Why Are DNA and Protein Electron Transfer So Different?

被引:78
作者
Beratan, David N. [1 ,2 ,3 ]
机构
[1] Duke Univ, Dept Chem, Durham, NC 27708 USA
[2] Duke Univ, Dept Phys, Durham, NC 27708 USA
[3] Duke Univ, Dept Biochem, Durham, NC 27710 USA
来源
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 70 | 2019年 / 70卷
关键词
electron transfer; flickering resonance; hopping; polaron; superexchange; PHOTOINDUCED CHARGE-TRANSFER; LONG-RANGE; DISTANCE DEPENDENCE; TRANSFER MECHANISM; MOLECULAR WIRE; BIOLOGICAL MOLECULES; SPIN SELECTIVITY; HOLE-TRANSPORT; TRANSFER RATES; CYTOCHROME-C;
D O I
10.1146/annurev-physchem-042018-052353
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The corpus of electron transfer (ET) theory provides considerable power to describe the kinetics and dynamics of electron flow at the nanoscale. How is it, then, that nucleic acid (NA) ET continues to surprise, while protein-mediated ET is relatively free of mechanistic bombshells? I suggest that this difference originates in the distinct electronic energy landscapes for the two classes of reactions. In proteins, the donor/acceptor-to-bridge energy gap is typically several-fold larger than in NAs. NA ET can access tunneling, hopping, and resonant transport among the bases, and fluctuations can enable switching among mechanisms; protein ET is restricted to tunneling among redox active cofactors and, under strongly oxidizing conditions, a few privileged amino acid side chains. This review aims to provide conceptual unity to DNA and protein ET reaction mechanisms. The establishment of a unified mechanistic framework enabled the successful design of NA experiments that switch electronic coherence effects on and off for ET processes on a length scale of multiple nanometers and promises to provide inroads to directing and detecting charge flow in soft-wet matter.
引用
收藏
页码:71 / 97
页数:27
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