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Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation
Reaction pathways of biochemical processes are influenced by the dissipative electrostatic interaction of the reagents with solvent water molecules. The simulation of these interactions requires a parametrization of the permanent and induced dipole moments. However, the underlying molecular polariza...
Autores principales: | , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2018
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5976729/ https://www.ncbi.nlm.nih.gov/pubmed/29849173 http://dx.doi.org/10.1038/s41467-018-04481-5 |
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author | Zalden, Peter Song, Liwei Wu, Xiaojun Huang, Haoyu Ahr, Frederike Mücke, Oliver D. Reichert, Joscha Thorwart, Michael Mishra, Pankaj Kr. Welsch, Ralph Santra, Robin Kärtner, Franz X. Bressler, Christian |
author_facet | Zalden, Peter Song, Liwei Wu, Xiaojun Huang, Haoyu Ahr, Frederike Mücke, Oliver D. Reichert, Joscha Thorwart, Michael Mishra, Pankaj Kr. Welsch, Ralph Santra, Robin Kärtner, Franz X. Bressler, Christian |
author_sort | Zalden, Peter |
collection | PubMed |
description | Reaction pathways of biochemical processes are influenced by the dissipative electrostatic interaction of the reagents with solvent water molecules. The simulation of these interactions requires a parametrization of the permanent and induced dipole moments. However, the underlying molecular polarizability of water and its dependence on ions are partially unknown. Here, we apply intense terahertz pulses to liquid water, whose oscillations match the timescale of orientational relaxation. Using a combination of terahertz pump / optical probe experiments, molecular dynamics simulations, and a Langevin dynamics model, we demonstrate a transient orientation of their dipole moments, not possible by optical excitation. The resulting birefringence reveals that the polarizability of water is lower along its dipole moment than the average value perpendicular to it. This anisotropy, also observed in heavy water and alcohols, increases with the concentration of sodium iodide dissolved in water. Our results enable a more accurate parametrization and a benchmarking of existing and future water models. |
format | Online Article Text |
id | pubmed-5976729 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2018 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-59767292018-06-01 Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation Zalden, Peter Song, Liwei Wu, Xiaojun Huang, Haoyu Ahr, Frederike Mücke, Oliver D. Reichert, Joscha Thorwart, Michael Mishra, Pankaj Kr. Welsch, Ralph Santra, Robin Kärtner, Franz X. Bressler, Christian Nat Commun Article Reaction pathways of biochemical processes are influenced by the dissipative electrostatic interaction of the reagents with solvent water molecules. The simulation of these interactions requires a parametrization of the permanent and induced dipole moments. However, the underlying molecular polarizability of water and its dependence on ions are partially unknown. Here, we apply intense terahertz pulses to liquid water, whose oscillations match the timescale of orientational relaxation. Using a combination of terahertz pump / optical probe experiments, molecular dynamics simulations, and a Langevin dynamics model, we demonstrate a transient orientation of their dipole moments, not possible by optical excitation. The resulting birefringence reveals that the polarizability of water is lower along its dipole moment than the average value perpendicular to it. This anisotropy, also observed in heavy water and alcohols, increases with the concentration of sodium iodide dissolved in water. Our results enable a more accurate parametrization and a benchmarking of existing and future water models. Nature Publishing Group UK 2018-05-30 /pmc/articles/PMC5976729/ /pubmed/29849173 http://dx.doi.org/10.1038/s41467-018-04481-5 Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
spellingShingle | Article Zalden, Peter Song, Liwei Wu, Xiaojun Huang, Haoyu Ahr, Frederike Mücke, Oliver D. Reichert, Joscha Thorwart, Michael Mishra, Pankaj Kr. Welsch, Ralph Santra, Robin Kärtner, Franz X. Bressler, Christian Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
title | Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
title_full | Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
title_fullStr | Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
title_full_unstemmed | Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
title_short | Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
title_sort | molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5976729/ https://www.ncbi.nlm.nih.gov/pubmed/29849173 http://dx.doi.org/10.1038/s41467-018-04481-5 |
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