title: Range, Magnitude, and Ultrafast Dynamics of Electric Fields at the Hydrated DNA Surface.
abstract: 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.
authors.affiliation: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie , D-12489 Berlin, Germany.
authors.forename: Torsten
authors.initials: T
authors.lastname: Siebert
authors.affiliation: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie , D-12489 Berlin, Germany.
authors.forename: Biswajit
authors.initials: B
authors.lastname: Guchhait
authors.affiliation: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie , D-12489 Berlin, Germany.
authors.forename: Yingliang
authors.initials: Y
authors.lastname: Liu
authors.affiliation: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie , D-12489 Berlin, Germany.
authors.forename: Benjamin P
authors.initials: BP
authors.lastname: Fingerhut
authors.affiliation: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie , D-12489 Berlin, Germany.
authors.forename: Thomas
authors.initials: T
authors.lastname: Elsaesser
mesh_terms: D004247:DNA / Q000737:chemistry*; D004560:Electricity; D004574:Electromagnetic Fields; D006860:Hydrogen Bonding; D056004:Molecular Dynamics Simulation; D014732:Vibration; D014867:Water / Q000737:chemistry
chemical_list: D014867:Water; D004247:DNA