Rigorous theory of molecular orientational nonlinear optics

Classical statistical mechanics of the molecular optics theory proposed by Buckingham [A. D. Buckingham and J. A. Pople, Proc. Phys. Soc. A 68, 905 (1955)] has been extended to describe the field induced molecular orientational polarization effects on nonlinear optics. In this paper, we present the...

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Main Authors: Chong Hoon Kwak, Gun Yeup Kim
Format: Article
Language:English
Published: AIP Publishing LLC 2015-01-01
Series:AIP Advances
Online Access:http://dx.doi.org/10.1063/1.4906521
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author Chong Hoon Kwak
Gun Yeup Kim
author_facet Chong Hoon Kwak
Gun Yeup Kim
author_sort Chong Hoon Kwak
collection DOAJ
description Classical statistical mechanics of the molecular optics theory proposed by Buckingham [A. D. Buckingham and J. A. Pople, Proc. Phys. Soc. A 68, 905 (1955)] has been extended to describe the field induced molecular orientational polarization effects on nonlinear optics. In this paper, we present the generalized molecular orientational nonlinear optical processes (MONLO) through the calculation of the classical orientational averaging using the Boltzmann type time-averaged orientational interaction energy in the randomly oriented molecular system under the influence of applied electric fields. The focal points of the calculation are (1) the derivation of rigorous tensorial components of the effective molecular hyperpolarizabilities, (2) the molecular orientational polarizations and the electronic polarizations including the well-known third-order dc polarization, dc electric field induced Kerr effect (dc Kerr effect), optical Kerr effect (OKE), dc electric field induced second harmonic generation (EFISH), degenerate four wave mixing (DFWM) and third harmonic generation (THG). We also present some of the new predictive MONLO processes. For second-order MONLO, second-order optical rectification (SOR), Pockels effect and difference frequency generation (DFG) are described in terms of the anisotropic coefficients of first hyperpolarizability. And, for third-order MONLO, third-order optical rectification (TOR), dc electric field induced difference frequency generation (EFIDFG) and pump-probe transmission are presented.
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spelling doaj.art-51dc00dedbd6488d8bd35b1fbea7c2312022-12-22T01:51:44ZengAIP Publishing LLCAIP Advances2158-32262015-01-0151017124017124-2810.1063/1.4906521023501ADVRigorous theory of molecular orientational nonlinear opticsChong Hoon Kwak0Gun Yeup Kim1Department of Physics, Yeungnam University, Kyongsan 712-749, KoreaDepartment of Physics, Yeungnam University, Kyongsan 712-749, KoreaClassical statistical mechanics of the molecular optics theory proposed by Buckingham [A. D. Buckingham and J. A. Pople, Proc. Phys. Soc. A 68, 905 (1955)] has been extended to describe the field induced molecular orientational polarization effects on nonlinear optics. In this paper, we present the generalized molecular orientational nonlinear optical processes (MONLO) through the calculation of the classical orientational averaging using the Boltzmann type time-averaged orientational interaction energy in the randomly oriented molecular system under the influence of applied electric fields. The focal points of the calculation are (1) the derivation of rigorous tensorial components of the effective molecular hyperpolarizabilities, (2) the molecular orientational polarizations and the electronic polarizations including the well-known third-order dc polarization, dc electric field induced Kerr effect (dc Kerr effect), optical Kerr effect (OKE), dc electric field induced second harmonic generation (EFISH), degenerate four wave mixing (DFWM) and third harmonic generation (THG). We also present some of the new predictive MONLO processes. For second-order MONLO, second-order optical rectification (SOR), Pockels effect and difference frequency generation (DFG) are described in terms of the anisotropic coefficients of first hyperpolarizability. And, for third-order MONLO, third-order optical rectification (TOR), dc electric field induced difference frequency generation (EFIDFG) and pump-probe transmission are presented.http://dx.doi.org/10.1063/1.4906521
spellingShingle Chong Hoon Kwak
Gun Yeup Kim
Rigorous theory of molecular orientational nonlinear optics
AIP Advances
title Rigorous theory of molecular orientational nonlinear optics
title_full Rigorous theory of molecular orientational nonlinear optics
title_fullStr Rigorous theory of molecular orientational nonlinear optics
title_full_unstemmed Rigorous theory of molecular orientational nonlinear optics
title_short Rigorous theory of molecular orientational nonlinear optics
title_sort rigorous theory of molecular orientational nonlinear optics
url http://dx.doi.org/10.1063/1.4906521
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AT gunyeupkim rigoroustheoryofmolecularorientationalnonlinearoptics