Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Polyelectrolyte Surface Diffusion in a Nanoslit Geometry

Journal Article · · Macromolecules
The surface diffusion of poly-l-lysine (PLL) in a planar nanoslit was studied using convex lens-induced confinement (CLiC) single-molecule tracking microscopy. Here, three surface chemistries were employed to understand the interplay of electrostatic and short-range interactions: an amine-functionalized silica surface, an oligo(ethylene oxide) (OEG)-modified surface, and a 1:1 mixture of the two ligands. Effective surface diffusion coefficients increased rapidly with slit height until saturating for slit heights <30 nm. While diffusion at a semi-infinite interface was significantly faster for OEG surfaces, the diffusion coefficient increased most rapidly with slit height for amine-functionalized surfaces, resulting in surface diffusion within very thin slits being nearly independent of surface chemistry. Intermittent random walks were simulated within a planar slit geometry, using experimentally measured parameters obtained from diffusion at a single interface to account for the characteristic short-range interactions between PLL and each surface chemistry, and were in good agreement with experimental measurements.
Research Organization:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Organization:
Defense Threat Reduction Agency (DTRA); National Institute of Standards and Technology (NIST); National Institutes of Health (NIH); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001854
OSTI ID:
1773872
Journal Information:
Macromolecules, Journal Name: Macromolecules Journal Issue: 10 Vol. 53; ISSN 0024-9297
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (66)

Nanomedicine and its potential in diabetes research and practice journal November 2008
Prediction models for the Abraham hydrogen bond donor strength: comparison of semi-empirical, ab initio , and DFT methods: HYDROGEN BOND DONOR STRENGTH journal April 2011
Charged polypeptide diffusion at a very high ionic strength journal January 2005
Development of a pressure-driven nanofluidic control system and its application to an enzymatic reaction journal June 2008
Detecting proteins complex formation using steady-state diffusion in a nanochannel journal December 2008
Biomimetic nanochannels based biosensor for ultrasensitive and label-free detection of nucleic acids journal December 2016
Comparison of protein A affinity sorbents journal November 2005
Surface diffusion in reversed-phase liquid chromatography journal March 2010
Mass transfer kinetics, band broadening and column efficiency journal January 2012
Molecular simulation studies of reversed-phase liquid chromatography journal April 2013
Mass transport properties of second-generation silica monoliths with mean mesopore size from 5 to 25nm journal October 2014
Mass-transfer properties of insulin on core–shell and fully porous stationary phases journal October 2014
Adsorption of poly(l-lysine) on silica probed by optical reflectometry journal May 2010
New developments and possibilities of wide-pore superficially porous particle technology applied for the liquid chromatographic analysis of therapeutic proteins journal September 2018
Simultaneous Observation of Enzyme Surface Diffusion and Surface Reaction Using Microfluidic Patterning of Substrate Surfaces journal December 2005
Convex Lens-Induced Confinement for Imaging Single Molecules journal July 2010
Nanofluidic Devices with Two Pores in Series for Resistive-Pulse Sensing of Single Virus Capsids journal December 2011
Direct Observation of Transitions between Surface-Dominated and Bulk Diffusion Regimes in Nanochannels journal July 2009
Electrochemical Correlation Spectroscopy in Nanofluidic Cavities journal October 2009
A Rheological Study of the Association and Dynamics of MUC5AC Gels journal October 2017
Surface Diffusion of Aromatic Hydrocarbon Analytes in Reversed-Phase Liquid Chromatography journal August 2017
Multiscale Simulation of Diffusion in Porous Media: From Interfacial Dynamics to Hierarchical Porosity journal May 2019
Tuning the Flight Length of Molecules Diffusing on a Hydrophobic Surface journal May 2015
Electrostatic Interactions Influence Protein Adsorption (but Not Desorption) at the Silica–Aqueous Interface journal June 2015
Complex Salt Dependence of Polymer Diffusion in Polyelectrolyte Multilayers journal February 2019
Cadherin Extracellular Domain Clustering in the Absence of Trans -Interactions journal July 2019
Free Energy of a Polymer in Slit-like Confinement from the Odijk Regime to the Bulk journal November 2016
Three Regimes of Polymer Surface Dynamics under Crowded Conditions journal January 2018
Polymer Surface Transport Is a Combination of in-Plane Diffusion and Desorption-Mediated Flights journal March 2016
Grafting Density Impacts Local Nanoscale Hydrophobicity in Poly(ethylene glycol) Brushes journal March 2018
Surface-Mediated Protein Unfolding as a Search Process for Denaturing Sites journal November 2015
Influence of Oligonucleotide Grafting Density on Surface-Mediated DNA Transport and Hybridization journal June 2019
Spatial Analysis of Nanofluidic-Embedded Biosensors for Wash-Free Single-Nucleotide Difference Discrimination journal February 2018
Predicting Hydrogen-Bond Strengths from Acid−Base Molecular Properties. The p K a Slide Rule: Toward the Solution of a Long-Lasting Problem journal January 2009
Single-Molecule Tracking of Polymer Surface Diffusion journal November 2013
Adsorption and Ion Exchange: Basic Principles and Their Application in Food Processing journal January 2011
Prediction of the Intrinsic Hydrogen Bond Acceptor Strength of Chemical Substances from Molecular Structure journal September 2009
Effect of Pore Size on Adsorption of a Polyelectrolyte to Porous Glass journal February 2007
The Role of Electrostatic Interactions in Protease Surface Diffusion and the Consequence for Interfacial Biocatalysis journal December 2010
Double-Stranded DNA Diffusion in Slitlike Nanochannels journal September 2006
Diffusion of DNA in Nanoslits journal October 2008
Layer-by-Layer Assembly of Polyelectrolytes in Nanofluidic Devices journal March 2010
Ionic Transport Phenomena in Nanofluidics:  Experimental and Theoretical Study of the Exclusion-Enrichment Effect on a Chip journal June 2005
Single-Molecule Observation of Long Jumps in Polymer Adsorption journal October 2013
Protein diffusion through charged nanopores with different radii at low ionic strength journal January 2014
Polymers under confinement: single polymers, how they interact, and as model chromosomes journal January 2015
Inverted critical adsorption of polyelectrolytes in confinement journal January 2015
Continuous high throughput nanofluidic separation through tangential-flow vertical nanoslit arrays journal January 2016
Standalone interferometry-based calibration of convex lens-induced confinement microscopy with nanoscale accuracy journal January 2019
Non-Gaussian, non-ergodic, and non-Fickian diffusion of tracers in mucin hydrogels journal January 2019
Physics and technological aspects of nanofluidics journal January 2014
Nonequilibrium separation of short DNA using nanoslit arrays journal July 2009
A new approach to the problem of bulk-mediated surface diffusion journal August 2015
Bulk-mediated surface transport in the presence of bias journal July 2017
Transport in nanofluidic systems: a review of theory and applications journal January 2010
Bulk-mediated surface diffusion: non-Markovian desorption dynamics journal January 2005
Dynamics and limitations of spontaneous polyelectrolyte intrusion into a charged nanocavity journal December 2014
Intermittent Molecular Hopping at the Solid-Liquid Interface journal June 2013
Interfacial Molecular Searching Using Forager Dynamics journal March 2016
Three-Dimensional Tracking of Interfacial Hopping Diffusion journal December 2017
Anomalous Diffusion at Liquid Surfaces journal March 1995
Transport phenomena in nanofluidics journal July 2008
Intermittent search strategies journal March 2011
The Ins and Outs of DNA Transfer in Bacteria journal December 2005
Bulk mediated surface diffusion: finite bulk case journal January 2003
Packaging of a Polymer by a Viral Capsid: The Interplay between Polymer Length and Capsid Size journal February 2008

Similar Records

Three Regimes of Polymer Surface Dynamics under Crowded Conditions
Journal Article · Tue Jan 23 19:00:00 EST 2018 · Macromolecules · OSTI ID:1773866

Standalone interferometry-based calibration of convex lens-induced confinement microscopy with nanoscale accuracy
Journal Article · Wed Feb 27 19:00:00 EST 2019 · Analyst · OSTI ID:1773869

Synthesis and adsorption of polymers: Control of polymer and surface structure
Thesis/Dissertation · Tue Dec 31 23:00:00 EST 1991 · OSTI ID:5154604