Title

Theory of Molecular Nonlinear Optics

Authors

Authors

M. G. Kuzyk; K. D. Singer;G. I. Stegeman

Comments

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Abbreviated Journal Title

Adv. Opt. Photonics

Keywords

2ND HARMONIC-GENERATION; HYPER-RAYLEIGH-SCATTERING; NEMATISCHEN; KRISTALLINFLUSSIGEN PHASE; OXYGEN-OCTAHEDRA FERROELECTRICS; MOLEKULAR-STATISTISCHE THEORIE; CONJUGATED ORGANIC-MOLECULES; LANGMUIR-BLODGETT-FILMS; BOND-LENGTH ALTERNATION; POLED POLYMER-FILMS; PUSH-PULL POLYMERS; Optics

Abstract

The theory of molecular nonlinear optics based on the sum-over-states (SOS) model is reviewed. The interaction of radiation with a single wtpisolated molecule is treated by first-order perturbation theory, and expressions are derived for the linear (alpha(ij)) polarizability and nonlinear (beta(ijk), gamma(ijkl)) molecular hyperpolarizabilities in terms of the properties of the molecular states and the electric dipole transition moments for light-induced transitions between them. Scale invariance is used to estimate fundamental limits for these polarizabilities. The crucial role of the spatial symmetry of both the single molecules and their ordering in dense media, and the transition from the single molecule to the dense medium case (susceptibilities. chi((1))(ij), chi((2))(ijk), chi((3))(ijkl), is discussed. For example, for beta(ijk), symmetry determines whether amolecule can support second-order nonlinear processes or not. For asymmetric molecules, examples of the frequency dispersion based on a two-level model (ground state and one excited state) are the simplest possible for beta(ijk) and examples of the resulting frequency dispersion are given. The third-order susceptibility is too complicated to yield simple results in terms of symmetry properties. It will be shown that whereas a two-level model suffices for asymmetric molecules, symmetric molecules require a minimum of three levels in order to describe effects such as two-photon absorption. The frequency dispersion of the third-order susceptibility will be shown and the importance of one and two-photon transitions will be discussed. (C) 2013 Optical Society of America

Journal Title

Advances in Optics and Photonics

Volume

5

Issue/Number

1

Publication Date

1-1-2013

Document Type

Article

Language

English

First Page

4

Last Page

82

WOS Identifier

WOS:000330189200001

ISSN

1943-8206

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