Sequential electron transfer governs the UV-induced self-repair of DNA photolesions

Result code in IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F68081707%3A_____%2F18%3A00492425" target="_blank" >RIV/68081707:_____/18:00492425 - isvavai.cz</a>

Alternative codes found

RIV/61989592:15310/18:73591647

Result on the web

<a href="http://dx.doi.org/10.1039/c8sc00024g" target="_blank" >http://dx.doi.org/10.1039/c8sc00024g</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/c8sc00024g" target="_blank" >10.1039/c8sc00024g</a>

Result language

angličtina

Original language name

Sequential electron transfer governs the UV-induced self-repair of DNA photolesions

Original language description

Cyclobutane pyrimidine dimers (CpDs) are among the most common DNA lesions occurring due to the interaction with ultraviolet light. While photolyases have been well known as external factors repairing CpDs, the intrinsic self-repairing capabilities of the GAT=T DNA sequence were discovered only recently and are still largely obscure. Here, we elucidate the mechanistic details of this self-repair process by means of MD simulations and QM/MM computations involving the algebraic diagrammatic construction to the second order [ADC(2)] method. We show that local UV-excitation of guanine may be followed by up to three subsequent electron transfers, which may eventually enable efficient CpD ring opening when the negative charge resides on the T=T dimer. Consequently, the molecular mechanism of GAT=T self-repair can be envisaged as sequential electron transfer (SET) occurring downhill along the slope of the S-1 potential energy surface. Even though the general features of the SET mechanism are retained in both of the studied stacked conformers, our optimizations of different S-1/S-0 state crossings revealed minor differences which could influence their self-repair efficiencies. We expect that such assessment of the availability and efficiency of the SET process in other DNA oligomers could hint towards other sequences exhibiting similar photochemical properties. Such explorations will be particularly fascinating in the context of the origins of biomolecules on Earth, owing to the lack of external repairing factors in the Archean age.

Czech name

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Czech description

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Type

J_imp - Article in a specialist periodical, which is included in the Web of Science database

CEP classification

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OECD FORD branch

10608 - Biochemistry and molecular biology

Project

<a href="/en/project/GA16-13721S" target="_blank" >GA16-13721S: Multi-scale modeling of structure, dynamics and folding of DNA.</a><br>

Continuities

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Publication year

2018

Confidentiality

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

Name of the periodical

Chemical Science

ISSN

2041-6520

e-ISSN

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Volume of the periodical

9

Issue of the periodical within the volume

12

Country of publishing house

GB - UNITED KINGDOM

Number of pages

10

Pages from-to

3131-3140

UT code for WoS article

000428987200006

EID of the result in the Scopus database

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