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Abstract:

Lifetimes of the first electronic excited state (S1) of fluorine and methyl (o-, m-, and p-) substituted phenols and their complexes with one ammonia molecule have been measured for the 00 transition and for the intermolecular stretching σ1 levels in complexes using picosecond pump-probe spectroscopy. Excitation energies to the S1 (π π *) and S2 (π σ*) states are obtained by quantum chemical calculations at the MP2 and CC2 level using the aug-cc-pVDZ basis set for the ground-state and the S1 optimized geometries. The observed lifetimes and the energy gaps between the π π * and π σ* states show a good correlation, the lifetime being shorter for a smaller energy gap. This propensity suggests that the major dynamics in the excited state concerns an excited state hydrogen detachment or transfer (ESHD/T) promoted directly by a S1 / S2 conical intersection, rather than via internal conversion to the ground-state. A specific shortening of lifetime is found in the o-fluorophenol-ammonia complex and explained in terms of the vibronic coupling between the π π * and π σ* states occurring through the out-of-plane distortion of the C-F bond. © 2010 American Institute of Physics.

Registro:

Documento: Artículo
Título:Excited state hydrogen transfer dynamics in substituted phenols and their complexes with ammonia: π π * -π σ*energy gap propensity and ortho-substitution effect
Autor:Pino, G.A.; Oldani, A.N.; Marceca, E.; Fujii, M.; Ishiuchi, S.-I.; Miyazaki, M.; Broquier, M.; Dedonder, C.; Jouvet, C.
Filiación:INFIQC-Dpto. de Fisicoquímica, Fac. de Cs. Químicas, Universidad Nacional de Córdoba, Córdoba 5000, Argentina
INQUIMAE-DQIAQF, Universidad de Buenos Aires, Ciudad Universitaria, Pabellón II, Buenos Aires C1428EHA, Argentina
Chemical Resources Laboratory, Integrated Research Institute, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan
Centre Laser de l'Universit́ Paris Sud (CLUPS), ISMO-CNRS, Univ. Paris Sud 11, Orsay Cedex F-91405, France
Palabras clave:Ammonia complexes; Ammonia molecules; Basis sets; C-F bonds; Conical intersection; Electronic excited state; Good correlations; Hydrogen transfer; Intermolecular stretching; Internal conversions; Optimized geometries; Ortho-substitution; Out-of-plane distortions; Picoseconds; Pump-probe spectroscopy; Quantum chemical calculations; State concerns; Substituted phenol; Vibronic coupling; Ammonia; Diamond films; Energy gap; Fluorine; Ground state; Hydrogen; Organic polymers; Phenols; Pumps; Quantum chemistry; Quantum theory; Solids; Excited states
Año:2010
Volumen:133
Número:12
DOI: http://dx.doi.org/10.1063/1.3480396
Título revista:Journal of Chemical Physics
Título revista abreviado:J Chem Phys
ISSN:00219606
CODEN:JCPSA
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00219606_v133_n12_p_Pino

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Citas:

---------- APA ----------
Pino, G.A., Oldani, A.N., Marceca, E., Fujii, M., Ishiuchi, S.-I., Miyazaki, M., Broquier, M.,..., Jouvet, C. (2010) . Excited state hydrogen transfer dynamics in substituted phenols and their complexes with ammonia: π π * -π σ*energy gap propensity and ortho-substitution effect. Journal of Chemical Physics, 133(12).
http://dx.doi.org/10.1063/1.3480396
---------- CHICAGO ----------
Pino, G.A., Oldani, A.N., Marceca, E., Fujii, M., Ishiuchi, S.-I., Miyazaki, M., et al. "Excited state hydrogen transfer dynamics in substituted phenols and their complexes with ammonia: π π * -π σ*energy gap propensity and ortho-substitution effect" . Journal of Chemical Physics 133, no. 12 (2010).
http://dx.doi.org/10.1063/1.3480396
---------- MLA ----------
Pino, G.A., Oldani, A.N., Marceca, E., Fujii, M., Ishiuchi, S.-I., Miyazaki, M., et al. "Excited state hydrogen transfer dynamics in substituted phenols and their complexes with ammonia: π π * -π σ*energy gap propensity and ortho-substitution effect" . Journal of Chemical Physics, vol. 133, no. 12, 2010.
http://dx.doi.org/10.1063/1.3480396
---------- VANCOUVER ----------
Pino, G.A., Oldani, A.N., Marceca, E., Fujii, M., Ishiuchi, S.-I., Miyazaki, M., et al. Excited state hydrogen transfer dynamics in substituted phenols and their complexes with ammonia: π π * -π σ*energy gap propensity and ortho-substitution effect. J Chem Phys. 2010;133(12).
http://dx.doi.org/10.1063/1.3480396