ArticleJournal of the American Chemical Society2012
Entropic and electrostatic effects on the folding free energy of a surface-attached biomolecule: an experimental and theoretical study.
Article in Journal of the American Chemical Society, 2012. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 16 papers.
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Who cites it
16 citing papers in PubMed, 52 citations in OpenAlex.
- Cyclooctyne-Functionalized N-Heterocyclic Carbenes for Click Coupling of Sensing Oligonucleotides to Gold Surfaces.ACS sensors · 2025Article
- Using Spectroscopy to Guide the Adaptation of Aptamers into Electrochemical Aptamer-Based Sensors.Bioconjugate chemistry · 2023Article
- Interplay of Affinity and Surface Tethering in Protein Recognition.The journal of physical chemistry letters · 2022Article
- Ultrasensitive DNA-Biomacromolecule Sensor for the Detection Application of Clinical Cancer Samples.Advanced science (Weinheim, Baden-Wurttemberg, Germany) · 2022Article
- The effect of charged residue substitutions on the thermodynamics of protein-surface interactions.Protein science : a publication of the Protein Society · 2021Article
- Elucidating the Mechanisms Underlying the Signal Drift of Electrochemical Aptamer-Based Sensors in Whole Blood.ACS sensors · 2021Article
- Programming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework.Nature communications · 2020Article
- Seconds-resolved pharmacokinetic measurements of the chemotherapeutic irinotecanChemical science · 2019Article
- Surface Attachment Enhances the Thermodynamic Stability of Protein L.Angewandte Chemie (International ed. in English) · 2019Article
- Experimental Measurement of Surface Charge Effects on the Stability of a Surface-Bound Biopolymer.Langmuir : the ACS journal of surfaces and colloids · 2018Article
- Quantitative measurements of protein-surface interaction thermodynamics.Proceedings of the National Academy of Sciences of the United States of America · 2018Article
- 3D single-molecule tracking enables direct hybridization kinetics measurement in solution.Nanoscale · 2017Article
- Activity modulation and allosteric control of a scaffolded DNAzyme using a dynamic DNA nanostructure.Chemical science · 2016Article
- Effects of crowding on the stability of a surface-tethered biopolymer: an experimental study of folding in a highly crowded regime.Journal of the American Chemical Society · 2014Article
- DNA hairpin stabilization on a hydrophobic surface.Small (Weinheim an der Bergstrasse, Germany) · 2013Article
- Bioelectrochemical switches for the quantitative detection of antibodies directly in whole blood.Journal of the American Chemical Society · 2012Article
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Authors and funding
5 authors at 1 institution in 1 country.
Funding
Abstract
Surface-tethered biomolecules play key roles in many biological processes and biotechnologies. However, while the physical consequences of such surface attachment have seen significant theoretical study, to date this issue has seen relatively little experimental investigation. In response we present here a quantitative experimental and theoretical study of the extent to which attachment to a charged-but otherwise apparently inert-surface alters the folding free energy of a simple biomolecule. Specifically, we have measured the folding free energy of a DNA stem loop both in solution and when site-specifically attached to a negatively charged, hydroxylalkane-coated gold surface. We find that whereas surface attachment is destabilizing at low ionic strength, it becomes stabilizing at ionic strengths above ~130 mM. This behavior presumably reflects two competing mechanisms: excluded volume effects, which stabilize the folded conformation by reducing the entropy of the unfolded state, and electrostatics, which, at lower ionic strengths, destabilizes the more compact folded state via repulsion from the negatively charged surface. To test this hypothesis, we have employed existing theories of the electrostatics of surface-bound polyelectrolytes and the entropy of surface-bound polymers to model both effects. Despite lacking any fitted parameters, these theoretical models quantitatively fit our experimental results, suggesting that, for this system, current knowledge of both surface electrostatics and excluded volume effects is reasonably complete and accurate.
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Registered trials
Read under generation 80e0d062 · epoch 390. Bibliography from PubMed, PubMed Central and OpenAlex; grants from NIH RePORTER; trial links from ClinicalTrials.gov; estimates, votes and beliefs from the OpenQuestion graph.