OSA's Digital Library

Advances in Optics and Photonics

Advances in Optics and Photonics

| BRINGING REVIEWS AND TUTORIALS TO LIGHT

  • Editor: Bahaa E. A. Saleh
  • Vol. 5, Iss. 1 — Mar. 31, 2013

Theory of Molecular Nonlinear Optics

Mark G. Kuzyk, Kenneth D. Singer, and George I. Stegeman  »View Author Affiliations


Advances in Optics and Photonics, Vol. 5, Issue 1, pp. 4-82 (2013)
http://dx.doi.org/10.1364/AOP.5.000004


View Full Text Article

Enhanced HTML    Acrobat PDF (1893 KB)





Browse Journals / Lookup Meetings

Browse by Journal and Year


   


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools

Share
Citations

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 ( α i j ) polarizability and nonlinear ( β i j k , γ i j k l ) 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 χ i j ( 1 ) , χ i j k ( 2 ) , χ i j k l ( 3 ) ), is discussed. For example, for β i j k , symmetry determines whether a molecule 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 β i j k 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.

© 2013 Optical Society of America

OCIS Codes
(020.4180) Atomic and molecular physics : Multiphoton processes
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials

ToC Category:
Nonlinear Optics

History
Original Manuscript: July 16, 2012
Revised Manuscript: October 31, 2012
Manuscript Accepted: November 1, 2012
Published: March 26, 2013

Virtual Issues
(2013) Advances in Optics and Photonics

Citation
Mark G. Kuzyk, Kenneth D. Singer, and George I. Stegeman, "Theory of Molecular Nonlinear Optics," Adv. Opt. Photon. 5, 4-82 (2013)
http://www.opticsinfobase.org/aop/abstract.cfm?URI=aop-5-1-4

You do not have subscription access to this journal. Citation lists with outbound citation links are available to subscribers only. You may subscribe either as an OSA member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Log in to access OSA Member Subscription

You do not have subscription access to this journal. Cited by links are available to subscribers only. You may subscribe either as an OSA member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Log in to access OSA Member Subscription

You do not have subscription access to this journal. Figure files are available to subscribers only. You may subscribe either as an OSA member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Log in to access OSA Member Subscription

You do not have subscription access to this journal. Article level metrics are available to subscribers only. You may subscribe either as an OSA member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Log in to access OSA Member Subscription

Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited