Ultrafast vibrational dynamics of the DNA backbone at different hydration levels mapped by two-dimensional infrared spectroscopy
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TLDR
Two-dimensional infrared spectroscopy of DNA backbone modes between 920 and 1120 cm−1 maps fluctuating interactions at the DNA surface to reveal a significant contribution of water to the fluctuating forces.Abstract:
DNA oligomers are studied at 0% and 92% relative humidity, corresponding to N 20 water molecules per base pair. Two-dimensional (2D) infrared spectroscopy of DNA backbone modes between 920 and 1120 cm−1 maps fluctuating interactions at the DNA surface. At both hydration levels, a frequency fluctuation correlation function with a 300 fs decay and a slow decay beyond 10 ps is derived from the 2D lineshapes. The fast component reflects motions of DNA helix, counterions, and water shell. Its higher amplitude at high hydration level reveals a significant contribution of water to the fluctuating forces. The slow component reflects disorder-induced inhomogeneous broadening.read more
Citations
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Water Dynamics in the Hydration Shells of Biomolecules
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Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy
TL;DR: Some of the basic principles behind 2D IR and how they have, and can, impact the field of protein biophysics are presented and technological developments in 2DIR are highlighted that continue to expand the scope of scientific problems that can be accessed in the biomedical sciences.
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DNA’s Chiral Spine of Hydration
TL;DR: Here, chiral nonlinear vibrational spectroscopy of two DNA sequences shows that not only do such structural water molecules exist in solution at ambient conditions but that they form a chiral superstructure: aChiral spine of hydration, the first observation of a Chiral water superstructure templated by a biomolecule.
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Range, Magnitude, and Ultrafast Dynamics of Electric Fields at the Hydrated DNA Surface
TL;DR: It is shown that 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 are decisive for biochemical structure and function.
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Multiple Decay Mechanisms and 2D-UV Spectroscopic Fingerprints of Singlet Excited Solvated Adenine-Uracil Monophosphate.
Quansong Li,Angelo Giussani,Javier Segarra-Martí,Artur Nenov,Ivan Rivalta,Alexander A. Voityuk,Shaul Mukamel,Daniel Roca-Sanjuán,Marco Garavelli,Marco Garavelli,Lluís Blancafort +10 more
TL;DR: The results reveal the complexity of the photophysics of the relatively small ApU system, and the potential of 2D‐UV spectroscopy to disentangle the photrophysics of multichromophoric systems.
References
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