In solid state physics, electronic excitations are often classified as plasmons or single-particle excitations. The former class of states refers to collective oscillations of the electron density. The random-phase approximation allows for a quantum-theoretical treatment and a characterization on a microscopic level as a coherent superposition of a large number of particle-hole transitions with the same momentum transfer. However, small systems such as molecules or small nanoclusters lack the basic properties (momentum conservation and uniform exchange interaction) responsible for the formation of plasmons in the solid-state case. Despite an enhanced interest in plasmon-based technologies and an increasing number of studies regarding plasmons in molecules and small nanoclusters, their definition on a microscopic level of theory remains ambiguous. In this work, we analyze the microscopic properties of molecular plasmons in comparison with the homogeneous electron gas as a model system. Subsequently, the applicability of the derived characteristics is validated by analyzing the electronic excitation vectors with respect to orbital transitions for two linear polyenes within second order versions of the algebraic diagrammatic construction scheme for the polarization propagator.
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14 September 2014
Research Article|
September 08 2014
Plasmons in molecules: Microscopic characterization based on orbital transitions and momentum conservation
Caroline M. Krauter;
Caroline M. Krauter
a)
1Theoretical Chemistry,
Heidelberg University
, Im Neuenheimer Feld 229, D-69120 Heidelberg, Germany
2Interdisciplinary Center for Scientific Computing,
Heidelberg University
, Im Neuenheimer Feld 368, 69120 Heidelberg, Germany
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Jochen Schirmer;
Jochen Schirmer
1Theoretical Chemistry,
Heidelberg University
, Im Neuenheimer Feld 229, D-69120 Heidelberg, Germany
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Christoph R. Jacob;
Christoph R. Jacob
3Center for Functional Nanostructures and Institute of Physical Chemistry,
Karlsruhe Institute of Technology (KIT)
, Wolfgang-Gaede-Strasse 1a, 76131 Karlsruhe, Germany
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Markus Pernpointner;
Markus Pernpointner
1Theoretical Chemistry,
Heidelberg University
, Im Neuenheimer Feld 229, D-69120 Heidelberg, Germany
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Andreas Dreuw
Andreas Dreuw
2Interdisciplinary Center for Scientific Computing,
Heidelberg University
, Im Neuenheimer Feld 368, 69120 Heidelberg, Germany
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a)
Present address: Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, New Jersey 08544-5263, USA. Electronic mail: [email protected].
J. Chem. Phys. 141, 104101 (2014)
Article history
Received:
June 13 2014
Accepted:
August 19 2014
Citation
Caroline M. Krauter, Jochen Schirmer, Christoph R. Jacob, Markus Pernpointner, Andreas Dreuw; Plasmons in molecules: Microscopic characterization based on orbital transitions and momentum conservation. J. Chem. Phys. 14 September 2014; 141 (10): 104101. https://doi.org/10.1063/1.4894266
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