Experimental developments continue to challenge the theoretical description of molecular interactions. One key arena in which these advances have taken place is in rotationally inelastic scattering. Electric fields have been used with great success to select the initial quantum state and slow molecules for scattering studies, revealing novel stereodynamics, diffraction oscillations and scattering resonances. These have enjoyed excellent agreement with quantum scattering calculations performed on state-of-the-art coupled-cluster potential energy surfaces. To date these studies have largely employed reactants in the ground vibrational state (v = 0) and the lowest low-field-seeking quantum state. Here we describe the use of stimulated emission pumping to prepare NO molecules in arbitrary single rotational and parity states of v = 10 for inelastic scattering studies. These are employed in a near-copropagating molecular beam geometry that permits the collision energy to be tuned from above room temperature to 1 K or below, with product differential cross-sections obtained by velocity map imaging. This extremely nonequilibrium condition, not found in nature, tests current theoretical methods in a new regime.
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Raw scattering images, MC simulated images, extracted DCSs and theoretical DCSs are publicly available in the Zenodo data repository at https://doi.org/10.5281/zenodo.3703096.
The quantum 2D scattering algorithm used for open-shell systems such as Ar-NO is publicly available. The MC forward-convolution program used to simulate experimental conditions is available from the author upon reasonable request.
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We thank S. Y. T. van de Meerakker for valuable discussions. This work was supported by the Army Research Office under awards W911NF-14-1-0378 and W911NF-19-1-0283 and the AFOSR under award FA9550-16-1-0018. J.K. acknowledges financial support from the US National Science Foundation, grant no. CHE-1565872 to Millard Alexander. M.B. acknowledges support from the Dutch Astrochemistry Network programme of the Netherlands Organization for Scientific Research and support from the European Research Council under the European Union’s Horizon 2020 Research and Innovation Program (grant agreement no. 817947 FICOMOL awarded to S. Y. T. van de Meerakker).
The authors declare no competing interests.
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Amarasinghe, C., Li, H., Perera, C.A. et al. State-to-state scattering of highly vibrationally excited NO at broadly tunable energies. Nat. Chem. 12, 528–534 (2020). https://doi.org/10.1038/s41557-020-0466-8
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