Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 16, Pages 3131-3136Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b01369
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- DFG within the Emmy Noether Programme [Fl 2034/1-1]
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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.
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