Size-Dependent Surface Plasmon Dynamics in Metal Nanoparticles

Shahbazyan, Tigran V.; Perakis, I. E.; Bigot, Jean‐Yves

doi:10.1103/physrevlett.81.3120

Cited by 106 publications

(89 citation statements)

References 19 publications

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“…Nevertheless, there have been, to the best of our knowledge, no first-principles calculations of the dielectric response function of Cu that include the full effects of the crystal lattice. Furthermore, the dynamical density-response function is well-known to be a key quantity in discussing one-electron properties in real metals, and it is also of basic importance in the description of low-dimensional copper systems studied in optical and time-resolved femtosecond experiments 9,10 .…”

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confidence: 99%

Ab initiocalculations of the dynamical response of copper

1999

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The role of localized d-bands in the dynamical response of Cu is investigated, on the basis of ab initio pseudopotential calculations. The density-response function is evaluated in both the random-phase approximation (RPA) and a time-dependent local-density functional approximation (TDLDA). Our results indicate that in addition to providing a polarizable background which lowers the free-electron plasma frequency, d-electrons are responsible, at higher energies and small momenta, for a doublepeak structure in the dynamical structure factor. These results are in agreement with the experimentally determined optical response of copper. We also analyze the dependence of dynamical scattering cross sections on the momentum transfer.PACS numbers: 71.45. Gm, 72.30.+q, 78.70.Ck Noble-metal systems have been the focus of much experimental and theoretical work in order to get a better understanding of how electronic properties of delocalized, free-electron-like, electrons are altered by the presence of localized d-electrons. Silver is one of the best understood systems, where the free-electron plasma frequency is strongly renormalized (red-shifted) by the presence of a polarizable background of d-electrons 1 . Unlike silver, copper presents no decoupling between sp and d orbitals, and a combined description of these oneelectron states is needed to address both structural and electronic properties of this material. Though in the case of other materials, as semiconductors, electron-hole interactions (excitonic renormalization) strongly modify the single-particle optical absorption profile 2 , metals offer a valuable playground for investigations of dynamical exchange-correlation effects of interacting many-electron systems within a quasiparticle picture 3 . Indeed, ab initio calculations of the dynamical response of a variety of simple metals, as obtained within the random-phaseapproximation (RPA), successfully account for the experimentally determined plasmon dispersion relations 4 and scattering cross sections 5 . Within the same many-body framework, ab initio calculations of the electronic stopping power of real solids have also been reported 6 .Since the pioneering investigations by Ehrenreich and Philipp 7 on the optical absorption and reflectivity of Ag an Cu, a variety of measurements of the optical properties of copper has been reported 8 . Nevertheless, there have been, to the best of our knowledge, no first-principles calculations of the dielectric response function of Cu that include the full effects of the crystal lattice. Furthermore, the dynamical density-response function is well-known to be a key quantity in discussing one-electron properties in real metals, and it is also of basic importance in the description of low-dimensional copper systems studied in optical and time-resolved femtosecond experiments 9,10 .In this Rapid Communication we report a firstprinciples evaluation of the dynamical density-response function of Cu, as computed in the RPA and a timedependent extension of local-density functional th...

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confidence: 99%

Ab initiocalculations of the dynamical response of copper

1999

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“…[126] revealed that, for sizes smaller than ∼ 5nm, the decay times of the pump-probe signal depend strongly on the probe frequency in the immediate vicinity of the SP resonance. In particular, the relaxation is considerably slower at the SP resonance, and becomes faster right above and right below the SP frequency [126,152,153]. This and other observations suggest that collective surface excitations play an important role in the electron dynamics in small metal particles.…”

Section: Ultrafast Dynamicsmentioning

confidence: 68%

“…Despite the similarities to the bulk-like behavior, observed, e.g., in metal films, certain aspects of the optical dynamics in nanoparticles are significantly different [126,152,153]. For example, the experimental studies of copper nanoparticles by Bigot et.…”

Section: Ultrafast Dynamicsmentioning

confidence: 99%

Many-body correlation effects in the ultrafast non-linear optical response of confined Fermi seas

Perakis

Shahbazyan

2000

Surface Science Reports

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The dynamics of electrons and atoms interacting with intense and ultrashort optical pulses presents an important problem in physics that cuts across different materials such as semiconductors and metals. The currently available laser pulses, as short as 5 fs, provide a time resolution shorter than the dephasing and relaxation times in many materials. This allows for a systematic study of many-body effects using nonlinear optical spectroscopy. In this review article, we discuss the role of Coulomb correlations in the ultrafast dynamics of modulation-doped quantum wells and metal nanoparticles. We focus in particular on the manifestations of non-Markovian memory effects induced by strong electron-hole and electron-plasmon correlations.

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“…31 Namely, an electron-hole pair can nonradiatively recombine by transferring its energy to SP (and vice versa) via dynamically-screened Coulomb interaction. 32 Feynman diagrams of processes contributing to polarizability of molecule-nanoparticle system,α, are shown in Fig. 1: (a) incident photon with energy ω is absorbed by the molecule and reemitted with Stokesshifted energy ω s ; (b) after absorbing a photon, excited molecule nonradiatively recombines transferring its energy to SP in the nanoparticle, which emits a photon; (c) SP, excited by incident light, transfers its energy to the molecule, which emits a photon; and (d) after energy transfer from SP to molecule, the latter transfers the energy back to SP, which emits a photon.…”

Section: Polarizability Of Molecule-nanoparticle Systemmentioning

confidence: 99%

Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles

Pustovit

Shahbazyan

2006

Phys. Rev. B

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We present a microscopic model for surface-enhanced Raman scattering (SERS) from molecules adsorbed on small noble-metal nanoparticles. In the absence of direct overlap of molecular orbitals and electronic states in the metal, the main enhancement source is the strong electric field of the surface plasmon resonance in a nanoparticle acting on a molecule near the surface. In small particles, the electromagnetic enhancement is strongly modified by quantum-size effects. We show that, in nanometer-sized particles, SERS magnitude is determined by a competition between several quantum-size effects such as the Landau damping of surface plasmon resonance and reduced screening near the nanoparticle surface. Using time-dependent local density approximation, we calculate spatial distribution of local fields near the surface and enhancement factor for different nanoparticles sizes.

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Size-Dependent Surface Plasmon Dynamics in Metal Nanoparticles

Cited by 106 publications

References 19 publications

Ab initiocalculations of the dynamical response of copper

Ab initiocalculations of the dynamical response of copper

Many-body correlation effects in the ultrafast non-linear optical response of confined Fermi seas

Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles

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