Electric Field Modulation of Semiconductor Quantum Dot Photoluminescence: Insights Into the Design of Robust Voltage-Sensitive Cellular Imaging Probes

Rowland, Clare E.; Susumu, Kimihiro; Stewart, Michael H.; Oh, Eunkeu; Mäkinen, Antti; O’Shaughnessy, Thomas J.; Kushto, Gary P.; Wolak, Mason A.; Erickson, Jeffrey S.; Efros, Alexander L.; Huston, Alan L.; Delehanty, James B.

doi:10.1021/acs.nanolett.5b02725

Cited by 84 publications

(100 citation statements)

References 54 publications

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“…This configuration was selected to promote enhanced sensitivity to applied electric fields, as we have reported previously. 38 The C 60 is an efficient electron acceptor that quenches the PL of the photoexcited QD quantitatively as a function of the number of C 60 acceptors assembled on the QD surface. 31 Finally, the alanine/leucinerich peptide bridge serves to append the C 60 acceptor at discrete fixed distances while also mediating membrane insertion as confirmed by CD analysis and immunostaining.…”

Section: Discussionmentioning

confidence: 99%

Quantum Dot–Peptide–Fullerene Bioconjugates for Visualization of in Vitro and in Vivo Cellular Membrane Potential

Nag¹,

Stewart²,

Deschamps³

et al. 2017

ACS Nano

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We report the development of a quantum dot (QD)–peptide–fullerene (C60) electron transfer (ET)-based nanobioconjugate for the visualization of membrane potential in living cells. The bioconjugate is composed of (1) a central QD electron donor, (2) a membrane-inserting peptidyl linker, and (3) a C60 electron acceptor. The photoexcited QD donor engages in ET with the C60 acceptor, resulting in quenching of QD photoluminescence (PL) that tracks positively with the number of C60 moieties arrayed around the QD. The nature of the QD-capping ligand also modulates the quenching efficiency; a neutral ligand coating facilitates greater QD quenching than a negatively charged carboxylated ligand. Steady-state photophysical characterization confirms an ET-driven process between the donor–acceptor pair. When introduced to cells, the amphiphilic QD–peptide–C60 bioconjugate labels the plasma membrane by insertion of the peptide–C60 portion into the hydrophobic bilayer, while the hydrophilic QD sits on the exofacial side of the membrane. Depolarization of cellular membrane potential augments the ET process, which is manifested as further quenching of QD PL. We demonstrate in HeLa cells, PC12 cells, and primary cortical neurons significant QD PL quenching (ΔF/F0 of 2–20% depending on the QD–C60 separation distance) in response to membrane depolarization with KCl. Further, we show the ability to use the QD–peptide–C60 probe in combination with conventional voltage-sensitive dyes (VSDs) for simultaneous two-channel imaging of membrane potential. In in vivo imaging of cortical electrical stimulation, the optical response of the optimal QD–peptide–C60 configuration exhibits temporal responsivity to electrical stimulation similar to that of VSDs. Notably, however, the QD–peptide–C60 construct displays 20- to 40-fold greater ΔF/F0 than VSDs. The tractable nature of the QD–peptide–C60 system offers the advantages of ease of assembly, large ΔF/F0, enhanced photostability, and high throughput without the need for complicated organic synthesis or genetic engineering, respectively, that is required of traditional VSDs and fluorescent protein constructs.

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Section: Discussionmentioning

confidence: 99%

Quantum Dot–Peptide–Fullerene Bioconjugates for Visualization of in Vitro and in Vivo Cellular Membrane Potential

Nag¹,

Stewart²,

Deschamps³

et al. 2017

ACS Nano

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“…A prime example of this is monitoring electric signaling in neuronal cells which is foundational to neuroscience and yet still incredibly challenging in practice. 885 …”

Section: Special Case Of Benzenediolsmentioning

confidence: 99%

Energy Transfer with Semiconductor Quantum Dot Bioconjugates: A Versatile Platform for Biosensing, Energy Harvesting, and Other Developing Applications

Spillmann²,

et al. 2016

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Luminescent semiconductor quantum dots (QDs) are one of the more popular nanomaterials currently utilized within biological applications. However, what is not widely appreciated is their growing role as versatile energy transfer (ET) donors and acceptors within a similar biological context. The progress made on integrating QDs and ET in biological configurations and applications is reviewed in detail here. The goal is to provide the reader with (1) an appreciation for what QDs are capable of in this context, (2) how this field has grown over a relatively short time span, and, in particular, (3) how QDs are steadily revolutionizing the development of new biosensors along with a myriad of other photonically active nanomaterial-based bioconjugates. An initial discussion of QD materials along with key concepts surrounding their preparation and bioconjugation is provided given the defining role these aspects play in the QDs ability to succeed in subsequent ET applications. The discussion is then divided around the specific roles that QDs provide as either Förster resonance energy transfer (FRET) or charge/electron transfer donor and/or acceptor. For each QD-ET mechanism, a working explanation of the appropriate background theory and formalism is articulated before examining their biosensing and related ET utility. Other configurations such as incorporation of QDs into multistep ET processes or use of initial chemical and bioluminescent excitation are treated similarly. ET processes that are still not fully understood such as QD interactions with gold and other metal nanoparticles along with carbon allotropes are also covered. Given their maturity, some specific applications ranging from in vitro sensing assays to cellular imaging are separated and discussed in more detail. Finally a perspective on how this field will continue to evolve is provided.

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“…In particular, we have shown that charge separation across one (or more) heterostructure interface(s) with type-II band alignment (and the associated induced dipole) is crucial for an enhanced QCSE (12). The feasibility of utilizing such vsNPs for membrane voltage sensing was soon after theoretically investigated and favorably compared to organic VSDs (13, 14). Here we utilize self-consistent Schrödinger-Poisson calculations for vsNPs embedded in the membrane to further explore the feasibility and performance of vsNPs as voltage sensors, and to provide guiding principles for their design.…”

Section: Introductionmentioning

confidence: 99%

Design Rules for Membrane-Embedded Voltage-Sensing Nanoparticles

Park

Weiss

2017

Biophysical Journal

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Voltage-sensing dyes and voltage-sensing fluorescence proteins have been continually improved and as a result have provided a wealth of insights into neuronal circuits. Further improvements in voltage-sensing dyes and voltage-sensing fluorescence proteins are needed, however, for routine detection of single action potentials across a large number of individual neurons in a large field-of-view of a live mammalian brain. On the other hand, recent experiments and calculations suggest that semiconducting nanoparticles could act as efficient voltage sensors, suitable for the above-mentioned task. This study presents quantum mechanical calculations, including Auger recombination rates, of the quantum-confined Stark effect in membrane-embedded semiconducting nanoparticles, examines their possible utility as membrane voltage sensors, and provide design rules for their structure and composition.

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Electric Field Modulation of Semiconductor Quantum Dot Photoluminescence: Insights Into the Design of Robust Voltage-Sensitive Cellular Imaging Probes

Cited by 84 publications

References 54 publications

Quantum Dot–Peptide–Fullerene Bioconjugates for Visualization of in Vitro and in Vivo Cellular Membrane Potential

Quantum Dot–Peptide–Fullerene Bioconjugates for Visualization of in Vitro and in Vivo Cellular Membrane Potential

Energy Transfer with Semiconductor Quantum Dot Bioconjugates: A Versatile Platform for Biosensing, Energy Harvesting, and Other Developing Applications

Design Rules for Membrane-Embedded Voltage-Sensing Nanoparticles

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