Preparation and electronic structure of phase pure K3C60

Phase pure K₃C₆₀ films have been grown using vacuum distillation. The structure of such films could be shown to be face centered cubic consistent with X-ray diffraction studies. The electronic structure of the films has been studied using electron energy-loss spectroscopy in transmission. From C1s core excitation measurements the unoccupied density of states has been determined. Performing the dielectric function has been derived in a wide energy range (0–45 eV). It is shown that the low energy part of the optical conductivity cannot be understood within a simple free electron model but that interband transitions between the three conduction bands have to be taken into account. The spectral weight of interband transitions between valence and conduction bands shows strong momentum dependence due to optical selection rules demonstrating the molecular-like nature of the electronic states.     

Optical Properties of Hexagonal and Cubic ZnS Nanoribbons: Experiment and Theory

Optical properties of hexagonal and cubic ZnS nanoribbons are studied by using valence electron energy loss spectroscopy （VEELS） and ab initio band structure calculations. The peaks in VEELS are assigned to interband transitions by comparing the interband transition strengths with the calculated densities of states. The optical properties are deduced from the experimental VEELS, and the theoretical calculations give consistent results. This combination of experimental and theoretical approaches provides a comprehensive understanding of the optical properties of polytype ZnS.     

Optical and spectral tunability of multilayer spherical and cylindrical nanoshells

This theoretical work presents a comparative study of the optical properties and spectral tunability of hybrid multilayer spherical and cylindrical nanoshells based on the quasi-static approximation of classical electrodynamics. The interband transitions have been considered using the Drude–Lorentz model for the complex dielectric function of metallic layers because the optical properties of metals arise from both the optical excitation of interband transitions and the free-electron response. A general formula for N-ayer concentric nanoshells is arranged, and numerical calculations are performed for the four-layer nanoshells as an example. We have analyzed in detail different configurations of nanoshells such as dielectric-metal-dielectric-metal with dielectric core, metal-dielectric-metal-dielectric with metal core and semiconductor-metal-dielectric-metal with semiconductor core because composition of nanoshells have dramatic influence on their optical properties. The absorbance spectrum behavior of the shell thicknesses, surrounding medium, shape and composition of each layer of the nanoshell is numerically investigated.     

Microscopic theory of optical dephasing in semiconductors

Dephasing, i.e. the decay of the optical interband polarization in a semiconductor results from destructive interference effects between different microscopic contributions. For a system without any disorder it is shown that the many-body Coulomb correlations lead to excitation-induced dephasing which becomes increasingly important at elevated excitation levels. The effect of disorder-induced dephasing is analyzed for low excitation levels, where the combined influence of excitonic, biexcitonic, and disorder scattering contributions lead to a temporal decay of the four-wave-mixing signal. Received: 30 March 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

Second-harmonic interferometric spectroscopy of buried interfaces of column IV semiconductors

The technique of combined optical second-harmonic (SH) intensity and phase spectroscopy, which is the spectroscopic modification of SH phase measurements, is proposed to study the nonlinear optical response of semiconductor interfaces with spectrally close resonant contributions. The spectral dependences of SH intensity and phase from oxidised Si (111) and Ge (111) surfaces are studied in the range of 3.5- to 5-eV SH photon energy. The resonant behaviour of combined SH spectra is associated with a superposition of contributions from direct interband transitions at several critical points of Si and Ge band structures. Received: 16 October 2001 / Revised version: 16 April 2002 / Published online: 6 June 2002     

Band-dependent quasiparticle dynamics in the hole-doped Ba-122 iron pnictides

We report on band-dependent quasiparticle dynamics in the hole-doped Ba-122 pnictides measured by ultrafast pump-probe spectroscopy. In the superconducting state of the optimal and over hole-doped samples, we observe two distinct relaxation processes: a fast component whose decay rate increases linearly with excitation density and a slow component whose relaxation is independent of excitation strength. We argue that these two components reflect the recombination of quasiparticles in the two hole bands through intraband and interband processes. We also find that the thermal recombination rate of quasiparticles increases quadratically with temperature in all samples. The temperature and excitation density dependence of the decays indicates fully gapped hole bands and nodal or very anisotropic electron bands.     

Ab initio simulation of the electron structure and optical spectroscopy of ErRhGe compound

The results of investigation of the electronic structure and optical properties of ErRhGe are presented. The band spectrum of this compound is calculated in the local electron spin density approximation with correction for strong electron interactions in the 4f shell of the rare-earth metal (LSDA + U method) with allowance for the spin polarization. The optical constants of the compound are measured, and a number of spectral and electronic characteristics are determined by the ellipsometric method in a wide range of wave-lengths. Structural features of the optical conductivity spectrum in the interband absorption region are interpreted on the basis of the calculated electron state density.     

Defect state model for localized excitations in LiF

We find that a defect state treatment of localized excitations in LiF within the local density functional formalism accounts remarkably well for the observed experimental (core plus optical gap) excitations — in contrast to the failure of the one-electron band model. We show that when electron relaxation, self-interaction and charge polarization effects are taken into account by treating the excitation as a localized points defect, the improved band model predicts the correct excitation and interband states.     

Broadening of resonances in yttrium nanoparticle optical spectra

The dielectric function of yttrium in the range between 0.2 μm and 2 μm is composed of a harmonic oscillator contribution due to a discrete interband transition and the contribution of free electrons. Hence, it is possible to discuss surface plasmon polaritons as well as other electronic resonances in the optical extinction spectra of yttrium nanoparticles. For the latter, we discuss the broadening of the resonance caused by the aggregation of particles. When particles are lumped into aggregates, the color of the particle system also changes. Aggregation also affects the surface plasmon resonance in yttrium nanoparticles in a way comparable to silver or gold nanoparticle aggregates. Comparison is made with the first experimental results on yttriumnanoparticles, showing that aggregation is the dominant effect for the broad resonance in the measured extinction spectra. Received: 2 July 2001 / Revised version: 10 September 2001 / Published online: 15 October 2001     

Optical oscillation modes of plasmon particles observed in direct space by phase-contrast near-field microscopy

Light distributions near resonant metal nanoparticles are recorded by a scattering-type scanning near-field optical microscope (s-SNOM), for the first time with a sub-particle-size resolution (<10 nm) and with simultaneous amplitude and phase contrast. The images depict the optical oscillation patterns of single plasmon particles. Examples are presented of particles excited in dominantly dipolar and quadrupolar modes, and also of closely spaced particles sustaining a gap mode. The gap mode can provide enhanced optical fields in nanometric spots for non-linear and single-molecule spectroscopy applications. Received: 20 June 2001 / Revised version: 3 August 2001 / Published online: 19 September 2001     

Optical properties of gold metal clusters: A time-dependent local-density-approximation investigation

The optical response of free and matrix-embedded gold metal clusters Au_N is investigated in the framework of the time-dependent local-density-approximation (TDLDA). The characteristics of the surface plasmon resonance are carefully analyzed as a function of the model parameters and the particle radius. The strong influence of the frequency-dependence of the 5d core-electron dielectric function in the vicinity of the interband threshold is emphasized. The size evolution of the Mie-frequency in free gold clusters exhibits a noticeable blue-shift trend as the particle size decreases, much stronger than in silver clusters. The width and shape of the resonance, essentially ruled by the decay via the interband transitions, are found closely correlated to the imaginary component of the core-electron dielectric function. In presence of a surrounding matrix the blue-shift trend is largely rubbed out. Agreement with recent experimental results on size-selected gold clusters embedded in an alumina matrix may be achieved by taking into account the porosity effects at the metal/matrix interface. The comparison with the predictions of classical models is also provided. Received: 9 March 1998 / Revised: 5 June 1998 / Accepted: 3 July 1998     

Charge carrier recombination mechanisms in Sb-containing quantum well laser structures

The dynamics of interband luminescence in structures with InGaAsSb-based quantum wells and barriers of different types was studied at different temperatures and excitation levels. The lifetime of optically injected charge carriers in quantum wells at different temperatures and optical excitation levels was determined. An increased recombination rate in structures with deep electron quantum wells was discovered; it is associated with the occurrence of resonance Auger recombination. It was concluded that the application of quinary solid solutions as barriers in laser structures for a 3—4 fum wavelength range is to be preferred.     

Interband optical excitation of space-charge waves in high-resistance semiconductors

A fairly complete theory is proposed for trap recharging waves upon their optical excitation under conditions of dominant interband transitions. It is demonstrated that the occurrence of interband transitions reduces the role of trapping centers existing in the crystal and the carrier lifetime. This leads to a decrease in the lifetime of trap recharging waves and can result in their complete disappearance as eigenmodes of electron oscillations in the semiconductor crystal. It is shown that a large number of specific cases can occur depending on the illumination intensity and the ratio of recombination parameters. The physical meaning of the effective trap concentration and its relation to the screening length of the internal electric field are discussed.     

Photoluminescence of Er3+ ions in amorphous silicon layers under intensive laser excitation

Transients of the photoluminescence (1.54 μm) of Er³⁺ ions embedded in an amorphous silicon matrix excited with intensive laser pulses are simulated using a phenomenological model which takes into account both the defect-related excitation mechanism and stimulated optical transitions in the ions. The simulated transients are compared with the experimental ones observed in Er-doped amorphous silicon layers under pulsed laser excitation. The modeling and the experimental results demonstrate a possibility to realize a regime of superradiance in the system of Er³⁺ ions pumped via an electronic excitation of the amorphous matrix. Received: 7 August 2001 / Revised version: 1 November 2001 / Published online: 17 January 2002     

Nonlinear optical studies of the transient coherence in the Quantum Hall system

We review recent investigations of the femtosecond nonlinear optical response of the two-dimensional electron gas (2DEG) in a strong magnetic field. We probe the Quantum Hall (QH) regime for filling factors ν∼1. Our focus is on the transient coherence induced via optical excitation and on its time evolution during early femtosecond timescales. We simultaneously study the interband and intraband coherence in this system by using a nonlinear spectroscopic technique, transient three-pulse four wave mixing optical spectroscopy, and a many-body theory. We observe striking differences in the temporal and spectral profile of the nonlinear optical signal between a modulation doped quantum well system (with the 2DEG) and a similar undoped quantum well (without a 2DEG). We attribute these qualitative differences to Coulomb correlations between the photoexcited electron-hole pairs and the 2DEG. We show, in particular, that intraband many-particle coherences assisted by the inter-Landau-level magnetoplasmon excitations of the 2DEG dominate the femtosecond nonlinear optical response. The most striking effect of these exciton-magnetoplasmon coherences is a large off-resonant four-wave-mixing signal in the case of very low photoexcited carrier densities, not observed in the undoped system, with strong temporal oscillations and unusually symmetric temporal profile.     

Electronic excitations on clean and adsorbate covered Pd(111) by angle resolved electron energy loss spectroscopy

Electronic excitations on clean and adsorbate covered Pd(111) have been investigated by angle resolved electron energy loss spectroscopy. Primary energies in the range of 50–1000 eV were chosen for strong specular reflection to emphasize elastic diffraction-before-loss processes. The clean Pd spectra are compared with optical data, and good correspondence is found for the optical limit (q ? 0). The loss features are interpreted in terms of plasmon resonances and interband transitions within the framework of a recent band structure calculation. Virtually no dispersion is observed for the intrinsic Pd losses, but vertical interband transitions decay fast in the dispersive (q ≠ 0) spectra. Two adsorbate systems are investigated in this study: CO in a disordered adsorbate layer and bromine in a well-ordered $\text{(}\text{3×}\text{3 )R30°}$ structure. Adsorbate derived loss features are generally prominent in the nonspecular (q ≠ 0) spectra. While no dispersion is seen for the intramolecular 13.5 eV excitation of adsorbed CO, dispersion up to 1 eV is found for the Br 4p derived loss feature of the ordered overlayer. This is discussed in terms of a two-dimensional adsorbate band structure of bromine.     

The role of electron scattering in the surface enhanced Raman effect on AgAu alloys

We have observed SERS from AgAu alloys using incident photon energies above and below the onset for interband transitions. Below the onset, electron scattering processes due to alloying cause a decrease in SERS intensity below that observed on either pure metal. This behavior is most easily explained by theories which are based on the optical properties of the substrate.     

Theoretical investigation on near-infrared and visible absorption spectra of nanometallic aluminium with oxide coating in nanoenergetic materials: size and shape effects

The effects of metal core dimension, oxide shell thickness and ellipsoid aspect ratio of Al-Al2O3 core-shell nanoparticles on the near-infrared and visible absorption spectra of nanocomposite Al-Al2O3/nitrocellulose（NC） film are investigated by numerical calculations. Both the size-dependent interband transitions and frequency-dependent free electron damping of the nanometallic aluminium are taken into account in the calculations. Oxidation effect of nanoaluminium is also analysed. It is shown that oxidation may enhance but may also reduce the optical absorption, depending on the excited light energy and initial dimension of nanoparticle. Metal core size and excited light energy dominate the absorption characteristic. The absorption ability of ellipsoidal nanoparticles is larger than that of spheroidal nanoparticles and increases by the square index as the aspect ratio increases. These calculations will provide some significant theoretical guidance for the preparation and laser ignition of nanoenergetic materials.     

胶体金纳米颗粒的荧光光谱特性

研究了胶体金纳米颗粒的荧光激发光谱和荧光发射光谱特性.增大激发光的波长,发射峰相应红移并在629nm达到最强,对应的灵敏激发波长为473nm.增加金纳米颗粒粒径,观察到发射谱的峰值先增大然后减小.发射峰产生的原因在于电子与带间空穴的复合导致非线性共振光散射.发射峰强度和金颗粒粒径的关系可以用表面等离子体震荡引起的局域场增强来解释,数值计算结果和实验结果能较好的吻合.     

Strong ultraviolet and violet photoluminescence from Si-based anodic porous alumina films

We have investigated photoluminescence (PL) from Si-based anodic porous alumina films formed by real-time controlled anodization of electron-beam evaporated Al films. As-anodized samples show three strong PL bands at 295, 340, and 395 nm. These bands blueshift and their intensities decrease after the samples are annealed. When the annealing temperature increases to 1000 °C, the blueshift becomes specially pronounced and meanwhile the structures of the films develop toward crystalline Al₂O₃. Based on discussions on the thermal annealing behaviors of the PL and PL excitation spectra, we suggest that optical transitions in oxygen-related defects, F⁺ (oxygen vacancy with one electron) centers, are responsible for the observed ultraviolet and violet PL. Received: 24 July 2000 / Accepted: 24 February 2001 / Published online: 3 May 2001