Experimental Evidence for a Cluster Glass Transition in Concentrated Lysozyme Solutions

The Journal of Physical Chemistry. B
Maxime J BergmanAnna Stradner

Abstract

Lysozyme is known to form equilibrium clusters at pH ≈ 7.8 and at low ionic strength as a result of a mixed potential. While this cluster formation and the related dynamic and static structure factors have been extensively investigated, its consequences on the macroscopic dynamic behavior expressed by the zero shear viscosity η0 remain controversial. Here we present results from a systematic investigation of η0 using two complementary passive microrheology techniques, dynamic light scattering based tracer microrheology, and multiple particle tracking using confocal microscopy. The combination of these techniques with a simple but effective evaporation approach allows for reaching concentrations close to and above the arrest transition in a controlled and gentle way. We find a strong increase of η0 with increasing volume fraction ϕ with an apparent divergence at ϕ ≈ 0.35, and unambiguously demonstrate that this is due to the existence of an arrest transition where a cluster glass forms. These findings demonstrate the power of tracer microrheology to investigate complex fluids, where weak temporary bonds and limited sample volumes make measurements with classical rheology challenging.

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Citations

Jun 24, 2019·The Journal of Chemical Physics·M Litniewski, A Ciach
Dec 13, 2019·Soft Matter·Anna Stradner, Peter Schurtenberger
Jan 16, 2020·The Journal of Physical Chemistry. B·Chiho WatanabeMiho Yanagisawa
Nov 17, 2020·ACS Nano·Jasper N ImminkPeter Schurtenberger
Aug 14, 2020·Molecular Pharmaceutics·Tuan Phan-XuanVitaly Kocherbitov

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Methods Mentioned

BETA
rheology
dynamic light scattering
rheometry

Software Mentioned

MPT
IDL

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