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Phys Chem Chem Phys ; 18(45): 31260-31267, 2016 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-27819104

RESUMO

The gas phase structure and excited state lifetime of the p-aminophenolp-cresol heterodimer have been investigated by REMPI and LIF spectroscopy with nanosecond laser pulses and pump-probe experiments with picosecond laser pulses as a model system to study the competition between π-π and H-bonding interactions in aromatic dimers. The excitation is a broad and unstructured band. The excited state of the heterodimer is long lived (2.5 ± 0.5) ns with a very broad fluorescence spectrum red-shifted by 4000 cm-1 with respect to the excitation spectrum. Calculations at the MP2/RI-CC2 and DFT-ωB97X-D levels indicate that hydrogen-bonded (HB) and π-stacked isomers are almost isoenergetic in the ground state while in the excited state only the π-stacked isomer exists. This suggests that the HB isomer cannot be excited due to negligible Franck-Condon factors and therefore the excitation spectrum is associated with the π-stacked isomer that reaches vibrationally excited states in the S1 state upon vertical excitation. The excited state structure is an exciplex responsible for the fluorescence of the complex. Finally, a comparison was performed between the π-stacked structure observed for the p-aminophenolp-cresol heterodimer and the HB structure reported for the (p-cresol)2 homodimer indicating that the differences are due to different optical properties (oscillator strengths and Franck-Condon factors) of the isomers of both dimers and not to the interactions involved in the ground state.

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