Self-Assembled Soft Matter

Liquid-liquid phase separation offer a strategy for targeting biomaterial scaffolds, but controlling assembly to form functional materials is challenging. Here, the authors transform native proteins into amyloid fibres for assembly, and use the materials as a gastric ulcer protective agent.

Aqueous two-phase systems form interfaces and compartments, but converting the liquid structures to functional solids is challenging. Here, the authors use poly(ionic liquids) to form such systems, which can then be converted to gels and used for desalination.

Preparing heterogeneous hydrogels with distinct phases is desirable for the mimicking of biological tissues, but generally requires complex techniques. Here, the authors report a method that uses phase separation to fabricate two-aqueous phase soft materials with distinct properties at different length scales.

Coacervate droplets have potential as components for cell-like materials, but are limited by complex molecular structure and control of the internal microenvironment. Here, the authors report stable dipeptide-based coacervates with a microenvironment for the encapsulation of hydrophobic species.

Coacervate-based compartments are attractive as potential protocells, but formation and control of the compartments can be challenging. Here, the authors report the spontaneous formation of core-shell, cell-sized coacervate compartments driven by droplet evaporation.

Biomolecular condensates with internal structure allow cells to further organise their processes. In this work the authors investigate how condensates can obtain an internal structure with droplets of dilute phase inside via kinetic, rather than purely thermodynamic driving forces.

The molecular mechanisms underlying the formation of biomolecular condensates have not been fully elucidated. Here the authors show that the LLPS propensity, dynamics, and encapsulation efficiency of designed peptide condensates can be tuned by subtle changes to the peptide composition.

Earlier methods for droplet network stabilization require extremely precise control and manipulation with considerable energy consumption, making them difficult to implement. Here, the authors present 2D interfacial networks, formed by irreversible interfacial interactions between polymer chains dissolved in one liquid and ligands dissolved in a second immiscible liquid at random points along the chains.

Under-oil open microfluidic systems have potential for studying multi-phase chemical reactions but have so far demonstrated largely only for biological applications. Here, the authors report the development of a system for in situ characterization of gas-liquid reactions by Raman spectroscopy.

Native spider silk has desirable mechanical properties, but these are challenging to replicate in an artificial material. Here, the authors report the use of a microfluidic system to create continuous fibers based on recombinant spidroin.

Coacervate droplets are promising protocells that sequester nutrients, but how new peptides could be synthesized inside coacervates remains a mystery. Here, the authors develop redox-active coacervates that facilitate the formation of new peptide bonds.

Stimuli-responsive emulsions are useful for long-term storage combined with controlled release, but the fundamental mechanism behind this release is not established. Here, the authors report a study into the effect of individual microgel morphology on the destabilisation of responsive emulsions.

Liquid–liquid phase separation is known in cell biology as an underlying mechanism of intracellular organization. The authors study a complex interplay between phase separation, network mechanics, and condensate capillarity, providing explanation for the phenomena in complex environments like the cellular interior.

Phase separation is driven by the component activity, elasticity, or composition of a homogeneous mixture. Here the authors, develop heterogeneous colloidal suspensions exhibiting both liquid-liquid phase separation of polymers and liquid crystal phase separation of nanoparticles controlled by the trade-off between thermodynamics and kinetics.

Three-dimensional conductive hydrogels have promise in bioelectronics, yet achieving the desired conductivity and mechanical properties in 3D structured hydrogels is challenging. Here, the authors report a liquid-in-liquid 3D printing process for preparation of desirable PEDOT:PSS hydrogels.

Producing functional soft fibers via existing spinning methods is environmentally and economically costly due to the complexity of spinning equipment, involvement of copious solvents, intensive consumption of energy. Here, the authors report a nonsolvent vapor-induced phase separation spinning approach under ambient conditions, which resembles the native spider silk fibrillation’.

In heterogeneous colloidal systems, composition, shape, structure and physical properties result from the trade-off between thermodynamic and kinetic effects during nucleation and growth. Here, the authors demonstrate that kinetic and thermodynamic effects can be disentangled by careful selection of a colloidal systems and controlling phase separation in microfluidic devices

Water/water phase separation in cells facilitates the spatial localization of biological components, but its influence on mechanical processes driven by protein motors has been largely overlooked. Here, the interface of water/water phase separation is shown to produce mechanical motion by spontaneously entrapping kinesins and microtubules and generating a micrometre-scale vortex flow inside cell-sized droplets.

The dynamic regulation of supramolecular chirality in non-equilibrium systems can provide valuable insights into molecular self-assembly in living systems. Here, the authors demonstrate the use of chemical fuels for regulating self-assembly pathway, which thereby controls the supramolecular chirality of a non-equilibrium assembled system.

Assembly of amyloids is important in neurodegenerative diseases, but there is limited understanding of how supramolecular chirality is controlled. Here, the authors report the design of peptide derivatives that allow chirality inversion at biologically relevant temperatures.

Janus particles commonly exhibit a high-symmetry patch, constraining the range of possible assemblies. Here, the authors devise a synthetic approach to fine-tune the patch symmetry in Janus particles and showcase the assembly of these particles into chiral colloidal clusters.

Achieving close contact between organic and inorganic components in nanostructures is critical for performance. Here, the interfacial interaction in titanium oxide-based organic-inorganic nanoheterojunctions is promoted by host-guest interactions, which are obtained through chiral recognition.

Polymeric vesicles are promising candidates for use in a range of applications including drug delivery and cell mimics, however, control over the shape is still a challenge. Here, the authors report control over local curvature formation by addition of salt ions and stimuli responsive polymer to modulate its interaction with polymeric membrane.

Bio-inspired assembly of mesoscale materials presents a unique challenge due to complex machinery or labor-intensive processing involved in engineering. Barber et al. report chiral filaments self-assembled into free-standing, anisotropic bundles through pre-programmed, light-mediated structural deformations.

Polymersomes, as analogues of liposomes, have interesting physical and chemical properties, but have not yet been translated into clinical or industrial applications. Here, the authors report the development of a continuous flow process for the production of polymersomes at scale.

Materials with tunable modulus, viscosity, and complex viscoelastic spectra are crucial in various applications but it remains challenging to design polymer networks with predicted hierarchical relaxation processes. Here, the authors synthesize networks with both pendant and telechelic architectures using mixed orthogonal dynamic bonds to understand how the network connectivity and bond exchange mechanisms govern the overall relaxation spectrum.

Synthetic hydrogels composed of covalent polymers and supramolecular fibers have been investigated for controlled delivery of biopharmaceuticals, but characterisation of the structures and properties can be challenging. Here, the authors report an imaging study for the composite network, categorizing into four distinct patterns controlled by network formation kinetics and interactions between

Mechanically interlocked structures in polymer backbones can give interesting functionality, but can be challenging to prepare and control. Here, the authors report the development of polymers with a daisy chain unit in the backbone that are capable of shape memory behaviour.

Defects and disordered local domains in soft, self-assembled aggregates determine their dynamic and adaptive properties, and enable communication between entities, but characterizing and classifying such intricate dynamic behaviors is highly complex. Here, the authors report on a data-driven workflow to identify objective criteria for the comparison of complex dynamic features in soft supramolecular materials, deriving a data-driven ’defectometer’ that allows to classify soft self-assembled materials based on the structural dynamics of the ordered/disordered molecular environments that statistically emerge within them.

Polymerisation induced self assembly can lead to unusual morphology and dynamics of resultant structures. Here the mechanism of the collective dynamics of a self-assembled polymer system under light irradiation, including self-replication, is eludicated.