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Chemical Physics Letters
Volume 392, Issues 4-6, 11 July 2004, Pages 444-451
 
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doi:10.1016/j.cplett.2004.05.078    How to Cite or Link Using DOI (Opens New Window)
Copyright © 2004 Elsevier B.V. All rights reserved.

Calculations of the third-order nonlinear optical responses in push–pull chromophores with a time-dependent density functional theory

Nadya Kobko1, Artëm Masunov and Sergei TretiakCorresponding Author Contact Information, E-mail The Corresponding Author

Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM 87545, USA

Received23 March 2004; 
Revised 24 May 2004. 
Available online 19 June 2004.

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Abstract

The third-order resonant and static nonlinear optical polarizabilities of the donor–donor and donor–acceptor substituted π conjugated molecules are calculated using the third-order response formalism in combination with time-dependent Hartree–Fock (TD-HF) and density functional theory (TD-DFT) methods. Performance of different levels of theory for excited state structure and nonlinear optical responses has been analyzed. Since the exact computations are fairly expensive, and only a few components of the cubic polarizability (corresponding to the Liouville space paths) are important, numerically efficient approximations are suggested.

Article Outline

1. Introduction
2. Computational methodology
3. Results and discussions
4. Conclusion
Acknowledgements
References





 
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