Quantum chemical study of the enzymatic repair of T(6-4)C/C(6-4)T UV-photolesions by DNA photolyases
Several strategies have evolved to repair one of the abundant UV radiation-induced damages caused to DNA, namely the mutagenic pyrimidine (6-4) pyrimidone photolesions. DNA (6-4)-photolyases are enzymes repairing these lesions by a photoinitiated electron transfer. An important aspect of a possible...
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| Main Authors: | , , |
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| Format: | Article (Journal) |
| Language: | English |
| Published: |
2 July 2013
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| In: |
ChemPhysChem
Year: 2013, Volume: 14, Issue: 12, Pages: 2817-2824 |
| ISSN: | 1439-7641 |
| DOI: | 10.1002/cphc.201300223 |
| Online Access: | Verlag, Volltext: http://dx.doi.org/10.1002/cphc.201300223 Verlag, Volltext: http://onlinelibrary.wiley.com/doi/10.1002/cphc.201300223/abstract 
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| Author Notes: | Shirin Faraji, Lukas Wirz, and Andreas Dreuw |
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| 520 | |a Several strategies have evolved to repair one of the abundant UV radiation-induced damages caused to DNA, namely the mutagenic pyrimidine (6-4) pyrimidone photolesions. DNA (6-4)-photolyases are enzymes repairing these lesions by a photoinitiated electron transfer. An important aspect of a possible repair mechanism is its generality and transferability to different (6-4) lesions. Therefore, previously suggested mechanisms for the repair of the T(6-4)T lesion are here transferred to the T(6-4)C and C(6-4)T lesions and investigated theoretically using quantum chemical methods. Despite the different functional groups of the pyrimidine bases involved, a general valid molecular mechanism was identified, in which the initial step is an electron transfer coupled to a proton transfer from the protonated HIS365 to the N3′ nitrogen of the 3′ pyrimidine, followed by an intramolecular OH/NH2 transfer in one concerted step, which does not require an oxetane/azetidine or isolated water/ammonia intermediate. | ||
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