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Single Molecule Tracking Studies of Lower Critical Solution Temperature Transition Behavior in Poly(N-isopropylacrylamide)

Journal Article · · Langmuir
DOI:https://doi.org/10.1021/la201753v· OSTI ID:2480681
 [1];  [2];  [2];  [3]
  1. University of Illinois at Urbana−Champaign, IL (United States)
  2. University of Utah, Salt Lake City, UT (United States)
  3. University of Notre Dame, IN (United States)

Spatial and temporal heterogeneities in expanded and collapsed surface bound poly(N-isopropylacrylamide), pNIPAAm, films are studied by single molecule tracking (SMT) experiments. Tracking data are analyzed using both radius of gyration (Rg) evolution and confinement level calculations to elucidate the range of behaviors displayed by single Rhodamine6G (R6G) molecules. Furthermore, confined diffusion that is dictated by the free volume within surface tethered chains is observed with considerable dispersion among individual R6G molecules. Thus, the distribution of probe behavior reflects nanometer-scale information about the behavior of the probe–polymer system at temperatures above (T > TLCST) and below (T < TLCST) the lower critical solution temperature (LCST). In this context, confinement-level analysis and Rg evolution both show a larger degree of confinement of the probe in pNIPAAm at T > TLCST. Temperature-dependent changes in confinement are evidenced at T > TLCST by a higher percentage of confined steps, longer periods of confined events, and smaller area of confined zones, as well as a shift in the overall distribution of Rg evolution paths and final Rg distributions.

Research Organization:
University of Utah, Salt Lake City, UT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)
Grant/Contract Number:
FG03-93ER14333
OSTI ID:
2480681
Journal Information:
Langmuir, Journal Name: Langmuir Journal Issue: 17 Vol. 27; ISSN 0743-7463
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (43)

Reversible Switching between Superhydrophilicity and Superhydrophobicity journal January 2004
In Situ Characterization of Thermo‐Responsive Poly(N‐Isopropylacrylamide) Films with Sum‐Frequency Generation Spectroscopy journal May 2010
Synthesis of Near‐Infrared Responsive Gold Nanorod/PNIPAAm Core/Shell Nanohybrids via Surface Initiated ATRP for Smart Drug Delivery journal April 2008
Methods of Digital Video Microscopy for Colloidal Studies journal April 1996
Preparation of aqueous latices with N-isopropylacrylamide journal October 1986
A closer look at how membrane proteins move journal November 1993
Confined lateral diffusion of membrane receptors as studied by single particle tracking (nanovid microscopy). Effects of calcium-induced differentiation in cultured epithelial cells journal November 1993
Lateral diffusion measurement at high spatial resolution by scanning microphotolysis in a confocal microscope journal September 1994
Automated detection and tracking of individual and clustered cell surface low density lipoprotein receptor molecules journal May 1994
Single-particle tracking: effects of corrals journal August 1995
Detection of temporary lateral confinement of membrane proteins using single-particle tracking analysis journal September 1995
Single molecule photobleaching: increasing photon yield and survival time through suppression of two-step photolysis journal November 2002
Discrimination of photoblinking and photobleaching on the single molecule level journal November 2007
Real-time observation of coil-to-globule transition in thermosensitive poly(N-isopropylacrylamide) brushes by quartz crystal microbalance journal September 2007
Stimuli-reponsive polymers and their bioconjugates journal December 2004
Smart polymeric gels: Redefining the limits of biomedical devices journal August 2007
Single-Molecule Fluorescence Trajectories for Investigating Molecular Transport in Thin Silica Sol−Gel Films journal September 2003
Stimulus-Responsive Poly( N -isopropylacrylamide) Brushes and Nanopatterns Prepared by Surface-Initiated Polymerization journal September 2004
Polymer Brushes via Surface-Initiated Controlled Radical Polymerization: Synthesis, Characterization, Properties, and Applications journal November 2009
Surface-Initiated Atom Transfer Radical Polymerization on Gold at Ambient Temperature journal August 2000
Probing Hydrophobic Interactions Using Trajectories of Amphiphilic Molecules at a Hydrophobic/Water Interface journal April 2009
Combining Optical Trapping and Single-Molecule Fluorescence Spectroscopy:  Enhanced Photobleaching of Fluorophores journal April 2004
Quasi-Elastic Neutron Scattering Study on Water and Polymer Dynamics in Thermo/Pressure Sensitive Polymer Solutions journal September 2009
Thermosensitive Behavior of Poly(N-isopropylacrylamide) and Release of Incorporated Hemoglobin journal August 2009
Thermal Response of Poly( N -isopropylacrylamide) Brushes Probed by Surface Plasmon Resonance journal April 2003
Patterned Poly( N -isopropylacrylamide) Brushes on Silica Surfaces by Microcontact Printing Followed by Surface-Initiated Polymerization journal August 2004
Temperature-Controlled Flow Switching in Nanocapillary Array Membranes Mediated by Poly( N -isopropylacrylamide) Polymer Brushes Grafted by Atom Transfer Radical Polymerization journal January 2007
Fabrication of Thermosensitive Polymer Nanopatterns through Chemical Lithography and Atom Transfer Radical Polymerization journal February 2007
Density Effects on Collapse, Compression, and Adhesion of Thermoresponsive Polymer Brushes journal December 2009
Effects of Grafting Density and Molecular Weight on the Temperature-Dependent Conformational Change of Poly(N-isopropylacrylamide) Grafted Chains in Water journal April 2006
Temperature Induced Volume-Phase Transitions in Surface-Tethered Poly( N -isopropylacrylamide) Networks journal February 2008
Effect of Grafting Density on Phase Transition Behavior for Poly( N -isopropylacryamide) Brushes in Aqueous Solutions Studied by AFM and QCM-D journal September 2010
Emerging applications of stimuli-responsive polymer materials journal January 2010
Dynamic multiple-target tracing to probe spatiotemporal cartography of cell membranes journal July 2008
Trajectory analysis of single molecules exhibiting non-Brownian motion journal January 2011
Stimuli-responsive polymer gels journal January 2008
Diffusion processes of single fluorescent molecules in a polymer-based thin material with three-dimensional network journal January 2009
Molecular diffusion on surface tethered polymer layers: coupling of molecular thermal fluctuation and polymer chain dynamics journal January 2010
Detection of Dimers of Dimers of Human Leukocyte Antigen (HLA)–DR on the Surface of Living Cells by Single-Particle Fluorescence Imaging journal January 1998
Three-Dimensional Imaging of Single Molecules Solvated in Pores of Poly(acrylamide) Gels journal November 1996
SINGLE-PARTICLE TRACKING:Applications to Membrane Dynamics journal June 1997
A spatially restricted increase in receptor mobility is involved in directional sensing during Dictyostelium discoideum chemotaxis journal May 2008
Detection of Non-Brownian Diffusion in the Cell Membrane in Single Molecule Tracking journal March 2005