Single-molecule spectroelectrochemical cross-correlation during redox cycling in recessed dual ring electrode zero-mode waveguides

Han, Donghoon; Crouch, Garrison M.; Fu, Kaiyu; Zaino, Lawrence P.; Bohn, Paul W.

doi:10.1039/c7sc02250f

Cited by 37 publications

(53 citation statements)

References 59 publications

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“…The recent rapid development of solid‐state nanopores represents a robust and durable sensing platform to perform single biomolecule detection, DNA sequencing, and proteomic profiling . Synthetic nanopores not only approach the small size of biological ion channels, but can also be designed to incorporate voltage‐gating properties and biorecognition capabilities to mediate analyte transport into the nanopore, where chemical signals can be generated .…”

Section: Introductionmentioning

confidence: 99%

Voltage‐Gated Nanoparticle Transport and Collisions in Attoliter‐Volume Nanopore Electrode Arrays

Han

Crouch

et al. 2018

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Single nanoparticle analysis can reveal how particle‐to‐particle heterogeneity affects ensemble properties derived from traditional bulk measurements. High‐bandwidth, low noise electrochemical measurements are needed to examine the fast heterogeneous electron‐transfer behavior of single nanoparticles with sufficient fidelity to resolve the behavior of individual nanoparticles. Herein, nanopore electrode arrays (NEAs) are fabricated in which each pore supports two vertically spaced, individually addressable electrodes. The top ring electrode serves as a particle gate to control the transport of silver nanoparticles (AgNPs) within individual attoliter volume NEAs nanopores, as shown by redox collisions of AgNPs collisions at the bottom disk electrode. The AgNP‐nanoporeis system has wide‐ranging technological applications as well as fundamental interest, since the transport of AgNPs within the NEA mimics the transport of ions through cell membranes via voltage‐gated ion channels. A voltage threshold is observed above which AgNPs are able to access the bottom electrode of the NEAs, i.e., a minimum potential at the gate electrode is required to switch between few and many observed collision events on the collector electrode. It is further shown that this threshold voltage is strongly dependent on the applied voltage at both electrodes as well as the size of AgNPs, as shown both experimentally and through finite‐element modeling. Overall, this study provides a precise method of monitoring nanoparticle transport and in situ redox reactions within nanoconfined spaces at the single particle level.

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Section: Introductionmentioning

confidence: 99%

Voltage‐Gated Nanoparticle Transport and Collisions in Attoliter‐Volume Nanopore Electrode Arrays

Han

Crouch

et al. 2018

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“…Raman is a technique with low sensitivity but it can be largely improved using surface enhanced Raman scattering (SERS) substrates . Finally, fluorescence is a really sensitive and selective technique making it easy to work at a suitable time‐scale.…”

Section: Whatmentioning

confidence: 99%

“…Other alternatives have been proposed to enhance the sensitivity in PL‐SEC. By using an array of nanopore ring electrodes fixed on an optically transparent support, bifunctional nanopores with nanophotonic and nanoelectrochemical behavior were obtained , Figure . Using this analytical strategy and repeating cycles of oxidation and reduction of the analyte, based on the cross‐correlation of single molecule fluctuations in electrochemical and photon‐emission responses, single‐molecule detection was achieved.…”

Section: Whymentioning

confidence: 99%

Spectroelectrochemical Sensing: Current Trends and Challenges

et al. 2019

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Spectroelectrochemistry (SEC) has been used for more than 50 years, but this set of techniques has not been widely used for quantitative analysis. For many years, no commercial instruments were available, which made very difficult to spread the use of SEC. Nowadays, only the creativity of the researchers is required to exploit the capabilities of SEC. This review is written with the aim of showing the potential of SEC, mainly for analytical chemistry. Here, we explain what SEC is, how analytical responses can be obtained, why these techniques are useful for sensors, with a brief description of its advantages in use, and, finally, we try to show the challenges that must be addressed in the next years. SEC can resolve interesting analytical problems using the high amount of data provided by this intrinsic trilinear technique. Given the quantitative analysis point of view of this review, the discussion of the SEC techniques is focused on UV/Vis absorption, photoluminescence and Raman SEC.

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“…Panel b reproduced with permission from ref ( 90 ) (Copyright 2016 American Chemical Society) and ref ( 89 ) (Copyright 2014 American Chemical Society). Panel c reproduced with permission from ref ( 103 ). Copyright 2017 Royal Society of Chemistry.…”

Section: Nanopore Electrode Capabilitiesmentioning

confidence: 99%

Nanopore Electrochemistry: A Nexus for Molecular Control of Electron Transfer Reactions

Bohn

2018

ACS Cent. Sci.

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Pore-based structures occur widely in living organisms. Ion channels embedded in cell membranes, for example, provide pathways, where electron and proton transfer are coupled to the exchange of vital molecules. Learning from mother nature, a recent surge in activity has focused on artificial nanopore architectures to effect electrochemical transformations not accessible in larger structures. Here, we highlight these exciting advances. Starting with a brief overview of nanopore electrodes, including the early history and development of nanopore sensing based on nanopore-confined electrochemistry, we address the core concepts and special characteristics of nanopores in electron transfer. We describe nanopore-based electrochemical sensing and processing, discuss performance limits and challenges, and conclude with an outlook for next-generation nanopore electrode sensing platforms and the opportunities they present.

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Single-molecule spectroelectrochemical cross-correlation during redox cycling in recessed dual ring electrode zero-mode waveguides

Abstract: The ability of zero-mode waveguides (ZMW) to guide light into subwavelength-diameter nanoapertures has been exploited for studying electron transfer dynamics in zeptoliter-volume nanopores under single-molecule occupancy conditions.

Cited by 37 publications

References 59 publications

Voltage‐Gated Nanoparticle Transport and Collisions in Attoliter‐Volume Nanopore Electrode Arrays

Voltage‐Gated Nanoparticle Transport and Collisions in Attoliter‐Volume Nanopore Electrode Arrays

Spectroelectrochemical Sensing: Current Trends and Challenges

Nanopore Electrochemistry: A Nexus for Molecular Control of Electron Transfer Reactions

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