Neurotransmitter detection using corona phase molecular recognition on fluorescent single-walled carbon nanotube sensors

Sebastian Kruss, Markita P. Landry, Emma Vander Ende, Barbara M.A. Lima, Nigel F. Reuel, Jingqing Zhang, Justin Nelson, Bin Mu, Andrew Hilmer, Michael Strano

Research output: Contribution to journalArticle

137 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)713-724
Number of pages12
JournalJournal of the American Chemical Society
Volume136
Issue number2
DOIs
StatePublished - Jan 15 2014

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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    Kruss, S., Landry, M. P., Vander Ende, E., Lima, B. M. A., Reuel, N. F., Zhang, J., Nelson, J., Mu, B., Hilmer, A., & Strano, M. (2014). Neurotransmitter detection using corona phase molecular recognition on fluorescent single-walled carbon nanotube sensors. Journal of the American Chemical Society, 136(2), 713-724. https://doi.org/10.1021/ja410433b