Chiral plasmonic fields probe structural order of biointerfaces

Kelly, C., Tullius, R., Lapthorn, A. J. , Gadegaard, N. , Cooke, G. , Barron, L. D., Karimullah, A. S. , Rotello, V. M. and Kadodwala, M. (2018) Chiral plasmonic fields probe structural order of biointerfaces. Journal of the American Chemical Society, 140(27), pp. 8509-8517. (doi:10.1021/jacs.8b03634) (PMID:29909628)

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Abstract

The structural order of biopolymers, such as proteins, at interfaces defines the physical and chemical interactions of biological systems with their surroundings and is hence a critical parameter in a range of biological problems. Known spectroscopic methods for routine rapid monitoring of structural order in biolayers are generally only applied to model single-component systems that possess a spectral fingerprint which is highly sensitive to orientation. This spectroscopic behavior is not a generic property and may require the addition of a label. Importantly, such techniques cannot readily be applied to real multicomponent biolayers, have ill-defined or unknown compositions, and have complex spectroscopic signatures with many overlapping bands. Here, we demonstrate the sensitivity of plasmonic fields with enhanced chirality, a property referred to as superchirality, to global orientational order within both simple model and “real” complex protein layers. The sensitivity to structural order is derived from the capability of superchiral fields to detect the anisotropic nature of electric dipole–magnetic dipole response of the layer; this is validated by numerical simulations. As a model study, the evolution of orientational order with increasing surface density in layers of the antibody immunoglobulin G was monitored. As an exemplar of greater complexity, superchiral fields are demonstrated, without knowledge of exact composition, to be able to monitor how qualitative changes in composition alter the structural order of protein layers formed from blood serum, thereby establishing the efficacy of the phenomenon as a tool for studying complex biological interfaces.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Barron, Professor Laurence and Lapthorn, Dr Adrian and TULLIUS, Ryan and Gadegaard, Professor Nikolaj and Kadodwala, Professor Malcolm and Karimullah, Dr Affar and Cooke, Professor Graeme
Authors: Kelly, C., Tullius, R., Lapthorn, A. J., Gadegaard, N., Cooke, G., Barron, L. D., Karimullah, A. S., Rotello, V. M., and Kadodwala, M.
College/School:College of Science and Engineering > School of Chemistry
College of Science and Engineering > School of Engineering > Biomedical Engineering
Journal Name:Journal of the American Chemical Society
Publisher:American Chemical Society
ISSN:0002-7863
ISSN (Online):1520-5126
Published Online:18 June 2018
Copyright Holders:Copyright © 2018 American Chemical Society
First Published:First published in Journal of the American Chemical Society 140(27): 8509-8517
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
618701Plasmon-Enhanced Chiroptical SensorsMalcolm KadodwalaEngineering and Physical Sciences Research Council (EPSRC)EP/K034936/1CHEM - CHEMISTRY
726421Mapping the mesoscale structural landscape using "sculpted" chiral plasmonic fieldsMalcolm KadodwalaEngineering and Physical Sciences Research Council (EPSRC)EP/P00086X/1CHEM - CHEMISTRY
3024060High-Throughput Diagnostics with Chiral Plasmonic AssaysAffar KarimullahEngineering and Physical Sciences Research Council (EPSRC)EP/S001514/1Chemistry
683531Consortium for advanced materials based on spin chiralityRobert StampsEngineering and Physical Sciences Research Council (EPSRC)EP/M024423/1S&E P&A - PHYSICS & ASTRONOMY