Glucose Sensing Using Surface-Enhanced Raman-Mode Constraining
Abstract
Diabetes mellitus is a chronic disease, and its management focuses on monitoring and lowering a patient's glucose level to prevent further complications. By tracking the glucose-induced shift in the surface-enhanced Raman-scattering (SERS) emission of mercaptophenylboronic acid (MPBA), we have demonstrated fast and continuous glucose sensing in the physiologically relevant range from 0.1 to 30 mM and verified the underlying mechanism using numerical simulations. Bonding of glucose to MPBA suppresses the "breathing" mode of MPBA at 1071 cm^(–1) and energizes the constrained-bending mode at 1084 cm^(–1), causing the dominant peak to shift from 1071 to 1084 cm^(–1). MPBA–glucose bonding is also reversible, allowing continuous tracking of ambient glucose concentrations, and the MPBA-coated substrates showed very stable performance over a 30 day period, making the approach promising for long-term continuous glucose monitoring. Using Raman-mode-constrained, miniaturized SERS implants, we also successfully demonstrated intraocular glucose measurements in six ex vivo rabbit eyes within ±0.5 mM of readings obtained using a commercial glucose sensor.
Additional Information
© 2018 American Chemical Society. Received: July 31, 2018; Accepted: October 28, 2018; Published: October 29, 2018. The authors thank Dr. Robert Grubbs (Department of Chemistry, California Institute of Technology) and Dr. Massimo Olivucci (Department of Chemistry, Bowling Green State University) for helpful discussions on boronic acid and computational modeling with solvents, respectively. The research was funded by a Samsung Grand Research Opportunity and the Heritage Medical Research Institute Inaugural Principle Investigator Program. Computational resources were provided by the Texas Advanced Computer Center (XSEDE Program) and the Ohio Supercomputer Center (OSC). Author Contributions: D.Y., J.O.L., and H. Choo conceived the study. D.Y. performed most of sample fabrication, experiments, and data processing under the supervision of H. Choo. S.A. conducted DFT simulations to identify the mode-shifting mechanism under the supervision of A.T.Z. J.O.L., H. Cho, and S.K. contributed at various stages during sample fabrication and measurements. R.H.S. contributed to the optical simulation and spectroscopy of the SERS substrates. S.K., V. N., and Y.-Z.Y. contributed to data-processing-algorithm development. D.Y. and H. Choo wrote the manuscript with S.A. and A.T.Z. and with a significant contribution from S.K. J.O.L., H. Cho., and Y.-Z.Y. also assisted with manuscript preparation. All authors discussed the results and commented on the manuscript. The authors declare no competing financial interest.Attached Files
Supplemental Material - ac8b03420_si_001.pdf
Supplemental Material - ac8b03420_si_002.avi
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Additional details
- Eprint ID
- 90455
- DOI
- 10.1021/acs.analchem.8b03420
- Resolver ID
- CaltechAUTHORS:20181029-094838503
- Samsung Grand Research Opportunity
- Heritage Medical Research Institute
- Created
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2018-10-29Created from EPrint's datestamp field
- Updated
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2021-11-16Created from EPrint's last_modified field
- Caltech groups
- Heritage Medical Research Institute