Anisotropic Polarizability-Induced Plasmon Transfer

Greta Donati; David B. Lingerfelt; Christine M. Aikens; Xiaosong Li

doi:10.1021/acs.jpcc.8b02425

Anisotropic Polarizability-Induced Plasmon Transfer

Greta Donati, David B. Lingerfelt, Christine M. Aikens, Xiaosong Li

Research output: Contribution to journal › Article › peer-review

22 Scopus citations

Abstract

Despite the large number of technological applications relying on noble metal nanoparticles' collective electron oscillations, or localized surface plasmon resonances (LSPR), a complete understanding of all factors affecting their dynamics has not yet been achieved. In this paper, a nonadiabatic Ehrenfest dynamics approach is employed to investigate the dynamics of a linear chain of silver atoms initialized in the transverse LSPR state. Out-of-chain motions are shown to cause the increase of one specific off-diagonal component of the molecular polarizability, inducing a polarization orthogonal to the direction of the transverse LSPR oscillation and consistent with the molecule's geometrical orientation. These geometry changes allow the transfer from the initially excited transverse plasmon to a multipolar longitudinal plasmon. This unique plasmon transfer mechanism, allowed only by the symmetry change of the system and never observed before, sheds light on a previously unknown feature of metal nanoparticles.

Original language	English
Pages (from-to)	10621-10626
Number of pages	6
Journal	Journal of Physical Chemistry C
Volume	122
Issue number	19
DOIs	https://doi.org/10.1021/acs.jpcc.8b02425
State	Published - May 17 2018
Externally published	Yes

Funding

The development of the first-principles electronic dynamics is supported by the US Department of Energy (DE-SC0006863). The development of LR TDDFT method for computational spectroscopy was supported by the National Science Foundation (CHE-1565520). C.M.A. is grateful to the US Department of Energy (DE-SC0012273) for the financial support. This work was facilitated though the use of advanced computational, storage, and networking infrastructure provided by the Hyak supercomputer system and funded by the STF at the University of Washington and the National Science Foundation (MRI-1624430).

Funders	Funder number
US Department of Energy	DE-SC0006863
National Science Foundation	1565520, DE-SC0012273, 1624430, CHE-1565520
University of Washington	MRI-1624430

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10.1021/acs.jpcc.8b02425

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title = "Anisotropic Polarizability-Induced Plasmon Transfer",

abstract = "Despite the large number of technological applications relying on noble metal nanoparticles' collective electron oscillations, or localized surface plasmon resonances (LSPR), a complete understanding of all factors affecting their dynamics has not yet been achieved. In this paper, a nonadiabatic Ehrenfest dynamics approach is employed to investigate the dynamics of a linear chain of silver atoms initialized in the transverse LSPR state. Out-of-chain motions are shown to cause the increase of one specific off-diagonal component of the molecular polarizability, inducing a polarization orthogonal to the direction of the transverse LSPR oscillation and consistent with the molecule's geometrical orientation. These geometry changes allow the transfer from the initially excited transverse plasmon to a multipolar longitudinal plasmon. This unique plasmon transfer mechanism, allowed only by the symmetry change of the system and never observed before, sheds light on a previously unknown feature of metal nanoparticles.",

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AU - Li, Xiaosong

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AB - Despite the large number of technological applications relying on noble metal nanoparticles' collective electron oscillations, or localized surface plasmon resonances (LSPR), a complete understanding of all factors affecting their dynamics has not yet been achieved. In this paper, a nonadiabatic Ehrenfest dynamics approach is employed to investigate the dynamics of a linear chain of silver atoms initialized in the transverse LSPR state. Out-of-chain motions are shown to cause the increase of one specific off-diagonal component of the molecular polarizability, inducing a polarization orthogonal to the direction of the transverse LSPR oscillation and consistent with the molecule's geometrical orientation. These geometry changes allow the transfer from the initially excited transverse plasmon to a multipolar longitudinal plasmon. This unique plasmon transfer mechanism, allowed only by the symmetry change of the system and never observed before, sheds light on a previously unknown feature of metal nanoparticles.

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Anisotropic Polarizability-Induced Plasmon Transfer

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