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Deciphering the scaling of single-molecule interactions using Jarzynski's equality

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Raman,  Sangeetha
Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Utzig,  Thomas
Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Baimpos,  Theodoros
Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Shrestha,  Buddha Ratna
Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Valtiner,  Markus
Interaction Forces and Functional Materials, Interface Chemistry and Surface Engineering, Max-Planck-Institut für Eisenforschung GmbH, Max Planck Society;

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Citation

Raman, S., Utzig, T., Baimpos, T., Shrestha, B. R., & Valtiner, M. (2014). Deciphering the scaling of single-molecule interactions using Jarzynski's equality. Nature Communications, 5: 5539. doi:10.1038/ncomms6539.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0025-02E6-0
Abstract
Unravelling the complexity of the macroscopic world relies on understanding the scaling of single-molecule interactions towards integral macroscopic interactions. Here, we demonstrate the scaling of single acid-amine interactions through a synergistic experimental approach combining macroscopic surface forces apparatus experiments and single-molecule force spectroscopy. This experimental framework is ideal for testing the well-renowned Jarzynski's equality, which relates work performed under non-equilibrium conditions with equilibrium free energy. Macroscopic equilibrium measurements scale linearly with the number density of interfacial bonds, providing acid-amine interaction energies of 10.9 +/- 0.2 kT. Irrespective of how far from equilibrium single-molecule experiments are performed, the Jarzynski's free energy converges to 11 +/- 1 kT. Our results validate the applicability of Jarzynski's equality to unravel the scaling of non-equilibrium single-molecule experiments to scenarios where large numbers of molecules interacts simultaneously in equilibrium. The developed scaling strategy predicts large-scale properties such as adhesion or cell-cell interactions on the basis of single-molecule measurements.