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Width of cluster plasmon resonances: Bulk dielectric functions and chemical interface damping
(1993)
The damping of collective electron resonances in clusters which develop into plasmon polaritons at larger sizes is investigated for free, supported, and embedded neutral metal clusters. Embedding of free 2 nm Ag clusters of 2-nm diameter into a SiO2 matrix leads to an increase of the width of the resonances by more than a factor of 3. The optical spectra are compared with the Mie theory using size-effect-modified dielectric functions of the solid state. The results corroborate the assumption that the widths of the resonances strongly depend on chemical interface effects. The results are briefly discussed with regard to limited-mean-free-path and quantum-size-effect theories and a recent approach by Persson. It is demonstrated that the widths of the spectra of supported and embedded clusters have to be interpreted with care since true intrinsic size effects of the clusters appear to be less effective than previously believed and can be obscured by the chemical interface damping.
© 1993 The American Physical Society
Laser-induced desorption of metal atoms from the surface of small metal particles has been investigated as a function of the shape of the particles and the polarization of the incident laser light. The particles were supported on LiF, quartz or sapphire substrates. In a first set of experiments, the shape of the particles was determined by recording optical transmission spectra with s- and p-polarized light incident under an angle of typically 40° with respect to the surface normal. The metal particles turn out to be oblate, the ratio of the axes perpendicular and parallel to the substrate surface being on the order of 0.5. This ratio decreases with increasing particle size. Also, the particles change shape if the temperature is raised. In further experiments, s- and p-polarized light has been used to stimulate desorption of atoms via surface plasmon excitation. It is found that the desorption rate markedly depends on the polarization of the light. This is explained by excitation of the collective electron oscillation along different axes of the non-spherical particles.
Results on laser-induced desorption of metal atoms from small metal particles are presented. Experiments have been performed on sodium, potassium, and silver particles supported on a LiF(100) single-crystal surface under ultrahigh vacuum conditions. Measurements include the determination of the desorption rate as a function of laser wavelength, laser intensity, average particle size, and substrate temperature, the determination of the kinetic energy of the desorbed atoms, the investigation of the optical spectra of the supported metal particles, and the study of the influence of adsorbate molecules on the desorption rate. Furthermore, theoretical extinction and absorption spectra of the metal particles have been calculated with the classical electrodynamical Mie theory as a function of average particle size and excitation wavelength. Also, the radial electric field at the particle surface was computed. The results of the experiments and theoretical calculations are combined to give a consistent picture of the mechanism of metal-atom desorption by electronic excitation with laser light. A realistic surface potential from which the atoms escape and nonlocal optical effects are taken into account. The latter introduce additional absorption channels by the formation of electron-hole pairs in the surface layer of the particle which relax into antibonding states before desorption occurs. Finally, the mechanism is discussed in the light of similar phenomena observed for thin metal films. Possibilities for future work are outlined.
© 1993 The American Physical Society
Beleuchtet man die Oberfläche eines Festkörpers mit Laserlicht, können darauf adsorbierte Atome oder Moleküle abgelöst werden. Solche Desorptionsprozesse sind in jüngster Zeit in zahlreichen Experimenten untersucht worden, wobei sich das Interesse sowohl auf die Erforschung der zugrundeliegenden Mechanismen als auch auf mögliche Anwendungen dieser Reaktionen, zum Beispiel zur gezielten Modifizierung von Oberflächen, konzentriert. Besonders interessant ist das laserinduzierte Aufbrechen von Bindungen zur Oberfläche dann, wenn es nicht einfach als thermischer Prozeß durch eine Temperaturerhöhung hervorgerufen wird, sondern direkt auf einer elektronischen Anregung beruht. Solche nichtthermischen Prozesse werden selbst für Metalle beobachtet, obwohl die Kopplung der elektronischen Anregung an das Substrat hier besonders schnell abläuft. Der zugrundeliegende Mechanismus beruht auf dem Zusammenspiel einer kollektiven Elektronenoszillation und einer lokalisierten Einzelelektronenanregung, wobei auch nichtlokale optische Effekte in der Metalloberfläche eine wichtige Rolle spielen.
The results of an experimental study of the optical and photoelectrical properties of Eu-containing lead chalcogenides and superlattices are presented. From both sets of experiments band offset data for the lead chalcogenide-europium chalcogenide heterojunction are derived. The results are compared with the data obtained from a linear interpolation of the band structures between those of the binaries.