We report on the first photochemical use of a continuous-wave optical parametric oscillator (OPO) in a matrix isolation experiment. The narrow-band high-power OPO light promotes efficient conformational changes of matrix-isolated formic acid by selective vibrational excitation, which is combined with thermal annealing of matrices. This approach allows us to find five new dimers of formic acid in an argon matrix (presumably two trans−trans and three trans−cis structures), as shown by infrared spectroscopy. The assignment of the newly observed absorptions is discussed on the basis of the recent ab initio calculations. As a result of this work, all of the trans−trans and trans−cis dimers of formic acid theoretically predicted to date have now been observed in matrix isolation experiments. The structure of dimers can be influenced by the solid matrix surrounding, which may explain differences from the computational spectra obtained for species in vacuum.
Highly sensitive cantilever-enhanced photoacoustic detection of hydrogen cyanide and methane in the mid-infrared region is demonstrated. A mid-infrared continuous-wave frequency tunable optical parametric oscillator was used as a light source in the experimental setup. Noise equivalent detection limits of 190 ppt (1 s) and 65 ppt (30 s) were achieved for HCN and CH(4), respectively. The normalized noise equivalent absorption coefficient is 1.8 × 10(-9) W cm(-1) Hz(-1/2).
The authors demonstrate that a dielectric resonant waveguide grating can enhance optical second-harmonic generation by a factor of 550 compared to a similar flat surface. Their structure, which consists of purely dielectric and thereby transparent materials, has a low index silicon dioxide grating covered by a high index titanium dioxide layer and it is optimized for the fundamental wavelength of 1064nm. Polarization dependence of the second-harmonic response suggests that the enhancement arises from the favorable interaction of the resonant waveguide mode and its strong local field with the inherent surface nonlinearity of the dielectric materials.
We report a continuous-wave singly resonant optical parametric oscillator pumped by a widely tunable titanium-doped sapphire ring laser. It produces up to 0.8 W of mid-infrared power. The wavelength can be tuned in a few seconds from 2.5 to 3.5 microm or from 3.4 to 4.4 microm and scanned up to 40 GHz without mode-hops by only changing the pump beam wavelength. Spectroscopic capability is demonstrated by measuring parts of the photoacoustic absorption spectrum of NH(3) near 3196 cm(-1).
We provide a detailed investigation of the second-order nonlinear optical and structural properties of Langmuir-Blodgett (LB) films of nonracemic thiohelicenebisquinone (THBQ). We prepare both X- and Y-type films of different thicknesses and characterize them using optical second-harmonic generation and atomic-force microscopy (AFM). We find that the overall nonlinear properties of the samples are essentially independent of the film thickness and the deposition type and arise from susceptibility tensor components associated with chirality. Both X- and Y-type films can be described by D2 symmetry, which is a higher symmetry than the previously assumed C2 of LB films of THBQ and a similar helicenebisquinone (HBQ). However, the two types of films are shown to differ significantly with respect to the orientation of the in-plane axis. For Y type, the axis follows the direction of vertical sample deposition, but for X type, the direction of the axis varies randomly and significantly between different samples. The Y-type samples are therefore more ordered than the X-type samples. This was confirmed by AFM measurements in which the Y type exhibits uniform ordering into columnar structures. Similar structures in X type, on the other hand, are shorter and more randomly oriented, like those earlier observed for racemic samples of HBQ [Verbiest, T., et al. Science 1998, 282, 913]. The common nonlinear properties and different high-level ordering observed here for two different types of nonracemic samples reinforces that the nonlinearity of THBQ (and probably HBQ, as well) originates from the low-level columnar aggregation of the molecules with the higher-level structures playing a lesser role. In addition, within the columns, the molecules likely assume fairly random azimuthal orientations so that the columns themselves exhibit approximate Dinfinity symmetry.
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