Capturing roaming molecular fragments in real time

Author:

Endo Tomoyuki12ORCID,Neville Simon P.3,Wanie Vincent1,Beaulieu Samuel1ORCID,Qu Chen4ORCID,Deschamps Jude1ORCID,Lassonde Philippe1,Schmidt Bruno E.5,Fujise Hikaru6ORCID,Fushitani Mizuho6ORCID,Hishikawa Akiyoshi67ORCID,Houston Paul L.89ORCID,Bowman Joel M.10ORCID,Schuurman Michael S.311ORCID,Légaré François1ORCID,Ibrahim Heide1ORCID

Affiliation:

1. Centre Énergie Matériaux Télécommunications, Institut National de la Recherche Scientifique, Varennes, Quebec J3X 1S2, Canada.

2. Kansai Photon Science Institute, National Institutes for Quantum and Radiological Science and Technology, Kizugawa, Kyoto 619-0215, Japan.

3. Department of Chemistry and Biomolecular Sciences, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada.

4. Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA.

5. few-cycle Inc., Montreal, Quebec H1L 5W5, Canada.

6. Department of Chemistry, Graduate School of Science, Nagoya University, Nagoya, Aichi 464-8602, Japan.

7. Research Center for Materials Science, Nagoya University, Nagoya, Aichi 464-8602, Japan.

8. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY 14852, USA.

9. School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA 30332, USA.

10. Department of Chemistry and Cherry L. Emerson Center for Scientific Computation, Emory University, Atlanta, GA 30322, USA.

11. National Research Council of Canada, Ottawa, Ontario K1A 0R6, Canada.

Abstract

Roaming dynamics in real time Roaming is distinct from conventional reaction channels because of the unusual geometries that chemical systems use to bypass the minimum energy pathway. It is a relatively new phenomenon that is usually determined in experiments through spectroscopic characterization of the roaming products. Using a combination of time-resolved Coulomb explosion imaging and quasiclassical trajectory analysis, Endo et al. report real-time observation of individual fragments of the prototypical reaction of deuterated formaldehyde (D 2 CO) dissociation as they roam on ultrafast time scales. They show that roaming not only occurs several orders of magnitude earlier than previously expected but also that it can terminate in a radical (D + DCO) rather than the well-known molecular (D 2 + CO) product channel. Science , this issue p. 1072

Funder

Natural Sciences and Engineering Research Council of Canada

Canada Foundation for Innovation

Fonds de Recherche du Québec - Nature et Technologies

Japan Society for the Promotion of Science

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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