Time-space-resolved origami hierarchical electronics for ultrasensitive detection of physical and chemical stimuli.

Recent years have witnessed thriving progress of flexible and portable electronics, with very high demand for cost-effective and tailor-made multifunctional devices. Here, we report on an ingenious origami hierarchical sensor array (OHSA) written with a conductive ink. Thanks to origami as a controllable hierarchical framework for loading ink material, we have demonstrated that OHSA possesses unique time-space-resolved, high-discriminative pattern recognition (TSR-HDPR) features, qualifying it as a smart sensing device for simultaneous sensing and distinguishing of complex physical and chemical stimuli, including temperature, relative humidity, light and volatile organic compounds (VOCs). Of special importance, OSHA has shown very high sensitivity in differentiating between structural isomers and chiral enantiomers of VOCs - opening a door for wide variety of unique opportunities in several length scales.

Three-dimensional simulations of liquid bridges between two cylinders: forces, energies, and torques.

We present numerical simulations of three-dimensional liquid bridges between two identical smooth and chemically homogeneous cylinders held at a fixed distance and angle one with respect to the other. Despite the limited range of parameters studied, an analysis of resultant forces, energies, and torques reveals a rich level of detail. For large enough separations between the cylinders, the bridges appear symmetric and stable in shape and are found to yield a negligible torque on the cylinders. The force of adhesion is found to be positive in this case (the cylinders are attracted one to the other). A reduction in the distance between the cylinders reveals different behavior depending on the particular value of the set of parameters considered. For example, it appears that while relatively low contact angle systems favor attractive (positive) forces and stable symmetric bridges for small separation distances, larger contact angles lead to the coexistence of stable asymmetric and (apparently) unstable symmetric solutions, mostly (and respectively) associated with near-zero and negative (repulsive) forces of adhesion. In addition, while the larger values of contact angles studied here (90 degrees, 110 degrees) are associated with barely detectable torques, smaller values of contact angle are found to be associated with torques acting to rotate cylinders into a position where they are parallel one with respect to the other.

Corresponding-states laws for protein solutions.

The solvent around protein molecules in solutions is structured and this structuring introduces a repulsion in the intermolecular interaction potential at intermediate separations. We use Monte Carlo simulations with isotropic, pair-additive systems interacting with such potentials. We test if the liquid-liquid and liquid-solid phase lines in model protein solutions can be predicted from universal curves and a pair of experimentally determined parameters, as done for atomic and colloid materials using several laws of corresponding states. As predictors, we test three properties at the critical point for liquid-liquid separation: temperature, as in the original van der Waals law, the second virial coefficient, and a modified second virial coefficient, all paired with the critical volume fraction. We find that the van der Waals law is best obeyed and appears more general than its original formulation: A single universal curve describes all tested nonconformal isotropic pair-additive systems. Published experimental data for the liquid-liquid equilibrium for several proteins at various conditions follow a single van der Waals curve. For the solid-liquid equilibrium, we find that no single system property serves as its predictor. We go beyond corresponding-states correlations and put forth semiempirical laws, which allow prediction of the critical temperature and volume fraction solely based on the range of attraction of the intermolecular interaction potential.

Multiple extrema in the intermolecular potential and the phase diagram of protein solutions.

Recent experiments have revealed several surprising features of the phase equilibria in protein solutions: liquid-liquid phase separation which is, in some cases, metastable with respect to the liquid-solid equilibrium, and in others-unobservable; widely varying crystallization enthalpies, including completely athermal crystallization; the co-existence of several crystalline polymorphs; and others. Other studies have shown that the solvent molecules at the hydrophobic and polar patches on the protein molecular surfaces are structured, introducing repulsive forces at surface separations equal to several water molecule sizes. In search of a causal link between the latter and former findings, we apply Monte Carlo simulation techniques in the investigation of phase diagrams associated with globular biological molecules in solution. We account for the solvent structuring via short-range isotropic two-body intermolecular potentials exhibiting multiple extrema. We show that the introduction of a repulsive maximum or a secondary attractive minimum at separations longer than the primary attractive minimum has dramatic effects on the phase diagram: liquid-liquid separation curves are driven to lower or higher temperatures, the sensitivity of the solubility curve (liquidus) to temperature, i.e., the enthalpy of crystallization, is significantly reduced or enhanced, metastable liquid-liquid separation may become stable and vice versa, and both low- and high-density crystalline phases are observed. The similarity of these features of the simulated phase behavior to those observed experimentally suggests that at least some of the mysteries of the protein phase equilibria may be due to the structuring of the solvent around the protein molecular surfaces. Another conclusion is that at least some of the dense liquids seen in protein solutions may be stable and not metastable with respect to a solid phase.

Partial wetting of chemically patterned surfaces: the effect of drop size.

Partial wetting of chemically heterogeneous substrates is simulated. Three-dimensional sessile drops in equilibrium with smooth surfaces supporting ordered chemical patterns are considered. Significant features are observed as a result of changing the drop volume. The number of equilibrated drops is found either to remain constant or to increase with growing drop volume. The shape of larger drops appears to approach that of a spherical cap and their three-phase contact line seems, on a larger scale, more circular in shape than that of smaller drops. In addition, as the volume is increased, the average contact angle of drops whose free energy is lowest among all equilibrium-shaped drops of the same volume appears to approach the angle predicted by Cassie. Finally, contrary to results obtained with two-dimensional drops, contact angle hysteresis observed in this system is shown to exhibit a degree of volume dependence in the advancing and receding angles. Qualitative differences in the wetting behavior associated with the two different chemical patterns considered here, as well as differences between results obtained with two-dimensional and three-dimensional drops, can possibly be attributed to variations in the level of constraint imposed on the drop by the different patterns and by the dimensionality of the system.