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Range, Magnitude, and Ultrafast Dynamics of Electric Fields at the Hydrated DNA Surface
T. Siebert, , Y. Liu, B.P. Fingerhut, T. Elsaesser
Published in American Chemical Society
PMID: 27468144
Volume: 7
Issue: 16
Pages: 3131 - 3136
Range and magnitude of electric fields at biomolecular interfaces and their fluctuations in a time window down to the subpicosecond regime have remained controversial, calling for electric-field mapping in space and time. Here, we trace fluctuating electric fields at the surface of native salmon DNA via their interactions with backbone vibrations in a wide range of hydration levels by building the water shell layer by layer. Femtosecond two-dimensional infrared spectroscopy and ab initio based theory establish water molecules in the first two layers as the predominant source of interfacial electric fields, which fluctuate on a 300 fs time scale with an amplitude of 25 MV/cm due to thermally excited water motions. The observed subnanometer range of these electric interactions is decisive for biochemical structure and function. © 2016 American Chemical Society.
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Published in American Chemical Society
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