Theoretical Studies of Plasmonics using Electronic Structure Methods

Morton, Seth M.; Silverstein, D.; Jensen, Lasse

doi:10.1021/cr100265f

Cited by 430 publications

(506 citation statements)

References 518 publications

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“…[3][4][5] This phenomenon, called surface plasmon resonance (SPR), has been intensively studied both experimentally [6][7][8][9][10] and theoretically. [11][12][13][14][15][16] Applications include high-sensitivity chemical and biological sensing [17][18][19][20][21][22][23][24][25] as well as energy conversion and storage. 26,27 Anisotropic systems such as nanorods and nanowires are especially useful for certain applications such as photothermal cancer therapy.…”

Section: Introductionmentioning

confidence: 99%

Quantum coherent plasmon in silver nanowires: A real-time TDDFT study

Ding

Guidez

Aikens

et al. 2014

The Journal of Chemical Physics

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A plasmon-like phenomenon, arising from coinciding resonant excitations of different electronic characteristics in 1D silver nanowires, has been proposed based on theoretical linear absorption spectra. Such a molecular plasmon holds the potential for anisotropic nanoplasmonic applications. However, its dynamical nature remains unexplored. In this work, quantum dynamics of longitudinal and transverse excitations in 1D silver nanowires are carried out within the real-time time-dependent density functional theory framework. The anisotropic electron dynamics confirm that the transverse transitions of different electronic characteristics are collective in nature and oscillate in-phase with respect to each other. Analysis of the time evolutions of participating one-electron wave functions suggests that the transverse transitions form a coherent wave packet that gives rise to a strong plasmon resonance at the molecular level. © 2014 AIP Publishing LLC. [http://dx

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Section: Introductionmentioning

confidence: 99%

Quantum coherent plasmon in silver nanowires: A real-time TDDFT study

Ding

Guidez

Aikens

et al. 2014

The Journal of Chemical Physics

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“…Therefore, there is a need to address the influence of the atomic configuration in the plasmonic response at the nanoscale. In this Rapid Communication we present ab initio calculations including the atomic structure, in accordance with the current paradigm in computational condensed matter physics [32] and physical chemistry [33]. We study one of the canonical cases in nanoplasmonics: the hybridization of LSPs in a metallic-cluster dimer.…”

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confidence: 99%

Ab initionanoplasmonics: The impact of atomic structure

et al. 2014

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We present an ab initio study of the hybridization of localized surface plasmons in a metal nanoparticle dimer. The atomic structure, which is often neglected in theoretical studies of quantum nanoplasmonics, has a strong impact on the optical absorption properties when subnanometric gaps between the nanoparticles are considered. We demonstrate that this influences the hybridization of optical resonances of the dimer, and leads to significantly smaller electric field enhancements as compared to the standard jellium model. In addition, we show that the corrugation of the metal surface at a microscopic scale becomes as important as other well-known quantum corrections to the plasmonic response, implying that the atomic structure has to be taken into account to obtain quantitative predictions for realistic nanoplasmonic devices. There is a growing interest in the development and implementation of nanoplasmonic devices such as nanosensors [1,2], nanophotonic lasers [3][4][5], optoelectronic [6,7] and light-harvesting [8,9] structures, and nanoantennas [10,11]. Therefore, it is essential to have theoretical techniques with a sufficient predictive value to understand the physical processes of light-matter interactions at the nanoscale. In this regime, the standard analysis of the plasmonic response to external electromagnetic (EM) fields using the classical macroscopic Maxwell equations must be undertaken with caution. Indeed, genuine quantum effects such as the nonlocal nature of the electron-density response, the inhomogeneity of the conduction-electron density, or the possibility of charge transfer by tunneling have to be considered [12]. These effects can be incorporated into Maxwell equations in an approximate manner using, e.g., nonlocal dielectric functions [13][14][15][16][17][18][19] or the ad hoc inclusion of "virtual" dielectric materials [20][21][22]. While these semiclassical approximations have been successfully applied in many cases, they do not achieve the precision provided by first-principle calculations.A number of recent publications [20,[23][24][25][26][27] have treated the electronic response of plasmonic structures using stateof-the-art time-dependent density functional theory (TDDFT) [28,29]. However, the ionic structure is typically neglected and replaced by a homogeneous jellium background or by an unstructured effective potential. Although this approximation is sometimes justified by the collective nature of plasmon excitations [30,31], the charge oscillations associated with a localized surface plasmon (LSP) are mainly concentrated on the metal-vacuum interface. One may thus expect that the ionic structure in this region will have a quantitative and even qualitative impact. Therefore, there is a need to address the influence of the atomic configuration in the plasmonic response at the nanoscale. In this Rapid Communication we present ab initio calculations including the atomic structure, in accordance with the current paradigm in computational condensed matter physics [32] and physical chem...

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“…nanopolaritonics), [1][2][3][4] a new field investigating the interaction between molecules and surface plasmons, requires modeling of a large number of electrons coupled to an electromagnetic field. Time dependent density functional theory (TDDFT) has been widely used to study quantum effects in plasmonics [5][6][7] that are missing in conventional classical electrodynamics models. [8][9][10] However, TDDFT is expensive so a multiscale approach bridging the molecular and plasmonic scales is needed.…”

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confidence: 99%