We present ab initio calculations of frequency-dependent linear and nonlinear optical responses based on real-time time-dependent density functional theory for arbitrary photonic molecules. This approach is based on an extension of an approach previously implemented for a linear response using the electronic structure program SIESTA. Instead of calculating excited quantum states, which can be a bottleneck in frequency-space calculations, the response of large molecular systems to time-varying electric fields is calculated in real time. This method is based on the finite field approach generalized to the dynamic case. To speed the nonlinear calculations, our approach uses Gaussian enveloped quasimonochromatic external fields. We thereby obtain the frequency-dependent second harmonic generation , the dc nonlinear rectification , and the electro-optic effect . The method is applied to nanoscale photonic nonlinear optical molecules, including -nitroaniline and the FTC chromophore, i.e., 2-[3-Cyano-4-(2-{5-[2-(4-diethylamino-phenyl)-vinyl] - thiophen-2-yl} - vinyl)-5,5-dimethyl-5H-furan-2-ylidene]- malononitrile, and yields results in good agreement with experiment.
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21 October 2007
Research Article|
October 19 2007
Real-time time-dependent density functional theory approach for frequency-dependent nonlinear optical response in photonic molecules
Y. Takimoto;
Y. Takimoto
Department of Physics,
University of Washington
, Seattle, Washington 98195, USA
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F. D. Vila;
F. D. Vila
Department of Physics,
University of Washington
, Seattle, Washington 98195, USA
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J. J. Rehr
J. J. Rehr
a)
Department of Physics,
University of Washington
, Seattle, Washington 98195, USA
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a)
Electronic mail: [email protected]
J. Chem. Phys. 127, 154114 (2007)
Article history
Received:
July 11 2007
Accepted:
September 04 2007
Citation
Y. Takimoto, F. D. Vila, J. J. Rehr; Real-time time-dependent density functional theory approach for frequency-dependent nonlinear optical response in photonic molecules. J. Chem. Phys. 21 October 2007; 127 (15): 154114. https://doi.org/10.1063/1.2790014
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