Calculating Nonlocal Optical Properties of Structures with Arbitrary Shape

In a recent Letter [Phys. Rev. Lett. 103, 097403 (2009)], we outlined a computational method to calculate the optical properties of structures with a spatially nonlocal dielectric function. In this Article, we detail the full method, and verify it against analytical results for cylindrical nanowires. Then, as examples of our method, we calculate the optical properties of Au nanostructures in one, two, and three dimensions. We first calculate the transmission, reflection, and absorption spectra of thin films. Because of their simplicity, these systems demonstrate clearly the longitudinal (or volume) plasmons characteristic of nonlocal effects, which result in anomalous absorption and plasmon blueshifting. We then study the optical properties of spherical nanoparticles, which also exhibit such nonlocal effects. Finally, we compare the maximum and average electric field enhancements around nanowires of various shapes to local theory predictions. We demonstrate that when nonlocal effects are included, significant decreases in such properties can occur.Comment: 30 pages, 12 figures, 1 tabl

Surface plasmon lifetime in metal nanoshells

The lifetime of localized surface plasmon plays an important role in many aspects of plasmonics and its applications. In small metal nanostructures, the dominant mechanism restricting plasmon lifetime is size-dependent Landau damping. We performed quantum-mechanical calculations of Landau damping for the bright surface plasmon mode in a metal nanoshell. In contrast to the conventional model based on the electron surface scattering, we found that the damping rate decreases as the nanoshell thickness is reduced. The origin of this behavior is traced to the spatial distribution of plasmon local field inside the metal shell. We also found that, due to interference of electron scattering amplitudes from nanoshell's two metal surfaces, the damping rate exhibits pronounced quantum beats with changing shell thickness.Comment: 9 pages, 4 Figure

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

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.Comment: 8 pages, 6 figures. Considerably extended final versio

Photothermal heterodyne imaging of individual nonfluorescent nanoclusters and nanocrystals

We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual nonfluorescent nanoclusters and nanocrystals. A 2 order of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or nonluminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle

Landau damping in thin films irradiated by a strong laser field

The rate of linear collisionless damping (Landau damping) in a classical electron gas confined to a heated ionized thin film is calculated. The general expression for the imaginary part of the dielectric tensor in terms of the parameters of the single-particle self-consistent electron potential is obtained. For the case of a deep rectangular well, it is explicitly calculated as a function of the electron temperature in the two limiting cases of specular and diffuse reflection of the electrons from the boundary of the self-consistent potential. For realistic experimental parameters, the contribution of Landau damping to the heating of the electron subsystem is estimated. It is shown that for films with a thickness below about 100 nm and for moderate laser intensities it may be comparable with or even dominate over electron-ion collisions and inner ionization.Comment: 15 pages, 2 figure

Mie-resonances, infrared emission and band gap of InN

Mie resonances due to scattering/absorption of light in InN containing clusters of metallic In may have been erroneously interpreted as the infrared band gap absorption in tens of papers. Here we show by direct thermally detected optical absorption measurements that the true band gap of InN is markedly wider than currently accepted 0.7 eV. Micro-cathodoluminescence studies complemented by imaging of metallic In have shown that bright infrared emission at 0.7-0.8 eV arises from In aggregates, and is likely associated with surface states at the metal/InN interfaces.Comment: 4 pages, 5 figures, submitted to PR

Transport and optical response of molecular junctions driven by surface plasmon-polaritons

We consider a biased molecular junction subjected to external time-dependent electromagnetic field. The field for two typical junction geometries (bowtie antennas and metal nanospheres) is calculated within finite-difference time-domain technique. Time-dependent transport and optical response of the junctions is calculated within non-equilibrium Green's function approach expressed in a form convenient for description of multi-level systems. We present numerical results for a two-level (HOMO-LUMO) model, and discuss influence of localized surface plasmon polariton modes on transport.Comment: 9 pages, 6 figure

Coherently tunable third-order nonlinearity in a nanojunction

A possibility of tuning the phase of the third-order Kerr-type nonlinear susceptibility in a system consisting of two interacting metal nanospheres and a nonlinearly polarizable molecule is investigated theoretically and numerically. It is shown that by varying the relative inter-sphere separation, it is possible to tune the phase of the effective nonlinear susceptibility \chi^{(3)}(\omega;\omega,\omega,-\omega)$in the whole range from 0 to$2\pi$.Comment: 10 pages 5 figure

Size-Dependent Surface Plasmon Dynamics in Metal Nanoparticles

We study the effect of Coulomb correlations on the ultrafast optical dynamics of small metal particles. We demonstrate that a surface-induced dynamical screening of the electron-electron interactions leads to quasiparticle scattering with collective surface excitations. In noble-metal nanoparticles, it results in an interband resonant scattering of d-holes with surface plasmons. We show that this size-dependent many-body effect manifests itself in the differential absorption dynamics for frequencies close to the surface plasmon resonance. In particular, our self-consistent calculations reveal a strong frequency dependence of the relaxation, in agreement with recent femtosecond pump-probe experiments.Comment: 8 pages + 4 figures, final version accepted to PR

Local anisotropy and giant enhancement of local electromagnetic fields in fractal aggregates of metal nanoparticles

We have shown within the quasistatic approximation that the giant fluctuations of local electromagnetic field in random fractal aggregates of silver nanospheres are strongly correlated with a local anisotropy factor S which is defined in this paper. The latter is a purely geometrical parameter which characterizes the deviation of local environment of a given nanosphere in an aggregate from spherical symmetry. Therefore, it is possible to predict the sites with anomalously large local fields in an aggregate without explicitly solving the electromagnetic problem. We have also demonstrated that the average (over nanospheres) value of S does not depend noticeably on the fractal dimension D, except when D approaches the trivial limit D=3. In this case, as one can expect, the average local environment becomes spherically symmetrical and S approaches zero. This corresponds to the well-known fact that in trivial aggregates fluctuations of local electromagnetic fields are much weaker than in fractal aggregates. Thus, we find that, within the quasistatics, the large-scale geometry does not have a significant impact on local electromagnetic responses in nanoaggregates in a wide range of fractal dimensions. However, this prediction is expected to be not correct in aggregates which are sufficiently large for the intermediate- and radiation-zone interaction of individual nanospheres to become important.Comment: 9 pages 9 figures. No revisions from previous version; only figure layout is change