Nanoparticle‐Templated Molecular Recognition Platforms for Detection of Biological Analytes

Beyene, Abraham G.; Demirer, Gözde S.; Landry, Markita P.

doi:10.1002/cpch.10

Cited by 30 publications

(20 citation statements)

References 34 publications

(56 reference statements)

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“…21,28,29 Motivated by the goal of producing an in vivo compatible neuromodulator nanosensor for a broader dynamic range of physiological relevance, we synthesized a (GT)N based ssDNA-SWNT library for N = 4, 6,7,8,12,15,19,22,26, and 30 with a previously described protocol. 30 Near infrared fluorescence and absorption spectroscopy confirm that all sequences from N = 4 to N = 30 produced stable DNA-SWNT suspensions, as evidenced by sharply defined spectral line shapes corresponding to known SWNT electronic transitions ( Figure S1). We Our experimental results thus identify polymer length as a key modulator of SWNT fluorescence quantum yield, which can be exploited for maximizing nanosensor sensitivity and improving selectivity for neuromodulators.…”

Section: Strong Fluorescent "Turn-on" Neuromodulator Nanosensorsmentioning

confidence: 69%

Ultralarge Modulation of Single Wall Carbon Nanotube Fluorescence Mediated by Neuromodulators Adsorbed on Arrays of Oligonucleotide Rings

Beyene

Alizadehmojarad

Dorlhiac

et al. 2018

Preprint

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Non-covalent interactions between single-stranded DNA (ssDNA) oligonucleotides and single wall carbon nanotubes (SWNTs) have provided a unique class of tunable chemistries for a variety of applications. However, mechanistic insight into both the photophysical and intermolecular phenomena underlying their utility is lacking, resulting in obligate heuristic approaches for producing ssDNA-SWNT based technologies. In this work, we present an ultrasensitive "turn-on" nanosensor for neuromodulators dopamine and norepinephrine with strong ΔF/F0 of up to 3500%, a signal appropriate for in vivo imaging, and uncover the photophysical principles and intermolecular interactions that govern the molecular recognition and fluorescence modulation of this nanosensor synthesized from the non-covalent conjugation of (GT)6 ssDNA strands on SWNTs. The fluorescence modulation of the ssDNA-SWNT conjugate is shown to exhibit remarkable sensitivity to the ssDNA sequence chemistry, length, and surface density, providing a wealth of parameters with which to tune nanosensor dynamic range and strength of fluorescence turn-on. We employ classical and quantum mechanical molecular dynamics simulations to rationalize our experimental findings.Calculations show that (GT)6 ssDNA form ordered loops around SWNT, inducing periodic surface potentials that modulate exciton recombination lifetimes. Further evidence is presented to elucidate how analyte binding modulates SWNT fluorescence. We discuss the implications of our findings for SWNT-based molecular sensing applications. MainSingle wall carbon nanotubes exhibit advantageous electronic and photophysical properties that make them attractive for a diverse field of applications in electronics 1-5 , sensing 6-9 , imaging [10][11][12]13 ,and molecular transport [14][15][16] . SWNT fluorescence originates from radiative

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Section: Strong Fluorescent "Turn-on" Neuromodulator Nanosensorsmentioning

confidence: 69%

Ultralarge Modulation of Single Wall Carbon Nanotube Fluorescence Mediated by Neuromodulators Adsorbed on Arrays of Oligonucleotide Rings

Beyene

Alizadehmojarad

Dorlhiac

et al. 2018

Preprint

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“…measured with a UV-3600 Plus absorption spectrophotometer (Shimadzu). Our custom near-infrared spectrometer and microscope have been described in detail in previous works 44,45 .…”

Section: Methodsmentioning

confidence: 99%

High Throughput Evolution of Near Infrared Serotonin Nanosensors

Jeong¹,

Yang²,

Beyene³

et al. 2019

Preprint

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Release and reuptake of neuromodulator serotonin, 5-HT, is central to mood regulation and neuropsychiatric disorders, whereby imaging serotonin is of fundamental importance to study the brain's serotonin signaling system. We introduce a reversible near-infrared nanosensor for serotonin (nIRHT), for which synthetic molecular recognition toward serotonin is systematically evolved from ssDNA-carbon nanotube constructs generated from large libraries of 6.9 × 10 10 unique ssDNA sequences. nIRHT produces a ~200% fluorescence enhancement upon exposure to serotonin with a Kd = 6.3 µM affinity.nIRHT shows selective responsivity towards serotonin over serotonin analogs, metabolites, and receptortargeting drugs, and a 5-fold increased affinity for serotonin over dopamine. Further, nIRHT can be introduced into the brain extracellular space in acute slice, and can be used to image exogenous serotonin reversibly. Our results suggest evolution of nanosensors could be generically implemented to rapidly develop other neuromodulator probes, and that these probes can image neuromodulator dynamics at spatiotemporal scales compatible with endogenous neuromodulation.Serotonin, or 5-hydroxytryptamine (5-HT) is a monoamine neuromodulator that plays diverse roles in the central nervous system and is critically implicated in the etiology and treatment of mood and psychiatric disorders 1 . 5-HT also plays critical roles in modulating memory and learning 2, 3 , and in the regulation of mood 4 , sleep 5 , and appetite 5 . As such, aberrations in 5-HT signaling are thought to underlie multiple mental health disorders including major depressive disorder 6 , bipolar disorder 7 , autism 8 , schizophrenia 9 , anxiety 10 , and addiction 11 . Classical neurotransmission occurs through rapid activation of ligand-gated ion channels in which neurotransmitter signaling is confined at the synaptic cleft and thus to singular synaptic partners 12 . However, 5-HT acts primarily as a neuromodulator and may undergo signaling through extrasynaptic diffusion, enabling few neurons to affect broader networks of neuronal activity through 5-HT volume transmission. As such, there is great interest in monitoring the spatial component of 5-HT modulation in addition to its temporal dynamics. Current methods for measuring 5-HT include tools adapted from analytical chemistry to measure 5-HT in the brain extracellular space with varying levels of selectivity and spatiotemporal resolution: fast-scan cyclic voltammetry leverages redox chemistry to enable rapid temporal measurement of 5-HT by inserting a carbon electrode into brain tissue 13 .Microdialysis is an analytical chemistry method in which fluid samples from brain tissue are subject to downstream analysis with chromatography 14 . Recently, a field-effect transistor sensor modified with a 5-HT aptamer was reported to exhibit a highly sensitive and selective electrochemical response to 5-HT in physiological conditions 15 . However, previous methods suffer from limited spatial resolution, and microdialysis sampling oc...

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“…The conformation of the amphiphilic polymer, that is, the corona phase, can enable the binding of a specific analyte, resulting in spectral modulations (Figure 3c). In order to discover new corona phases for molecular recognition, a library of polymer-conjugated SWCNT is screened against a panel of analyses, and the nIR fluorescence emission is monitored for intensity changes or wavelength shifts [89,119,129,130]. A successful screen results in a corona phase that can specifically and selectively recognize a target Satishkumar et al [125] used fluorescent SWCNT sensors for the detection of avidin by conjugating redox-active dyes bound to a recognition element, biotin, to the SWCNT surface.…”

Section: Synthetic Protein Recognitionmentioning

confidence: 99%

Fluorescent Single-Walled Carbon Nanotubes for Protein Detection

Hendler‐Neumark

Bisker

2019

Sensors

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Nanosensors have a central role in recent approaches to molecular recognition in applications like imaging, drug delivery systems, and phototherapy. Fluorescent nanoparticles are particularly attractive for such tasks owing to their emission signal that can serve as optical reporter for location or environmental properties. Single-walled carbon nanotubes (SWCNTs) fluoresce in the near-infrared part of the spectrum, where biological samples are relatively transparent, and they do not photobleach or blink. These unique optical properties and their biocompatibility make SWCNTs attractive for a variety of biomedical applications. Here, we review recent advancements in protein recognition using SWCNTs functionalized with either natural recognition moieties or synthetic heteropolymers. We emphasize the benefits of the versatile applicability of the SWCNT sensors in different systems ranging from single-molecule level to in-vivo sensing in whole animal models. Finally, we discuss challenges, opportunities, and future perspectives.

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Nanoparticle‐Templated Molecular Recognition Platforms for Detection of Biological Analytes

Cited by 30 publications

References 34 publications

Ultralarge Modulation of Single Wall Carbon Nanotube Fluorescence Mediated by Neuromodulators Adsorbed on Arrays of Oligonucleotide Rings

Ultralarge Modulation of Single Wall Carbon Nanotube Fluorescence Mediated by Neuromodulators Adsorbed on Arrays of Oligonucleotide Rings

High Throughput Evolution of Near Infrared Serotonin Nanosensors

Fluorescent Single-Walled Carbon Nanotubes for Protein Detection

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