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

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...

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Main Authors: Kungwan N., Kerdpol K., Daengngern R., Hannongbua S., Barbatti M.
Format: Article
Language:English
Published: 2014
Online Access:http://www.scopus.com/inward/record.url?eid=2-s2.0-84896414947&partnerID=40&md5=ff3ef34d98760ed2d9d223ac1ed30cb9
http://cmuir.cmu.ac.th/handle/6653943832/4781
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Institution: Chiang Mai University
Language: English
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spelling th-cmuir.6653943832-47812014-08-30T02:55:45Z 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 Kungwan N. Kerdpol K. Daengngern R. Hannongbua S. Barbatti M. 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. © 2014 Springer-Verlag Berlin Heidelberg. 2014-08-30T02:55:45Z 2014-08-30T02:55:45Z 2014 Article in Press 1432881X 10.1007/s00214-014-1480-y http://www.scopus.com/inward/record.url?eid=2-s2.0-84896414947&partnerID=40&md5=ff3ef34d98760ed2d9d223ac1ed30cb9 http://cmuir.cmu.ac.th/handle/6653943832/4781 English
institution Chiang Mai University
building Chiang Mai University Library
country Thailand
collection CMU Intellectual Repository
language English
description 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. © 2014 Springer-Verlag Berlin Heidelberg.
format Article
author Kungwan N.
Kerdpol K.
Daengngern R.
Hannongbua S.
Barbatti M.
spellingShingle Kungwan N.
Kerdpol K.
Daengngern R.
Hannongbua S.
Barbatti M.
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
author_facet Kungwan N.
Kerdpol K.
Daengngern R.
Hannongbua S.
Barbatti M.
author_sort Kungwan N.
title 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
title_short 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
title_full 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
title_fullStr 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
title_full_unstemmed 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
title_sort 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
publishDate 2014
url http://www.scopus.com/inward/record.url?eid=2-s2.0-84896414947&partnerID=40&md5=ff3ef34d98760ed2d9d223ac1ed30cb9
http://cmuir.cmu.ac.th/handle/6653943832/4781
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