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State-resolved diffraction oscillations imaged for inelastic collisions of NO radicals with He, Ne and Ar

Abstract

Just as light scattering from an object results in diffraction patterns, the quantum mechanical nature of molecules can lead to the diffraction of matter waves during molecular collisions. This behaviour manifests itself as rapid oscillatory structures in measured differential cross-sections, and such observable features are sensitive probes of molecular interaction potentials. However, these structures have proved challenging to resolve experimentally. Here, we use a Stark decelerator to form a beam of state-selected and velocity-controlled NO radicals and measure state-to-state differential cross-sections for inelastic collisions of NO with He, Ne and Ar atoms using velocity map imaging. The monochromatic velocity distribution of the NO beam produced scattering images with unprecedented sharpness and angular resolution, thereby fully resolving quantum diffraction oscillations. We found excellent agreement with quantum close-coupling scattering calculations for these benchmark systems.

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Figure 1: Schematic representation of the experimental set-up.
Figure 2: Typical velocity-mapped ion images.
Figure 3: Velocity-mapped ion image for inelastic collisions of NO (1/2f) radicals with Ne atoms, probing simultaneously the final states (5/2f) and (11/2e).
Figure 4: Experimental and simulated ion images revealing quantum diffraction oscillations.
Figure 5: Diffraction oscillations for the scattering process NO (1/2f)+ Rg → NO (3/2e)+ Rg for Rg = He, Ne and Ar.
Figure 6: Diffraction oscillations for the scattering process NO (1/2f) + Ne → NO (3/2e) + Ne at a collision energy of 485 cm−1 and 600 cm−1.

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Acknowledgements

This work is part of the research programme of the Foundation for Fundamental Research on Matter (FOM), which is supported financially by the Netherlands Organization for Scientific Research (NWO). S.Y.T.v.d.M. acknowledges support from the NWO via a VIDI grant, and from the European Research Council via a Starting Grant. The authors thank D. Parker for discussions and general support and the Fritz-Haber-Institute in Berlin for loan of equipment. The authors thank K. Liu for discussions about the analysis of scattering images and J. Kłos, H. Cybulski, B. Fernández, Y. Endo and M. Alexander for providing their PESs. The authors thank B. Nichols and S. Chefdeville for assistance during part of the measurements, R. Rammeloo for developing software to simulate ion images, and A. van Roij, L. Gerritsen, C. Berkhout and P. Claus for expert technical support.

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The research project was conceived and supervised by S.Y.T.v.d.M. The experiments were carried out by A.v.Z. and J.O. Data analysis and interpretation was performed by A.v.Z., J.O., S.N.V. and S.Y.T.v.d.M. Theoretical calculations were performed by J.O., A.v.d.A. and G.C.G. The paper was written by S.Y.T.v.d.M. with contributions from all authors. All authors contributed to discussions about the content of the paper.

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Correspondence to Sebastiaan Y. T. van de Meerakker.

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von Zastrow, A., Onvlee, J., Vogels, S. et al. State-resolved diffraction oscillations imaged for inelastic collisions of NO radicals with He, Ne and Ar. Nature Chem 6, 216–221 (2014). https://doi.org/10.1038/nchem.1860

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