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Fickian yet non-Gaussian diffusion (FnGD), a most intriguing open issue in soft matter, is generically associated with some dynamical and/or structural heterogeneity of the environment. Here we investigate the features of FnGD in glass-forming liquids, the epitome of dynamical heterogeneity, drawing on experiments on hard-sphere colloidal suspensions and simulations of a simple model of molecular liquid. We demonstrate that FnGD strengthens on approaching the glass transition, by identifying distinct timescales for Fickianity, τ_{F}, and for restoring of Gaussianity, τ_{G}>τ_{F}, as well as their associated length scales, ξ_{F} and ξ_{G}. We find τ_{G}∝τ_{F}^{γ} with γ≃1.8 for both systems. In the deep FnGD regime, the displacement distributions display exponential tails. We show that, in simulations, the time-dependent decay lengths l(t) at different temperatures all collapse onto a power-law master curve [l(t)/(ξ_{G})]∝(t/τ_{G})^{α}, with α=0.33. A similar collapse, if less sharp, is also found in experiments, seemingly with the same exponent α. We further discuss the connections of the timescales and length scales characterizing FnGD with structural relaxation and dynamic heterogeneity.
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http://dx.doi.org/10.1103/PhysRevLett.128.168001 | DOI Listing |
Chem Sci
August 2025
Department of Chemistry, The Chinese University of Hong Kong Shatin, N. T. Hong Kong 999077 P. R. China
Protein corona can significantly alter the interfacial physico-chemical characteristics and hydrodynamics of microentities in crowded bio-fluids. However, how this soft boundary affects the confined motion and intersurface interaction remains unknown. In this study, we used total internal reflection microscopy to directly measure the mechanical coupling underlying the confinement.
View Article and Find Full Text PDFJ Chem Phys
July 2024
Solid State Physics Division, Bhabha Atomic Research Centre, Mumbai 400085, India.
Aqueous mixtures of deep eutectic solvents (DESs) have emerged as a subject of interest in recent years for their tailored physicochemical properties. However, a comprehensive understanding of water's multifaceted influence on the microscopic dynamics, including its impact on improved transport properties of the DES, remains elusive. Additionally, the diffusion mechanisms within DESs manifest heterogeneous behavior, intricately tied to the formation and dissociation kinetics of complexes and hydrogen bonds.
View Article and Find Full Text PDFPhys Chem Chem Phys
November 2023
Department of Chemistry, Indian Institute of Technology Patna, Bihar 801106, India.
A lipid membrane undergoes a phase transition from fluid to gel phase upon changing external thermodynamic conditions, such as decreasing temperature and increasing pressure. Extremophilic organisms face the challenge of preventing this deleterious phase transition. The main focus of their adaptive strategy is to facilitate effective temperature sensing through sensor proteins, relying on the drastic changes in packing density and membrane fluidity during the phase transition.
View Article and Find Full Text PDFJ Chem Phys
November 2023
Tata Institute of Fundamental Research, Hyderabad 500046, India.
Despite the enormous theoretical and application interests, a fundamental understanding of the glassy dynamics remains elusive. The static properties of glassy and ordinary liquids are similar, but their dynamics are dramatically different. What leads to this difference is the central puzzle of the field.
View Article and Find Full Text PDFPhys Rev Lett
September 2023
Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, USA.