Efficient implementation of isotropic cubic response functions for two-photon absorption cross sections within the self-consistent field approximation
Within the self-consistent field approximation, computationally tractable expressions for the isotropic second-order hyperpolarizability have been derived and implemented for the calculation of two-photon absorption cross sections. The novel tensor average formulation presented in this work allows f...
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| Hauptverfasser: | , , , , , , |
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| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
12 January 2021
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| In: |
The journal of chemical physics
Year: 2021, Jahrgang: 154, Heft: 2 |
| ISSN: | 1089-7690 |
| DOI: | 10.1063/5.0031851 |
| Online-Zugang: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1063/5.0031851 Verlag, lizenzpflichtig, Volltext: https://aip.scitation.org/doi/10.1063/5.0031851 
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| Verfasserangaben: | Karan Ahmadzadeh, Mikael Scott, Manuel Brand, Olav Vahtras, Xin Li, Zilvinas Rinkevicius, and Patrick Norman |
| Zusammenfassung: | Within the self-consistent field approximation, computationally tractable expressions for the isotropic second-order hyperpolarizability have been derived and implemented for the calculation of two-photon absorption cross sections. The novel tensor average formulation presented in this work allows for the evaluation of isotropic damped cubic response functions using only ∼3.3% (one-photon off-resonance regions) and ∼10% (one-photon resonance regions) of the number of auxiliary Fock matrices required when explicitly calculating all the needed individual tensor components. Numerical examples of the two-photon absorption cross section in the one-photon off-resonance and resonance regions are provided for alanine-tryptophan and 2,5-dibromo-1,4-bis(2-(4-diphenylaminophenyl)vinyl)-benzene. Furthermore, a benchmark set of 22 additional small- and medium-sized organic molecules is considered. In all these calculations, a quantitative assessment is made of the reduced and approximate forms of the cubic response function in the one-photon off-resonance regions and results demonstrate a relative error of less than ∼5% when using the reduced expression as compared to the full form of the isotropic cubic response function. |
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| Beschreibung: | Gesehen am 23.02.2021 |
| Beschreibung: | Online Resource |
| ISSN: | 1089-7690 |
| DOI: | 10.1063/5.0031851 |