title: Neurotransmitter detection using corona phase molecular recognition on fluorescent single-walled carbon nanotube sensors.
abstract: Temporal and spatial changes in neurotransmitter concentrations are central to information processing in neural networks. Therefore, biosensors for neurotransmitters are essential tools for neuroscience. In this work, we applied a new technique, corona phase molecular recognition (CoPhMoRe), to identify adsorbed polymer phases on fluorescent single-walled carbon nanotubes (SWCNTs) that allow for the selective detection of specific neurotransmitters, including dopamine. We functionalized and suspended SWCNTs with a library of different polymers (n = 30) containing phospholipids, nucleic acids, and amphiphilic polymers to study how neurotransmitters modulate the resulting band gap, near-infrared (nIR) fluorescence of the SWCNT. We identified several corona phases that enable the selective detection of neurotransmitters. Catecholamines such as dopamine increased the fluorescence of specific single-stranded DNA- and RNA-wrapped SWCNTs by 58-80% upon addition of 100 μM dopamine depending on the SWCNT chirality (n,m). In solution, the limit of detection was 11 nM [K(d) = 433 nM for (GT)15 DNA-wrapped SWCNTs]. Mechanistic studies revealed that this turn-on response is due to an increase in fluorescence quantum yield and not covalent modification of the SWCNT or scavenging of reactive oxygen species. When immobilized on a surface, the fluorescence intensity of a single DNA- or RNA-wrapped SWCNT is enhanced by a factor of up to 5.39 ± 1.44, whereby fluorescence signals are reversible. Our findings indicate that certain DNA/RNA coronae act as conformational switches on SWCNTs, which reversibly modulate the SWCNT fluorescence. These findings suggest that our polymer-SWCNT constructs can act as fluorescent neurotransmitter sensors in the tissue-compatible nIR optical window, which may find applications in neuroscience.
authors.affiliation: Department of Chemical Engineering, Massachusetts Institute of Technology , Cambridge, Massachusetts 02139, United States.
authors.forename: Sebastian
authors.initials: S
authors.lastname: Kruss
authors.forename: Markita P
authors.initials: MP
authors.lastname: Landry
authors.forename: Emma
authors.initials: E
authors.lastname: Vander Ende
authors.forename: Barbara M A
authors.initials: BM
authors.lastname: Lima
authors.forename: Nigel F
authors.initials: NF
authors.lastname: Reuel
authors.forename: Jingqing
authors.initials: J
authors.lastname: Zhang
authors.forename: Justin
authors.initials: J
authors.lastname: Nelson
authors.forename: Bin
authors.initials: B
authors.lastname: Mu
authors.forename: Andrew
authors.initials: A
authors.lastname: Hilmer
authors.forename: Michael
authors.initials: M
authors.lastname: Strano
mesh_terms: D000327:Adsorption; D005456:Fluorescent Dyes / Q000737:chemistry*; D008856:Microscopy, Fluorescence / Q000379:methods*; D015394:Molecular Structure; D037742:Nanotubes, Carbon / Q000737:chemistry*; D018377:Neurotransmitter Agents / Q000032:analysis*
chemical_list: D005456:Fluorescent Dyes; D037742:Nanotubes, Carbon; D018377:Neurotransmitter Agents