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Abstract
State-of-the-art ultra-sensitive blood glucose-monitoring biosensors, based on glucose oxidase (GOx) covalently linked to a single layer graphene (SLG), will be a valuable next generation diagnostic tool for personal glycemic level management. We report here our observations of sensor matrix structure obtained using a multi-physics approach towards analysis of small-angle neutron scattering (SANS) on graphene-based biosensor functionalized with GOx under different pH conditions for various hierarchical GOx assemblies within SLG. We developed a methodology to separately extract the average shape of GOx molecules within the hierarchical assemblies. The modeling is able to resolve differences in the average GOx dimer structure and shows that treatment under different pH conditions lead to differences within the GOx at the dimer contact region with SLG. The coupling of different analysis methods and modeling approaches we developed in this study provides a universal approach to obtain detailed structural quantifications, for establishing robust structure-property relationships. This is an essential step to obtain an insight into the structure and function of the GOx-SLG interface for optimizing sensor performance.
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1 Cornell High Energy Synchrotron Source, Cornell University, Ithaca, New York, USA
2 Institute for Cell and Molecular Biosciences, Newcastle University, Newcastle upon Tyne-NE1 7RU, UK
3 Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee, USA
4 Department of Bioengineering, University of California, Berkeley, Berkeley, California, USA
5 Department of Mechanical Engineering and Materials Science, Rice University, Houston, Texas, USA
6 Center for Life Sciences, Boston Children’s Hospital, Harvard Medical School, Boston, Massachusetts, USA
7 Tata Institute of Fundamental Research – Center for Interdisciplinary Sciences, Hyderabad, India
8 Department of Computational and Data Sciences, Indian Institute of Science, Bangalore, India
9 Universidade da Coruña, Grupo EXPRELA, F. Ciencias & Centro de Investigacións Científicas Avanzadas (CICA) & Instituto de Investigación Biomédica A Coruña (INIBIC), A Coruña, Spain
10 Newton Wellesley Hospital/Partners Healthcare System, Newton, Massachusetts, USA
11 Cellular Pathway Imaging Laboratory (CPIL), Dept. of Radiology, Stanford University School of Medicine, 3155 Porter Drive, Suite 2236, Palo Alto, California, USA
12 Center for Life Sciences, Boston Children’s Hospital, Harvard Medical School, Boston, Massachusetts, USA; Department of Chemistry and Chemical Biology, Northeastern University, Boston, Massachusetts, USA