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Frequencyhyphen;dependent hyperpolarizabilities for argon, krypton, and neon: Comparison with experiment

机译:Frequencyhyphen;dependent hyperpolarizabilities for argon, krypton, and neon: Comparison with experiment

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Accurate frequencyhyphen;dependent hyperpolarizabilities which incorporate the effects of electron correlation have been calculated for neon, argon, and krypton. Specifically, these values are derived from a previous lsquo;lsquo;best estimatersquo;rsquo; static value based on coupledhyphen;cluster calculations, and use of a secondhyphen;order perturbation theory frequencyhyphen;dependent correction. The values for ggr;K(minus;ohgr;;ohgr;,0,0) and ggr;par;(minus;2ohgr;;ohgr;,ohgr;,0) are compared with experiments for the d.c. Kerr effect and second harmonic generation, respectively. No negative dispersion is observed for either of these processes for neon, argon, and krypton. In particular, the second harmonic generation values for neon show a positive dispersion effect which is in agreement with other recent theoretical calculations and in line with recent measurements. This study demonstrates that it is possible to achieve quantitative accuracy for the frequencyhyphen;dependent hyperpolarizabilities of dilute gashyphen;phase manyhyphen;electron systems.

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