We demonstrate an ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure. Femtosecond excitation drastically alters the optical properties of a model system formed by coating a gold nanoslit array with a thin J-aggregated dye layer. Controlled and reversible transient switching from strong (Ω(R) ≃ 55 meV) to weak (Ω(R) ≈ 0) coupling on a sub-ps time scale is directly evidenced by mapping the nonequilibrium dispersion relations of the coupled excitations. Such a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plasmonic circuits.
We report measurements of a coherent coupling between surface plasmon polaritons (SPP) and quantum well excitons in a hybrid metal-semiconductor nanostructure. The hybrid structure is designed to optimize the radiative exciton-SPP interaction which is probed by low-temperature, angle-resolved, far-field reflectivity spectroscopy. As a result of the coupling, a significant shift of approximately 7 meV and an increase in broadening by approximately 4 meV of the quantum well exciton resonance are observed. The experiments are corroborated by a phenomenological coupled-oscillator model predicting coupling strengths as large as 50 meV in structures with optimized detunings between the coupled exciton and SPP resonances. Such a strong interaction can, e.g., be used to enhance the luminescence yield of semiconductor quantum structures or to amplify SPP waves.
We consider the spin reorientation transition in a ferromagnetic Heisenberg monolayer with a second order single ion anisotropy as a function of temperature and external field. Up to now analytical methods give satisfying results only for the special case that the external field is aligned parallel to the easy axis of the crystal. We propose a theory based on a generalization of the Callen decoupling, which can be used for arbritrary direction of the external field. Excellent agreement between our results and Quantum Monte Carlo data is found for the field induced reorientation at finite temperatures. Additionally, we discuss the temperature dependence of the transition in detail.
Unbiased gold nanoparticles are negatively charged in aqueous solution but not hydrated. Optical spectroscopy of voltage-clamped single gold nanoparticles reveals evidence that anion adsorption starts at positive potentials above the point of zero charge, causing severe but reversible plasmon damping in combination with a spectral red shift exceeding the linear double layer charging effect. Plasmon damping by adsorbate is relevant for the use of nanoparticles in catalysis, in biodiagnostics, and in surface enhanced Raman scattering.
We study the influence of collective magnetic excitations on the interlayer exchange coupling (IEC) in metallic multilayers. The results are compared to other models that explain the temperature dependence of the IEC by mechanisms within the spacer or at the interfaces of the multilayers. As a main result we find that the reduction of the IEC with temperature shows practically the same functional dependence in all models. On the other hand the influence of the spacer thickness, the magnetic material, and an external field are quite different. Based on these considerations we propose experiments, that are able to determine the dominating mechanism that reduces the IEC at finite temperatures.
Recent photoemission experiments have shown strong surface modifications in the spectra from vanadium oxides as (V, Cr)2O3 or (Sr, Ca)VO3. The effective mass is enhanced at the surface and the coherent part of the surface spectrum is narrowed as compared to the bulk. The quasiparticle weight is more sensitive at the surface than in the bulk against bandwidth variations. We investigate these effects theoretically considering the single-band Hubbard model for a film geometry. A simplified dynamical mean-field scheme is used to calculate the main features of the interacting layer-dependent spectral function. It turns out that the experimentally confirmed effects are inherent properties of a system of strongly correlated electrons. The reduction of the weight and the variance of the coherent part of the surface spectrum can be traced back to the reduced surface coordination number. Surface correlation effects can be strongly amplified by changes of the hopping integrals at the surface.
Quantum mechanical calculations based on an extended Heisenberg model are compared with ferromagnetic resonance experiments on prototype trilayer systems Ni(7)/Cu(n)/Co(2)/Cu(001) in order to determine and separate for the first time quantitatively the sources of the temperature dependence of interlayer exchange coupling. Magnon excitations are responsible for about 75% of the reduction of the coupling strength from zero to room temperature. The remaining 25% are due to temperature effects in the effective quantum well and the spacer-magnet interfaces.
We investigate the influence of s-d or p-d hybridization to d-band ferromagnetism to estimate the importance of hybridization for the magnetic properties of transition metals. To focus our attention to the interplay between hybridization and correlation we investigate a simple model system consisting of two non-degenerated hybridized bands, one strongly correlated, the other one quasi-free. To solve this extended Hubbard model, we apply simple approximations, namely SDA and MAA, that, concerning ferromagnetism in the single-band model, are known to give qualitatively satisfactory results. This approach allows us to discuss the underlying mechanism, by which dband ferromagnetism is influenced by the hybridization on the basis of analytical expressions. The latter clearly display the order and the functional dependencies of the important effects. It is found, that spin-dependent inter-band particle fluctuations cause a spin-dependent band shift and a spin-dependent band broadening of the Hubbard bands. The shift stabilizes, the broadening tends to destabilize ferromagnetism. Stabilization requires relatively high band distances and small hybridization matrix elements. Super-exchange and RKKY coupling are of minor importance.
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