title: Deciphering the scaling of single-molecule interactions using Jarzynski's equality.
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.
authors.affiliation: Department of Interface Chemistry and Surface Engineering, Max-Planck Institut für Eisenforschung GmbH, Max-Planck-Straße 1, D-40237 Düsseldorf, Germany.
authors.forename: Sangeetha
authors.initials: S
authors.lastname: Raman
authors.affiliation: Department of Interface Chemistry and Surface Engineering, Max-Planck Institut für Eisenforschung GmbH, Max-Planck-Straße 1, D-40237 Düsseldorf, Germany.
authors.forename: Thomas
authors.initials: T
authors.lastname: Utzig
authors.affiliation: Department of Interface Chemistry and Surface Engineering, Max-Planck Institut für Eisenforschung GmbH, Max-Planck-Straße 1, D-40237 Düsseldorf, Germany.
authors.forename: Theodoros
authors.initials: T
authors.lastname: Baimpos
authors.affiliation: Department of Interface Chemistry and Surface Engineering, Max-Planck Institut für Eisenforschung GmbH, Max-Planck-Straße 1, D-40237 Düsseldorf, Germany.
authors.forename: Buddha
authors.initials: B
authors.lastname: Ratna Shrestha
authors.affiliation: Department of Interface Chemistry and Surface Engineering, Max-Planck Institut für Eisenforschung GmbH, Max-Planck-Straße 1, D-40237 Düsseldorf, Germany.
authors.forename: Markus
authors.initials: M
authors.lastname: Valtiner
mesh_terms: D000143:Acids / Q000378:metabolism; D000588:Amines / Q000378:metabolism; D002448:Cell Adhesion / Q000502:physiology*; D002450:Cell Communication; D002462:Cell Membrane / Q000502:physiology*; D004735:Energy Transfer; D008051:Lipid Bilayers / Q000378:metabolism; D018625:Microscopy, Atomic Force; D036103:Nanotechnology; D013054:Spectrophotometry, Atomic; D013816:Thermodynamics
chemical_list: D000143:Acids; D000588:Amines; D008051:Lipid Bilayers