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Register a new userImaging the onset of the resonance regime in low-energy NO-He collisions
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At low energies, the quantum wave-like nature of molecular interactions result in unique scattering behavior, ranging from the universal Wigner laws near zero Kelvin to the occurrence of scattering resonances at higher energies. It has proven challenging to experimentally probe the individual waves underlying these phenomena. We report measurements of state-to-state integral and differential cross sections for inelastic NO-He collisions in the 0.2 - 8.5 cm$^{-1}$ range with 0.02 cm$^{-1}$ resolution. We study the onset of the resonance regime by probing the lowest-lying resonance dominated by s and p waves only. The highly structured differential cross sections directly reflect the increasing number of contributing waves as the energy is increased. A new NO-He potential calculated at the CCSDT(Q) level was required to reproduce our measurements.
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In molecular collisions, resonances occur at specific energies where the colliding particles temporarily form quasi-bound complexes, resulting in rapid variations in the energy dependence of scattering cross sections. Experimentally, it has proven challenging to observe such scattering resonances, especially in differential cross sections. We report the observation of resonance fingerprints in the state-to-state differential cross sections for inelastic NO-He collisions in the 13 to 19 cm$^{-1}$ energy range with 0.3 cm$^{-1}$ resolution. The observed structures were in excellent agreement with quantum scattering calculations. They were analyzed by separating the resonance contributions to the differential cross sections from the background through a partitioning of the multichannel scattering matrix. This revealed the partial wave composition of the resonances, and their evolution during the collision.
The experimental characterization of scattering resonances in low energy collisions has proven to be a stringent test for quantum chemistry calculations. Previous measurements on the NO-H$_2$ system at energies down to $10$ cm$^{-1}$ challenged the most sophisticated calculations of potential energy surfaces available. In this report, we continue these investigations by measuring the scattering behavior of the NO-H$_2$ system in the previously unexplored $0.4 - 10$ cm$^{-1}$ region for the parity changing de-excitation channel of NO. We study state-specific inelastic collisions with both textit{para}- and textit{ortho}-H$_2$ in a crossed molecular beam experiment involving Stark deceleration and velocity map imaging. We are able to resolve resonance features in the measured integral and differential cross sections. Results are compared to predictions from two previously available potential energy surfaces and we are able to clearly discriminate between the two potentials. We furthermore identify the partial wave contributions to these resonances, and investigate the nature of the differences between collisions with textit{para}- and textit{ortho}-H$_2$. Additionally, we tune the energy spreads in the experiment to our advantage to probe scattering behavior at energies beyond our mean experimental limit.
The vibrational quenching cross sections and corresponding low-temperature rate constants for the v = 1 and v = 2 states of CN- colliding with He and Ar atoms have been computed ab initio using new three dimensional potential energy surfaces. Little work has so far been carried out on low-energy vibrationally inelastic collisions for anions with neutral atoms. The cross sections and rates calculated at energies and temperatures relevant for both ion traps and astrochemical modelling, are found by the present calculations to be even smaller than those of the similar C2- /He and C2-/Ar systems which are in turn of the order of those existing for the collisions involving neutral diatom-atom systems. The implications of our finding in the present case rather small computed rate constants are discussed for their possible role in the dynamics of molecular cooling and in the evolution of astrochemical modelling networks.
The dicarbon molecular anion is currently of interest as a candidate for laser cooling due to its electronic structure and favorable branching ratios to the ground electronic and vibrational states. Helium has been proposed as a buffer gas to cool the molecules internal motion. We calculate the cross sections and corresponding rates for rovibrational inelastic collisions of the dicarbon anion with He, and also with Ne and Ar, on three-dimensional ab initio potential energy surfaces using quantum scattering theory. The rates for vibrational quenching with He and Ne are very small and are similar to those for small neutral molecules in collision with helium. The quenching rates for Ar, however, are far larger than those with the other noble gases, suggesting that this may be a more suitable gas for driving vibrational quenching in traps. The implications of these results for laser cooling of the dicarbon anion are discussed.
We present an experimental study on the rotational inelastic scattering of OH ($X^2Pi_{3/2}, J=3/2, f$) radicals with He and D$_2$ at collision energies between 100 and 500 cm$^{-1}$ in a crossed beam experiment. The OH radicals are state selected and velocity tuned using a Stark decelerator. Relative parity-resolved state-to-state inelastic scattering cross sections are accurately determined. These experiments complement recent low-energy collision studies between trapped OH radicals and beams of He and D$_2$ that are sensitive to the total (elastic and inelastic) cross sections (Sawyer emph{et al.}, emph{Phys. Rev. Lett.} textbf{2008}, emph{101}, 203203), but for which the measured cross sections could not be reproduced by theoretical calculations (Pavlovic emph{et al.}, emph{J. Phys. Chem. A} textbf{2009}, emph{113}, 14670). For the OH-He system, our experiments validate the inelastic cross sections determined from rigorous quantum calculations.
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