Exit-channel recoil resonances by imaging the photodissociation of single quantum-state-selected OCS molecules

Dimitris Sofikitis, Jaime Suarez, Johan A. Schmidt, T. Peter Rakitzis, Stavros C. Farantos, Maurice H.M. Janssen

Research output: Contribution to JournalArticleAcademicpeer-review


In a recent letter [Phys. Rev. Lett. 118, 253001 (2017)PRLTAO0031-900710.1103/PhysRevLett.118.253001] we have described how studies of the recoil velocity distribution in the photodissociation of OCS in the energy interval 42 600-42 900 cm-1 revealed an unexpected behavior: the recoil velocity distribution of only the lowest-kinetic-energy photofragments exhibited rapid, resonantlike variations with energy and caused complete inversion of the recoil direction. Periodic orbit analysis and quantum nonadiabatic calculations unveiled the existence of a resonance state localized at large bending angles towards the exit of the dissociation channel. In this article, we present an extensive theoretical study and we show how the fingerprints of these resonances are identified by the analysis of the nonadiabatic transitions and the stereodynamics of photofragments trajectories. Additionally, the experimental study is extended to a second photolysis energy region, 43 300-43 650 cm-1, where a similar rapid variation of the recoil direction is detected. The energy separation between this second resonance region and the one previously reported is ∼800cm-1, which is twice the calculated period of the localized resonant state, offering a second point of convergence between the experiment and the theory.

Original languageEnglish
Article number033417
Pages (from-to)1-11
Number of pages11
JournalPhysical Review A
Issue number3
Publication statusPublished - 26 Sept 2018


This research has been financially supported by the division of Chemical Sciences of the Netherlands Organization for Scientific Research (NWO). D.S. acknowledges support by the EC's Seventh Framework Program via the Marie Curie Initial Training Network ICONIC. D.S. and T.P.R. also acknowledge support by the project “HELLAS-CH” (MIS 5002735), which is implemented under the “Action for Strengthening Research and Innovation Infrastructures,” funded by the Operational Program “Competitiveness, Entrepreneurship and Innovation” (NSRF 2014-2020) and cofinanced by Greece and the European Union (European Regional Development Fund). J.S. acknowledges support from the Laserlab-Europe through Grant No. ULF-FORTH002179. J.A.S. acknowledges funding from a Carlsberg Foundation postdoctoral fellowship (CF14-0519). J.S. thanks George McBane for providing the nonadiabatic coupling elements. D.S. thanks George McBane and Luis Rubio-Lago for useful discussions.

FundersFunder number
Seventh Framework ProgrammeMIS 5002735
European Commission
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
European Regional Development Fund


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