Coupled cluster evaluation of the frequency dispersion of the first and second hyperpolarizabilities of water, methanol, and dimethyl ether

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Abstract

The static and dynamic first (β) and second (γ) hyperpolarizabilities of water, methanol, and dimethyl ether have been evaluated within the response function approach using a hierarchy of coupled cluster levels of approximation and doubly augmented correlation consistent atomic basis sets. For the three compounds, the electronic β and γ values calculated at the CCSD and CC3 levels are in good agreement with gas phase electric field-induced second harmonic generation (EFISHG) measurements. In addition, for dimethyl ether, the frequency dispersion of both properties follows closely recent experimental values [V. W. Couling and D. P. Shelton, J. Chem. Phys. 143, 224307 (2015)] demonstrating the reliability of these methods and levels of approximation. This also suggests that the vibrational contributions to the EFISHG responses of these molecules are small.
Original languageEnglish
Article number044311
Number of pages9
JournalJ. Chem. Phys.
Volume145
Issue number4
DOIs
Publication statusPublished - 28 Jul 2016

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Harmonic generation
Methanol
ethers
methyl alcohol
Electric fields
Water
evaluation
harmonic generations
water
electric fields
Gases
approximation
Molecules
hierarchies
vapor phases
electronics
dimethyl ether
molecules

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abstract = "The static and dynamic first (β‖) and second (γ‖) hyperpolarizabilities of water, methanol, and dimethyl ether have been evaluated within the response function approach using a hierarchy of coupled cluster levels of approximation and doubly augmented correlation consistent atomic basis sets. For the three compounds, the electronic β‖ and γ‖ values calculated at the CCSD and CC3 levels are in good agreement with gas phase electric field-induced second harmonic generation (EFISHG) measurements. In addition, for dimethyl ether, the frequency dispersion of both properties follows closely recent experimental values [V. W. Couling and D. P. Shelton, J. Chem. Phys. 143, 224307 (2015)] demonstrating the reliability of these methods and levels of approximation. This also suggests that the vibrational contributions to the EFISHG responses of these molecules are small.",
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