Understanding how defects are generated and propagate during operation in modern vertical cavity surface emitting lasers (VCSEL) is an important challenge in order to develop the next generation of highly reliable semiconductor lasers. Undesired oxidation processes or performance degrading dislocation networks are typically investigated by conventional failure analysis after damage formation. In this works new approach to VCSEL failure analysis, oxide confined high power VCSELs are investigated in-situ at elevated temperatures in a transmission electron microscope.
View Article and Find Full Text PDFThe two-dimensional (2D) temporal evolution of the NO-concentration over a NOx-storage catalyst is investigated in situ with planar laser-induced fluorescence (PLIF) in an optically accessible parallel wall channel reactor. Signal accumulated phase-correlated 2D-recordings of repetitive adsorption/desorption cycles are obtained by synchronizing the switching of the NO gas flow (on/off) with the laser and detection system, thereby significantly increasing the signal-to-noise ratio. The gas compositions at the reactor outlet are additionally monitored by ex-situ analytics.
View Article and Find Full Text PDFThe fundamental dependence between process parameters during focused electron beam induced deposition and the chemistry of functional PtC nanostructures have been studied via a multi-technique approach using SEM, (S)TEM, EELS, AFM, and EFM. The study reveals that the highest Pt contents can only be achieved by an ideal balance between potentially dissociating electrons and available precursor molecules on the surface. For precursor regimes apart from this situation, an unwanted increase of carbon is observed which originates from completely different mechanisms: (1) an excess of electrons leads to polymerization of precursor fragments whereas (2) a lack of electrons leads to incompletely dissociated precursor molecules incorporated into the nanostructures.
View Article and Find Full Text PDFIsomer- and mass-selective UV and IR-UV double resonance spectra of the BA3, B2A, and B2A2 clusters of benzene (B) and acetylene (A) are presented. Cluster structures are assigned by comparison with the UV and IR spectra of benzene, the benzene dimer, as well as the BA, BA2, and B2A clusters. The intermolecular vibrations of BA are identified by dispersed fluorescence spectroscopy.
View Article and Find Full Text PDFThis study shows that the morphology of organic/metal interfaces strongly depends on process parameters and the involved materials. The interface between organic n-type blocking layer materials and the top Ag cathode within an organic photodiode was investigated. Ag was deposited on either amorphous tris-8-hydroxyquinolinato-aluminum (Alq(3)) or crystalline 4,7-diphenyl-1,10-phenanthroline (Bphen) using different deposition techniques such as electron beam deposition, ion beam sputtering, and vacuum thermal evaporation at various deposition rates.
View Article and Find Full Text PDFFundamental proximity effects for electron beam induced deposition processes on nonflat surfaces were studied experimentally and via simulation. Two specific effects were elucidated and exploited to considerably increase the volumetric growth rate of this nanoscale direct write method: (1) increasing the scanning electron pitch to the scale of the lateral electron straggle increased the volumetric growth rate by 250% by enhancing the effective forward scattered, backscattered, and secondary electron coefficients as well as by strong recollection effects of adjacent features; and (2) strategic patterning sequences are introduced to reduce precursor depletion effects which increase volumetric growth rates by more than 90%, demonstrating the strong influence of patterning parameters on the final performance of this powerful direct write technique.
View Article and Find Full Text PDFThe formation of crystalline para-sexiphenyl (6P) films on Cu(110) and Cu(110)-(2 × 1)O (Cu-O) has been studied by low energy electron diffraction, X-ray absorption spectroscopy and both in situ and ex situ X-ray diffraction methods to elucidate the transition from the initial monolayers to crystalline thin films. It is found that, for Cu-O, a single and, for Cu(110), a double wetting layer is formed which then acts as a template for the subsequent 3D crystal growth. For both substrates the orientation of the long molecular axes of the 6P molecules in the first layers is conserved for the molecules in the bulk crystals growing on them.
View Article and Find Full Text PDFWe investigated the self-aggregation of 2'-deoxy-3',5'-bis(tert-butyldimethylsilyl)-cytidine dC(TBDMS)(2) in CDCl(3) solutions by Fourier transform infrared (FT-IR) spectroscopy and report the formation of larger aggregates than dimers in this solvent for the first time. The hydrogen bonding patterns in these complexes, which occur with increasing concentration may serve as a model for DNA super-structures such as triplexes. From the IR spectra, wavelength dependent absolute extinction coefficients of the monomer, dimer as well as a contribution from larger clusters which are supposedly trimers are deduced on the basis of a simple deconvolution method.
View Article and Find Full Text PDFWe reinvestigated the self-aggregation of 1-cyclohexyluracil (1CHU) in CDCl(3) solutions. Wavelength dependent absolute extinction coefficients of the monomer and of dimers are presented on the basis of a simple deconvolution method. Two isomeric dimer structures coexist in a solution with similar abundance.
View Article and Find Full Text PDFElectronic and vibrational gas phase spectra of 1-methylthymine (1MT) and 1-methyluracil (1MU) and their clusters with water are presented. Mass selective IR/UV double resonance spectra confirm the formation of pyrimidine-water clusters and are compared to calculated vibrational spectra obtained from ab initio calculations. In contrast to Y.
View Article and Find Full Text PDFWe reinvestigated the self-association of 9-substituted adenine derivatives in CDCl3 solutions and present the infrared spectra of 9-ethyladenine and N-methyl-9-ethyladenine and its aggregates in the spectral regions between 1500 and 1800 cm(-1) and between 2700 and 3600 cm(-1). Wavelength dependent absolute extinction coefficients of the monomer and dimers are presented on the basis of a simple deconvolution method. Comparison of the deconvoluted dimer spectra with quantum chemical calculations allows for a structural assignment of the two dimer structures that coexist in 9-ethyladenine/CDCl3 solutions.
View Article and Find Full Text PDFWe present infrared-UV double resonance spectra and quantum chemical calculations of the natural di-peptide H-Trp-Ser-OH. Two conformers are present in the supersonic expansions. They have a compact folded structure with two hydrogen bonds and with the serin residue stacked above the indole ring and an unusual NH(Trp).
View Article and Find Full Text PDFWe reinvestigated the assignment of the three major guanine conformers detected via resonance enhanced two-photon ionization (R2PI) in supersonic expansions and present IR/UV double resonance spectra in the spectral region between 1500 and 1800 cm(-1). Comparison with B3LYP/TZVPP and RI-MP2/cc-pVQZ calculations shows that both conformers B and C are 7H-keto tautomers with an imine group in the 2-position. They differ only in the local conformation of the imine group but are otherwise identical.
View Article and Find Full Text PDFWe present near- and mid-infrared-UV double resonance spectra of the natural dipeptide H-Pro-Trp-OH. Two conformers are present in the supersonic expansion: a stretched conformer with fully extended backbone and a folded conformer with an OH..
View Article and Find Full Text PDF2,2,2-Trifluoroethanol molecules synchronize their transiently chiral gauche configurations upon dimerization in supersonic jet expansions, while they avoid an energetically competitive heteroconfigurational hydrogen bonded dimer topology predicted by extensive quantum chemical calculations.
View Article and Find Full Text PDFAn apparatus for detailed study of quantum state-resolved inelastic energy transfer dynamics at the gas-liquid interface is described. The approach relies on supersonic jet-cooled molecular beams impinging on a continuously renewable liquid surface in a vacuum and exploits sub-Doppler high-resolution laser absorption methods to probe rotational, vibrational, and translational distributions in the scattered flux. First results are presented for skimmed beams of jet-cooled CO(2) (T(beam) approximately 15 K) colliding at normal incidence with a liquid perfluoropolyether (PFPE) surface at E(inc) = 10.
View Article and Find Full Text PDFHighly crystalline organic heteroepitaxial layers with controlled molecular orientations and morphologies are one of the keys for optimum organic device performance. With studies of molecular orientation, structure, and morphology, we have investigated the ability of oriented organic films to act as substrate templates for the growth of a second organic layer. Depending on the molecular orientation in the sexiphenyl substrate, crystalline sexithiophene nanostructures of either pyramidal or needlelike morphology, with either near vertical or parallel molecular orientations, respectively, grow.
View Article and Find Full Text PDFHigh-resolution IR absorption spectra of supersonically cooled ethyl radicals (Trot approximately 20 K) have been obtained in a slit supersonic jet discharge expansion, revealing first rotationally resolved data for CH-stretch excitation of the methyl group. Three different vibrational bands are observed, one parallel (k=0<--0) and two perpendicular (/k/1<--0), which for a nearly decoupled methyl rotor framework would correspond to symmetric and (nearly degenerate) asymmetric CH-stretch excitations. However, the splitting between the two asymmetric CH-stretch excitations is anomalously large (approximately 125 cm(-1)), signaling the presence of interactions between the CH2 radical moiety and the opposing CH bond on the methyl group.
View Article and Find Full Text PDFWe present resonant two-photon ionization (R2PI), IR-UV, and UV-UV double resonance spectra of jet-cooled 2-aminopurine (2AP) as well as Fourier transform infrared (FTIR) gas phase spectra. 2AP is a fluorescing isomer of the nucleobase adenine. The results show that there is only one tautomer of 2AP which absorbs in the wavelength range 32,300-34,500 cm(-1).
View Article and Find Full Text PDFTo understand the intrinsic properties of peptides, which are determined by factors such as intramolecular hydrogen bonding, van der Waals bonding and electrostatic interactions, the conformational landscape of isolated protein building blocks in the gas phase was investigated. Here, we present IR-UV double-resonance spectra of jet-cooled, uncapped peptides containing a tryptophan (Trp) UV chromophore in the 1000-2000 cm(-1) spectral range. In the series Trp, Trp-Gly and Trp-Gly-Gly (where Gly stands for glycine), the number of detected conformers was found to decrease from six (Snoek et al.
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