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Timon Kratzenberg

Publications and source records attributed to Timon Kratzenberg.

3 recordsLinked to original sources

Substrate contact angle governs microgel shape, stiffness and deposition pattern

Soft microgels are widely used as deformable building blocks for two-dimensional assemblies, yet solid substrates are often treated as passive supports after interfacial deposition. Here, we show that substrate wettability mechanically preconditions soft microgels before drying. Using in-liquid force-volume atomic force microscopy, we find that the same microgels adopt markedly different hydrated shapes and stiffness profiles depending on substrate contact angle: hydrophobic substrates induce spreading, flattening, and internal stiffening, whereas hydrophilic substrates preserve taller, softer microgels with smaller contact areas. These single-microgel states can explain how Langmuir-Blodgett-deposited monolayers respond during drying. On hydrophilic substrates, the observed assemblies are consistent with soft and weakly immobilized microgels rearranging under immersion-capillary forces, producing distinct corona-corona and core-core contact states and an apparent isostructural transition. On hydrophobic substrates, the flattened and stiffened microgels are more strongly immobilized, likely suppressing capillary-driven rearrangements and largely preserving the transferred interfacial assembly structure. These findings establish substrate-controlled microgel mechanics as the missing link between interfacial self-assembly and the final structures observed after transfer and drying.

cond-mat.soft

Unraveling the Mechanisms of Ultrasound-Induced Mechanical Degradation of Microgels: Effects of Mechanoresponsive Crosslinks, Softness, and Core-Shell Architecture

Ultrasound-induced degradation of soft polymeric colloids, like microgels, as well as a controlled drug release enabled by mechanoresponsive bonds, has recently attracted considerable attention. However, most examples in the literature focus primarily on the applications rather than examining the underlying mechanisms of the structural changes occurring in microgels due to cavitation - changes that are crucial for developing effective drug delivery systems. In this work, we provide a comprehensive view on how microgel structure governs the susceptibility to rupture and mass loss upon cavitation, investigating both conventional microgels containing mechanoresponsive disulfide bonds and more complex asymmetrically crosslinked core-shell microgels. By combining dynamic and static light scattering, small-angle X-ray scattering, and atomic force microscopy, we demonstrate that an interplay between mechanoresponsive crosslinks and the swelling degree determines the microgels susceptibility to ultrasound-induced damage. Our findings indicate that local stress from cavitation bubbles varies strongly within the microgel dispersion. The majority of microgels undergo gradual erosion at their periphery, resulting in smaller yet structurally intact particles over time, observable by light scattering and AFM. In contrast, microgels closer to a cavitation bubble can experience partial rupture or completely disintegrate, producing smaller, more polydisperse fragments, which contributes substantially to the overall mass loss observed. In the core-shell microgels with different crosslinkers in the core and shell, degradation occurs nearly uniformly across both regions, instead of selectively targeting the weaker part. These observations highlight the complexity of the degradation dynamics as well as the similarity to processes seen in linear polymers and bulk hydrogels.

cond-mat.soft

Anisotropic Microgels show their Soft Side

Anisotropic, submicrometer sized particles are versatile systems providing interesting features in creating ordering in 2-dimensional systems. Combining hard ellipsoids with a soft shell further enhances the opportunities to trigger and control order and alignment. In this work, we report a rich 2D phase behavior and show how softness affects the ordering of anisotropic particles at fluid oil-water interfaces. Three different core-shell systems were synthesized such that they have the same elliptical hematite-silica core but differ with respect to thickness and stiffness of the soft microgel shell. Compression isotherms, the shape of individual core-shell microgel as well as their 2D order at a decane-water interface are investigated by means of the Langmuir-Blodgett technique combined with ex-situ Atomic Force Microscopy (AFM) imaging, as well as by Disspiative Particle Dynamics (DPD) simulations. We show how softness, size and anisotropy of the microgel shell affect the side-to-side vs. tip-to-tip ordering of anisotropic hybrid microgels as well as the alignment with respect to the direction of compression in the Langmuir trough. A large and soft microgel shell leads to an ordered structure with a tip-to-tip alignment directed perpendicular to the direction of compression. In contrast, a thin and harder microgel shell leads to side-to-side ordering orientated parallel to the compression direction. In addition, the thin and harder microgel shell induces clustering of the microgels in the dilute state indicating the presence of strong capillary interactions. Our findings highlight the relevance of softness for the complex ordering of anisotropic hybrid microgels at interfaces.

cond-mat.soft