Electronic structure and optical properties of metallic nanoshells

The electronic structure and optical properties of metallic nanoshells are investigated using a jellium model and the Time Dependent Local Density Approximation (TDLDA). An efficient numerical implementation enables applications to nanoshells of realistic size with up to a million electrons. We demonstrate how a frequency dependent background polarizability of the jellium shell can be included in the TDLDA formalism. The energies of the plasmon resonances are calculated for nanoshells of different sizes and with different dielectric cores, dielectric embedding media, and dielectric shell backgrounds. The plasmon energies are found to be in good agreement with the results from classical Mie scattering theory using a Drude dielectric function. A comparison with experimental data shows excellent agreement between theory and the measured frequency dependent absorption spectra

Effective temperature determinations of late-type stars based on 3D non-LTE Balmer line formation

Hydrogen Balmer lines are commonly used as spectroscopic effective temperature diagnostics of late-type stars. However, the absolute accuracy of classical methods that are based on one-dimensional (1D) hydrostatic model atmospheres and local thermodynamic equilibrium (LTE) is still unclear. To investigate this, we carry out 3D non-LTE calculations for the Balmer lines, performed, for the first time, over an extensive grid of 3D hydrodynamic STAGGER model atmospheres. For H$\alpha$, H$\beta$, and H$\gamma$, we find significant 1D non-LTE versus 3D non-LTE differences (3D effects): the outer wings tend to be stronger in 3D models, particularly for H$\gamma$, while the inner wings can be weaker in 3D models, particularly for H$\alpha$. For H$\alpha$, we also find significant 3D LTE versus 3D non-LTE differences (non-LTE effects): in warmer stars ($T_{\text{eff}}\approx6500$K) the inner wings tend to be weaker in non-LTE models, while at lower effective temperatures ($T_{\text{eff}}\approx4500$K) the inner wings can be stronger in non-LTE models; the non-LTE effects are more severe at lower metallicities. We test our 3D non-LTE models against observations of well-studied benchmark stars. For the Sun, we infer concordant effective temperatures from H$\alpha$, H$\beta$, and H$\gamma$; however the value is too low by around 50K which could signal residual modelling shortcomings. For other benchmark stars, our 3D non-LTE models generally reproduce the effective temperatures to within $1\sigma$ uncertainties. For H$\alpha$, the absolute 3D effects and non-LTE effects can separately reach around 100K, in terms of inferred effective temperatures. For metal-poor turn-off stars, 1D LTE models of H$\alpha$ can underestimate effective temperatures by around 150K. Our 3D non-LTE model spectra are publicly available, and can be used for more reliable spectroscopic effective temperature determinations.Comment: 19 pages, 10 figures, abstract abridged; accepted for publication in Astronomy & Astrophysic

Transient currents and universal timescales for a fully time-dependent quantum dot in the Kondo regime

Using the time-dependent non-crossing approximation, we calculate the transient response of the current through a quantum dot subject to a finite bias when the dot level is moved suddenly into a regime where the Kondo effect is present. After an initial small but rapid response, the time-dependent conductance is a universal function of the temperature, bias, and inverse time, all expressed in units of the Kondo temperature. Two timescales emerge: the first is the time to reach a quasi-metastable point where the Kondo resonance is formed as a broad structure of half-width of the order of the bias; the second is the longer time required for the narrower split peak structure to emerge from the previous structure and to become fully formed. The first time can be measured by the gross rise time of the conductance, which does not substantially change later while the split peaks are forming. The second time characterizes the decay rate of the small split Kondo peak (SKP) oscillations in the conductance, which may provide a method of experimental access to it. This latter timescale is accessible via linear response from the steady stateand appears to be related to the scale identified in that manner [A. Rosch, J. Kroha, and P. Wolfle, Phys. Rev. Lett. 87, 156802 (2001)].Comment: Revtex with 15 eps figures. Compiles to 11 page

Kondo time scales for quantum dots - response to pulsed bias potentials

The response of a quantum dot in the Kondo regime to rectangular pulsed bias potentials of various strengths and durations is studied theoretically. It is found that the rise time is faster than the fall time, and also faster than time scales normally associated with the Kondo problem. For larger values of the pulsed bias, one can induce dramatic oscillations in the induced current with a frequency approximating the splitting between the Kondo peaks that would be present in steady state. The effect persists in the total charge transported per pulse, which should facilitate the experimental observation of the phenomenon.Comment: 5 pages with 4 encapsulated figures which come in separate postscript files: latex file: text.tex figures: fig1.eps, fig2.eps, fig3.eps, fig4.ep

Robust Subnanometric Plasmon Ruler by Rescaling of the Nonlocal Optical Response

We present the optical response of two interacting metallic nanowires calculated for separation distances down to angstrom range. State-of-the-art local and nonlocal approaches are compared with full quantum time-dependent density functional theory calculations that give an exact account of nonlocal and tunneling effects. We find that the quantum results are equivalent to those from classical approaches when the nanoparticle separation is defined as the separation between centroids of the screening charges. This establishes a universal plasmon ruler for subnanometric distances. Such a ruler not only impacts the basis of many applications of plasmonics, but also provides a robust rule for subnanometric metrology

Resonance Lifetimes from Complex Densities

The ab-initio calculation of resonance lifetimes of metastable anions challenges modern quantum-chemical methods. The exact lifetime of the lowest-energy resonance is encoded into a complex "density" that can be obtained via complex-coordinate scaling. We illustrate this with one-electron examples and show how the lifetime can be extracted from the complex density in much the same way as the ground-state energy of bound systems is extracted from its ground-state density

Electronic structure of small GaAs clusters

The electronic structure of small Ga_xAs_y clusters (x+y≤10) are calculated using the local density method. The calculation shows that even‐numbered clusters tend to be singlets, as opposed to odd‐numbered clusters which are open shell systems. This is in agreement with the experimental observations of even/odd alternations of the electron affinity and ionization potential. In the larger clusters, the atoms prefer an alternating bond arrangement; charge transfers are observed from Ga sites to As sites. This observation is also in agreement with recent chemisorption studies of ammonia on GaAs clusters. The close agreement between theoretical calculations and experimental results, together with the rich variation of electronic properties of GaAs clusters with composition makes GaAs clusters an ideal prototype system for the study of how electronic structure influences chemical reactivity