Probing the location of the unpaired electron in spin–orbit changing collisions of NO with Ar

Heid, Cornelia G.; Bentham, Imogen P.; Walpole, Victoria; Gheorghe, Razvan; Jambrina, Pablo G.; Aoiz, F. J.; Brouard, M.

doi:10.1039/d0cp04228e

Cited by 10 publications

(26 citation statements)

References 88 publications

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“…The spin-orbit changing collisions exhibit an overall preference for positive ISAs, that is, a preference for N-side/N-end collisions. We have observed the same trend in our previous work on the NO + Ar system, in which we attributed the N-side/N-end preference to the location of the unpaired electron closer to the N atom of the molecule [33]. Since the incoming rare gas atom can more efficiently interact with the unpaired electron at shorter distances, a change in spin-orbit quantum number is more likely to occur for collisions towards the N-side/N-end.…”

Section: Integral Steric Asymmetriessupporting

confidence: 85%

“…As observed previously for NO + Ar [27,[30][31][32][33], the orientational preferences of the DCSs alternate between even and odd j transitions. This is readily seen in the difference images in Figures 2-5, where red indicates a positive and blue a negative intensity.…”

Section: Velocity-map Ion Images and Dcsssupporting

confidence: 82%

“…The differences between the experimental and computational DCSs may also be partly due to small inaccuracies in the PESs used for the calculations [47]. For higher lying final states, for which the scattering distributions become broader and more backward scattered, the experimental resolution is less of a limiting factor and far-side scattering becomes highly unlikely [33]. In addition to the increasingly backward scattered DCSs, the Newton spheres of the scattered NO molecules become smaller as j increases, since more of the initially available energy is converted into rotational, and consequently less into translational, degrees of freedom.…”

Section: Velocity-map Ion Images and Dcssmentioning

confidence: 99%

“…Since then, different groups have used variations of this methodology to orient linear, symmetric, and asymmetric tops such as CD 3 I [6], OH [7], SO [18], and NO [21]. Following on from work by Stolte and coworkers [21,[24][25][26], our group has combined hexapole state selection with electric field orientation to study the stereodynamics of Ar atoms colliding with end-on [27][28][29][30] and, more recently, side-on [31][32][33] oriented NO molecules. In the current work, we extend these studies to collisions of oriented NO molecules with Kr atoms to investigate the effect the increased mass and the higher polarisability of the rare gas atom (compared to Ar) has on the orientation dependence of the scattering dynamics.…”

Section: Introductionmentioning

confidence: 99%

“…Interestingly, a sharp forward scattered peak appears in the Kr DCSs for both spin-orbit manifolds, but only in the spin-orbit changing DCSs for NO + Ar. In our previous work on spin-orbit changing collisions of NO + Ar, we have attributed this prominent feature to trajectories on the A PES that are efficiently funnelled from the Oend through the attractive well on the side of the NO molecule and closely approach the extended width at the N-end, where the unpaired electron lies within the plane of the three atoms [33].…”

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confidence: 98%

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Inelastic collision dynamics of oriented NO molecules with Kr atoms

et al. 2021

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Building on our previous work on NO + Ar, this paper presents a complete set of orientation measurements and quantum mechanical calculations for the NO + Kr collision system, including both spin-orbit conserving and changing collisions, and both side-on (x-axis) and end-on (z-axis) orientations. While many of the trends observed in the oriented differential and integral scattering distributions, as well as in the spin-orbit branching fractions, are similar to the ones seen previously for NO + Ar, a direct comparison with the Ar data reveals subtle differences in the scattering dynamics, which we rationalise with the more extended attractive regions on the NO + Kr potential energy surfaces. High-impact parameter collisions that lead to low scattering angles in the spin-orbit conserving manifold are particularly sensitive to the topology in the attractive parts of the potential, whereas more impulsive, low-impact parameter trajectories, which sample the repulsive parts of the potential, produce very similar features in the oriented differential cross sections for the Ar and Kr systems, especially for spin-orbit changing collisions.

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Section: Integral Steric Asymmetriessupporting

confidence: 85%

Section: Velocity-map Ion Images and Dcsssupporting

confidence: 82%

Section: Velocity-map Ion Images and Dcssmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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confidence: 98%

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Inelastic collision dynamics of oriented NO molecules with Kr atoms

et al. 2021

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Collision‐induced spin‐orbit relaxation of highly vibrationally excited NO near 1 K

Amarasinghe

Perera

et al. 2021

Natural Sciences

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State-to-state scattering studies of vibrationally excited molecules in the cold regime extend inelastic scattering investigations into a new territory. Here, we present differential cross-sections for superelastic scattering of spin-orbit excited nitric oxide (NO) (v = 10, Ω = 1.5, j = 1.5) with argon near 1 K utilizing our recently developed nearcopropagating beam technique, and compare these to quantum scattering calculations on coupled cluster and multi-reference potential energy surfaces. At these collision energies, the scattering is mainly governed by resonances and provides a platform to assess the accuracy of the attractive part of the difference potential for the NO-Ar system, which has remained untested. Quantum scattering calculations for such inelastic processes on high-quality potential energy surfaces at thermal energies have largely been successful at reproducing the key features of experimental results, but cold spin-orbit changing collisions are shown to test the limits of the current theoretical state-of-the-art. The experimental results clearly exhibit backscattering centered around 3.5 cm −1 collision energy suggesting a scattering resonance; such resonances have never been detected for the well-studied NO-Ar system. A partial wave analysis based on a multireference potential energy surface suggests the enhanced backscattering arises from overlapping resonances associated with the highest partial wave contributions.

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Gas sensing of fibrous red phosphorene towards inorganic air pollutants: Insights from first-principles calculations

Zhang

Mao

2021

Applied Surface Science

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Probing the location of the unpaired electron in spin–orbit changing collisions of NO with Ar

Abstract: Understanding the molecular forces that drive a reaction or scattering process lies at the heart of molecular dynamics. Here, we present a combined experimental and theoretical study of the spin-orbit...

Cited by 10 publications

References 88 publications

Inelastic collision dynamics of oriented NO molecules with Kr atoms

Inelastic collision dynamics of oriented NO molecules with Kr atoms

Collision‐induced spin‐orbit relaxation of highly vibrationally excited NO near 1 K

Gas sensing of fibrous red phosphorene towards inorganic air pollutants: Insights from first-principles calculations

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