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Control and imaging of O(1D2) precession

Nature Chemistry volume 3, pages 28–33 (2011)Cite this article

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Abstract

Larmor precession of a quantum mechanical angular momentum vector about an applied magnetic field forms the basis for a range of magnetic resonance techniques, including nuclear magnetic resonance spectroscopy and magnetic resonance imaging. We have used a polarized laser pump–probe scheme with velocity-map imaging detection to visualize, for the first time, the precessional motion of a quantum mechanical angular momentum vector. Photodissociation of O2 at 157 nm provides a clean source of fast-moving O(1D2) atoms, with their electronic angular momentum vector strongly aligned perpendicular to the recoil direction. In the presence of an external magnetic field, the distribution of atomic angular momenta precesses about the field direction, and polarization-sensitive images of the atomic scattering distribution recorded as a function of field strength yield ‘time-lapse-photography’ style movies of the precessional motion. We present movies recorded in various experimental geometries, and discuss potential consequences and applications in atmospheric chemistry and reaction dynamics.

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Figure 1: The O(1D2) MJ state population distribution following photodissociation of O2 at 157 nm.
Figure 2: Schematic of the VMI setup.
Figure 3: Montage of 2D sliced images from Supplementary Movie 1.
Figure 4: Experimentally measured and simulated images for the subset of images from Fig. 3 spanning Helmholtz coil currents of 200–450 mA.
Figure 5: Calibration showing the dependence of the magnetic field strength experienced by the scattered O(1D2) atoms on Helmholtz coil current.

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Acknowledgements

The authors acknowledge support from the European Union under training network ITN 238671 ‘ICONIC’, the European Research Council under Starting Independent Research Grant 200733 ‘ImageMS’, the Dutch National Science Foundation FOM-NWO program Molecular Atmospheric Processes, and the National Science Foundation under NSF CHE 0650414.

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Authors and Affiliations

  1. Radboud University Nijmegen, Institute for Molecules and Materials (IMM), Heyendaalseweg 135, Nijmegen, 6525, AJ, The Netherlands

    Shiou-Min Wu, Dragana Č. Radenovic, Wim J. van der Zande, Gerrit C. Groenenboom & David H. Parker

  2. Department of Chemistry, University of Oxford, Chemistry Research Laboratory, 12 Mansfield Road, Oxford, OX1 3TA, UK

    Claire Vallance

  3. Department of Chemistry, Stanford University, 333 Campus Drive, Stanford, 94305-5080, California, USA

    Richard N. Zare

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Contributions

D.P., W.Z. and, independently, R.Z., conceived and designed the experiments. S.W. and D.R. performed the experiments. C.V. and G.G. analysed the data. C.V., D.P. and S.W. wrote the manuscript, with contributions from W.Z., G.G. and R.Z.

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Correspondence to David H. Parker, Claire Vallance or Richard N. Zare.

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The authors declare no competing financial interests.

Supplementary information

Supplementary information

Supplementary information (PDF 329 kb)

Supplementary information

Supplementary Movie S1 (MOV 341 kb)

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Supplementary Movie S2 (MOV 249 kb)

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Supplementary Movie S3 (MOV 209 kb)

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Supplementary Movie S4 (MOV 371 kb)

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Supplementary Movie S5 (MOV 310 kb)

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Supplementary Movie S6 (MOV 224 kb)

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Wu, SM., Radenovic, D., van der Zande, W. et al. Control and imaging of O(1D2) precession. Nature Chem 3, 28–33 (2011). https://doi.org/10.1038/nchem.929

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