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Non-Markov bond model for dynamic force spectroscopy.

Jakob Tómas Bullerjahn1, Sebastian Sturm1, Klaus Kroy1

  • 1Universität Leipzig, Institut für Theoretische Physik, Postfach 100 920, 04009 Leipzig, Germany.

The Journal of Chemical Physics
|February 17, 2020
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Summary
This summary is machine-generated.

This study reveals that "hidden modes" in molecular dynamics explain anomalous bond-breaking kinetics in force spectroscopy. The new theory accurately predicts experimental results, especially at high loading rates.

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Area of Science:

  • Chemical Physics
  • Biophysics
  • Materials Science

Background:

  • Conventional single-molecule force spectroscopy analysis uses a simplified 1D model.
  • This model fails to explain anomalous bond-breaking kinetics like non-exponential bond lifetime distributions.

Purpose of the Study:

  • To develop a more rigorous theoretical framework for analyzing single-molecule force spectroscopy data.
  • To explain the origins of anomalous bond-breaking kinetics observed experimentally and in simulations.

Main Methods:

  • Extended the 1D diffusion model to include transient dynamics of coupled degrees of freedom ('hidden modes').
  • Derived exact analytical expressions for key observables in two asymptotic limits.
  • Investigated the influence of hidden mode relaxation spectra and loading protocols.

Main Results:

  • Anomalous kinetics, including apparent static and dynamic disorder, arise naturally from hidden mode dynamics.
  • Exact analytical solutions were found for mean rupture force and rupture-force distribution in specific limits.
  • The theory accurately describes rapid force spectroscopy, bypassing the Markov assumption.

Conclusions:

  • The extended theory provides a microscopically consistent explanation for complex bond-breaking behaviors.
  • The findings offer a more accurate analytical tool for interpreting single-molecule force spectroscopy experiments.
  • The developed framework is particularly powerful for analyzing high loading rate regimes.