Hans-Jürgen Eisler

Color-selective semiconductor nanocrystal laser

Theoretical predictions of the benefits of three-dimensional quantum confinement have provided motivation for the development of quantum-dot lasers. Such lasers, developed in the case of self-assembled quantum dots, have not been successfully demonstrated with quantum-confined colloidal nanocrystals (NCs). Here, using recently developed NC-titania chemistry, we report the successful development of an optically pumped, NC-based distributed feedback laser, in which the narrow gain profiles of these nanoparticles have been matched with the feedback of a second-order distributed feedback laser. This laser, whose output color can be selected by choosing appropriately sized nanocrystals, operates at 80 K and at room temperature.

Nanoengineering and characterization of gold dipole nanoantennas with enhanced integrated scattering properties

In this paper we present our approach for engineering gold dipole nanoantennas. Using electron-beam lithography we have been able to produce arrays of single gold antennas with dimensions from 70 to 300 nm total length with a highly reproducible nanoengineering protocol. Characterizing these gold nanoantenna architectures by optical means via dark-field microscopy and scattering spectroscopy gives the linear optical response function as a figure-of-merit for the antenna resonances, spectral linewidth and integrated scattering intensity. We observe an enhanced integrated scattering probability for two arm gold dipole nanoantennas with an antenna feed gap compared to antennas of the size of one arm without a gap.

Linear and nonlinear optical characterization of aluminum nanoantennas.

We experimentally determine the order of multiphoton induced luminescence of aluminum nanoantennas fabricated on a nonconductive substrate using electron-beam lithography to be 2.11 (±0.10). Furthermore, we optically characterize these nanostructures via linear dark-field microscopy and nonlinear multiphoton laser excitation. We hereby observe different spectral response functions that can be seen as a splitting of peak positions when the antenna arm length is increased to Larm > 150 nm which has not yet been reported for aluminum nanostructures.

Quantum molecular dynamics calculations and experimental Raman spectra confirm the proposed structure of the odd-numbered dimeric fullerene C119

A first-principles quantum molecular dynamics (QMD) method and a bond polarizability model, whose parameters were optimized on the basis of C60 data, have been used to calculate theoretical Raman spectra for four possible low-energy isomers of the odd-numbered dimeric fullerene C119 produced by thermolysis of C60 oxides. Comparison of the calculated and experimentally determined spectra provides strong evidence that the structure obtained by thermolysis is indeed the thermodynamically most stable isomer with C2 symmetry, as proposed earlier on the basis of semiempirical molecular modeling and 13C-NMR spectroscopy. This isomer has the structure originally predicted for C119 on the basis of QMD simulations.

Novel pyridinium dyes that enable investigations of peptoids at the single-molecule level.

Single-molecule microscopy is a powerful tool for investigating various uptake mechanisms of cell-penetrating biomolecules. A particularly interesting class of potential transporter molecules are peptoids. Fluorescence labels for such experiments need to comply with several physical, chemical, and biological requirements. Herein, we report the synthesis and photophysical investigation of new fluorescent pyridinium derived dyes. These fluorescent labels have advantageous structural variations and spacer units in order to avoid undesirable interactions with the labeled molecule and are able to easily functionalize biomolecules. In our case, cell-penetrating peptoids are successfully labeled on solid supports, and in ensemble measurements the photophysical properties of the dyes and the fluorescently labeled peptoids are investigated. Both fluorophores and peptoids are imaged at the single-molecule level in thin polymer gels. With respect to bleaching times and fluorescence lifetimes the dye molecules and the peptoids show only slightly perturbed optical behaviors. These investigations indicate that the new fluorophores fulfill well single-molecule microscopy and solid-phase synthesis requirements.

Photophysical properties of fluorescently-labeled peptoids

Fluorescently-labeled biomolecules are often utilized in biochemical or cellular experiments without further detailed spectroscopical characterization. This report is intended to narrow this gap and therefore presents the photophysical investigation of a library of 17 fluorescently-labeled molecules, namely peptoid transporters. First, one peptoid structure is labeled with seven different fluorophores and the spectroscopical properties are examined. Absorption and fluorescence maxima are almost identical for free dyes and conjugated dyes, suggesting free choice of a spectrally suitable fluorophore for different applications. Otherwise, extinction coefficients and quantum yields, and therefore the brightness of all seven dyes are strongly influenced. For the fluorophores, e.g. rhodamine B, the extent of this influence depends on the peptoid itself. This is shown by comparing different structures in the second part of this report. Especially the side chain functionalities influence the brightness. And finally, peptoids having two identical fluorescent labels are presented, which show decreased quantum yields. Possible reasons for the observed photophysical properties are discussed.

Gold nanoantenna resonance diagnostics via transversal particle plasmon luminescence

We perform two-photon excitation confocal experiments on coupled gold nanoantennas and observe time-integrated luminescence spectra that match plasmonic mode emission in the far-field. We show that the transversal particle plasmon mode can be excited, using excitation light that is cross-polarized with respect to the gold luminescence signal and therefore oriented along the long axis of the dipole gold antenna. We provide evidence for losses in polarization information from the excitation channel to the luminescence response due to the nature of the energy and momentum transfer. Finally, we map out the two-photon induced luminescence intensity profile for a fixed excitation wavelength λ and varying antenna arm length L.

Investigating the influences of the precise manufactured shape of dipole nanoantennas on their optical properties

Fabrication of small nanoantennas with high aspect ratios via electron beam lithography is at the current technical limit of nanofabrication and hence significant deviations from the intended shape of small nanobars occur. Via numerical simulations, we investigate the influence of geometrical variations of gap nanoantennas, having dimensions on the order of only a few tens of nanometers. We show that those deviations have a significant influence on the performance of such nanoantennas. In particular, their resonance wavelength as well as the magnitude of absorption and scattering cross section and the electric field distribution in the near field is strongly altered. Our findings are thus of importance for applications based on near field as well as those based on far field interactions with nanoantennas and have to be carefully and individually considered in both cases.

Superresolution optical fluctuation imaging (SOFI) aided nanomanipulation of quantum dots using AFM for novel artificial arrangements of chemically functionalized colloidal quantum dots and plasmonic structures

For single photon experiments or research on novel hybrid structures consisting of several colloidal quantum dots (Qdots) and plasmonic nanoparticles both the precise localization and the optical behavior of the emitters need to be correlated. Therefore, the gap between the high spatial resolution topography information that provides detailed localization of single Qdots and the diffraction limited fluorescence image needs to be overcome. In this paper, we demonstrate the combination of atomic force microscopy (AFM) with wide-field fluorescence microscopy improved by superresolution optical fluctuation imaging (SOFI). With this approach the topography and the superresolution image can be overlaid with sub-diffraction precision. Consequently, we discriminate between single Qdots that are optically active and dark ones. Additionally, the optical time-dependent behavior of molecular emitters can be selectively investigated. This method is, furthermore, useful for an advanced manipulation and characterization toolbox of Qdots in general. In summary, our findings represent an easily adaptable, highly reproducible and comparatively cheap subdiffraction limit imaging method and they facilitate the efficient selection of bright Qdots in a standard lab environment for proof-of-principle nanostructures containing Qdots and for nanomanipulation experiments.

Optical gain and lasing in colloidal quantum dots

Summary form only given. Semiconductor quantum dots (QDs) promise the lowest lasing threshold for semiconductor media. Additionally, QDs in the strong confinement regime have an emission wavelength that is a pronounced function of size, adding the advantage of continuous spectral tunability simply by changing the dot radius. Lasing has previously been demonstrated for epitaxially grown III-V QDs. Large lateral dimensions and difficulties in size control limit their spectral tunability using quantum confinement effects. An alternative approach to fabricating QDs is through chemical synthesis which can produce semiconductor nanoparticles (colloidal QDs) with radii from 1 to 6 nm and with size dispersions as small as 5%. Such dots show strong quantum confinement and permit size-controlled spectral tunability over an energy range as wide as 1 eV. The combination of tunable electronic energies and chemical flexibility make colloidal QDs ideal building blocks for the bottom-up assembly of optical device structures, including optical amplifiers and lasers. However, despite more than a decade of effort, lasing in small-size colloidal nanoparticles has not been realized. To determine what hinders lasing action, we performed extensive dynamical studies of radiative and nonradiative processes in CdSe colloidal QDs.