The plasmonic signals of quasi-1D electron systems are a clear and direct measure of their metallic behavior. Due to the finite size of such systems in reality, plasmonic signals from a gold-induced superstructure on Si(5 5 3) can be studied with infrared spectroscopy. The infrared spectroscopic features have turned out to be extremely sensitive to adsorbates. Even without geometrical changes of the surface superstructure, the effects of doping, of the adsorbate induced electronic surface scattering, and of the electronic polarizability changes on top of the substrate surface give rise to measurable changes of the plasmonic signal. Especially strong changes of the plasmonic signal have been observed for gold, oxygen, and hydrogen exposure. The plasmonic resonance gradually disappears under these exposures, indicating the transion to an insulating behavior, which is in accordance with published results obtained from other experimental methods. For C 70 and, as shown here for the first time, TAPP-Br, the plasmonic signal almost retains its original intensity even up to coverages of many monolayers. For C 70 , the changes of the spectral shape, e.g. of electronic damping and of the resonance position, were also found to be marginal. On the other hand, TAPP-Br adsorption shifts the plasmonic resonance to higher frequencies and strongly increases the electronic damping. Given the dispersion relation for plasmonic resonances of 1D electron systems, the findings for TAPP-Br indicate a push-back effect and therefore stronger confinement of the free charge carriers in the quasi-one-dimensonal channel due to the coverage by the flat TAPP-Br molecules. On the gold-doped Si(5 5 3)-Au surface TAPP-Br acts as counter dopant and increases the plasmonic signal.
Product imaging of O((3)P2) following dissociation of ozone has been used to determine the relative yields of the product channels O((3)P2) + O2(X (3)Σg(-)) of ozone. All three channels are prominent at all wavelengths investigated. O2 vibrational distributions for each channel and each wavelength are also estimated assuming Boltzmann rotational distributions. Averaged over wavelength in the measured range, the yields of the O((3)P2) + O2(X (3)Σg(-)), O((3)P2) + O2(a (1)Δg), and O((3)P2) + O2(b (1)Σg(+)) channels are 0.36, 0.31,and 0.34, respectively. Photofragment distributions in the spin-allowed channel O((3)P) + O2(X (3)Σg(-)) are compared with the results of quantum mechanical calculations on the vibronically coupled PESs of the singlet states B (optically bright) and R (repulsive). The experiments suggest that considerably more vibrational excitation and less rotational excitation occur than predicted by the quantum calculations. The rotational distributions, adjusted to fit the experimental images, suggest that the dissociation takes place from a more linear configuration than the Franck-Condon bending angle of 117°. The dissociation at most wavelengths results in a positive value of the anisotropy parameter, β, both in the experiment and in the calculations. Calculations indicate that both nonadiabatic transitions and intersystem crossings substantially reduce β below the nominal value of 2.
The O((1)D) + N(2)O → 2NO(X (2)Π) reaction has been studied in a molecular beam experiment in which O(3) and N(2)O were coexpanded. The precursor O((1)D) was prepared by O(3) photodissociation at 266 nm, and the NO(X (2)Π) molecules born from the reaction as the O((1)D) recoiled out of the beam were detected by 1+1 REMPI over the 220-246 nm probe laser wavelength range. The resulting spectrum was simulated to extract rotational and vibrational distributions of the NO(X (2)Π) molecules. The product rotational distribution is found to be characterized by a constant rotational temperature of ≈4500 K for all observed bands, v = 0-9. An inverted vibrational distribution is observed. A consistent explanation of this and previous experimental results is possible if there are two channels for the reaction, one producing a nearly statistical vibrational distribution for low O((1)D)-N(2)O relative velocity collisions and a second producing the inverted distribution observed here for high relative velocity collisions. The former might correspond to an insertion/complex-formation reaction, while the latter might correspond to a stripping reaction. Velocity relaxation of the O((1)D) is argued to compete strongly with reaction in most bulb studies, so that these studies see predominantly the nearly statistical distribution. In contrast, the beam experiments do not detect the part of the vibrational distribution produced in low relative velocity reactions because the O((1)D) is not relaxed from its initial velocity before it either reacts or leaves the beam.
The behaviour of an organic semiconductor (TAPP-Br) is found to be variable upon condensation on various surfaces and as mixtures with typical dopants.
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