Mapping the electric field distribution of tightly focused cylindrical vector beams with gold nanorings.

In this paper gold nanorings (NRs) are applied as particularly well-suited sensing elements for mapping the radially symmetric electric fields in the high numerical aperture focus of cylindrical vector beams. The optical properties of gold nanorings are analyzed by a combination of extinction and single particle dark field spectroscopy as well as confocal photoluminescence (PL) imaging. The results are compared to numerical calculations. The in-plane components in the focus of the cylindrical vector beams are estimated through the PL intensity distributions of the NRs. The optimum overlap between the structure and excitation is visualized by a narrow centre spot in the far-field PL scan.

Cold atmospheric pressure plasma for treatment of chronic wounds: drug or medical device?

OBJECTIVE: The use of cold atmospheric pressure plasma (CAPP) as a new therapeutic option to aid the healing of chronic wounds appears promising. Currently, uncertainty exists regarding their classification as medical device or medical drug. Because the classification of CAPP has medical, legal, and economic consequences as well as implications for the level of preclinical and clinical testing, the correct classification is not an academic exercise, but an ethical need. METHOD: A multidisciplinary team of physicians, surgeons, pharmacists, physicists and lawyers has analysed the physical and technical characteristics as well as legal conditions of the biological action of CAPP. RESULTS: It was concluded that the mode of action of the locally generated CAPP, with its main active components being different radicals, is pharmacological and not physical in nature. CONCLUSION: Depending on the intended use, CAPP should be classified as a drug, which is generated by use of a medical device directly at the point of therapeutic application.

Structure, transport and photoconductance of PbS quantum dot monolayers functionalized with a copper phthalocyanine derivative.

We simultaneously surface-functionalize PbS nanocrystals with Cu 4,4',4'',4'''-tetraaminophthalocyanine and assemble this hybrid material into macroscopic monolayers. Electron microscopy and X-ray scattering reveal a granular mesocrystalline structure with strong coherence between the atomic lattice and the superlattice of nanocrystals within each domain. Terahertz spectroscopy and field-effect transistor measurements indicate efficient coupling of holes throughout the hybrid thin film, in conjunction with a pronounced photoresponse. We demonstrate the potential of this material for optoelectronic applications by fabricating a light-effect transistor.

Combining ocFLIM and FIDSAM reveals fast and dynamic physiological responses at subcellular resolution in living plant cells.

For a deeper understanding of molecular mechanisms within cells and for the realization of predictive biology for intracellular processes at subcellular level, quantitative biology is required. Therefore, novel optical and spectroscopic technologies with quantitative and dynamic output are needed in cell biology. Here, we present a combined approach of novel one-chromophore fluorescence lifetime imaging microscopy to probe the local environment of fluorescent fusion proteins and fluorescence intensity decay shape analysis microscopy to suppress interfering autofluorescence. By applying these techniques, we are able to analyse the subcellular localization and partitioning of a green fluorescence protein fusion of the salt stress-induced protein low temperature induced (LTI)6b in great detail with high spatial and temporal resolution in living cells of Arabidopsis plants.

Nanoscale spectroscopic imaging of organic semiconductor films by plasmon-polariton coupling.

Tip-enhanced near-field optical images and correlated topographic images of an organic semiconductor film (diindenoperylene, DIP) on Si have been recorded with high optical contrast and high spatial resolution (17 nm) using a parabolic mirror with a high numerical aperture for tip illumination and signal collection. The DIP molecular domain boundaries being one to four molecular layers (1.5-6 nm) high are resolved topographically by a shear-force scanning tip and optically by simultaneously recording the 6x10{5} times enhanced photoluminescence (PL). The excitation is 4x10{4} times enhanced and the intrinsically weak PL-yield of the DIP-film is 15-fold enhanced by the tip. The Raman spectra indicate an upright orientation of the DIP molecules. The enhanced PL contrast results from the local film morphology via stronger coupling between the tip plasmon and the exciton-polariton in the DIP film.

Tailoring gold nanostructures for near-field optical applications.

A method of combined thin-film deposition, electron beam lithography, and ion milling is presented for the fabrication of gold and silver nanostructures. The flexibility of lithographical processes for the variation of geometric parameters is combined with three-dimensional control over the surface evolution. Depending on the etching angle, different shapes ranging from cones over rods to cups can be achieved. These size- and shape-tunable structures present a toolbox for nano-optical investigations. As an example, optical properties of systematically varying structures are examined in a parabolic mirror confocal microscope.

Tighter focusing with a parabolic mirror.

We demonstrate experimentally and theoretically that a parabolic mirror (PM) with a high numerical aperture (NA) of 1 focuses a radially polarized laser mode to the smallest diffraction-limited spot at a fixed NA and wavelength, having an area of 0.134 lambda(2). The measurements were performed with a confocal microscope, using the PM as a focusing and collecting element. The results stand in accordance with the theoretical calculations presented by Davidson and Bokor [Opt. Lett. 29, 1318 (2004)], who predicted a reduction in the total focal spot size of 43% as compared with an aplanatic lens.

High NA particle- and tip-enhanced nanoscale Raman spectroscopy with a parabolic-mirror microscope.

Detecting efficiently the plasmon-enhanced Raman signal of molecules created in the nanometre-sized gap between a metal nanoparticle or the apex of a sharp tip and a metal surface is the key problem in particle- or tip-enhanced local surface spectroscopy (Pettinger et al., 2004; Roth et al., 2006). The optical excitation field has to be polarized along the gap, and the field emerging from the gap has to be observed from the side. These geometrical restrictions usually limit the numerical aperture of the lens used for exciting the gap and collecting the scattered photons created in the gap. We present a novel method to overcome this problem. The solution is based on a confocal optical microscope with a high numerical aperture parabolic mirror for excitation and detection. Localized plasmons can be efficiently excited parallel to the surface normal by illuminating the parabolic mirror with a radially polarized doughnut mode and the field emerging sidewise from the gap can be efficiently collected by the rim of the parabolic mirror and directed to the detection system. First results on particle- and tip-enhanced Raman spectroscopic measurements of benzotriazole molecules adsorbed on gold films are presented.

A novel approach to detect and characterize the scattering patterns of single Au nanoparticles using confocal microscopy.

We demonstrate a novel optical method for characterizing single Au nanoparticles by acquiring their scattering patterns. This technique combines confocal microscopy and higher-order laser modes for detecting the light scattered by sub-wavelength-sized nanoobjects. The optical patterns are generated by the coherent superposition of the field scattered by individual metallic particles and the excitation field reflected at the cover slide-air interface and provide information about the particles' position, orientation, size and shape. Detectable changes in the full width at half maximum (FWHM) of the signal intensity permit to distinguish between 20- and 60-nm diameter Au spheres. The confocal images are also very sensitive to the particle's geometry and polarizability, that is, Au nanospheres, Au nanorods and triangular Au nanoplates give different characteristic patterns if the excitation wavelength is varied.

Conformational distribution of a ferroelectric liquid crystal revealed using fingerprint vibrational spectroscopy and the density functional theory.

The authors have investigated the conformational structure of the ferroelectric liquid crystal compound 4-3-methyl-2-chloropentanoyloxy-4"-hexyloxy-biphenyl also known under the abbreviations 3M2CPHOB and C6 using vibrational (IR and Raman) spectroscopy. The measured spectra exhibit two bands corresponding to the C=O stretching vibration that are separated by 20 cm(-1). In contrast, the molecular structure comprises only one such group. They assigned the two bands to different conformers that coexist in a temperature range between 25 and 65 degrees C covering the entire mesophase of this material. This assignment is strongly confirmed by calculated vibrational spectra based on the density functional theory.

Surface- and resonance-enhanced micro-Raman spectroscopy of xanthene dyes: from the ensemble to single molecules.

Surface-enhanced resonance Raman scattering (SERRS) spectra of various rhodamine dyes, of pyronine G and thiopyronine adsorbed on isolated silver clusters were recorded at the ensemble level and at the single-molecule level with a high-resolution confocal laser microscope equipped with a spectrograph and a CCD-detector. Comparing single-molecule spectra with ensemble spectra, various inhomogeneous spectral features, such as line splitting, spectral wandering, spectral diffusion and abrupt spectral jumps between different metastable spectral states, are revealed positions and the relative intensities of the vibronic bands. Resonance enhancement is investigated with respect to single-molecule surface-enhanced Raman scattering (SERS) spectroscopy and is found to be responsible for approximately three orders of magnitude in sensitivity. A significant influence of the substituents on the single-molecule SERRS sensitivity is found, showing that various chemical effects are responsible for surface enhancement in addition to the electromagnetic enhancement effect.

Probing highly confined optical fields in the focal region of a high NA parabolic mirror with subwavelength spatial resolution.

Parabolic mirrors with a high numerical aperture can be conveniently used to produce highly confined optical fields in the focal region. Furthermore, these fields can have interesting polarization behaviour due to the high numerical aperture. In particular, if the mirror is illuminated with a size matched radially polarized or azimuthally polarized doughnut mode, the electric field has in the focal region almost exclusively a longitudinal or a transverse polarization component. Such field distributions are interesting for applications in confocal or near-field optical microscopy. Here we present experimental results where we have probed some of these field distributions by raster scanning a fine gold tip in nanometer steps through the focal region and detecting the scattered light intensity. The measured intensity patterns are compared with corresponding vector-field calculations.

Near-field and confocal surface-enhanced resonance Raman spectroscopy at cryogenic temperatures.

For laser spectroscopy at variable temperatures with high spatial resolution a combined scanning near-field optical and confocal microscope was developed. Rhodamine 6G (R6G) dye molecules dispersed on silver nano-particles or nano-clusters were investigated. For optical excitation of the molecules, either an aperture probe or a focused laser spot in confocal arrangement were employed. Raman spectra in the wavenumber range between 300 cm-1 and 3000 cm-1 at room temperatures down to 8.5 K were recorded. Many of the observed Raman lines can be associated with the structure of the adsorbed molecule. Intensity fluctuations in spectral sequences were observed down to 77 K and are indicative of single molecule sensitivity.

Well-shaped fibre tips by pulling with a foil heater.

The length of the molten zone determines the length of pulled optical fibre tips. Tips produced by laser or filament heating are rather lengthy. By using a foil heater the taper length can be shortened and cone angles in the order of 30 degrees can reproducibly be obtained. For varying the drawing force there is an optimum temperature range where the taper shape is monotonic for the whole tip. The tip end diameter is well below 100 nm for optimized pulling conditions.

Dynamics of single dye molecules observed by confocal imaging and spectroscopy.

The fluorescence emission of single rhodamine dye molecules (rhodamine 6G and rhodamine 630) at room temperature was analyzed by using scanning confocal laser microscopy in conjunction with polarization analysis, fluorescence spectroscopy, time-resolved detection (minutes to microseconds), and excitation saturation. Results are presented and discussed 1) for samples with dye molecules at the glass-air interface and 2) covered with an additional thin protective polymer film (polyvinylbutyral). Under the polymer layer, the single-molecule fluorescence was more stable than the glass-air interface. This result may be explained by fewer spontaneous variations of the fluorescence rate, polarization changes, spectral shifts, and longer photochemical lifetimes.

Scanning near-field optical microscopy in cell biology and microbiology.

Scanning a point light source in close proximity over a sample and recording the scattered or transmitted light intensity point by point allows one to record optical images with a resolution not limited by diffraction. An overview of this technique called scanning near-field optical microscopy (SNOM or NSOM) is given with emphasis on cell- and microbiology. After an introduction, where the basic features of the technique are explained, illustrative examples are presented, such as a HeLa cell, fluorescence labelled human chromosomes, super resolution fluorescence imaging, single molecule imaging and fluorescence resonance energy transfer between a single pair of dye molecules.

Electric-field-modulated photon echoes in Pr(3+):YAlO(3).

We measured the Stark coefficient for the (3)H(4)(1) ? (1)D(2)(1) transition of Pr(3+):YAlO(3), using the technique of Stark-modulated photon echoes. This gave a value of 58 kHz/(V cm(-1)) for the vector difference between ground-and excited-state electric dipole moments. The resolution with which Stark shifts could be measured in these experiments was ~500 Hz, which is more than an order of magnitude less than the homogeneous linewidth.

Direct measurement of standing evanescent waves with a photon-scanning tunneling microscope.

We present a detailed analysis of a standing evanescent wave that is caused by total internal reflection of an Ar-ion laser beam on a glass prism and investigate the coupling to a subwavelength dielectric tip of a photon-scanning tunneling microscope that is raster scanned at a close distance over the prism surface. The intensity of the evanescent field is spatially modulated with a period of 239.2 nm. It decays exponentially with a constant of 103.9 nm with increasing distance from the prism surface. Precise measurements of the standing evanescent wave can be used to calibrate the scanner and permit one to determine the spatial resolution and the coupling efficiency of the tip.