Identification of plasmons in molecules with scaled ab initio approaches
For the electronic excitations in metallic systems under periodic boundary conditions, momentum conservation and a uniform electron-electron interaction imply a clear distinction of plasmons and single-particle excitations. For finite molecular systems, this distinction is less clear, but excitation...
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| Hauptverfasser: | , , |
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| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
September 25, 2015
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| In: |
The journal of physical chemistry. C, Energy, materials, and catalysis
Year: 2015, Jahrgang: 119, Heft: 43, Pages: 24564-24573 |
| ISSN: | 1932-7455 |
| DOI: | 10.1021/acs.jpcc.5b07659 |
| Online-Zugang: | Verlag, Volltext: http://dx.doi.org/10.1021/acs.jpcc.5b07659
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| Verfasserangaben: | Caroline M. Krauter, Stephan Bernadotte, Christoph R. Jacob, Markus Pernpointner, and Andreas Dreuw |
| Zusammenfassung: | For the electronic excitations in metallic systems under periodic boundary conditions, momentum conservation and a uniform electron-electron interaction imply a clear distinction of plasmons and single-particle excitations. For finite molecular systems, this distinction is less clear, but excitations formed by a coherent superposition of elementary particle-hole transitions that show a collective oscillation of the transition electron density have nevertheless been identified as plasmons in molecules. To aid this distinction, a scaling approach [Bernadotte, S.; Evers, F.; Jacob, C. R. J. Phys. Chem. C 2013, 117, 1863] has recently been developed that is based on the observation that, in contrast to single-particle excitations, plasmonic excitation energies strongly depend on the electron-electron interaction. In this work, we adapt the proposed scaling scheme to ab initio models, specifically configuration interaction singles and the second-order algebraic diagrammatic construction scheme of the polarization propagator. The resulting approach is applied to a series of linear polyenes and the characterization based on the scaling method is confirmed by inspection of the eigenvector components, transition density patterns, and transition strengths. |
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| Beschreibung: | Gesehen am 13.12.2017 |
| Beschreibung: | Online Resource |
| ISSN: | 1932-7455 |
| DOI: | 10.1021/acs.jpcc.5b07659 |