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

Content Provider	Semantic Scholar
Author	Baev, Alexander Autschbach, Jochen Boyd, Robert W. Prasad, Paras N.
Copyright Year	2010
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.
File Format	PDF HTM / HTML
DOI	10.1364/OE.18.008713
PubMed reference number	20588715
Journal	Medline
Volume Number	18
Issue Number	8
Alternate Webpage(s)	http://www.optics.rochester.edu/workgroups/boyd/assets/pdf/publications/Baev_OE_10.pdf
Alternate Webpage(s)	https://doi.org/10.1364/OE.18.008713
Journal	Optics express
Language	English
Access Restriction	Open
Content Type	Text
Resource Type	Article