An earlier proposed approach to molecular response functions based on the intermediate state representation (ISR) of polarization propagator and algebraic-diagrammatic construction (ADC) approximations is for the first time employed for calculations of nonlinear response properties. The two-photon absorption (TPA) spectra are considered. The hierarchy of the first- and second-order ADC/ISR computational schemes, ADC(1), ADC(2), ADC(2)-x, and ADC(3/2), is tested in applications to H2O, HF, and C2H4 (ethylene). The calculated TPA spectra are compared with the results of coupled cluster (CC) models and time-dependent density-functional theory (TDDFT) calculations, using the results of the CC3 model as benchmarks. As a more realistic example, the TPA spectrum of C8H10 (octatetraene) is calculated using the ADC(2)-x and ADC(2) methods. The results are compared with the results of TDDFT method and earlier calculations, as well as to the available experimental data. A prominent feature of octatetraene and other polyene molecules is the existence of low-lying excited states with increased double excitation character. We demonstrate that the two-photon absorption involving such states can be adequately studied using the ADC(2)-x scheme, explicitly accounting for interaction of doubly excited configurations. Observed peaks in the experimental TPA spectrum of octatetraene are assigned based on our calculations.
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14 February 2012
Research Article|
February 10 2012
Calculations of nonlinear response properties using the intermediate state representation and the algebraic-diagrammatic construction polarization propagator approach: Two-photon absorption spectra
S. Knippenberg;
S. Knippenberg
a)
1Institute for Physical and Theoretical Chemistry,
Goethe University Frankfurt
, Max-von-Laue-Str. 7, 60438 Frankfurt/Main, Germany
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D. R. Rehn;
D. R. Rehn
2Interdisciplinary Center for Scientific Computing,
Ruprecht-Karls University
, Im Neuenheimer Feld 368, 69120 Heidelberg, Germany
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M. Wormit;
M. Wormit
3Centre for Theoretical Chemistry and Physics, Institute for Advanced Study,
Massey University
, Auckland, New Zealand
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J. H. Starcke;
J. H. Starcke
1Institute for Physical and Theoretical Chemistry,
Goethe University Frankfurt
, Max-von-Laue-Str. 7, 60438 Frankfurt/Main, Germany
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I. L. Rusakova;
I. L. Rusakova
4A. E. Favorsky Irkutsk Institute of Chemistry,
Siberian Branch of the Russian Academy of Sciences
, 1 Favorsky Street, 664033 Irkutsk, Russia
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A. B. Trofimov;
A. B. Trofimov
5Laboratory of Quantum Chemistry,
Irkutsk State University
, Karl Marx Street 1, 664003 Irkutsk, Russia
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a)
Present address: Laboratory for Chemistry of Novel Materials, University of Mons, Place du Parc 20, B-7000 Mons, Belgium.
b)
Author to whom correspondence should be addressed. Electronic mail: [email protected].
J. Chem. Phys. 136, 064107 (2012)
Article history
Received:
November 30 2011
Accepted:
January 17 2012
Citation
S. Knippenberg, D. R. Rehn, M. Wormit, J. H. Starcke, I. L. Rusakova, A. B. Trofimov, A. Dreuw; Calculations of nonlinear response properties using the intermediate state representation and the algebraic-diagrammatic construction polarization propagator approach: Two-photon absorption spectra. J. Chem. Phys. 14 February 2012; 136 (6): 064107. https://doi.org/10.1063/1.3682324
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