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Optics Express

Optics Express

  • Editor: C. Martijn de Sterke
  • Vol. 18, Iss. 8 — Apr. 12, 2010
  • pp: 8713–8721

Microscopic cascading of second-order molecular nonlinearity: new design principles for enhancing third-order nonlinearity

Alexander Baev, Jochen Autschbach, Robert W. Boyd, and Paras N. Prasad  »View Author Affiliations


Optics Express, Vol. 18, Issue 8, pp. 8713-8721 (2010)
http://dx.doi.org/10.1364/OE.18.008713


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Abstract

Herein, we develop a phenomenological model for microscopic cascading and substantiate it with ab initio calculations. It is shown that the concept of local microscopic cascading of a second-order nonlinearity can lead to a third-order nonlinearity, without introducing any new loss mechanisms that could limit the usefulness of our approach. This approach provides a new molecular design protocol, in which the current great successes achieved in producing molecules with extremely large second-order nonlinearity can be used in a supra molecular organization in a preferred orientation to generate very large third-order response magnitudes. The results of density functional calculations for a well-known second-order molecule, (para)nitroaniline, show that a head-to-tail dimer configuration exhibits enhanced third-order nonlinearity, in agreement with the phenomenological model which suggests that such an arrangement will produce cascading due to local field effects.

© 2010 OSA

OCIS Codes
(000.1570) General : Chemistry
(190.4380) Nonlinear optics : Nonlinear optics, four-wave mixing
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials

ToC Category:
Nonlinear Optics

History
Original Manuscript: February 25, 2010
Manuscript Accepted: March 28, 2010
Published: April 9, 2010

Citation
Alexander Baev, Jochen Autschbach, Robert W. Boyd, and Paras N. Prasad, "Microscopic cascading of second-order molecular nonlinearity: new design principles for enhancing third-order nonlinearity," Opt. Express 18, 8713-8721 (2010)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-18-8-8713


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