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Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions

Decades after the birth of supramolecular chemistry, there are many techniques to measure noncovalent interactions, such as hydrogen bonding, under equilibrium conditions. As ensembles of molecules rapidly lose coherence, we cannot extrapolate bulk data to single-molecule events under non-equilibriu...

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Autores principales: Naranjo, Teresa, Cerrón, Fernando, Nieto-Ortega, Belén, Latorre, Alfonso, Somoza, Álvaro, Ibarra, Borja, Pérez, Emilio M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5625567/
https://www.ncbi.nlm.nih.gov/pubmed/28989633
http://dx.doi.org/10.1039/c7sc03044d
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author Naranjo, Teresa
Cerrón, Fernando
Nieto-Ortega, Belén
Latorre, Alfonso
Somoza, Álvaro
Ibarra, Borja
Pérez, Emilio M.
author_facet Naranjo, Teresa
Cerrón, Fernando
Nieto-Ortega, Belén
Latorre, Alfonso
Somoza, Álvaro
Ibarra, Borja
Pérez, Emilio M.
author_sort Naranjo, Teresa
collection PubMed
description Decades after the birth of supramolecular chemistry, there are many techniques to measure noncovalent interactions, such as hydrogen bonding, under equilibrium conditions. As ensembles of molecules rapidly lose coherence, we cannot extrapolate bulk data to single-molecule events under non-equilibrium conditions, more relevant to the dynamics of biological systems. We present a new method that exploits the high force resolution of optical tweezers to measure at the single molecule level the mechanical strength of a hydrogen bonded host–guest pair out of equilibrium and under near-physiological conditions. We utilize a DNA reporter to unambiguously isolate single binding events. The Hamilton receptor–cyanuric acid host–guest system is used as a test bed. The force required to dissociate the host–guest system is ∼17 pN and increases with the pulling rate as expected for a system under non-equilibrium conditions. Blocking one of the hydrogen bonding sites results in a significant decrease of the force-to-break by 1–2 pN, pointing out the ability of the method to resolve subtle changes in the mechanical strength of the binding due to the individual H-bonding components. We believe the method will prove to be a versatile tool to address important questions in supramolecular chemistry.
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spelling pubmed-56255672017-10-06 Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions Naranjo, Teresa Cerrón, Fernando Nieto-Ortega, Belén Latorre, Alfonso Somoza, Álvaro Ibarra, Borja Pérez, Emilio M. Chem Sci Chemistry Decades after the birth of supramolecular chemistry, there are many techniques to measure noncovalent interactions, such as hydrogen bonding, under equilibrium conditions. As ensembles of molecules rapidly lose coherence, we cannot extrapolate bulk data to single-molecule events under non-equilibrium conditions, more relevant to the dynamics of biological systems. We present a new method that exploits the high force resolution of optical tweezers to measure at the single molecule level the mechanical strength of a hydrogen bonded host–guest pair out of equilibrium and under near-physiological conditions. We utilize a DNA reporter to unambiguously isolate single binding events. The Hamilton receptor–cyanuric acid host–guest system is used as a test bed. The force required to dissociate the host–guest system is ∼17 pN and increases with the pulling rate as expected for a system under non-equilibrium conditions. Blocking one of the hydrogen bonding sites results in a significant decrease of the force-to-break by 1–2 pN, pointing out the ability of the method to resolve subtle changes in the mechanical strength of the binding due to the individual H-bonding components. We believe the method will prove to be a versatile tool to address important questions in supramolecular chemistry. Royal Society of Chemistry 2017-09-01 2017-07-31 /pmc/articles/PMC5625567/ /pubmed/28989633 http://dx.doi.org/10.1039/c7sc03044d Text en This journal is © The Royal Society of Chemistry 2017 http://creativecommons.org/licenses/by/3.0/ This is an Open Access article distributed under the terms of the Creative Commons Attribution 3.0 Unported License (http://creativecommons.org/licenses/by/3.0/) which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
spellingShingle Chemistry
Naranjo, Teresa
Cerrón, Fernando
Nieto-Ortega, Belén
Latorre, Alfonso
Somoza, Álvaro
Ibarra, Borja
Pérez, Emilio M.
Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
title Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
title_full Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
title_fullStr Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
title_full_unstemmed Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
title_short Mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
title_sort mechanical measurement of hydrogen bonded host–guest systems under non-equilibrium, near-physiological conditions
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5625567/
https://www.ncbi.nlm.nih.gov/pubmed/28989633
http://dx.doi.org/10.1039/c7sc03044d
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