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Abstract
Combined theoretical and experimental analysis of serotonin by quantum chemical density functional calculations and surface-enhanced Raman spectroscopy, respectively, is presented in this work to better understand phenomena related to this neurotransmitter’s detection and monitoring at very low concentrations specific to physiological levels. In addition to the successful ultrasensitive analyte detection on silver nanoparticles for concentrations as low as 10−11 molar, the relatively good agreement between the simulated and experimentally determined results indicates the presence of all serotonin molecular forms, such as neutral, ionic, and those oxidized through redox reactions. Obvious structural molecular deformations such as bending of lateral amino chains are observed for both ionic and oxidized forms. Not only does this combined approach reveal more probable adsorption of serotonin into the silver surface through hydroxyl/oxygen sites than through NH/nitrogen sites, but also that it does so predominantly in its neutral (reduced) form, somewhat less so in its ionic forms, and much less in its oxidized forms. If the development of opto-voltammetric biosensors and their effective implementation is envisioned for the future, this study provides some needed scientific background for comprehending changes in the vibrational signatures of this important neurotransmitter.
Highlights
Since this enhancement strongly depends on the roughness of the material used as a substrate, which can vary in scale from a few tens to hundreds of nanometers, as well as on the material type, both potentially being characteristics of electrodes currently employed in deep brain stimulation (DBS), the analysis presented here could shed some light on 5-HT monitoring, especially that of its unwanted oxidized forms
With a perspective that stems from a desire to obtain a reliable understanding of vibrational assignments as compared with experimentally observed phenomena, the current study presents a detailed investigation of serotonin detection using Ag NPs as the SERS substrate
Is it more probable that serotonin will be adsorbed onto the silver surface at its hydroxyl/oxygen site than at its NH/nitrogen site, but the adsorption occurs predominantly in the molecule’s neutral form, followed probabilistically by its ionic forms, and is much less likely in its oxidized form
Summary
Obvious structural molecular deformations such as bending of lateral amino chains are observed for both ionic and oxidized forms Does this combined approach reveal more probable adsorption of serotonin into the silver surface through hydroxyl/oxygen sites than through NH/nitrogen sites, and that it does so predominantly in its neutral (reduced) form, somewhat less so in its ionic forms, and much less in its oxidized forms. 5-hydroxytryptamine (5-HT), known as serotonin, is a neurotransmitter present in the central and peripheral nervous system It was first found in the early 20th century as a smooth-muscle-stimulating substance in extracts prepared from gastrointestinal tract (GI) tissue [1], and later on as a vasoconstrictive substance in blood serum [2], it has been studied less than dopamine, another key neurotransmitter.
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