Probing the interplay between chain diffusion and polymer crystal growth under nanoscale confinement: a study by single molecule fluorescence microscopy

Lü, Xi; Zheng, Kaikai; Yang, Jingfa; Zhao, Jiang

doi:10.1007/s11426-018-9290-3

Cited by 4 publications

(4 citation statements)

References 48 publications

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“…The negative C v (0.1 s) value reaches −0.31 at 8.5 c *, which agrees with the reptation behavior of DNA tubes confined in the entangled PEO network. Together, the increasingly subdiffusive and anticorrelation behavior suggests that the confinement effect becomes stronger at higher polymer concentrations, in agreement with the findings in other reports. − …”

Section: Resultssupporting

confidence: 92%

Crowding and Confinement Effects in Different Polymer Concentration Regimes and Their Roles in Regulating the Growth of Nanotubes

et al. 2019

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Among numerous research studies focusing on macromolecular crowding and confinement, few are concerned with the medium at a broad range of concentrations, let alone the interplay between the crowding effect and confinement effect. In this work, we systematically studied the assembly of DNA tiles into nanotubes in polyethylene oxide (PEO) and polyacrylamide (PAM) media covering the concentration range of dilute, semidilute, and concentrated regimes. In light of the structure and kinetics of DNA assembly, both the PEO and PAM media can be divided into three regimes with increasing polymer concentration: the crowding regime, double-effect regime, and confinement regime. In the crowding regime, DNA tiles only form clusters because the assembly into a tube structure is hindered. In the double-effect regime, polymer chains form a transient network whose pore size is close to the diameter of DNA nanotubes. The confinement effect, together with the crowding effect, facilitates the assembly of DNA tiles into a tube structure. In the confinement regime, the length of DNA tubes decreases with polymer concentration, which can be quantitatively described by a scaling relationship. The borderlines of the three regimes are polymer-specific. The PEO medium enters the double-effect regime and confinement regime at concentrations much lower than the PAM medium, suggesting that the PEO medium exhibits stronger macromolecular crowding and confinement effects. We attribute it to the special hydrophilicity of PEO, which has the capability to couple with the lattice structure of a water network, leading to a decrease in thermal motion and hence a mutual stabilization.

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Section: Resultssupporting

confidence: 92%

Crowding and Confinement Effects in Different Polymer Concentration Regimes and Their Roles in Regulating the Growth of Nanotubes

et al. 2019

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“…In the study presented here, the single-particle tracking was enabled by combining total internal reflection fluorescence microscopy with a high-throughput tracking algorithm, which involved the identification of fluorescence objects by convolving each image with a disk or Gaussian matrix and linking the identified objects to create trajectories. This algorithm enabled the accumulation of 10 5 –10 7 trajectories at an experimental-accessible timescale and was successfully applied to study diffusion in different scenarios such as in complex environments − and at interfaces. − The observation from a single-particle landscape allows one to go beyond the understanding of the average behavior and captures more details regarding subpopulations or transient dynamical phenomena through high temporal and spatial resolutions. By tracking nanoparticle diffusion at a surfactant-laden interface, we found that when the interfacial coverage of surfactant exceeded a threshold the nanoparticle diffusion exhibited a two-regime behavior, manifesting as short-time Brownian and long-time anomalous diffusion.…”

Section: Introductionmentioning

confidence: 99%

Tracking of Nanoparticle Diffusion at a Liquid–Liquid Interface Adsorbed by Nonionic Surfactants

Zhao

Wang

2021

Langmuir

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Emulsions stabilized by both nanoparticles and surfactants often display longer shelf life than those stabilized by nanoparticles or surfactants alone. Although numerous works have been conducted to understand the effect of nanoparticles and surfactants on the variation of interfacial tension, little is known about interfacial diffusion when both nanoparticles and surfactants are present at interfaces. In this work, we used single-particle fluorescence tracking to study the lateral diffusion of individual hydrophobic nanoparticles at hexane−glycerol interfaces adsorbed by different amounts of nonionic surfactants. When the surfactant concentration is over a threshold, we found that the nanoparticle diffusion exhibits a two-regime behavior involving short-time Brownian and the emergence of subdiffusive, non-Gaussian, and dynamically anticorrelated diffusion in the long lag time regime. A stepwise analysis rationalized diffusion in different lag time regimes, leading to a mechanistic interpretation regarding the two-regime behavior. These results could provide insight into the understanding of the synergistic effect for the surfactant-assistant Pickering emulsion.

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“…34−46 By combining TIRFM with a highly sensitive camera, this technique can exploit the evanescent field to illuminate fluorescent molecules within 100 nm of the interface. This makes it very suitable for studying the diffusion and adsorption of polymers, peptides, and proteins in ultrathin films, 47 on lipid bilayers, 48,49 at interfaces, 50−59 during chemical reaction, 60 and for quantifying the spatial/temporal heterogeneity upon protein adsorption. 27,61−63 In this study, we utilized TIRFM to investigate the adsorption and desorption processes of human serum albumin (HSA), the most abundant serum protein, on poly(L-lactic acid) (PLLA) film surfaces with different molar masses.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Protein adsorption has been extensively studied using various sensitive techniques such as quartz crystal microbalance, mass spectrometry, sum frequency generation spectroscopy, Fourier transform infrared spectroscopy, fluorescence correlation spectroscopy, isothermal titration calorimetry, and atomic force microscopy (AFM). ,, These techniques have greatly contributed to our understanding of protein adsorption. – Recently, total internal reflection fluorescence microscopy (TIRFM) has emerged as a powerful tool for studying the dynamics of fluorescent species in different environments at a spatial resolution of approximately 10 nm and a temporal resolution of a few milliseconds. – By combining TIRFM with a highly sensitive camera, this technique can exploit the evanescent field to illuminate fluorescent molecules within 100 nm of the interface. This makes it very suitable for studying the diffusion and adsorption of polymers, peptides, and proteins in ultrathin films, on lipid bilayers, , at interfaces, – during chemical reaction, and for quantifying the spatial/temporal heterogeneity upon protein adsorption. ,– …”

Section: Introductionmentioning

confidence: 99%

Tracking of Protein Adsorption on Poly(l-lactic acid) Film Surfaces: The Role of Molar Mass

Lyu,

Zhao,

Zhang

et al. 2023

Langmuir

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Poly(l-lactic acid) (PLLA) has been extensively utilized as a biomaterial for various biomedical applications. The first and one of the most critical steps upon contact with biological fluids is the adsorption of proteins on the material’s surface. Understanding the behavior of protein adsorption is vital for guiding the synthesis and preparation of PLLA for biomedical purposes. In this study, total internal reflection fluorescence microscopy was employed to investigate the adsorption of human serum albumin (HSA) on PLLA films with different molar masses. We found that molar mass affects HSA adsorption in such a way that it affects only the adsorption rate constants, but not the desorption rate constants. Additionally, we observed that HSA adsorption is spatially heterogeneous and exhibits many strong binding sites regardless of the molar mass of the PLLA films. We found that the free volume of PLLA plays a crucial role in determining its water uptake capacity and surface hydration, consequently impacting the adsorption of HSA.

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Probing the interplay between chain diffusion and polymer crystal growth under nanoscale confinement: a study by single molecule fluorescence microscopy

Cited by 4 publications

References 48 publications

Crowding and Confinement Effects in Different Polymer Concentration Regimes and Their Roles in Regulating the Growth of Nanotubes

Crowding and Confinement Effects in Different Polymer Concentration Regimes and Their Roles in Regulating the Growth of Nanotubes

Tracking of Nanoparticle Diffusion at a Liquid–Liquid Interface Adsorbed by Nonionic Surfactants

Tracking of Protein Adsorption on Poly(l-lactic acid) Film Surfaces: The Role of Molar Mass

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