We have studied the short-time dynamical behavior of polydimethylsiloxane (PDMS) bottlebrush polymers, PDMS--PDMS. The samples have similar backbone lengths but different side-chain lengths, resulting in a shape transition. Quasi-elastic neutron scattering was used to observe the dynamical changes inherent to these structural changes. The combination of data from three spectrometers enabled to follow the dynamics over broad frequency and temperature ranges, which included segmental relaxations and more localized motions. The latter, identified as the methyl group rotation, is described by a threefold jump model and shows higher activation energies compared to linear PDMS. The segmental relaxation times, τ, decrease with increasing molecular weight of the side chains but increase with momentum transfer, , following a power law, which suggests a non-Gaussian behavior for bottlebrush polymers.
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http://dx.doi.org/10.1021/acs.macromol.0c01846 | DOI Listing |
J Phys Chem Lett
December 2024
Institut Max von Laue-Paul Langevin, 71 Av. des Martyrs, 38042 Grenoble, France.
Liquid-liquid phase separation (LLPS) constitutes a crucial phenomenon in biological self-organization, not only intervening in the formation of membraneless organelles but also triggering pathological protein aggregation, which is a hallmark in neurodegenerative diseases. Employing incoherent quasi-elastic neutron spectroscopy (QENS), we examine the short-time self-diffusion of a model protein undergoing LLPS as a function of phase splitting and temperature to access information on the nanosecond hydrodynamic response to the cluster formation both within and outside the LLPS regime. We investigate the samples as they dissociate into microdroplets of a dense protein phase dispersed in a dilute phase as well as the separated dense and dilute phases obtained from centrifugation.
View Article and Find Full Text PDFJ Am Chem Soc
October 2024
Department of Materials Science and Engineering, North Carolina State University, Raleigh, North Carolina 27606, United States.
J Chem Phys
October 2024
Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-6100, USA.
We present a quasi-elastic neutron scattering study of liquid deuterium hydride carried out using the Disk Chopper Spectrometer at the National Institute of Standards and Technology. Under saturated vapor pressure, the self-diffusion constant of deuterium hydride obeys an Arrhenius law D=D0exp-EA/kBT, where the prefactor D0 is given by D0=9.5±1.
View Article and Find Full Text PDFJ Am Chem Soc
October 2024
STFC Rutherford Appleton Laboratory, ISIS Neutron and Muon Facility, Chilton, Didcot OX11 0QX, U.K.
Protein dynamics play a vital role in biology. Quasi elastic neutron scattering (QENS) is an ideal method to access these dynamics. To isolate protein dynamics, it is important to separate the signal of the buffer and the protein.
View Article and Find Full Text PDFJ Phys Chem B
July 2024
Materials Science and Engineering Division, Material Measurement Laboratory, National Institute of Standards and Technology, 100 Bureau Drive, Gaithersburg, Maryland 20899, United States.
The change in the transport properties (i.e., water diffusivity, shear viscosity, etc.
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