Surface plasmon in metallic nanoparticles: Renormalization effects due to electron-hole excitations

Weick, Guillaume; Ingold, Gert‐Ludwig; Jalabert, Rodolfo A.; Weinmann, Dietmar

doi:10.1103/physrevb.74.165421

Cited by 82 publications

(161 citation statements)

References 56 publications

(160 reference statements)

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“…The redshift of the surface-plasmon resonance in Na is linked to the electron spill-out in free space, or more precisely, to the fact that the centroid of the induced charge density r 1 associated with the SPR is placed outside the jellium edge 19,21,58 . Our selfconsistent calculations correctly reproduce this feature of r 1 at the SPR peak, as it is shown in Fig.…”

Section: Article Nature Communications | Doi: 101038/ncomms8132mentioning

confidence: 99%

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Resonance shifts and spill-out effects in self-consistent hydrodynamic nanoplasmonics

et al. 2015

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The standard hydrodynamic Drude model with hard-wall boundary conditions can give accurate quantitative predictions for the optical response of noble-metal nanoparticles. However, it is less accurate for other metallic nanosystems, where surface effects due to electron density spill-out in free space cannot be neglected. Here we address the fundamental question whether the description of surface effects in plasmonics necessarily requires a fully quantum-mechanical ab initio approach. We present a self-consistent hydrodynamic model (SC-HDM), where both the ground state and the excited state properties of an inhomogeneous electron gas can be determined. With this method we are able to explain the size-dependent surface resonance shifts of Na and Ag nanowires and nanospheres. The results we obtain are in good agreement with experiments and more advanced quantum methods. The SC-HDM gives accurate results with modest computational effort, and can be applied to arbitrary nanoplasmonic systems of much larger sizes than accessible with ab initio methods.

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Section: Article Nature Communications | Doi: 101038/ncomms8132mentioning

confidence: 99%

“…This approximation is more accurate for noble metals, that show a high work function 17 , than for alkali metals [18][19][20][21] , where the electron density spill-out in free-space characterizes the plasmonic response. This is a well-known limitation of the HDM 22 and many attempts have been made to overcome it, thus far with limited success.…”

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confidence: 99%

Resonance shifts and spill-out effects in self-consistent hydrodynamic nanoplasmonics

et al. 2015

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“…For example, in the approach where the environment is separated from the low-energy excitations that compose the collective plasmon excitation, the timescales that characterise the dynamics of the electronic environment [20] depend on the cutoff energy. Moreover, it was shown in [6] that the environment-induced redshift of the resonance frequency depends logarithmically on the cutoff. In the following we will provide an estimation of the cutoff energy separating the two subspaces.…”

Section: Introductionmentioning

confidence: 99%

“…The theoretical descriptions built to study this problem [5,6,13,18] treat the collective coordinate as a special degree of freedom, which is coupled to an environment constituted by the degrees of freedom of the relative coordinates. Friction arising from particle-hole pairs has been studied in bulk systems [19].…”

Section: Introductionmentioning

confidence: 99%

Friction of the surface plasmon by high-energy particle-hole pairs

et al. 2007

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Abstract. We show that the dynamics of the surface plasmon in metallic nanoparticles damped by its interaction with particle-hole excitations can be modelled by a single degree of freedom coupled to an environment. In this approach, the fast decrease of the dipole matrix elements that couple the plasmon to particle-hole pairs with the energy of the excitation allows a separation of the Hilbert space into low-and high-energy subspaces at a characteristic energy that we estimate. A picture of the spectrum consisting of a collective excitation built from low-energy excitations which interacts with high-energy particle-hole states can be formalised. The high-energy excitations yield an approximate description of a dissipative environment (or "bath") within a finite confined system. Estimates for the relevant timescales establish the Markovian character of the bath dynamics with respect to the surface plasmon evolution for nanoparticles with a radius larger than about 1 nm.PACS. 73.20.Mf Collective excitations -78.67.n Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures -71.45.Gm Exchange, correlation, dielectric and magnetic response functions, plasmons

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“…The set of relevant states includes the ground state a n = g n and the excited state a n = e n of the neutral molecule, as well as the negatively charged molecular (ground) state a n = f n , cf. Fig.1 The dipole plasmons of the left spherical lead can be modeled as three degenerate quantum harmonic oscillators [44] with the Hamiltonian…”

Section: Molecular Junction Modelmentioning

confidence: 99%

Theoretical study of plasmonic lasing in junctions with many molecules

2016

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We calculate the quantum state of the plasmon field excited by an ensemble of molecular emitters, which are driven by exchange of electrons with metallic nano-particle electrodes. Assuming identical emitters that are coupled collectively to the plasmon mode but are otherwise subject to independent relaxation channels, we show that symmetry constraints on the total system density matrix imply a drastic reduction in the numerical complexity. For N m three-level molecules we may thus represent the density matrix by a number of terms scaling as (N m + 8)!/(8!N m !) instead of 9 N m , and this allows exact simulations of up to N m = 10 molecules. Our simulations demonstrate that many emitters compensate strong plasmon damping and lead to the population of high plasmon number states and a narrowed linewidth of the plasmon field. For large N m , our exact results are reproduced by an approximate approach based on the plasmon reduced density matrix. With this approach, we have extended the simulations to more than 50 molecules and shown that the plasmon number state population follows a Poisson-like distribution. An alternative approach based on nonlinear rate equations for the molecular state populations and the mean plasmon number also reproduce the main lasing characteristics of the system.

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Surface plasmon in metallic nanoparticles: Renormalization effects due to electron-hole excitations

Cited by 82 publications

References 56 publications

Resonance shifts and spill-out effects in self-consistent hydrodynamic nanoplasmonics

Resonance shifts and spill-out effects in self-consistent hydrodynamic nanoplasmonics

Friction of the surface plasmon by high-energy particle-hole pairs

Theoretical study of plasmonic lasing in junctions with many molecules

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