Self-Diffusion and Cooperative Diffusion in Semidilute Polymer Solutions As Measured by Fluorescence Correlation Spectroscopy

Zettl, Ute; Hoffmann, Sebastian T.; Koberling, Felix; Krausch, Georg; Enderlein, Joerg; Harnau, Ludger; Ballauff, Matthias

doi:10.1021/ma901404g

Cited by 85 publications

(115 citation statements)

References 111 publications

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“…Fluorescence correlation spectroscopy (FCS) can also report the rate of the center-of-mass diffusion and the local relaxation of long and flexible molecules. [55][56][57][58] Due to the principle of the technique, the motion of a single molecule cannot be followed over a long time period with this approach, which makes Single molecule fluorescence imaging.…”

Section: Introductionmentioning

confidence: 99%

Single-Molecule Imaging Reveals Topology Dependent Mutual Relaxation of Polymer Chains

2015

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that the method provides an invaluable tool for characterizing topological interaction between the entangled chains. We further demonstrate that the current models proposed for the entanglement between cyclic polymers which are based on cyclic chains moving through an array of fixed obstacles cannot correctly describe the motion of the cyclic chain under the entangled conditions.Our results rather suggest the mutual relaxation of the cyclic chains, which underscore the necessity of developing a new model to describe the motion of cyclic polymer under the entangled conditions based on the mutual interaction of the chains.3

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Section: Introductionmentioning

confidence: 99%

Single-Molecule Imaging Reveals Topology Dependent Mutual Relaxation of Polymer Chains

2015

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“…in 1997 [1] proposed a simple explanation for the common occurrence of coffee-ring stains: enhanced evaporation at the pinned contact line induces outward flow to replenish solvent loss and sweeps suspended material to the contact line where it is deposited as a ring stain. In the subsequent years understanding the competing dynamic processes within evaporating sessile droplets has become an increasingly complex and interesting subject, encompassing many experimental factors such as: the solvent evaporation rate [2,3]; interactions between solvent, solute, vapour and substrate [4,5]; phase transitions within the droplet [6,7]; internal convection currents [8,9,10]; solute diffusion [11,12,13]; and the shape of suspended particles [14]. As well as to understand the fundamental science, motivation comes from a variety of industrial applications such as ink-jet printing [15], drying paints and varnishes, evaporative cooling [16], and effective chemical delivery in crop spraying.…”

Section: Introductionmentioning

confidence: 99%

The effects of molecular weight, evaporation rate and polymer concentration on pillar formation in drying poly(ethylene oxide) droplets

Baldwin

Fairhurst

2014

Colloids and Surfaces A: Physicochemical and Engineering Aspect

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Typically, when droplets of dilute suspensions are left to evaporate the final dry deposit is the familiar coffee-ring stain, with nearly all the solute deposited at the initial contact line. Contrastingly, in previous work we have shown that sessile droplets of poly(ethylene oxide) (PEO) solutions form tall central pillars (or monoliths) during a 4-stage drying process. We show that a dimensionless Péclet-type number P e, a ratio of the competing advective and diffusive motion of the dissolved polymer, which incorporates the effects of evaporation rate, initial concentration c 0 and the polymer diffusion coefficient, to determine whether the droplet will form a pillar or a flat deposit. In this work we vary concentration up to c 0 = 0.5 and molecular weight M w between 3.35kg/mol and 600kg/mol and find that in ambient conditions with c 0 = 0.1 pillars only form for a limited range, 35 ≤ M w ≤ 200 kg/mol. This observation is in contrast to the the Péclet argument in which high molecular weight polymers with a slow self-diffusion should still form pillars. We present various experimental measurements attempting to resolve this discrepancy: crossover time-scale for viscoelastic behaviour; fast diffusion of an entangled network; and droplet viscosity or contact line friction.

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“…In particular, fl uorescence correlation spectroscopy (FCS) is an excellent tool for measuring diffusion coeffi cients, because it allows access to a wide range of time scales. [28][29][30][31][32] FCS makes use of a confocal experimental setup to achieve high spatial and temporal resolution. Unlike confocal microscopy, FCS only requires a relatively low fl uorophore concentration.…”

Section: Introductionmentioning

confidence: 99%

Characterization of Diblock Copolymer Order-Order Transitions in Semidilute Aqueous Solution Using Fluorescence Correlation Spectroscopy

Clarkson

Lovett

Madsen

et al. 2015

Macromol. Rapid Commun.

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gels at relatively high concentrations. [ 1,2 ] Judicious choice of the copolymer allows the design of hydrogels that are responsive to temperature [ 3,4 ] or pH. [5][6][7][8] However, it is relatively unusual for such a copolymer to respond to both temperature and pH.In principle, biocompatible block copolymer gels can be used as a long-term cell storage medium. [ 9 ] One promising candidate for such applications is a diblock copolymer comprising poly(glycerol monomethacrylate) (PGMA) and poly(2-hydroxypropyl methacrylate) (PHPMA), which are conveniently prepared via polymerization-induced self-assembly [9][10][11][12][13] using reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization. [14][15][16] This versatile approach has enabled spherical, worm-like or vesicular copolymer morphologies to be generated in concentrated solution. [ 11,[17][18][19][20][21][22][23][24][25][26] Such a nonionic PGMA-PHPMA diblock copolymer exhibits a thermoreversibleThe temperature and pH-dependent diffusion of poly(glycerol monomethacrylate)-blockpoly(2-hydroxypropyl methacrylate) nanoparticles prepared via polymerization-induced self-assembly in water is characterized using fl uorescence correlation spectroscopy (FCS). Lowering the solution temperature or raising the solution pH induces a worm-to-sphere transition and hence an increase in diffusion coeffi cient by a factor of between four and eight. FCS enables morphological transitions to be monitored at relatively high copolymer concentrations (10% w/w) compared to those required for dynamic light scattering (0.1% w/w). This is important because such transitions are reversible at the former concentration, whereas they are irreversible at the latter. Furthermore, the FCS data suggest that the thermal transition takes place over a very narrow temperature range (less than 2 °C). These results demon strate the application of FCS to characterize orderorder transitions, as opposed to order-disorder transitions.

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Self-Diffusion and Cooperative Diffusion in Semidilute Polymer Solutions As Measured by Fluorescence Correlation Spectroscopy

Cited by 85 publications

References 111 publications

Single-Molecule Imaging Reveals Topology Dependent Mutual Relaxation of Polymer Chains

Single-Molecule Imaging Reveals Topology Dependent Mutual Relaxation of Polymer Chains

The effects of molecular weight, evaporation rate and polymer concentration on pillar formation in drying poly(ethylene oxide) droplets

Characterization of Diblock Copolymer Order-Order Transitions in Semidilute Aqueous Solution Using Fluorescence Correlation Spectroscopy

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