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| Content Provider | PubMed Central |
|---|---|
| Author | Liu, Yang Liu, Zhi Geacintov, Nicholas E. Vladimir, Shafirovich |
| Abstract | Nucleosomes were reconstituted from recombinant histones and a 147-mer DNA sequence containing the damage reporter sequence 5′-…d([2AP]T[GGG]1TT[GGG]2TTT[GGG]3TAT)… with 2-aminopurine (2AP) at position 27 from the dyad axis. Footprinting studies with •OH radicals reflect the usual effects of “in” and “out” rotational settings, while, interestingly, the guanine oxidizing one-electron oxidant CO3 •− radical does not. Site-specific hole injection was achieved by 308 nm excimer laser pulses to produce 2AP•+ cations, and superoxide via the trapping of hydrated electrons. Rapid deprotonation (~ 100 ns) and proton coupled electron transfer generates neutral guanine radicals, G(−H)• and hole hopping between the three groups of [GGG] on micro- to millisecond time scales. Hole transfer competes with hole trapping that involves the combination of O2 •− with G(−H)• radicals to yield predominantly 2,5-diamino-4H-imidazolone (Iz) and minor 8-oxo-7,8-dihydroguanine (8-oxoG) end-products in free DNA (Misiaszek et al. J. Biol. Chem. 2004, 279, 32106). Hole migration is less efficient in nucleosomal than in the identical protein-free DNA by a factor of 1.2 – 1.5. The Fpg/piperidine strand cleavage ratio is ~1.0 in free DNA at all three GGG sequences and at the “in” rotational settings [GGG]1,3 facing the histone core, and ~2.3 at the “out” setting at [GGG]2 facing away from the histone core. These results are interpreted in terms of competitive reaction pathways of O2 •− with G(−H)• radicals at the C5 (yielding Iz) and C8 (yielding 8-oxoG) positions. These differences in product distributions are attributed to variations in the local nucleosomal B-DNA base pair structural parameters that are a function of surrounding sequence context and rotational setting. |
| Related Links | http://dx.doi.org/10.1039/c2cp40759k |
| Starting Page | 7400 |
| File Format | |
| ISSN | 14639076 |
| e-ISSN | 14639084 |
| Journal | Physical chemistry chemical physics : PCCP |
| Issue Number | 20 |
| Volume Number | 14 |
| Language | English |
| Publisher Date | 2012-01-01 |
| Access Restriction | Open |
| Subject Keyword | Physical and Theoretical Chemistry Physics and Astronomy(all) Research in Higher Education |
| Content Type | Text |
| Resource Type | Article |
| Subject | Physics and Astronomy Physical and Theoretical Chemistry |
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