Theory of two-photon absorption in poly(diphenyl) polyacetylenes
DSpace at IIT Bombay
View Archive InfoField | Value | |
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
|
|