Anisotropic Decay Dynamics of Photoexcited Aligned Carbon Nanotube Bundles

We have performed polarization-dependent ultrafast pump-probe spectroscopy of a film of aligned single-walled carbon nanotube bundles. By taking into account imperfect nanotube alignment as well as anisotropic absorption cross sections, we quantitatively determined distinctly different photo-bleaching dynamics for polarizations parallel and perpendicular to the tube axis. For perpendicular polarization, we observe a slow (1.0-1.5 ps) relaxation process, previously unobserved in randomly-oriented nanotube bundles. We attribute this slower dynamics to the excitation and relaxation of surface plasmons in the radial direction of the nanotube bundles.Comment: 4 pages, 3 figure

Non-Fourier heat transport in metal-dielectric core-shell nanoparticles under ultrafast laser pulse excitation

Relaxation dynamics of embedded metal nanoparticles after ultrafast laser pulse excitation is driven by thermal phenomena of different origins the accurate description of which is crucial for interpreting experimental results: hot electron gas generation, electron-phonon coupling, heat transfer to the particle environment and heat propagation in the latter. Regardingthis last mechanism, it is well known that heat transport in nanoscale structures and/or at ultrashort timescales may deviate from the predictions of the Fourier law. In these cases heat transport may rather be described by the Boltzmann transport equation. We present a numerical model allowing us to determine the electron and lattice temperature dynamics in a spherical gold nanoparticle core under subpicosecond pulsed excitation, as well as that of the surrounding shell dielectric medium. For this, we have used the electron-phonon coupling equation in the particle with a source term linked with the laser pulse absorption, and the ballistic-diffusive equations for heat conduction in the host medium. Either thermalizing or adiabatic boundary conditions have been considered at the shell external surface. Our results show that the heat transfer rate from the particle to the matrix can be significantly smaller than the prediction of Fourier's law. Consequently, the particle temperature rise is larger and its cooling dynamics might be slower than that obtained by using Fourier's law. This difference is attributed to the nonlocal and nonequilibrium heat conduction in the vicinity of the core nanoparticle. These results are expected to be of great importance for analyzing pump-probe experiments performed on single nanoparticles or nanocomposite media

Off-resonance field enhancement by spherical nanoshells

We study light scattering by spherical nanoshells consistent of metal/dielectric composites. We consider two geometries of metallic nanoshell with dielectric core, and dielectric coated metallic nanoparticle. We demonstrate that for both geometries the local field enhancement takes place out of resonance regions ("dark states"), which, nevertheless, can be understood in terms of the Fano resonance. At optimal conditions the light is stronger enhanced inside the dielectric material. By using nonlinear dielectric materials it will lead to a variety nonlinear phenomena applicable for photonics applications

On-command enhancement of single molecule fluorescence using a gold nanoparticle as an optical nano-antenna

We investigate the coupling of a single molecule to a single spherical gold nanoparticle acting as a nano-antenna. Using scanning probe technology, we position the particle in front of the molecule with nanometer accuracy and measure a strong enhancement of more than 20 times in the fluorescence intensity simultaneous to a 20-fold shortening of the excited state lifetime. Direct comparison with three-dimensional calculations allow us to decipher the contributions of the excitation enhancement, spontaneous emission modification, and quenching. Furthermore, we provide direct evidence for the role of the particle plasmon resonance in the modification of the molecular emission.Comment: 5 pages, 4 figures. submitted to Phys.Rev.Lett. 12/04/200

Dynamics of femtosecond laser-induced melting and amorphization of indium phosphide

7 pages, 5 figures.-- PACS: 64.70.Dv; 81.30.Fb; 61.80.Ba; 78.66.Fd; 61.82.FkLaser-induced melting and resolidification of single-crystalline indium phosphide (InP) upon irradiation with 150 fs laser pulses at 800 nm has been investigated by means of real-time-reflectivity measurements with subnanosecond time resolution. Melting of the surface is observed to occur very rapidly on a time scale shorter than our experimental resolution while the lifetime of the liquid phase is several tens of nanoseconds. As a result of the subsequent rapid solidification process, a thin layer of amorphous material with a thickness of several tens of nanometers is formed on the surface. The formation of this amorphous layer has been observed for every fluence above the melting and below the ablation threshold. The evolution of the reflectivity has been modeled for several different solidification scenarios and compared to the experimental results. This comparison shows that solidification proceeds interfacially from the solid interface towards the surface. A lower limit for the critical solid-liquid interface velocity for amorphization in this compound semiconductor has been estimated to be in the range of 1–4 m/s.This work has been partially supported by the EU in the frame of the TMR Project XPOSE (Grant No. HPRN-CT- 2000-00160). S.M.W. acknowledges the funding in the frame of the same project. J.B. acknowledges the funding of the CSIC through a contract in the frame of the I3P programme (Ref. I3P-PC2002), co-funded by the European Social Fund.Peer reviewe

Structural, Vibrational and Thermodynamic Properties of AgnCu34-n Nanoparticles

We report results of a systematic study of structural, vibrational and thermodynamical properties of 34-atom bimetallic nanoparticles from the AgnCu34-n family using model interaction potentials as derived from the embedded atom method and in the harmonic approximation of lattice dynamics. Systematic trends in the bond length and dynamical properties can be explained largely on arguments based on local coordination and elemental environment. Thus increase in the number of silver atoms in a given neighborhood introduces a monotonic increase in bond length while increase of the copper content does the reverse. Moreover, based on bond lengths of the lowest coordinated (6 and 8) copper atoms with their nearest neighbors (Cu atoms), we find that the nanoparticles divide into two groups with average bond length either close to (~ 2.58 A) or smaller (~ 2.48 A) than that in bulk copper, accompanied by characteristic features in their vibrational density of states. For the entire set of nanoparticles, vibrational modes are found above the bulk bands of copper/silver. Furthermore, a blue shift in the high frequency end with increasing number of copper atoms in the nanoparticles is traced to a shrinkage of bond lengths from bulk values. The vibrational densities of states at the low frequency end of the spectrum scale linearly with frequency as for single element nanoparticles, however, the effect is more pronounced for these nanoalloys. The Debye temperature was found to be about one third of that of the bulk for pure copper and silver nanoparticles with a non-linear increase with increasing number of copper atoms in the nanoalloys.Comment: 37 pages, 12 figure

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

Photoemission Electron Microscopy as a tool for the investigation of optical near fields

Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiO$_{x}$). Photoemission was induced by illumination with a Hg UV-lamp (photon energy cutoff $\hbar\omega_{UV}=5.0$ eV, wavelength $\lambda_{UV}=250$ nm) and with a Ti:Sapphire femtosecond laser ($\hbar\omega_{l}=3.1$ eV, $\lambda_{l}=400$ nm, pulse width below 200 fs), respectively. While homogeneous photoelectron emission from the metal is observed upon illumination at energies above the silver plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signature of the local electrical field therefore providing a tool to map the optical near field with the resolution of emission electron microscopy.Comment: 10 pages, 4 figures; submitted to Physical Review Letter

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

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