Ximin He

Synthetic homeostatic materials with chemo-mechano-chemical self-regulation.

Living organisms have unique homeostatic abilities, maintaining tight control of their local environment through interconversions of chemical and mechanical energy and self-regulating feedback loops organized hierarchically across many length scales. In contrast, most synthetic materials are incapable of continuous self-monitoring and self-regulating behaviour owing to their limited single-directional chemomechanical or mechanochemical modes. Applying the concept of homeostasis to the design of autonomous materials would have substantial impacts in areas ranging from medical implants that help stabilize bodily functions to ‘smart’ materials that regulate energy usage. Here we present a versatile strategy for creating self-regulating, self-powered, homeostatic materials capable of precisely tailored chemo-mechano-chemical feedback loops on the nano- or microscale. We design a bilayer system with hydrogel-supported, catalyst-bearing microstructures, which are separated from a reactant-containing ‘nutrient’ layer. Reconfiguration of the gel in response to a stimulus induces the reversible actuation of the microstructures into and out of the nutrient layer, and serves as a highly precise ‘on/off’ switch for chemical reactions. We apply this design to trigger organic, inorganic and biochemical reactions that undergo reversible, repeatable cycles synchronized with the motion of the microstructures and the driving external chemical stimulus. By exploiting a continuous feedback loop between various exothermic catalytic reactions in the nutrient layer and the mechanical action of the temperature-responsive gel, we then create exemplary autonomous, self-sustained homeostatic systems that maintain a user-defined parameter—temperature—in a narrow range. The experimental results are validated using computational modelling that qualitatively captures the essential features of the self-regulating behaviour and provides additional criteria for the optimization of the homeostatic function, subsequently confirmed experimentally. This design is highly customizable owing to the broad choice of chemistries, tunable mechanics and its physical simplicity, and may lead to a variety of applications in autonomous systems with chemo-mechano-chemical transduction at their core.

A double droplet trap system for studying mass transport across a droplet-droplet interface

Here we present the design, fabrication and operation of a microfluidic device to trap droplets in a large array of droplet pairs in a controlled manner with the aim of studying the transport of small molecules across the resultant surfactant bilayers formed between the droplet pairs.

Exploiting the superior protein resistance of polymer brushes to control single cell adhesion and polarisation at the micron scale.

The control of the cell microenvironment on model patterned substrates allows the systematic study of cell biology in well defined conditions, potentially using automated systems. The extreme protein resistance of poly(oligo(ethylene glycol methacrylate)) (POEGMA) brushes is exploited to achieve high fidelity patterning of single cells. These coatings can be patterned by soft lithography on large areas (a microscope slide) and scale (substrates were typically prepared in batches of 200). The present protocol relies on the adsorption of extra-cellular matrix (ECM) proteins on unprotected areas using simple incubation and washing steps. The stability of POEGMA brushes, as examined via ellipsometry and SPR, is found to be excellent, both during storage and cell culture. The impact of substrate treatment, brush thickness and incubation protocol on ECM deposition, both for ultra-thin gold and glass substrates, is investigated via fluorescence microscopy and AFM. Optimised conditions result in high quality ECM patterns at the micron scale, even on glass substrates, that are suitable for controlling cell spreading and polarisation. These patterns are compatible with state-of-the-art technologies (fluorescence microscopy, FRET) used for live cell imaging. This technology, combined with single cell analysis methods, provides a platform for exploring the mechanisms that regulate cell behaviour.

An aptamer-functionalized chemomechanically modulated biomolecule catch-and-release system

The efficient extraction of (bio)molecules from fluid mixtures is vital for applications ranging from target characterization in (bio)chemistry to environmental analysis and biomedical diagnostics. Inspired by biological processes that seamlessly synchronize the capture, transport and release of biomolecules, we designed a robust chemomechanical sorting system capable of the concerted catch and release of target biomolecules from a solution mixture. The hybrid system is composed of target-specific, reversible binding sites attached to microscopic fins embedded in a responsive hydrogel that moves the cargo between two chemically distinct environments. To demonstrate the utility of the system, we focus on the effective separation of thrombin by synchronizing the pH-dependent binding strength of a thrombin-specific aptamer with volume changes of the pH-responsive hydrogel in a biphasic microfluidic regime, and show a non-destructive separation that has a quantitative sorting efficiency, as well as the systems stability and amenability to multiple solution recycling.

Synthesis and characterization of low bandgap conjugated donor-acceptor polymers for polymer: PCBM solar cells

We report on the synthesis, characterization and photovoltaic performance of three novel semiconducting polymers based on poly[bis-N,N′-(4-octylphenyl)-bis-N,N′-phenyl-1,4-phenylenediamine-alt-5,5′-4′,7′,-di-2-thienyl-2′,1′,3′-benzothiadiazole]. They differ only in the presence and position of hexyl side-chains on the thienyl groups. T8TBT-0 has no such side-chains, they face towards the benzothiadiazole in T8TBT-in and away in T8TBT-out. Based on electron-donating triarylamine and electron-accepting dithienyl-benzothiadiazole groups, the new polymers exhibit low bandgaps and enhanced absorption in the red part of the visible spectrum. Despite their identical backbone they differ in their synthesis and photophysics: T8TBT-0 and T8TBT-in can be synthesized by direct Suzuki coupling but a new synthesis procedure is necessary for T8TBT-out. In absorption and luminescence a blue shift is induced by the inward facing, and to a lesser extent by the outward-facing side-chains. From comparison of the photophysics in solutions and films, we conclude that the addition of side-chains reduces formation of aggregates in films and that this effect is stronger for inward-facing side-chains. By blending the three polymers with PCBM in a standard photovoltaic device architecture, T8TBT-0 performs best with a power conversion efficiency (PCE) of 1.0% (under AM1.5G illumination at 100 mW cm−2) compared to 0.17% and 0.27% for T8TBT-out and T8TBT-in, respectively.