Divalent Cation Dependence Enhances Dopamine Aptamer Biosensing.
Oligonucleotide receptors (aptamers), which change conformation upon target recognition, enable electronic biosensing under high ionic-strength conditions when coupled to field-effect transistors (FETs). Because highly negatively charged aptamer backbones are influenced by ion content and concentration, biosensor performance and target sensitivities were evaluated under application conditions. For a recently identified dopamine aptamer, physiological concentrations of Mg2+ and Ca2+ in artificial cerebrospinal fluid produced marked potentiation of dopamine FET-sensor responses. By comparison, divalent cation-associated signal amplification was not observed for FET sensors functionalized with a recently identified serotonin aptamer or a previously reported dopamine aptamer. Circular dichroism spectroscopy revealed Mg2+- and Ca2+-induced changes in target-associated secondary structure for the new dopamine aptamer, but not the serotonin aptamer nor the old dopamine aptamer. Thioflavin T displacement corroborated the Mg2+ dependence of the new dopamine aptamer for target detection. These findings imply allosteric binding interactions between divalent cations and dopamine for the new dopamine aptamer. Developing and testing sensors in ionic environments that reflect intended applications are best practices for identifying aptamer candidates with favorable attributes and elucidating sensing mechanisms.
['Nakatsuka|Nako|N|http://orcid.org/0000-0001-8248-5248', 'Abendroth|John M|JM|http://orcid.org/0000-0002-2369-4311', 'Yang|Kyung-Ae|KA|http://orcid.org/0000-0001-5575-4107', 'Andrews|Anne M|AM|http://orcid.org/0000-0002-1961-4833']
D052157:Aptamers, Nucleotide D052160:Benzothiazoles D015374:Biosensing Techniques D002118:Calcium D004298:Dopamine D055664:Electrochemical Techniques D054856:G-Quadruplexes D008274:Magnesium D012701:Serotonin D014173:Transistors, Electronic
oligonucleotides field-effect transistor Mg2+ Ca2+ serotonin circular dichroism spectroscopy Debye length neurotransmitter