A double-QM/MM method for investigating donor-acceptor electron-transfer reactions in solution

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F14%3A10286194" target="_blank" >RIV/00216208:11320/14:10286194 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1039/c4cp02307b" target="_blank" >http://dx.doi.org/10.1039/c4cp02307b</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/c4cp02307b" target="_blank" >10.1039/c4cp02307b</a>

Jazyk výsledku

angličtina

Název v původním jazyce

A double-QM/MM method for investigating donor-acceptor electron-transfer reactions in solution

Popis výsledku v původním jazyce

We developed a double-quantum mechanical/molecular mechanical (d-QM/MM) method for investigation of full outer-sphere electron transfer (ET) processes between a donor and an acceptor (DA) in condensed matter. In the d-QM/MM method, which employs the novel concept of multiple QM regions, one can easily specify the number of electrons, spin states and appropriate exchange-correlation treatment in each QM region, which is especially important in the cases of ET involving transition metal sites. We investigated Fe2+/3+ self-exchange and Fe3+ + Ru2+ -> Fe2+ + Ru3+ in aqueous solution as model reactions, and demonstrated that the d-QM/MM method gives reasonable accuracy for the redox potential, reorganization free energy and electronic coupling. In particular, the DA distance dependencies of those quantities are clearly shown at the density functional theory hybrid functional level. The present d-QM/MM method allows us to explore the intermediate DA distance region, important for long-range

Název v anglickém jazyce

A double-QM/MM method for investigating donor-acceptor electron-transfer reactions in solution

Popis výsledku anglicky

We developed a double-quantum mechanical/molecular mechanical (d-QM/MM) method for investigation of full outer-sphere electron transfer (ET) processes between a donor and an acceptor (DA) in condensed matter. In the d-QM/MM method, which employs the novel concept of multiple QM regions, one can easily specify the number of electrons, spin states and appropriate exchange-correlation treatment in each QM region, which is especially important in the cases of ET involving transition metal sites. We investigated Fe2+/3+ self-exchange and Fe3+ + Ru2+ -> Fe2+ + Ru3+ in aqueous solution as model reactions, and demonstrated that the d-QM/MM method gives reasonable accuracy for the redox potential, reorganization free energy and electronic coupling. In particular, the DA distance dependencies of those quantities are clearly shown at the density functional theory hybrid functional level. The present d-QM/MM method allows us to explore the intermediate DA distance region, important for long-range

Druh

J_x - Nezařazeno - Článek v odborném periodiku (Jimp, Jsc a Jost)

CEP obor

BJ - Termodynamika

OECD FORD obor

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Projekt

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Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2014

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Physical Chemistry Chemical Physics

ISSN

1463-9076

e-ISSN

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Svazek periodika

16

Číslo periodika v rámci svazku

36

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

10

Strana od-do

19530-19539

Kód UT WoS článku

000341299500054

EID výsledku v databázi Scopus

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