Dynamics of amphiphilic PEG-PDMS-PEG triblock copolymer assemblies

Sudipta Gupta; Rasangi M. Perera; Christopher J. Van Leeuwen; Tianyu Li; Laura Stingaciu; Markus Bleuel; Kunlun Hong; Gerald J. Schneider

doi:10.1088/1361-648X/adfd32

Dynamics of amphiphilic PEG-PDMS-PEG triblock copolymer assemblies

Sudipta Gupta
, Rasangi M. Perera
, Christopher J. Van Leeuwen
, Tianyu Li
, Laura Stingaciu
, Markus Bleuel
, Kunlun Hong
, Gerald J. Schneider

SANS & Spin Echo

Research output: Contribution to journal › Article › peer-review

Abstract

The size and stability of micelles and vesicles determine the uptake capacity of guest molecules, thereby influencing potential applications in drug/gene delivery, bioreactors, and templates for nanoparticle synthesis. Polyethylene glycol (PEG) and polydimethylsiloxane (PDMS) are commonly used in these applications. We discovered that PEG-PDMS-PEG triblock copolymers can assemble into micelles and vesicles, making them valuable for dynamic studies to derive the bending elasticity, κ η , which governs the stability these objects. We analyzed the structure using cryogenic transmission electron microscopy and small-angle neutron scattering. We investigated the dynamics through dynamic light scattering and neutron spin echo spectroscopy. By varying the number of repeating units in the hydrophilic block, we created micellar (PEG₂₈-PDMS₁₅-PEG₂₈) and vesicular systems (PEG₁₄-PDMS₁₅-PEG₁₄). For the vesicle, membrane rigidity was determined from experiments to be κ η = ( 16 ± 2) k B T , where k B T is the thermal energy ( k B Boltzmann’s constant and T is the temperature). According to Zilman and Granek’s concept, membrane rigidity reflects height-height fluctuations within the membrane layer. Compared to polymers at the oil-water interface of a microemulsion, the membrane rigidity in polymersomes is over an order of magnitude higher, indicatingsignificantly enhanced stability. This value closely aligns with that of liposomes, suggesting similar stability between polymersomes and liposomes.

Original language	English
Article number	355402
Journal	Journal of Physics Condensed Matter
Volume	37
Issue number	35
DOIs	https://doi.org/10.1088/1361-648X/adfd32
State	Published - Sep 1 2025

Funding

The authors express their sincere gratitude for the funding provided by the U.S. Department of Energy (DOE) through Grant DE-SC0019050. This funding enabled them to access the NSE spectrometer and small-angle scattering instruments at the Center for High-Resolution Neutron Scattering. This partnership was established between the NIST and the National Science Foundation (Agreement No. DMR-1508249). Additionally, research conducted at the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory (ORNL) was supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, DOE. Polymer synthesis and characterization were conducted at the Center for Nanophase Materials Sciences (CNMS), a DOE Office of Science User Facility. Furthermore, access to the NG7 SANS instrument was facilitated through a partnership between NIST and NSF under Agreement No. DMR-201079. Special appreciation goes to Jeff Krzywon for his invaluable support on the NG7 beamline, Rafael Cueto (LSU) for his assistance with dynamic light scattering experiments, and Jibao He (Tulane University) for his support with cryo-TEM imaging.

Keywords

Zilman and Granek model
copolymer nano-scale assemblies
membrane dynamics
neutron spin echo spectroscopy
small-angle neutron scattering

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10.1088/1361-648X/adfd32

Cite this

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title = "Dynamics of amphiphilic PEG-PDMS-PEG triblock copolymer assemblies",

abstract = "The size and stability of micelles and vesicles determine the uptake capacity of guest molecules, thereby influencing potential applications in drug/gene delivery, bioreactors, and templates for nanoparticle synthesis. Polyethylene glycol (PEG) and polydimethylsiloxane (PDMS) are commonly used in these applications. We discovered that PEG-PDMS-PEG triblock copolymers can assemble into micelles and vesicles, making them valuable for dynamic studies to derive the bending elasticity, κ η , which governs the stability these objects. We analyzed the structure using cryogenic transmission electron microscopy and small-angle neutron scattering. We investigated the dynamics through dynamic light scattering and neutron spin echo spectroscopy. By varying the number of repeating units in the hydrophilic block, we created micellar (PEG28-PDMS15-PEG28) and vesicular systems (PEG14-PDMS15-PEG14). For the vesicle, membrane rigidity was determined from experiments to be κ η = ( 16 ± 2) k B T , where k B T is the thermal energy ( k B Boltzmann{\textquoteright}s constant and T is the temperature). According to Zilman and Granek{\textquoteright}s concept, membrane rigidity reflects height-height fluctuations within the membrane layer. Compared to polymers at the oil-water interface of a microemulsion, the membrane rigidity in polymersomes is over an order of magnitude higher, indicatingsignificantly enhanced stability. This value closely aligns with that of liposomes, suggesting similar stability between polymersomes and liposomes.",

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AU - Hong, Kunlun

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AB - The size and stability of micelles and vesicles determine the uptake capacity of guest molecules, thereby influencing potential applications in drug/gene delivery, bioreactors, and templates for nanoparticle synthesis. Polyethylene glycol (PEG) and polydimethylsiloxane (PDMS) are commonly used in these applications. We discovered that PEG-PDMS-PEG triblock copolymers can assemble into micelles and vesicles, making them valuable for dynamic studies to derive the bending elasticity, κ η , which governs the stability these objects. We analyzed the structure using cryogenic transmission electron microscopy and small-angle neutron scattering. We investigated the dynamics through dynamic light scattering and neutron spin echo spectroscopy. By varying the number of repeating units in the hydrophilic block, we created micellar (PEG28-PDMS15-PEG28) and vesicular systems (PEG14-PDMS15-PEG14). For the vesicle, membrane rigidity was determined from experiments to be κ η = ( 16 ± 2) k B T , where k B T is the thermal energy ( k B Boltzmann’s constant and T is the temperature). According to Zilman and Granek’s concept, membrane rigidity reflects height-height fluctuations within the membrane layer. Compared to polymers at the oil-water interface of a microemulsion, the membrane rigidity in polymersomes is over an order of magnitude higher, indicatingsignificantly enhanced stability. This value closely aligns with that of liposomes, suggesting similar stability between polymersomes and liposomes.

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Dynamics of amphiphilic PEG-PDMS-PEG triblock copolymer assemblies

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