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Effects of the second hydration shell on excited-state multiple proton transfer: dynamics simulations of 7-azaindole:(H2O)1–5 clusters in the gas phase

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Abstract

Dynamics of the multiple excited-state proton transfer (ESPT) in clusters of 7-azaindole with up to five water molecules was investigated with quantum chemical methods. The ultrafast excited-state dynamics triggered by photoexcitation was simulated with the algebraic diagrammatic construction to the second-order scheme. Multiple ESPT through a hydrogen-bonded network is observed in the 100-fs scale. The probability of tautomerization is anti-correlated with the maximum free energy barrier in the excited state. An increasing number of water molecules tends to reduce the barrier by strengthening the hydrogen-bonded network. Barrierless reactions are found already for clusters with four waters. In structures presenting double hydrogen bond circuits, proton transfer happens mostly through the internal circuit by triple proton transfer. The overall role of the second hydration shell is of stabilizing the network, facilitating the proton transfer in the internal circuit. Proton transfers involving the second hydration shell were observed, but with small probability of occurrence. The proton-transfer processes tend to be synchronous, with two of them occurring within 10–15 fs apart.

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Acknowledgments

The authors wish to thank the Thailand Research Fund (MRG5480294 and TRG5680098) for financial support. K. Kerdpol and R. Daengngern thank the Science Achievement Scholarship of Thailand (SAST), Faculty of Science, Chiang Mai University, Chiang Mai, Thailand.

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Authors and Affiliations

  1. Department of Chemistry, Faculty of Science, Chiang Mai University, Chiang Mai, 50200, Thailand

    Nawee Kungwan, Khanittha Kerdpol & Rathawat Daengngern

  2. Department of Chemistry, Faculty of Science, Kasetsart University, Bangkhen Campus, Bangkok, 10930, Thailand

    Supa Hannongbua

  3. Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470, Mülheim an der Ruhr, Germany

    Mario Barbatti

Authors
  1. Nawee Kungwan
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  2. Khanittha Kerdpol
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  3. Rathawat Daengngern
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  4. Supa Hannongbua
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  5. Mario Barbatti
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Corresponding authors

Correspondence to Nawee Kungwan or Mario Barbatti.

Additional information

Dedicated to the memory of Professor Isaiah Shavitt and published as part of the special collection of articles celebrating his many contributions.

Electronic supplementary material

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214_2014_1480_MOESM1_ESM.pdf

Ground-state structures of the 7AI(H2O) n=1,1+1,2 complexes; snapshots of trajectories featuring HBR and tautomerization; time evolution of average potential energies and average bond lengths; average relative energies along the reaction pathways; relative energies of the three ground-state 7AI(H2O)3 isomers; Cartesian coordinates of all investigated complexes. (PDF 2693 kb)

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Kungwan, N., Kerdpol, K., Daengngern, R. et al. Effects of the second hydration shell on excited-state multiple proton transfer: dynamics simulations of 7-azaindole:(H2O)1–5 clusters in the gas phase. Theor Chem Acc 133, 1480 (2014). https://doi.org/10.1007/s00214-014-1480-y

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