Emergence of excited-state plasmon modes in linear hydrogen chains from time-dependent quantum mechanical methods
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Date
2011-11-03
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Citation of Original Publication
DePrince, A. Eugene, Matthew Pelton, Jeffrey R. Guest, and Stephen K. Gray. “Emergence of Excited-State Plasmon Modes in Linear Hydrogen Chains from Time-Dependent Quantum Mechanical Methods.” Physical Review Letters 107, no. 19 (November 3, 2011): 196806. https://doi.org/10.1103/PhysRevLett.107.196806.
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This work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law.
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Abstract
Explicitly time-dependent configuration-interaction theory is used to predict a new type of plasmonic behavior in linear hydrogen chains. After an intense ultrashort laser pulse brings the system into a broad superposition of excited states, the electronic dipole of the entire chain oscillates coherently, and the system is predicted to emit radiation at energies significantly lower than the first absorption band. A simple classical model accurately predicts the energy of this plasmon resonance for different hydrogen chain lengths and electron densities, demonstrating that collective, free-electron-like behavior can arise in chains of as few as 20 hydrogen atoms. The excitation mechanism for this plasmonic resonance is a highly nonlinear, multiphoton process, different from the linear excitation of ordinary surface plasmons.