Exploration of Excited State Deactivation Pathways of Adenine Monohydrates

Chaiwongwattana, Sermsiri; Sapunar, Marin; Ponzi, Aurora; Decleva, Piero; Došlić, Nađa (2015) Exploration of Excited State Deactivation Pathways of Adenine Monohydrates. The Journal of Physical Chemistry A, 119 (43). pp. 10637-10644. ISSN 1089-5639

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Abstract

Binding of a single water molecule has a dramatic effect on the excited state lifetime of adenine. Here we report a joint nonadiabatic dynamics and reaction paths study aimed at understanding the sub-100 fs lifetime of adenine in the monohydrates. Our nonadiabatic dynamics simulations, performed using the ADC(2) electronic structure method, show a shortening of the excited state lifetime in the monohydrates with respect to bare adenine. However, the computed lifetimes were found to be significantly longer that the observed one. By comparing the reaction pathways of several excited state deactivation processes in adenine and adenine monohydrates, we show that electron-driven proton transfer from water to nitrogen atom N3 of the adenine ring may be the process responsible for the observed ultrafast decay. The inaccessibility of the electron-driven proton transfer pathway to trajectory-based nonadiabatic dynamics simulation is discussed.

Item Type:	Article
Additional Information:	This document is the unedited Author’s version of a Submitted Manuscript subsequently accepted for publication in The Journal of Physical Chemistry A, copyright © 2015 American Chemical Society. To access the final published article, see ACS Articles on Request.
Uncontrolled Keywords:	photochemistry ; trajectory surface hopping ; nonadiabatic dynamics ; microsolvation
Subjects:	NATURAL SCIENCES > Chemistry > Theoretical Chemistry
Divisions:	Division of Physical Chemistry
Depositing User:	Marin Sapunar
Date Deposited:	30 Apr 2026 09:57
URI:	https://fulir.irb.hr:/id/eprint/11836
DOI:	10.1021/acs.jpca.5b07496

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