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Issue 3, 2011
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Photodissociation of pyrrole–ammonia clusters by velocity map imaging: mechanism for the H-atom transfer reaction

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Abstract

The photodissociation dynamics of pyrrole–ammonia clusters (PyH·(NH3)n, n = 2–6) has been studied using a combination of velocity map imaging and non-resonant detection of the NH4(NH3)n−1 products. The excited state hydrogen-atom transfer mechanism (ESHT) is evidenced through delayed ionization and presents a threshold around 236.6 nm, in agreement with previous reports. A high resolution determination of the kinetic energy distributions (KEDs) of the products reveals slow (∼0.15 eV) and structured distributions for all the ammonia cluster masses studied. The low values of the measured kinetic energy rule out the existence of a long-lived intermediate state, as it has been proposed previously. Instead, a direct N–H bond rupture, in the fashion of the photodissociation of bare pyrrole, is proposed. This assumption is supported by a careful analysis of the structure of the measured KEDs in terms of a discrete vibrational activity of the pyrrolyl co-fragment.

Graphical abstract: Photodissociation of pyrrole–ammonia clusters by velocity map imaging: mechanism for the H-atom transfer reaction

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Publication details

The article was received on 06 Aug 2010, accepted on 12 Oct 2010 and first published on 12 Nov 2010


Article type: Paper
DOI: 10.1039/C0CP01442G
Citation: Phys. Chem. Chem. Phys., 2011,13, 1082-1091
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    Photodissociation of pyrrole–ammonia clusters by velocity map imaging: mechanism for the H-atom transfer reaction

    L. Rubio-Lago, G. A. Amaral, A. N. Oldani, J. D. Rodríguez, M. G. González, G. A. Pino and L. Bañares, Phys. Chem. Chem. Phys., 2011, 13, 1082
    DOI: 10.1039/C0CP01442G

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