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Flip de Jong

Publications and source records attributed to Flip de Jong.

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Three-dimensional Optical Reconstruction of colloidal electrokinetics via multiplane imaging

Sorting, filtering, moving and controlling colloidal particles is crucial in many fields, ranging from chemistry to biology and physics. Dielectrophoresis is an outstanding tool for the manipulation of small particles by AC electric fields, due to its high selectivity and the absence of the need for labels. We use a new theoretical-experimental approach to study the dynamics of fluorescently labeled polystyrene nanoparticles of 200 nm under positive and negative dielectrophoresis conditions. Our multiplane widefield microscopy technique combined with single particle tracking offers real-time ($>$ 100 fps) superresolved visualization of colloidal dynamics in three spatial dimensions. This real-time 3D imaging technique allows the reconstruction of superresolved trajectories, enabling the visualisation of local forces with unprecedented detail. To interpret this data, a dedicated multiscale modeling approach was developed, targeting a direct comparison between theory and experiment. In the current model DEP and electro-osmotic forces were considered. Under positive DEP conditions, this resulted in a very good agreement with experiment. Under negative DEP conditions, the agreement is less clear, indicating the importance of other effects. This illustrates the potential of this combined 3D imaging and modeling approach to validate and refine our theoretical understanding of AC field induced colloidal dynamics. This framework is broadly applicable to other complex fluid or microfluidic motion.

cond-mat.soft

Amorphous to Crystalline Transformation: How Cluster Aggregation Drives the Multistep Nucleation of ZIF-8

Nucleation, the pivotal first step of crystallization, governs essential characteristics of crystallization products, including size distribution, morphology, and polymorphism. While understanding this process is paramount to the design of chemical, pharmaceutical and industrial production processes, major knowledge gaps remain, especially with respect to the crystallization of porous solids. Also for nanocrystalline ZIF-8, one of the most widely studied metal-organic frameworks, questions regarding the species involved in the nucleation pathway and their structural and chemical transformations remain unanswered. By combining harmonic light scattering, inherently sensitive to structural changes, with NMR spectroscopy, which reveals molecular exchanges between particles and solution, we were able to capture the crystallization mechanism of ZIF-8 in unprecedented detail. This dual approach provides concurrent structural and chemical insights, revealing key processes not previously observed in ZIF crystallization. Upon mixing small charged prenucleation clusters (PNCs) are formed, exhibiting an excess of ligands and net positive charge. We show that nucleation is initiated by aggregation of PNCs, through the release of ligands and associated protons to the liquid. This leads to the formation of charge neutral amorphous precursor particles (APPs) which incorporate neutral monomers from solution, and crystallize ZIF-8. Our work highlights chemical dynamics as a vital, yet often overlooked, dimension in the multi-stage structural evolution of MOFs. By establishing the critical role of PNCs in the nucleation of ZIF-8, new pathways open up for controlling crystallization of metal-organic frameworks through targeted chemical interactions with these species.

cond-mat.mtrl-sci