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Theory of two-photon absorption in poly(diphenyl) polyacetylenes

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Title Theory of two-photon absorption in poly(diphenyl) polyacetylenes
 
Creator SHUKLA, ALOK
 
Subject conjugated polymer
nonlinear optics
two-photon spectra
absorption
 
Description In this paper, we present a theoretical study of the nonlinear optical response of the newly discovered conjugated polymer poly(diphenyl)polyacetylene (PDPA). In particular, we compute the third-order nonlinear susceptibility corresponding to two-photon absorption process in PDPA using: (a) independent-particle Hückel model, and (b) using the correlated-electron Pariser-Parr-Pople (P-P-P) model coupled with various configuration-interaction methodologies such as the singles-configuration-interaction (SCI), the multi-reference-singles-doubles CI (MRSDCI), and the quadruples-CI (QCI) method. At all levels of theory, the polymer is found to exhibit highly anisotropic nonlinear optical response, distributed over two distinct energy scales. The low-energy response is predominantly polarized in the conjugation direction, and can be explained in terms of chain-based orbitals. The high-energy response of the polymer is found to be polarized perpendicular to the conjugation direction, and can be explained in terms of orbitals based on the side phenylene rings. Moreover, the intensity of the nonlinear optical response is also enhanced as compared to the corresponding polyenes, and can be understood in terms of reduced optical gap.
 
Publisher Elsevier
 
Date 2009-04-03T09:07:53Z
2011-11-25T20:42:32Z
2011-12-26T13:08:30Z
2011-12-27T05:56:27Z
2009-04-03T09:07:53Z
2011-11-25T20:42:32Z
2011-12-26T13:08:30Z
2011-12-27T05:56:27Z
2004
 
Type Article
 
Identifier Chemical Physics 300(1-3), 177-188
0301-0104
http://dx.doi.org/10.1016/j.chemphys.2004.02.004
http://hdl.handle.net/10054/1136
http://dspace.library.iitb.ac.in/xmlui/handle/10054/1136
 
Language en