Ballistic Brownian Motion of Nanoconfined DNA

被引:5
作者
Madrid, Ignacio [1 ]
Zheng, Zhiyong [2 ]
Gerbelot, Cedric [3 ]
Fujiwara, Akira [3 ]
Li, Shuo [1 ]
Grall, Simon [1 ]
Nishiguchi, Katsuhiko [3 ]
Kim, Soo Hyeon [1 ]
Chovin, Arnaud [2 ]
Demaille, Christophe [2 ]
Clement, Nicolas [1 ,3 ]
机构
[1] Univ Tokyo, IIS, LIMMS, CNRS,IIS UMI2820, Meguro Ku, Tokyo 1538505, Japan
[2] Univ Paris Cite, Lab Electrochim Mol, CNRS, UMR 7591, F-75205 Paris, France
[3] NTT Corp, NTT Basic Res Labs, Atsugi, 2430198, Japan
关键词
DNA; Brownian motion; ballistic motion; nanoconfinement; molecular dynamics; nanoelectrochemistry; nanogap; ELECTRON-TRANSPORT; MOLECULAR DIODES; DIFFUSION-MODEL; DYNAMICS; MICROSCOPY; SURFACES; CHAINS;
D O I
10.1021/acsnano.3c04349
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Theoretical treatments of polymer dynamics in liquid generally start with the basic assumption that motion at the smallest scale is heavily overdamped; therefore, inertia can be neglected. We report on the Brownian motion of tethered DNA under nanoconfinement, which was analyzed by molecular dynamics simulation and nanoelectrochemistry-based single-electron shuttle experiments. Our results show a transition into the ballistic Brownian motion regime for short DNA in sub-5 nm gaps, with quality coefficients as high as 2 for double-stranded DNA, an effect mainly attributed to a drastic increase in stiffness. The possibility for DNA to enter the underdamped regime could have profound implications on our understanding of the energetics of biomolecular engines such as the replication machinery, which operates in nanocavities that are a few nanometers wide.
引用
收藏
页码:17031 / 17040
页数:10
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