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Abstract Several actin-binding proteins form phase-separated condensates that promote actin filament assembly and bundling. However, the mechanism by which crosslinker multivalency, actin growth, and condensate mechanics regulate actin organization and droplet shape is not well understood. Here, using a combination of agent-based simulations and experiments, we show that a dynamically deformable droplet interface enables the emergence of tightly-bundled actin rings and weakly-bundled actin discs. We find that crosslinked bundle thickness and droplet diameter follow a power law, consistent with measurements in condensates formed by vasodilator-stimulated phosphoprotein. In addition, the dynamics of droplet deformation exhibit a dynamic snapping behavior that depends on droplet surface tension and crosslinker binding kinetics. We assess the generalizability of these predictions in condensates formed by lamellipodin and RGG. Together, these results indicate that mechanochemical feedback between droplet interfacial mechanics and crosslinker multivalency tunes actin organization and controls the dynamics of droplet deformation driven by actin networks.more » « lessFree, publicly-accessible full text available December 1, 2027
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Abstract A deeper understanding of resistive switching (RS) in 2D materials is essential for advancing neuromorphic computing. The Dissociation-Diffusion-Adsorption (DDA) model offers a useful framework for probing RS mechanisms in non-volatile memory (NVM) and in-memory computing. We have employed first-principles density functional theory (DFT) to explore dissociation, diffusion, and adsorption phenomena within the DDA model, focusing on the interactions between exemplary metal atoms (Au, Ag, Cu) and monolayer MoS2. Nudged elastic band (NEB) calculations evaluated diffusion barriers in pristine and sulfur-vacancy MoS2. Charged systems were modeled to assess the impact of applied bias on migration pathways. We also examined metal dissociation from bulk electrodes and adsorption at S vacancies. Ag/MoS2shows the lowest dissociation barrier (~0.034 eV), while Au and Cu exhibit similar values (~0.32 eV). These insights highlight Ag as a promising candidate for low-energy RS applications and provide guidance for optimizing switching efficiency in 2D memory devices.more » « lessFree, publicly-accessible full text available December 1, 2026
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Abstract Spin- and valley flavor polarization plays a central role in the many-body physics of flat band graphene, with Fermi surface reconstruction — often accompanied by quantized anomalous Hall and superconducting state — observed in a variety of experimental systems. Here we describe an optical technique that sensitively and selectively detects flavor textures via the exciton response of a proximal transition metal dichalcogenide layer. Through a systematic study of rhombohedral and rotationally faulted graphene bilayers and trilayers, we show that when the semiconducting dichalcogenide is in direct contact with the graphene, the exciton response is most sensitive to the large momentum rearrangement of the Fermi surface, providing information that is distinct from and complementary to electrical compressibility measurements. The wide-field imaging capability of optical probes allows us to obtain spatial maps of flavor order with high throughput, and with broad temperature and device compatibility. Our work helps pave the way for optical probing and imaging of flavor orders in flat band graphene systems.more » « lessFree, publicly-accessible full text available December 1, 2026
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Abstract Colloidal nanocrystal gels offer tunable optical properties governed by both the nature of the building blocks and their spatial arrangement. When assembled via reversible molecular linkers, their phase behavior and structure are primarily dictated by bond strength and lability. However, precise control over these interactions remains a significant synthetic challenge and is often system‐specific. Here, we present a simple, broadly tunable linking strategy that modulates nanocrystal phase behavior and assembly structure by leveraging competitive metal–ligand equilibria. We achieve programmable control over gelation temperature and network structure by tuning competitive metal–terpyridine and metal–halide equilibria in terpyridine‐functionalized tin‐doped indium oxide (ITO) nanocrystals, governed by metal and halide identity, concentration, and temperature, enabling wide‐range infrared optical modulation. Combined kinetic Monte Carlo and optical simulations reveal that weaker, more labile links facilitate particle crawling, leading to denser gel structures with enhanced plasmon coupling. This strategy eliminates the need for complex ligand or linker design and establishes competitive coordination chemistry as a versatile platform for engineering dynamic, stimuli‐responsive colloidal assemblies.more » « lessFree, publicly-accessible full text available November 4, 2026
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Abstract Helical spin structures are expressions of magnetically induced chirality, entangling the dipolar and magnetic orders in materials1–4. The recent discovery of helical van der Waals multiferroics down to the ultrathin limit raises prospects of large chiral magnetoelectric correlations in two dimensions5,6. However, the exact nature and magnitude of these couplings have remained unknown so far. Here we perform a precision measurement of the dynamical magnetoelectric coupling for an enantiopure domain in an exfoliated van der Waals multiferroic. We evaluate this interaction in resonance with a collective electromagnon mode, capturing the impact of its oscillations on the dipolar and magnetic orders of the material with a suite of ultrafast optical probes. Our data show a giant natural optical activity at terahertz frequencies, characterized by quadrature modulations between the electric polarization and magnetization components. First-principles calculations further show that these chiral couplings originate from the synergy between the non-collinear spin texture and relativistic spin–orbit interactions, resulting in substantial enhancements over lattice-mediated effects. Our findings highlight the potential for intertwined orders to enable unique functionalities in the two-dimensional limit and pave the way for the development of van der Waals magnetoelectric devices operating at terahertz speeds.more » « less
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Abstract An extremely rapid process for self‐assembling well‐ordered, nano, and microparticle monolayers via a novel aerosolized method is presented. The novel technique can reach monolayer self‐assembly rates as high as 268 cm2min−1from a single aerosolizing source and methods to reach faster monolayer self‐assembly rates are outlined. A new physical mechanism describing the self‐assembly process is presented and new insights enabling high‐efficiency nanoparticle monolayer self‐assembly are developed. In addition, well‐ordered monolayer arrays from particles of various sizes, surface functionality, and materials are fabricated. This new technique enables a 93× increase in monolayer self‐assembly rates compared to the current state of the art and has the potential to provide an extremely low‐cost option for submicron nanomanufacturing.more » « less
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Abstract Block polyethers comprised of poly(propylene oxide) (PPO) and poly(ethylene oxide) (PEG or PEO) segments form the basis of ABA‐type PEO‐b‐PPO‐b‐PEO poloxamer materials. The inverse architecture with an internal hydrophilic PEO segment flanked by hydrophobic blocks can be difficult to prepare with control of architecture by use of traditional anionic polymerization. These oxyanionic polymerizations are plagued by chain‐transfer‐to‐monomer side reactions that occur with substituted epoxides such as propylene oxide (PO). Herein, we report a new method for the preparation of block polymers through a controlled polymerization involving a N‐Al Lewis adduct catalyst and an aluminum alkoxide macroinitiator. The Lewis pair catalyst was able to chain‐extend commercial PEO macroinitiators to prepare di‐, tri‐, and pentablock polyethers with low dispersity and reasonable monomer tolerance. Chain extension was confirmed using size exclusion chromatography and diffusion ordered nuclear magnetic resonance spectroscopy. The resulting block polymers were additionally analyzed with small‐angle X‐ray scattering to correlate the morphology to molecular architecture.more » « less
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Controlling the structure and function of colloidal gels requires a detailed understanding of how the various components govern network formation and aging. In particular, molecular additives like salts are widely used to tune interparticle interactions, yet their influence on gelation pathways in complex systems such as colloidal nanocrystal gels remains inadequately understood. Here, we investigate how noncoordinating salts modulate the evolution of gels formed using chemically linked tin-doped indium oxide nanocrystals. Through combined structural, dynamic, and kinetic analyses, we demonstrate that increasing salt concentration accelerates gelation. When rescaled by salt-dependent characteristic times, the evolution collapses onto universal trajectories, revealing a time-salt superposition principle. The universality extends across length scales, suggesting a consistent salt-dependent mechanism that controls both local structuring and macroscopic network formation. This observed salt modulation of structure and dynamics provides a predictive basis for controlling the kinetics of nonequilibrium nanocrystal gel assembly, enhancing the rational design of functional nanomaterials with tunable properties.more » « lessFree, publicly-accessible full text available March 13, 2027
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Soft and active condensed matter represent a class of fascinating materials that we encounter in our everyday lives—and constitute life itself. Control signals interact with the dynamics of these systems, and this influence is formalized in control theory and optimal control. Recent advances have employed various control-theoretical methods to design desired dynamics, properties, and functionality. Here, we provide an introduction to optimal control aimed at physicists working with soft and active matter. We describe two main categories of control, feedforward control and feedback control, and their corresponding optimal control methods. We emphasize their parallels to Lagrangian and Hamiltonian mechanics and provide a worked example problem. Finally, we review recent studies of control in soft, active, and related systems. Applying control theory to soft, active, and living systems will lead to an improved understanding of the signal processing, information flows, and actuation that underlie the physics of life.more » « lessFree, publicly-accessible full text available March 13, 2027
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Dynamic covalent cross-links impart hydrogels with viscoelastic and self-healing properties, motivating applications as biomimetic cell scaffolds and injectable materials. The long bond lifetime results in complex rheological behavior including shear thickening. We hypothesized that this behavior applies broadly across dynamic covalent hydrogels and can be engineered through reaction rate constants. Thus, we synthesized multiarm poly(ethylene glycol) (PEG) hydrogels with conjugate addition, boronate ester, or terpyridine-zinc cross-links, which tune bond dissociation kinetics and hydrogel relaxation times over four orders of magnitude. All formulations exhibited shear thickening, with the onset dictated by the relaxation time. Although multiple mechanisms may underlie this behavior, chain stretching is hypothesized to contribute to shear thickening, as the cross-linking concentration remained constant under shear and networks with more defects correlated with increased shear thickening. These molecular and structural drivers of shear thickening apply across dilute dynamic covalent tetra-PEG hydrogels, clarifying their suitability for applications under shear.more » « lessFree, publicly-accessible full text available March 6, 2027
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