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Imaging the onset of the resonance regime in low-energy NO-He collisions

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Science  08 May 2020:
Vol. 368, Issue 6491, pp. 626-630
DOI: 10.1126/science.aba3990

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Ultracold molecular collision dynamics

Ultracold collision dynamics are of great importance in understanding the quantum nature of chemical interactions, but achieving the ultracold regime for molecules is challenging. Traditional techniques based on alternative routes to assemble the ultracold atomic constituents are only able to produce a type of ultracold molecules that cannot probe state-selective dynamics. Using Stark deceleration and velocity map–imaging techniques, de Jongh et al. achieved the ultracold regime directly for a nitric oxide–helium system and measured the state-to-state cross sections for inelastic scattering with high precision (see the Perspective by Yang and Yang). The observed scattering resonances confirmed high sensitivity to the underlying interaction potential because only the most accurate electronic structure theory could reproduce their structure.

Science, this issue p. 626; see also p. 582

Abstract

At low energies, the quantum wave–like nature of molecular interactions results in distinctive scattering behavior, ranging from the universal Wigner laws near 0 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 to 8.5 centimeter–1 range with 0.02 centimeter–1 resolution. We studied 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. Only with CCSDT(Q) level of theory was it possible to reproduce our measurements.

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