State-to-State Differential and Relative Integral Cross Sections for Rotationally Inelastic Scattering of H2O by Hydrogen

State-to-state differential cross sections (DCSs) for rotationally inelastic scattering of H2O by H2 have been measured at 71.2 meV (574 cm-1) and 44.8 meV (361 cm-1) collision energy using crossed molecular beams combined with velocity map imaging. A molecular beam containing variable compositions of the (J = 0, 1, 2) rotational states of hydrogen collides with a molecular beam of argon seeded with water vapor that is cooled by supersonic expansion to its lowest para or ortho rotational levels (JKaKc= 000 and 101, respectively). Angular speed distributions of fully specified rotationally excited final states are obtained using velocity map imaging. Relative integral cross sections are obtained by integrating the DCSs taken with the same experimental conditions. Experimental state-specific DCSs are compared with predictions from fully quantum scattering calculations on the most complete H2O-H2 potential energy surface. Comparison of relative total cross sections and state-specific DCSs show excellent agreement with theory in almost all detailsComment: 46 page

Random matrix description of decaying quantum systems

This contribution describes a statistical model for decaying quantum systems (e.g. photo-dissociation or -ionization). It takes the interference between direct and indirect decay processes explicitely into account. The resulting expressions for the partial decay amplitudes and the corresponding cross sections may be considered a many-channel many-resonance generalization of Fano's original work on resonance lineshapes [Phys. Rev 124, 1866 (1961)]. A statistical (random matrix) model is then introduced. It allows to describe chaotic scattering systems with tunable couplings to the decay channels. We focus on the autocorrelation function of the total (photo) cross section, and we find that it depends on the same combination of parameters, as the Fano-parameter distribution. These combinations are statistical variants of the one-channel Fano parameter. It is thus possible to study Fano interference (i.e. the interference between direct and indirect decay paths) on the basis of the autocorrelation function, and thereby in the regime of overlapping resonances. It allows us, to study the Fano interference in the limit of strongly overlapping resonances, where we find a persisting effect on the level of the weak localization correction.Comment: 16 pages, 2 figure

Exploring Renner-Teller Induced Quenching in the Reaction H(\u3csup\u3e2\u3c/sup\u3e\u3ci\u3eS\u3c/i\u3e)+NH(\u3ci\u3ea\u3c/i\u3e\u3csup\u3e1\u3c/sup\u3eΔ): A Combined Experimental and Theoretical Study

Experimental rate coefficients for the removal of NH(a1Δ) and ND(a1Δ) in collisions with H and D atoms are presented; all four isotope combinations are considered: NH+H, NH+D, ND+H, and ND+D. The experiments were performed in a quasistatic laser-flash photolysis/laser-induced fluorescence system at low pressures. NH(a1Δ) and ND(a1Δ) were generated by photolysis of HN3 and DN3, respectively. The total removal rate coefficients at room temperature are in the range of (3-5) x 1013 cm3 mol-1 s-1. For two isotope combinations, NH+H and NH+D, quenching rate coefficients for the production of NH(X 3Σ-) or ND(X 3Σ-) were also determined; they are in the range of 1x1013 cm3 mol-1 s-1. The quenching rate coefficients directly reflect the strength of the Renner-Teller coupling between the 2A and 2A\u27 electronic states near linearity and so can be used to test theoretical models for describing this nonadiabatic process. The title reaction was modeled with a simple surface-hopping approach including a single parameter, which was adjusted to reproduce the quenching rate for NH+H; the same parameter value was used for all isotope combinations. The agreement with the measured total removal rate is good for all but one isotope combination. However, the quenching rates for the NH+D combination are only in fair (factor of 2) agreement with the corresponding data

Statistics of S-matrix poles in Few-Channel Chaotic Scattering: Crossover from Isolated to Overlapping Resonances

We derive the explicit expression for the distribution of resonance widths in a chaotic quantum system coupled to continua via M equivalent open channels. It describes a crossover from the $\chi^2$ distribution (regime of isolated resonances) to a broad power-like distribution typical for the regime of overlapping resonances. The first moment is found to reproduce exactly the Moldauer-Simonius relation between the mean resonance width and the transmission coefficient. This fact may serve as another manifestation of equivalence between the spectral and the ensemble averaging.Comment: 4 two-column pages, RevTex. text is slightly modified; some misprints are correcte

The decay of photoexcited quantum systems: a description within the statistical scattering model

The decay of photoexcited quantum systems (examples are photodissociation of molecules and autoionization of atoms) can be viewed as a half-collision process (an incoming photon excites the system which subsequently decays by dissociation or autoionization). For this reason, the standard statistical approach to quantum scattering, originally developed to describe nuclear compound reactions, is not directly applicable. Using an alternative approach, correlations and fluctuations of observables characterizing this process were first derived in [Fyodorov YV and Alhassid Y 1998 Phys. Rev. A 58, R3375]. Here we show how the results cited above, and more recent results incorporating direct decay processes, can be obtained from the standard statistical scattering approach by introducing one additional channel.Comment: 7 pages, 2 figure

Instrumentation-related uncertainty of reflectance and transmittance measurements with a two-channel spectrophotometer

Spectrophotometers are operated in numerous fields of science and industry for a variety of applications. In order to provide confidence for the measured data, analyzing the associated uncertainty is valuable. However, the uncertainty of the measurement results is often unknown or reduced to sample-related contributions. In this paper, we describe our approach for the systematic determination of the measurement uncertainty of the commercially available two-channel spectrophotometer Agilent Cary 5000 in accordance with the Guide to the expression of uncertainty in measurements. We focus on the instrumentation-related uncertainty contributions rather than the specific application and thus outline a general procedure which can be adapted for other instruments. Moreover, we discover a systematic signal deviation due to the inertia of the measurement amplifier and develop and apply a correction procedure. Thereby we increase the usable dynamic range of the instrument by more than one order of magnitude. We present methods for the quantification of the uncertainty contributions and combine them into an uncertainty budget for the device. © 2017 Author(s)

O18O and C18O observations of rho Oph A

Observations of the (N_J=1_1-1_0) ground state transition of O_2 with the Odin satellite resulted in a about 5 sigma detection toward the dense core rho Oph A. At the frequency of the line, 119 GHz, the Odin telescope has a beam width of 10', larger than the size of the dense core, so that the precise nature of the emitting source and its exact location and extent are unknown. The current investigation is intended to remedy this. Telluric absorption makes ground based O_2 observations essentially impossible and observations had to be done from space. mm-wave telescopes on space platforms were necessarily small, which resulted in large, several arcminutes wide, beam patterns. Although the Earth's atmosphere is entirely opaque to low-lying O_2 transitions, it allows ground based observations of the much rarer O18O in favourable conditions and at much higher angular resolution with larger telescopes. In addition, rho Oph A exhibits both multiple radial velocity systems and considerable velocity gradients. Extensive mapping of the region in the proxy C18O (J=3-2) line can be expected to help identify the O_2 source on the basis of its line shape and Doppler velocity. Line opacities were determined from observations of optically thin 13C18O (J=3-2) at selected positions. During several observing periods, two C18O intensity maxima in rho Oph A were searched for in the 16O18O (2_1-0_1) line at 234 GHz with the 12m APEX telescope. Our observations resulted in an upper limit on the integrated O18O intensity of < 0.01 K km/s (3 sigma) into the 26.5" beam. We conclude that the source of observed O_2 emission is most likely confined to the central regions of the rho Oph A cloud. In this limited area, implied O_2 abundances could thus be higher than previously reported, by up to two orders of magnitude.Comment: 7 pages, 6 figures (5 colour), Astronomy & Astrophysic