A new method for quantifying lipid–lipid interactions within biomimetic membranes undergoing electrocompression is demonstrated by coupling droplet mechanics and membrane biophysics. The membrane properties are varied by altering the lipid packing through the introduction of cholesterol. Pendant drop tensiometry is used to measure the lipid monolayer tension at an oil–water interface. Next, two lipid-coated aqueous droplets are manipulated into contact to form a bilayer membrane at their adhered interface. The droplet geometries are captured from two angles to provide accurate measurements of both the membrane area and the contact angle between the adhered droplets. Combining the monolayer tension and contact angle measurements enables estimations of the membrane tension with respect to lipid composition. Then, the membrane is electromechanically compressed using a transmembrane voltage. Electrostatic pressure, membrane tension and the work necessary for bilayer thinning are tracked, and a model is proposed to capture the mechanics of membrane compression. The results highlight that a previously unaccounted for energetic term is produced during compression, potentially reflecting changes in the lateral membrane structure. This residual energy is eliminated in cases with cholesterol mole fractions of 0.2 and higher, suggesting that cholesterol diminishes these adjustments.

Exchange governed by membrane structure within a network of aqueous subcompartments provides a foundation for materials inspired by cellular mechanics.

The droplet interface bilayer platform allows for the fabrication of stimuli-responsive microfluidic materials, using phospholipids as an organic surfactant in water-in-oil mixtures. In this approach, lipid-coated droplets are adhered together in arranged networks, forming lipid bilayer membranes with embedded transporters and establishing selective exchange pathways between neighboring aqueous subcompartments. The resulting material is a biologically inspired droplet-based material that exhibits emergent properties wherein different droplets accomplish different functions, similar to multicellular organisms. These networks have been successfully applied towards biomolecular sensing and energy harvesting applications. However, unlike their source of inspiration, these droplet structures are often static. This limitation not only renders the networks unable to adapt or modify their structure and function after formation but also limits their long term use as passive ionic exchange between neighboring droplet pairs may initiate immediately after the membranes are established. This work addresses this shortcoming by rupturing selected sacrificial membranes within the collections of droplets to rearrange the remaining droplets into new configurations, redirecting the droplet-droplet exchange pathways. This is accomplished through electrical shocks applied between selected droplets. Experimental outcomes are compared to predictions provided by a coupled mechanical-electrical model for the droplet networks, and then advanced configurations are proposed using this model.

Droplet interface bilayer (DIB) networks allow for the construction of stimuli-responsive, membrane-based materials. Traditionally used for studying cellular transport phenomena, the DIB technique has proven its practicality when creating structured droplet networks. These structures consist of aqueous compartments capable of exchanging their contents across membranous barriers in a regulated fashion via embedded biomolecules, thus approximating the activity of natural cellular systems. However, lipid bilayer networks are often static and incapable of any reconfiguration in their architecture. In this study, we investigate the incorporation of a magnetic fluid or ferrofluid within the droplet phases for the creation of magnetically responsive DIB arrays. The impact of adding ferrofluid to the aqueous phases of the DIB networks is assessed by examining the bilayers' interfacial tensions, thickness, and channel activity. Once compatibility is established, potential applications of the ferrofluid-enabled DIBs are showcased by remotely modifying membrane qualities through magnetic fields. Ferrofluids do not significantly alter the bilayers' properties or functionality and can therefore be safely embedded within the DIB platform, allowing for remote manipulation of the interfacial bilayer properties.