Optical stark effects in j-aggregate-metal hybrid nanostructures exhibiting a strong exciton-surface-plasmon-polariton interaction.

We report on the observation of optical Stark effects in J-aggregate-metal hybrid nanostructures exhibiting strong exciton-surface-plasmon-polariton coupling. For redshifted nonresonant excitation, pump-probe spectra show short-lived dispersive line shapes of the exciton-surface-plasmon-polariton coupled modes caused by a pump-induced Stark shift of the polariton resonances. For larger coupling strengths, the sign of the Stark shift is reversed by a transient reduction in normal mode splitting. Our studies demonstrate an approach to coherently control and largely enhance optical Stark effects in strongly coupled hybrid systems. This may be useful for applications in ultrafast all-optical switching.

Ultrasmall bullets of light--focusing few-cycle light pulses to the diffraction limit.

We demonstrate an essentially dispersion-free and diffraction-limited focusing of few-cycle laser pulses through all-reflective microscope objectives. By transmitting 6-fs-pulses from a Ti:sapphire oscillator through an all-reflective 0.5 NA objective, we reach a focus with a beam diameter of 1.0 µm, preserving the time structure of the pulses. The temporal and spatial pulse profile is recorded simultaneously using a novel tip-enhanced electron emission autocorrelator, indicating a focal volume of these pulses of only 1.8 µm3. We anticipate that the demonstrated technique is of considerable interest for inducing and probing optical nonlinearities of individual nanostructures.

Bethe-hole polarization analyser for the magnetic vector of light.

The nature of light as an electromagnetic wave with transverse components has been confirmed using optical polarizers, which are sensitive to the orientation of the electric field. Recent advances in nanoscale optical technologies demand their magnetic counterpart, which can sense the orientation of the optical magnetic field. Here we report that subwavelength metallic apertures on infinite plane predominantly sense the magnetic field of light, establishing the orientation of the magnetic component of light as a separate entity from its electric counterpart. A subwavelength aperture combined with a tapered optical fibre probe can also serve as a nanoscale polarization analyser for the optical magnetic field, analogous to a nanoparticle sensing the local electric polarization. As proof of its functionality, we demonstrate the measurement of a magnetic field orientation that is parallel to the electric field, as well as a circularly polarized magnetic field in the presence of a linearly polarized electric field.

Distinguishing between ultrafast optical harmonic generation and multi-photon-induced luminescence from ZnO thin films by frequency-resolved interferometric autocorrelation microscopy.

The nonlinear optical properties of thin ZnO film are studied using interferometric autocorrelation (IFRAC) microscopy. Ultrafast, below-bandgap excitation with 6-fs laser pulses at 800 nm focused to a spot size of 1 µm results in two emission bands in the blue and blue-green spectral region with distinctly different coherence properties. We show that an analysis of the wavelength-dependence of the interference fringes in the IFRAC signal allows for an unambiguous assignment of these bands as coherent second harmonic emission and incoherent, multiphoton-induced photoluminescence, respectively. More generally our analysis shows that IFRAC allows for a complete characterization of the coherence properties of the nonlinear optical emission from nanostructures in a single-beam experiment. Since this technique combines a very high temporal and spatial resolution we anticipate broad applications in nonlinear nano-optics.

Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures.

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.

Coherent exciton-surface-plasmon-polariton interaction in hybrid metal-semiconductor nanostructures.

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.

Femtosecond phase control of spatial localization of the optical near-field in a metal nanoslit array.

We demonstrate spatial control of optical near-fields by femtosecond phase shaping in one-dimensional plasmonic structures. The near-field images display striking temporal-phase dependence, switching between double- and single-peak images within one lattice constant. The change of the near-field distribution is studied in the time and spectral domain. The spectral composition change observed by varying the time delay between two phase-locked femtosecond pulses explains the spatial control of the near-field images. Modal expansion calculations of linear light transmission using the surface impedance boundary condition are in excellent agreement with experiments.

Broadband optical near-field microscope for nanoscale absorption spectroscopy of organic materials.

Conjugated organic materials in the solid state are generally amorphous or polycrystalline, with local order only achieved in mesoscopic domains with size ranging from a few tens to a few hundreds of nanometres. Understanding the interplay between mesoscopic order and macroscopic behaviour of these materials calls for a spatially resolved study of their optical properties. Near-field scanning optical microscopy allows one in principle to beat the diffraction limit in optical imaging. A quantitative measurement of nanoscale absorption spectra is, however, complicated by the difficulty of obtaining broadband near-field illumination with sufficiently high intensity. Here we demonstrate a near-field spectrometer with 100-nm spatial resolution based on an ultrabroadband Ti : sapphire oscillator coupled to an aperture-based near-field scanning optical microscopy, enabling structural phase-selective imaging of organic materials at the nanoscale. In polycrystalline phtalocyanine films we can distinguish between the crystalline and the amorphous phase, thus providing previously unavailable information on their mesoscopic texture.

Grating-coupling of surface plasmons onto metallic tips: a nanoconfined light source.

We describe and demonstrate a new nanometer-scale broadband light source. It is based on the grating-coupled excitation of surface plasmon polaritons (SPPs) on the shaft of a sharp conical metal taper with a tip radius of few tens of nanometers. Far-field excitation of linear nanoslit gratings results in the resonant generation of SPPs traveling over more than 10 mum to the tip apex and converging to an intense radiative local light spot. Such nanofabricated tips are expected to find various applications in nanospectroscopy, overcoming problems with background illumination in apertureless microscopy.

Localized multiphoton emission of femtosecond electron pulses from metal nanotips.

Intense multiphoton electron emission is observed from sharp (approximately 20 nm radius) metallic tips illuminated with weak 100-pJ, 7-fs light pulses. Local field enhancement, evidenced by concurrent nonlinear light generation, confines the emission to the tip apex. Electrons are emitted from a highly excited nonequilibrium carrier distribution, resulting in a marked change of the absolute electron flux and its dependence on optical power with the tip bias voltage. The strong optical nonlinearity of the electron emission allows us to image the local optical field near a metallic nanostructure with a spatial resolution of a few tens of nanometers in a novel tip-enhanced electron emission microscope.

Vector field mapping of local polarization using gold nanoparticle functionalized tips: independence of the tip shape.

We have measured local electric field vectors of local polarizaton on the nanoscale using gold nanoparticle functionalized tips as local field scatterers. In our experiments, the local field induces a dipole-moment in the gold nanoparticle functionalized tip, which then radiates into the far-field, transferring the full information about the local electric field from the near into the far field. The polarization characteristics of the scattered fields are analyzed using a conventional ellipsometry method. The tip dependent scattering function- the polarizability tensor- is fully determined by far field scattering measurements. Once the polarizability tensor for each tip is correctly accounted for in the data analysis, our results show that the finally determined local field polarization vectors are essentially independent of the tip shape.

Femtosecond light transmission and subradiant damping in plasmonic crystals.

We report the first observation of subradiance in plasmonic nanocrystals. Amplitude- and phase-resolved ultrafast transmission experiments directly reveal the coherent coupling between surface plasmon polaritons (SPPs) induced by periodic variations in the dielectric function. This interaction results in the formation of plasmonic band gaps and coupled SPP eigenmodes with different symmetries, as directly shown by near-field imaging. In antisymmetric modes, radiative SPP damping is strongly suppressed, increasing the SPP lifetime from 30 fs to more than 200 fs. The findings are analyzed within a coupled resonance model.

Microscopic origin of surface-plasmon radiation in plasmonic band-gap nanostructures.

We report spatial domain measurements of the damping of surface-plasmon excitations in metal films with periodic nanohole arrays. The measurements reveal a short coherent propagation length of a few microm inside nanohole arrays, consistent with delays of about 10 fs in ultrafast transmission experiments. This implies that the transmission spectra of the entire plasmonic band-gap structure are homogeneously broadened by radiative damping of surface-plasmon excitations. We show that a Rayleigh-like scattering of surface plasmons by the periodic hole array is the microscopic origin of this damping, allowing the reradiation rate to be controlled.

Quantum mechanical repulsion of exciton levels in a disordered quantum well.

Spatially resolved photoluminescence spectra of a single quantum well are recorded by near-field spectroscopy. A set of over four hundred spectra displaying sharp emission lines from localized excitons is subject to a statistical analysis of the two-energy autocorrelation function. An accurate comparison with a quantum theory of the exciton center-of-mass motion in a two-dimensional spatially correlated disordered potential reveals clear signatures of quantum mechanical energy level repulsion, giving the spatial and energetic correlations of excitons in disordered quantum systems.

Three-dimensional analysis of light propagation through uncoated near-field fibre probes.

The near-field emission from uncoated tapered fibre probes is investigated for different probe geometries. The three-dimensional model calculations are based on Maxwell's curl equations and describe the propagation of a 10 fs optical pulse (lambda = 805 nm) through tapers of different lengths and different diameters of the taper exit. The numerical evaluation is done with a finite difference time domain code. Two tapers with cone angles of 50 degrees, with taper lengths of 1.5 microm and 1.0 microm and exit diameters of 100 nm and 520 nm, respectively, are considered. We find that without sample the short taper with large exit diameter optimizes both light transmission and spatial resolution. In the presence of a sample with a high dielectric constant, however, the spatial near-field distribution changes drastically for both taper geometries. We find a pronounced increase in spatial resolution, down to about 250 nm inside the medium. This collimation of the near-field distribution arises from interferences between emitted and reflected light from the sample surface and from a collimation effect that the field experiences in the high-index semiconductor material. The combination of high spatial resolution and transmission and collection efficiencies makes such probes interesting for spectroscopic investigations, as demonstrated by recent experiments.

Low temperature near-field luminescence studies of localized and delocalized excitons in quantum wires.

Excitons in a GaAs quantum wire were studied in high-resolution photoluminescence experiments performed at a temperature of about 10 K with a spatial resolution of 160 nm and a spectral resolution of 100 microeV. We report the observation of quasi-one-dimensional excitons which are delocalized over a length of up to several micrometres along the quantum wire. Such excitons give rise to a 10 meV broad luminescence band, representing a superposition of transitions between different delocalized states. In addition, we find a set of sharp luminescence peaks from excitons localized on a sub150 nm length scale. Theoretical calculations of exciton states in a disordered quasi-one-dimensional potential reproduce the experimental results.

Femtosecond near-field spectroscopy: carrier relaxation and transport in single quantum wires.

Quasi-two-colour femtosecond pump and probe spectroscopy and near-field scanning optical microscopy are combined to study the carrier dynamics in single semiconductor nanostructures. In temporally, spectrally and spatially resolved measurements with a time resolution of 200 fs and a spatial resolution of 200 nm, the non-linear change in reflectivity of a single quantum wire is mapped in real space and time. The experiments show that carrier relaxation into a single quantum wire occurs on a 100 fs time scale at room temperature. Evidence is given for a transient unipolar electron transport along the wire axis on a picosecond time and 100 nm length scale.

Time-resolved near-field optics: exciton transport in semiconductor nanostructures.

We present a systematic, temperature-dependent study of excitonic real-space transfer into single GaAs quantum wires using time-resolved low-temperature near-field luminescence spectroscopy. Excitons generated by local short pulse optical excitation in a 250 nm spot undergo diffusive transport over a length of several micrometres and are subsequently trapped into the quantum wire by optical phonon emission. The effect of local energy barriers in the vicinity of the quantum wire on the real-space transfer dynamics is monitored directly by mapping the time-resolved quantum wire luminescence. Experiments at variable temperatures are compared to numerical simulations based on drift-diffusive model calculations, and the spatio-temporal evolution of the two-dimensional exciton distribution within the nanostructure is visualized.

[Fibrinolysis with rt-PA in peripheral arterial occlusions]. / Fibrinolyse mit rt-PA bei peripheren arteriellen Verschlüssen.

First experiences using rt-PA for the local lysis of peripheral arterial occlusions have shown that it is a potent activator of the fibrinolytic system. 2 to 5 mg of rt-PA administered for 1 to 1 1/2 hours are sufficient to completely dissolve even long occlusions. With doses up to 20 mg over 2 hours no systemic bleeding was observed. With 50 mg given within 5 hours and with an infusion of 2.5 mg per hour for 48 hours there were two cases of systemic haemorrhaging entirely due to the fibrinolysis. No appreciable defects in the coagulation system and no other side effects were observed.