Polymeric particles with complex shapes are required for biomedical therapies, colloidal self‐assembly, and micro‐robotics. It has been challenging to synthesize particles beyond simple shapes (e.g., spheres, cubes) with high structural accuracy using existing methods. Here, a method for fabricating polymeric microparticles of complex 3D shapes is reported using two‐photon lithography, and dispersing the particles in an aqueous solution on a glass substrate. The fabrication of polyhedrons (e.g., tetrahedron, pyramid), polypods (e.g., tetrapod, hexapod), and other shapes of 5–10 µm in size is demonstrated. Confocal microscopy is used to track the motion of the sphere, tetrahedron, tetrapod, and screw‐shaped particles near the substrate, and determine their translational diffusion coefficients. HYDRO++ is used to simulate the motion of the particles far from the substrate. The influence of particle size and substrate effects on diffusion in the spherical particles is determined and finds that the non‐spherical particles have increased hindrance at the substrate compared to the spherical particles.
This content will become publicly available on May 15, 2025
- Award ID(s):
- 2223084
- NSF-PAR ID:
- 10530561
- Publisher / Repository:
- Royal Society of Chemistry
- Date Published:
- Journal Name:
- Soft Matter
- Volume:
- 20
- Issue:
- 19
- ISSN:
- 1744-683X
- Page Range / eLocation ID:
- 3942-3953
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Abstract -
The dynamics of viscoelastic fluids are governed by a memory function, essential yet challenging to compute, especially when diffusion faces boundary restrictions. We propose a computational method that captures memory effects by analyzing the time-correlation function of the pressure tensor, a viscosity indicator, through the Stokes–Einstein equation’s analytic continuation into the Laplace domain. We integrate this equation with molecular dynamics simulations to derive necessary parameters. Our approach computes nuclear magnetic resonance (NMR) line shapes using a generalized diffusion coefficient, accounting for temperature and confinement geometry. This method directly links the memory function with thermal transport parameters, facilitating accurate NMR signal computation for non-Markovian fluids in confined geometries.
-
This study explores the impact of electric field and temperature on flash sintering of zirconia nanoparticles using molecular dynamics simulations. The findings suggest that the electric field effect is secondary to the temperature effect. A comparison of simulations varying temperature and electric field reveals a more significant difference in diffusion coefficient with temperature variations. Furthermore, the electric field effect does not exhibit a consistent monotonic trend, as seen in the changing order of curves when temperature increases. The induced electric field contributes to crystal orientation alignment and promotes surface mechanisms throughout sintering stages. While a higher electric field leads to greater atomic motion in the initial stage, the relationship is not strictly monotonic. However, it consistently enhances the diffusion coefficient of surface atoms, highlighting its role in surface mechanisms. Further research is warranted to fully understand the interplay between electric field, temperature, and sintering mechanisms.more » « less
-
Abstract We investigate the effect of steric and hydrodynamic interactions (HI) on quiescent diffusion and flow‐driven transport of finite‐sized nanoparticles through periodic 2D (two‐dimensional) and 3D (three‐dimensional) nanopost arrays using Stokesian dynamics simulations. We find that steric and HI hinder particle diffusivity under quiescent conditions and enhance longitudinal dispersion under flow. Moreover, the presence of HI leads to a power‐law increase in the longitudinal dispersion coefficient with Pe due to spatial variations in the fluid velocity. Lastly, our simulations reveal that longitudinal particle dispersion coefficients behave similarly in 2D and 3D when HI are included.
-
The first paper of this series [J. Chem. Phys. 158, 034103 (2023)] demonstrated that excess entropy scaling holds for both fine-grained and corresponding coarse-grained (CG) systems. Despite its universality, a more exact determination of the scaling relationship was not possible due to the semi-empirical nature. In this second paper, an analytical excess entropy scaling relation is derived for bottom-up CG systems. At the single-site CG resolution, effective hard sphere systems are constructed that yield near-identical dynamical properties as the target CG systems by taking advantage of how hard sphere dynamics and excess entropy can be analytically expressed in terms of the liquid packing fraction. Inspired by classical equilibrium perturbation theories and recent advances in constructing hard sphere models for predicting activated dynamics of supercooled liquids, we propose a new approach for understanding the diffusion of molecular liquids in the normal regime using hard sphere reference fluids. The proposed “fluctuation matching” is designed to have the same amplitude of long wavelength density fluctuations (dimensionless compressibility) as the CG system. Utilizing the Enskog theory to derive an expression for hard sphere diffusion coefficients, a bridge between the CG dynamics and excess entropy is then established. The CG diffusion coefficient can be roughly estimated using various equations of the state, and an accurate prediction of accelerated CG dynamics at different temperatures is also possible in advance of running any CG simulation. By introducing another layer of coarsening, these findings provide a more rigorous method to assess excess entropy scaling and understand the accelerated CG dynamics of molecular fluids.more » « less