Observation of coherent delocalized phonon-like modes in DNA under physiological conditions

Underdamped terahertz-frequency delocalized phonon-like modes have long been suggested to play a role in the biological function of DNA. Such phonon modes involve the collective motion of many atoms and are prerequisite to understanding the molecular nature of macroscopic conformational changes and...

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Main Authors: González-Jiménez, Mario, Ramakrishnan, Gopakumar, Harwood, Thomas, Lapthorn, Adrian J., Kelly, Sharon M., Ellis, Elizabeth M., Wynne, Klaas
Format: Online
Language:English
Published: Nature Publishing Group 2016
Online Access:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4895446/
id pubmed-4895446
recordtype oai_dc
spelling pubmed-48954462016-06-21 Observation of coherent delocalized phonon-like modes in DNA under physiological conditions González-Jiménez, Mario Ramakrishnan, Gopakumar Harwood, Thomas Lapthorn, Adrian J. Kelly, Sharon M. Ellis, Elizabeth M. Wynne, Klaas Article Underdamped terahertz-frequency delocalized phonon-like modes have long been suggested to play a role in the biological function of DNA. Such phonon modes involve the collective motion of many atoms and are prerequisite to understanding the molecular nature of macroscopic conformational changes and related biochemical phenomena. Initial predictions were based on simple theoretical models of DNA. However, such models do not take into account strong interactions with the surrounding water, which is likely to cause phonon modes to be heavily damped and localized. Here we apply state-of-the-art femtosecond optical Kerr effect spectroscopy, which is currently the only technique capable of taking low-frequency (GHz to THz) vibrational spectra in solution. We are able to demonstrate that phonon modes involving the hydrogen bond network between the strands exist in DNA at physiologically relevant conditions. In addition, the dynamics of the solvating water molecules is slowed down by about a factor of 20 compared with the bulk. Nature Publishing Group 2016-06-01 /pmc/articles/PMC4895446/ /pubmed/27248361 http://dx.doi.org/10.1038/ncomms11799 Text en Copyright © 2016, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
repository_type Open Access Journal
institution_category Foreign Institution
institution US National Center for Biotechnology Information
building NCBI PubMed
collection Online Access
language English
format Online
author González-Jiménez, Mario
Ramakrishnan, Gopakumar
Harwood, Thomas
Lapthorn, Adrian J.
Kelly, Sharon M.
Ellis, Elizabeth M.
Wynne, Klaas
spellingShingle González-Jiménez, Mario
Ramakrishnan, Gopakumar
Harwood, Thomas
Lapthorn, Adrian J.
Kelly, Sharon M.
Ellis, Elizabeth M.
Wynne, Klaas
Observation of coherent delocalized phonon-like modes in DNA under physiological conditions
author_facet González-Jiménez, Mario
Ramakrishnan, Gopakumar
Harwood, Thomas
Lapthorn, Adrian J.
Kelly, Sharon M.
Ellis, Elizabeth M.
Wynne, Klaas
author_sort González-Jiménez, Mario
title Observation of coherent delocalized phonon-like modes in DNA under physiological conditions
title_short Observation of coherent delocalized phonon-like modes in DNA under physiological conditions
title_full Observation of coherent delocalized phonon-like modes in DNA under physiological conditions
title_fullStr Observation of coherent delocalized phonon-like modes in DNA under physiological conditions
title_full_unstemmed Observation of coherent delocalized phonon-like modes in DNA under physiological conditions
title_sort observation of coherent delocalized phonon-like modes in dna under physiological conditions
description Underdamped terahertz-frequency delocalized phonon-like modes have long been suggested to play a role in the biological function of DNA. Such phonon modes involve the collective motion of many atoms and are prerequisite to understanding the molecular nature of macroscopic conformational changes and related biochemical phenomena. Initial predictions were based on simple theoretical models of DNA. However, such models do not take into account strong interactions with the surrounding water, which is likely to cause phonon modes to be heavily damped and localized. Here we apply state-of-the-art femtosecond optical Kerr effect spectroscopy, which is currently the only technique capable of taking low-frequency (GHz to THz) vibrational spectra in solution. We are able to demonstrate that phonon modes involving the hydrogen bond network between the strands exist in DNA at physiologically relevant conditions. In addition, the dynamics of the solvating water molecules is slowed down by about a factor of 20 compared with the bulk.
publisher Nature Publishing Group
publishDate 2016
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4895446/
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