Abstract

The abundance of hotspots tuned via precise arrangement of coupled plasmonic nanostructures highly boost the surface-enhanced Raman scattering (SERS) signal enhancements, expanding their potential applicability to a diverse range of applications. Herein, nanoscale assembly of Ag coated Au nanostars in dimer and trimer configurations with tunable nanogap was achieved using programmable DNA origami technique. The resulting assemblies were then utilized for SERS-based ultra-sensitive detection of an important neurotransmitter, dopamine. The trimer assemblies were able to detect dopamine with picomolar sensitivity, and the assembled dimer structures achieved SERS sensitivity as low as 1 fM with a limit of detection of 0.225 fM. Overall, such coupled nanoarchitectures with superior plasmon tunability are promising to explore new avenues in biomedical diagnostic applications.

Highlights

  • Detection of alterations in the level of key neuromodulators in our body is of central importance for identification of most neurodegenerative disorders, such as Parkinson’s disease (Lotharius and Brundin, 2002), Alzheimer’s disease (Henstridge et al, 2019), schizophrenia (Breier et al, 1997), and Huntington’s disease (Chen et al, 2013)

  • L-DOPA was procured from SRL, and tyramine was purchased from TCI Chemicals. 1× TE buffer was purchased from Integrated DNA technologies (IDT) and 50× TAE buffer solution was procured from Himedia and used without further purification

  • We explored if the surface-enhanced Raman scattering (SERS) peaks correspond to the dopamine molecule only by recording the reference spectrum of dopamine solution with 50-nm Au nanoparticles deposited on Si substrate

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Summary

Introduction

Detection of alterations in the level of key neuromodulators in our body is of central importance for identification of most neurodegenerative disorders, such as Parkinson’s disease (Lotharius and Brundin, 2002), Alzheimer’s disease (Henstridge et al, 2019), schizophrenia (Breier et al, 1997), and Huntington’s disease (Chen et al, 2013). A significant catecholamine neurotransmitter is responsible for the control and regulation of various brain functions in mammals (Beninger, 1983; Klein et al, 2019). Imbalances in dopamine level is a diagnostic indicator to neural dysfunctions that can aid in monitoring and control of many neurological diseases. Progress in sensitive detection of dopamine is reported in some methods (Sansuk et al, 2013; Ban et al, 2015; Talemi et al, 2017), these methods still pose a significant challenge in their potential practical applicability due to time-consuming, complicated sample preparation techniques, and limited accuracy (Pradhan et al, 2014; Tang et al, 2015). Development of highly sensitive detection techniques is required to design low-cost diagnostic platforms for dopamine detection

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