Electron-driven proton transfer enables nonradiative photodeactivation in microhydrated 2-aminoimidazole

Faraday Discussions
Mikołaj JanickiRobert W Góra

Abstract

2-Aminoimidazole (2-AIM) was proposed as a plausible nucleotide activating group in a nonenzymatic copying and polymerization of short RNA sequences under prebiotically plausible conditions. One of the key selection factors controlling the lifespan and importance of organic molecules on early Earth was ultraviolet radiation from the young Sun. Therefore, to assess the suitability of 2-AIM for prebiotic chemistry, we performed non-adiabatic molecular dynamics simulations and static explorations of potential energy surfaces of the photoexcited 2-AIM-(H2O)5 model system by means of the algebraic diagrammatic construction method to the second order [ADC(2)]. Our quantum mechanical simulations demonstrate that 1πσ* excited states play a crucial role in the radiationless deactivation of the UV-excited 2-AIM-(H2O)5 system. More precisely, electron-driven proton transfer (EDPT) along water wires is the only photorelaxation pathway leading to the formation of 1πσ*/S0 conical intersections. The availability of this mechanism and the lack of destructive photochemistry indicate that microhydrated 2-AIM is characterized by substantial photostability and resistance to prolonged UV irradiation.

References

Feb 12, 1993·Science·J F Kasting
Apr 15, 2004·Chemical Reviews·Carlos E Crespo-HernándezBern Kohler
Jun 25, 2005·The Journal of Chemical Physics·Zhenggang LanSusanta Mahapatra
Feb 24, 2006·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Andrzej L Sobolewski, Wolfgang Domcke
Apr 14, 2007·The Journal of Chemical Physics·Giovanni Granucci, Maurizio Persico
Nov 4, 2010·Journal of the American Chemical Society·Matthew W PownerJack W Szostak
Mar 4, 2011·Journal of Computational Chemistry·Stefan GrimmeLars Goerigk
Sep 10, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Rachel Crespo-OteroSusanne Ullrich
Mar 16, 2013·Physical Chemistry Chemical Physics : PCCP·Xiaojun LiuWolfgang Domcke
Jul 11, 2014·Journal of the American Chemical Society·Mario Barbatti
Jul 17, 2014·Physical Chemistry Chemical Physics : PCCP·Rafał SzablaRobert W Góra
Aug 20, 2014·The Journal of Physical Chemistry. a·Xiaojun LiuWolfgang Domcke
Mar 25, 2015·Nature Chemistry·Bhavesh H PatelJohn D Sutherland
May 30, 2015·The Journal of Physical Chemistry. a·Reza OmidyanGholamhassan Azimi
Jul 29, 2015·The Journal of Physical Chemistry. B·Xiaojun LiuWolfgang Domcke
Aug 12, 2015·The Journal of Physical Chemistry Letters·Rafał SzablaRobert W Góra
Oct 7, 2015·The Journal of Physical Chemistry. a·Sermsiri ChaiwongwattanaNađa Došlić
Jan 2, 2016·The Journal of Physical Chemistry Letters·Thomas A A OliverStephen E Bradforth
Jan 21, 2016·Astrobiology·Sukrit Ranjan, Dimitar D Sasselov
Feb 3, 2016·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Xiuxiu WuWolfgang Domcke
Jan 7, 2015·Chemical Science·Rafał SzablaJohn D Sutherland
Oct 11, 2016·Faraday Discussions·Rafał SzablaJiří Šponer
Jan 25, 2017·Journal of the American Chemical Society·Li LiJack W Szostak
Feb 15, 2017·The Journal of Physical Chemistry Letters·Juan J NogueiraVilly Sundström
Jun 9, 2017·The Journal of Physical Chemistry. a·Johannes EhrmaierWolfgang Domcke
Jun 24, 2017·Journal of the American Chemical Society·Albert C FahrenbachJack W Szostak
Jul 1, 2017·Physical Chemistry Chemical Physics : PCCP·Rafał SzablaRobert W Góra

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Citations

Aug 6, 2019·Chemical Communications : Chem Comm·Zoe R ToddDimitar D Sasselov
Dec 24, 2020·Physical Chemistry Chemical Physics : PCCP·Joanna Jankowska, Robert W Góra

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