skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Multifunctional nanopore electrode array method for characterizing and manipulating single entities in attoliter-volume enclosures

Journal Article · · Journal of Applied Physics
DOI:https://doi.org/10.1063/5.0101693· OSTI ID:1971653

Structurally regular nanopore arrays fabricated to contain independently controllable annular electrodes represent a new kind of architecture capable of electrochemically addressing small collections of matter—down to the single entity (molecule, particle, and biological cell) level. Furthermore, these nanopore electrode arrays (NEAs) can also be interrogated optically to achieve single entity spectroelectrochemistry. Larger entities such as nanoparticles and single bacterial cells are investigated by dark-field scattering and potential-controlled single-cell luminescence experiments, respectively, while NEA-confined molecules are probed by single molecule luminescence. By carrying out these experiments in arrays of identically constructed nanopores, massively parallel collections of single entities can be investigated simultaneously. The multilayer metal–insulator design of the NEAs enables highly efficient redox cycling experiments with large increases in analytical sensitivity for chemical sensing applications. NEAs may also be augmented with an additional orthogonally designed nanopore layer, such as a structured block copolymer, to achieve hierarchically organized multilayer structures with multiple stimulus-responsive transport control mechanisms. Finally, NEAs constructed with a transparent bottom layer permit optical access to the interior of the nanopore, which can result in the cutoff of far-field mode propagation, effectively trapping radiation in an ultrasmall volume inside the nanopore. Furthermore, the bottom metal layer may be used as both a working electrode and an optical cladding layer, thus, producing bifunctional electrochemical zero-mode waveguide architectures capable of carrying out spectroelectrochemical investigations down to the single molecule level.

Research Organization:
University of Notre Dame, IN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-07ER15851
OSTI ID:
1971653
Journal Information:
Journal of Applied Physics, Vol. 132, Issue 17; ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (88)

Acid–base chemistry at the single ion limit journal January 2020
Rectification of Ionic Current in a Nanofluidic Diode journal March 2007
Electrochemical attosyringe journal July 2007
Higher-Order Organization by Mesoscale Self-Assembly and Transformation of Hybrid Nanostructures journal May 2003
Mass Transport to Nanoelectrode Arrays and Limitations of the Diffusion Domain Approach: Theory and Experiment journal June 2009
Single-enzyme kinetics with fluorogenic substrates: lessons learnt and future directions journal June 2014
Selective Capture and Identification of Pathogenic Bacteria Using an Immobilized Siderophore journal October 2010
Asymmetric Nafion-Coated Nanopore Electrode Arrays as Redox-Cycling-Based Electrochemical Diodes journal August 2018
A programmable droplet-based microfluidic device applied to multiparameter analysis of single microbes and microbial communities journal April 2012
Isolation, incubation, and parallel functional testing and identification by FISH of rare microbial single-copy cells from multi-species mixtures using the combination of chemistrode and stochastic confinement journal January 2009
Electrowetting‐Mediated Transport to Produce Electrochemical Transistor Action in Nanopore Electrode Arrays journal April 2020
Manipulating Molecular Transport through Nanoporous Membranes by Control of Electrokinetic Flow:  Effect of Surface Charge Density and Debye Length journal October 2001
Electrochemical Detection of Single Molecules journal February 1995
Psl trails guide exploration and microcolony formation in Pseudomonas aeruginosa biofilms journal May 2013
World Health Organization Report: Current Crisis of Antibiotic Resistance journal August 2019
Surface plasmon subwavelength optics journal August 2003
Stimuli-responsive smart gating membranes journal January 2016
Intelligent Dual-Responsive Cellulose Surfaces via Surface-Initiated ATRP journal August 2008
Synthetic Proton-Gated Ion Channels via Single Solid-State Nanochannels Modified with Responsive Polymer Brushes journal July 2009
Electrochemical Desalination for a Sustainable Water Future journal March 2014
Perspective and Prospectus on Single-Entity Electrochemistry journal November 2018
A strategy for selective detection based on interferent depleting and redox cycling using the plane-recessed microdisk array electrodes journal October 2011
Three DNA sequencing methods using capillary gel electrophoresis and laser-induced fluorescence journal December 1991
Capture of Single Silver Nanoparticles in Nanopore Arrays Detected by Simultaneous Amperometry and Surface-Enhanced Raman Scattering journal March 2019
Electrokinetic Flow in a Narrow Cylindrical Capillary journal November 1965
(Poly)cation-induced protection of conventional and wireframe DNA origami nanostructures journal January 2018
Ultrafast Dynamics of Flavins in Five Redox States journal October 2008
Ozonolysis Is the Primary Cause of UV Photooxidation of Alkanethiolate Monolayers at Low Irradiance journal March 1998
Voltage-Gated Hydrophobic Nanopores journal August 2011
Rapid Identification of Pseudomonas spp. via Raman Spectroscopy Using Pyoverdine as Capture Probe journal January 2016
Construction and use of paired and triple band microelectrodes in solutions of low ionic strength journal October 1988
Light-Harvesting Conjugated Microporous Polymers: Rapid and Highly Efficient Flow of Light Energy with a Porous Polyphenylene Framework as Antenna journal March 2010
Digital simulation of the measured electrochemical response of reversible redox couples at microelectrode arrays: consequences arising from closely spaced ultramicroelectrodes journal August 1986
Emulsion Solvent Evaporation-Induced Self-Assembly of Block Copolymers Containing pH-Sensitive Block journal August 2017
Single-molecule spectroscopy of protein folding dynamics—expanding scope and timescales journal February 2013
Microfabricated Porous Membrane Structure for Sample Concentration and Electrophoretic Analysis journal May 1999
Electrochemical behavior of reversible redox species at interdigitated array electrodes with different geometries: consideration of redox cycling and collection efficiency journal March 1990
A Novel Glucose Biosensor Based on Hierarchically Porous Block Copolymer Film journal July 2018
Biomedical surface science: Foundations to frontiers journal March 2002
Potential-dependent single molecule blinking dynamics for flavin adenine dinucleotide covalently immobilized in zero-mode waveguide array of working electrodes journal January 2013
Recessed Ring–Disk Nanoelectrode Arrays Integrated in Nanofluidic Structures for Selective Electrochemical Detection journal September 2013
Single-Molecule Enzyme Dynamics of Monomeric Sarcosine Oxidase in a Gold-Based Zero-Mode Waveguide journal February 2012
Nanoscale Control and Manipulation of Molecular Transport in Chemical Analysis journal July 2009
Ion Gating in Nanopore Electrode Arrays with Hierarchically Organized pH-Responsive Block Copolymer Membranes journal November 2020
Self-Contained Microelectrochemical Immunoassay for Small Volumes Using Mouse IgG as a Model System journal July 2002
Optical-facilitated single-entity electrochemistry journal August 2022
Localized Surface Plasmon Resonance Spectroscopy and Sensing journal May 2007
Organization of Au Colloids as Monolayer Films onto ITO Glass Surfaces: Application of the Metal Colloid Films as Base Interfaces To Construct Redox-Active Monolayers journal April 1995
Light as Trigger for Biocatalysis: Photonic Wiring of Flavin Adenine Dinucleotide-Dependent Glucose Dehydrogenase to Quantum Dot-Sensitized Inverse Opal TiO 2 Architectures via Redox Polymers journal April 2018
The Antimicrobial Resistance Crisis: Causes, Consequences, and Management journal September 2014
Single Entity Electrochemistry in Nanopore Electrode Arrays: Ion Transport Meets Electron Transfer in Confined Geometries journal January 2020
Redox Cycling on Recessed Ring-Disk Nanoelectrode Arrays in the Absence of Supporting Electrolyte journal May 2014
Stochasticity in single-entity electrochemistry journal February 2021
Block Copolymers: Synthesis, Self-Assembly, and Applications journal October 2017
Controlled Vectorial Electron Transfer and Photoelectrochemical Applications of Layered Relay/Photosensitizer-Imprinted Au Nanoparticle Architectures on Electrodes journal January 2016
Electric-field-induced wetting and dewetting in single hydrophobic nanopores journal October 2011
Ion selective redox cycling in zero-dimensional nanopore electrode arrays at low ionic strength journal January 2017
Redox cycling with facing interdigitated array electrodes as a method for selective detection of redox species journal January 2007
Potential-induced wetting and dewetting in pH-responsive block copolymer membranes for mass transport control journal January 2022
The potential and challenges of nanopore sequencing journal October 2008
Single-molecule spectroelectrochemical cross-correlation during redox cycling in recessed dual ring electrode zero-mode waveguides journal January 2017
Chemical Noise Produced by Equilibrium Adsorption/Desorption of Surface Pyridine at Au–Ag–Au Bimetallic Atom-Scale Junctions Studied by Fluctuation Spectroscopy journal March 2013
A nanopore machine promotes the vectorial transport of DNA across membranes journal September 2013
Mediator-free triple-enzyme cascade electrocatalytic aptasensor with exonuclease-assisted target recycling and hybridization chain reaction amplification journal May 2014
Voltage-Gated Nanoparticle Transport and Collisions in Attoliter-Volume Nanopore Electrode Arrays journal January 2018
Directed Self-Assembly of Block Copolymers for the Fabrication of Functional Devices journal October 2020
Electrolytic transport through a synthetic nanometer-diameter pore journal July 2005
Selective protein trapping within hybrid nanowells journal January 2016
Nanofluidic Redox Cycling Amplification for the Selective Detection of Catechol journal February 2008
Microfluidic Confinement of Single Cells of Bacteria in Small Volumes Initiates High-Density Behavior of Quorum Sensing and Growth and Reveals Its Variability journal July 2009
Metal enhanced fluorescence improved protein and DNA detection by zigzag Ag nanorod arrays journal August 2016
Single Molecule Electrochemical Detection in Aqueous Solutions and Ionic Liquids journal October 2015
Redox Cycling in Nanoscale-Recessed Ring-Disk Electrode Arrays for Enhanced Electrochemical Sensitivity journal May 2013
Electrochemistry at single molecule occupancy in nanopore-confined recessed ring-disk electrode arrays journal January 2016
Single occupancy spectroelectrochemistry of freely diffusing flavin mononucleotide in zero-dimensional nanophotonic structures journal January 2015
Counting and Sizing of Submicron Particles by the Resistive Pulse Technique journal July 1970
Biological Nanopore Approach for Single‐Molecule Protein Sequencing journal February 2021
Redox Cycling in Individually Encapsulated Attoliter-Volume Nanopores journal November 2018
Enhanced Mass Transport of Electroactive Species to Annular Nanoband Electrodes Embedded in Nanocapillary Array Membranes journal May 2012
Zero-mode waveguides: Sub-wavelength nanostructures for single molecule studies at high concentrations journal September 2008
Porous block copolymer separation membranes for 21st century sanitation and hygiene journal January 2021
Sequence-specific detection of individual DNA strands using engineered nanopores journal July 2001
Engineered Asymmetric Heterogeneous Membrane: A Concentration-Gradient-Driven Energy Harvesting Device journal November 2015
Convective Delivery of Electroactive Species to Annular Nanoband Electrodes Embedded in Nanocapillary-Array Membranes journal August 2012
Ionic transport in nanocapillary membrane systems journal July 2012
Confined Nanopipette Sensing: From Single Molecules, Single Nanoparticles, to Single Cells journal March 2019
Graphene Nanopores for Protein Sequencing journal June 2016
Counting and Sizing of Single Vesicles/Liposomes by Electrochemical Events journal July 2018