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Effects of Multiple-Bond Ruptures in Force Spectroscopy Measurements of Interactions between Fullerene C_(60) Molecules in Water

Gu, Chao and Kirkpatrick, Andrea and Ray, Chad and Guo, Senli and Akhremitchev, Boris B. (2008) Effects of Multiple-Bond Ruptures in Force Spectroscopy Measurements of Interactions between Fullerene C_(60) Molecules in Water. Journal of Physical Chemistry C, 112 (13). pp. 5085-5092. ISSN 1932-7447. https://resolver.caltech.edu/CaltechAUTHORS:20170419-085108756

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Abstract

Interactions between fullerene C_(60) molecules in water were measured by force spectroscopy. Fullerene molecules were covalently connected to bifunctional water-soluble poly(ethylene glycol) (PEG) linkers and subsequently tethered to the substrate and to the tip of the atomic force microscope to facilitate single molecule detection and avoid spurious surface effects. The distributions of rupture forces for substrates prepared with different incubation times of C_(60)-PEG-NH_2 exhibit high rupture forces that cannot be explained by the theoretical distribution of single molecule binding. Moreover, the relative amplitude of the high force peak in the histogram increases with incubation time. These observations are explained by attributing the measured high forces to the rupture of multiple bonds between fullerene molecules. Force spectroscopy data analysis based on the most probable forces gives significantly different dissociation rates for samples that exhibit different amplitudes of the high force peak. An approximate analytical model that considers ruptures of two bonds that are simultaneously loaded by tethers with different lengths is proposed. This model successfully fits the distributions of the rupture forces using the same set of kinetic parameters for samples prepared with different grafting densities. It is proposed that this model can be used as a common tool to analyze the probability distributions of rupture forces that contain peaks or shoulders on the high force side of the distribution.


Item Type:Article
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http://dx.doi.org/10.1021/jp709593cDOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp709593cPublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/jp709593cPublisherSupporting Information
Additional Information:© 2008 American Chemical Society. Received: October 1, 2007; In Final Form: January 18, 2008. Publication Date (Web): March 12, 2008. The authors thank Duke University and National Science Foundation (Grant CHE-0719043) for financial support.
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Funding AgencyGrant Number
Duke UniversityUNSPECIFIED
NSFCHE-0719043
Issue or Number:13
Record Number:CaltechAUTHORS:20170419-085108756
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170419-085108756
Official Citation:Effects of Multiple-Bond Ruptures in Force Spectroscopy Measurements of Interactions between Fullerene C60 Molecules in Water Chao Gu, Andrea Kirkpatrick, Chad Ray, Senli Guo, and Boris B. Akhremitchev The Journal of Physical Chemistry C 2008 112 (13), 5085-5092 DOI: 10.1021/jp709593c
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:76659
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:19 Apr 2017 16:37
Last Modified:03 Oct 2019 17:03

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