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  Tether-Length Dependence of Bias in Equilibrium Free-Energy Estimates for Surface-to-Molecule Unbinding Experiments

Ostertag, L. M., Utzig, T., Klinger, C., & Valtiner, M. (2018). Tether-Length Dependence of Bias in Equilibrium Free-Energy Estimates for Surface-to-Molecule Unbinding Experiments. Langmuir, 34(3), 766-772. doi:10.1021/acs.langmuir.7b02844.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0001-5D73-6 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-5D74-5
Genre: Journal Article

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 Creators:
Ostertag, Laila Moreno1, Author              
Utzig, Thomas1, Author              
Klinger, Christine2, Author              
Valtiner, Markus1, 3, Author              
Affiliations:
1Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society, ou_1863357              
2Institut für Physikalische Chemie II, TU Bergakademie Freiberg, 09599 Freiberg, Germany, persistent22              
3Institute of Applied Synthetic Chemistry, Vienna University of Technology, Getreidemarkt 9/163-AC, A-1060 Vienna, Austria, ou_persistent22              

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Free keywords: ATOMIC-FORCE MICROSCOPY; SPACE OVERLAP MEASURES; SINGLE-MOLECULE; NONEQUILIBRIUM MEASUREMENTS; PERTURBATION CALCULATIONS; FLUCTUATION THEOREMS; SPECTROSCOPY; ADHESION; SCALE; SIMULATIONChemistry; Materials Science;
 Abstract: The capabilities of atomic force microscopes and optical tweezers to probe unfolding or surface-to-molecule bond rupture at a single-molecular level are widely appreciated. These measurements are typically carried out unidirectionally under nonequilibrium conditions. Jarzynski's equality has proven useful to relate the work obtained along these nonequilibrium trajectories to the underlying free energy of the unfolding or unbinding process. Here, we quantify biases that arise from the molecular design of the bond rupture experiment for probing surface-to-molecule bonds. In particular, we probe the well-studied amine/gold bond as a function of the linker's length which is used to anchor the specific amine functionality during a single molecule unbinding experiment. With increasing linker length, we observe a significant increase in the average work spent on polymer stretching and a strongly biased estimated interaction free energy. Our data demonstrate that free energy estimates converge well for linker lengths below 20 nm, where the bias is <10-15%. With longer linkers severe methodical limits of the method are reached, and convergence within a reasonable number of realizations of the bond rupture is not feasible. Our results also provide new insights into stability and work dissipation mechanisms at adhesive interfaces at the single-molecular level, and offer important design and analysis aspects for single-molecular surface-to-molecule experiments.

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Language(s): eng - English
 Dates: 2017-10-312018-01-23
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Degree: -

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Title: Langmuir
Source Genre: Journal
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Publ. Info: Columbus, OH : American Chemical Society
Pages: - Volume / Issue: 34 (3) Sequence Number: - Start / End Page: 766 - 772 Identifier: ISSN: 0743-7463
CoNE: https://pure.mpg.de/cone/journals/resource/954925541194