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There appear to be some differences in the probabilities for observing multiple force quanta, for example, for 3 (Figure 3B), which may arise from: (i) differences in solubilities and adsorptivities of the guest thiols leading to different guest-mercaptoethanol ratios on the tip than present in solution, (ii) different degrees of clustering of guests on the tip, rendering some guest molecules inaccessible for binding, and (iii) variations in tip geometry and tip-surface contact areas.
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53
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The data in the histograms were treated as described in refs 24 and 25.
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Noise levels were ∼15 pN. Plots of peak position from the histograms versus peak number yielded straight lines, with the force quantum as the slope (see also ref 25).
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The measured pull-off forces did not vary for nominal spacings of the data points between 1 and 10 A.
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61
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out-of-contact to the energy difference between the two minima, eliminating the need for the numerical integration (see the Supporting Information). Here, the interaction potential at the well of the "contact" minimum is also fitted to a harmonic potential. This analysis shows that the probability distribution depends only marginally on the "stiffness" of the complex (which governs the harmonic interaction potential and which is directly related to the well width s).
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62
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