–0 Q(J) overtone transitions (v, J = 0, J → 3, J for J = 0, 1, 2, and 3). The magnitude of the resonant contribution to γ was measured with 2% accuracy using the previously determined non-resonant γ for calibration. Pressure broadening and frequency shift for the transitions were also measured. A theoretical expression for the resonant vibrational γ contribution in terms of transition polarizabilities is compared to the observations. The measured γ resonance strength is 4%–14% larger than the results obtained from this theoretical expression evaluated using ab initio transition polarizabilities.
Biological and Chemical Physics
Ellis, R. M.,
Shelton, D. P.
Vibration Overtone Hyperpolarizability Measured for H2.
Journal of Chemical Physics, 152