Via event-driven molecular dynamics simulations and experiments, we study the packing-fraction and shear-rate dependence of single-particle fluctuations and dynamic correlations in hard-sphere glasses under shear. At packing fractions above the glass transition, correlations increase as shear rate decreases: the exponential tail in the distribution of single-particle jumps broadens and dynamic four-point correlations increase. Interestingly, however, upon decreasing the packing fraction, a broadening of the exponential tail is also observed, while dynamic heterogeneity is shown to decrease. An explanation for this behavior is proposed in terms of a competition between shear and thermal fluctuations. Building upon our previous studies [Chikkadi et al., Europhys. Lett. 100, 56001 (2012)], we further address the issue of anisotropy of the dynamic correlations.
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Nano Lett
January 2025
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, P.R. China.
Crystals with three-dimensional (3D) stereoscopic structures, characterized by diverse shapes, crystallographic planes, and morphologies, represent a significant advancement in catalysis. Differentiating and quantifying the catalytic activity of specific surface facets and sites at the single-particle level is essential for understanding and predicting catalytic performance. This study employs super-resolution radial fluctuations electrogenerated chemiluminescence microscopy (SRRF-ECLM) to achieve high-resolution mapping of electrocatalytic activity on individual 3D CuO crystals, including cubic, octahedral, and truncated octahedral structures.
View Article and Find Full Text PDFSuper-resolution optical fluctuation imaging (SOFI) rapidly generates super-resolution images by analyzing fluorescence intensity fluctuations. However, fluorophores for high-order SOFI applications are very rare. Here, we report ultrasmall semiconducting polymer dots (Pdots) to achieve high-order SOFI at single-particle and cellular levels.
View Article and Find Full Text PDFACS Nano
January 2025
Department of Chemistry, Indiana University, Bloomington, Indiana 47405, United States.
Nature
January 2025
Max-Planck-Institut für Quantenoptik, Garching, Germany.
J Chem Theory Comput
January 2025
Materials Science Department, Graduate School of Engineering, Chiba University, Chiba 263-8522, Japan.
The standard definition of particle number fluctuations based on point-like particles neglects the excluded volume effect. This leads to a large and systematic finite-size scaling and an unphysical surface term in the isothermal compressibility. We correct these errors by introducing a modified pair distribution function that takes account of the finite size of the particles.
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