Two switchable, palindromically constituted bistable [3]rotaxanes have been designed and synthesized with a pair of mechanically mobile rings encircling a single dumbbell. These designs are reminiscent of a "molecular muscle" for the purposes of amplifying and harnessing molecular mechanical motions. The location of the two cyclobis(paraquat-p-phenylene) (CBPQT 4+ ) rings can be controlled to be on either tetrathiafulvalene (TTF) or naphthalene (NP) stations, either chemically ( 1 H NMR spectroscopy) or electrochemically (cyclic voltammetry), such that switching of inter-ring distances from 4.2 to 1.4 nm mimics the contraction and extension of skeletal muscle, albeit on a shorter length scale. Fast scan-rate cyclic voltammetry at low temperatures reveals stepwise oxidations and movements of one-half of the [3]rotaxane and then of the other, a process that appears to be concerted at room temperature. The active form of the bistable [3]rotaxane bears disulfide tethers attached covalently to both of the CBPQT 4+ ring components for the purpose of its self-assembly onto a gold surface. An array of flexible microcantilever beams, each coated on one side with a monolayer of 6 billion of the active bistable [3]rotaxane molecules, undergoes controllable and reversible bending up and down when it is exposed to the synchronous addition of aqueous chemical oxidants and reductants. The beam bending is correlated with flexing of the surfacebound molecular muscles, whereas a monolayer of the dumbbell alone is inactive under the same conditions. This observation supports the hypothesis that the cumulative nanoscale movements within surface-bound "molecular muscles" can be harnessed to perform larger-scale mechanical work.
In the present study, it is shown that the spreading rate of a mixing layer can be greatly manipulated at very low forcing level if the mixing layer is perturbed near a subharmonic of the most-amplified frequency. The subharmonic forcing technique is able to make several vortices merge simultaneously and hence increases the spreading rate dramatically. A new mechanism, ‘collective interaction’, was found which can bypass the sequential stages of vortex merging and make a large number of vortices (ten or more) coalesce.A deeper physical insight into the evolution of the coherent structures is revealed through the investigation of a forced mixing layer. The stability and the forcing function play important roles in determining the initial formation of the vortices. The subharmonic starts to amplify at the location where the phase speed of the subharmonic matches that of the fundamental. The position where vortices are seen to align vertically coincides with the position where the measured subharmonic reaches its peak. This location is defined as the merging location, and it can be determined from the feedback equation (Ho & Nosseir 1981).The spreading rate and the velocity profiles of the forced mixing layer are distinctly different from the unforced case. The data show that the initial condition has a longlasting effect on the development of the mixing layer.
A macroscopic evaporating water droplet with suspended particles on a solid surface will form a ring-like structure at the pinned contact line due to induced capillary flow. As the droplet size shrinks, the competition between the time scales of the liquid evaporation and the particle movement may influence the resulting ring formation. When the liquid evaporates much faster than the particle movement, coffee ring formation may cease. Here, we experimentally show that there exists a lower limit of droplet size, D c , for the successful formation of a coffee ring structure. When the particle concentration is above a threshold value, D c can be estimated by considering the collective effects of the liquid evaporation and the particle diffusive motion within the droplet. For suspended particles of size ~100 nm, the minimum diameter of the coffee ring structure is found to be ~10 µm.
Fast advancements of microfabrication processes in past two decades have reached to a fairly matured stage that we can manufacture a wide range of microfluidic devices. At present, the main challenge is the control of nanoscale properties on the surface of lab-on-a-chip to satisfy the need for biomedical applications. For example, poly(dimethylsiloxane) (PDMS) is a commonly used material for microfluidic circuitry, yet the hydrophobic nature of PDMS surface suffers serious nonspecific protein adsorption. Thus the current major efforts are focused on surface molecular property treatments for satisfying specific needs in handling macro functional molecules. Reviewing surface modifications of all types of materials used in microfluidics will be too broad. This review will only summarize recent advances in nonbiofouling PDMS surface modification strategies applicable to microfluidic technology and classify them into two main categories: (1) physical approach including physisorption of charged or amphiphilic polymers and copolymers, as well as (2) chemical approach including self assembled monolayer and thick polymer coating. Pros and cons of a collection of available yet fully exploited surface modification methods are briefly compared among subcategories.
The coffee ring phenomenon has long been known for its ability to concentrate particles at the rim of a dried liquid droplet, yet little is known about its particle separation capability. Here, we elucidate the physics of particle separation during coffee ring formation, which is based on a particle-size selection mechanism near the contact line of an evaporating droplet. On the basis of this mechanism, we demonstrate nanochromatography of three relevant biological entities (proteins, micro-organisms, and mammalian cells) in a liquid droplet, with a separation resolution on the order of ∼100 nm and a dynamic range from ∼10 nm to a few tens of micrometers. These findings have direct implications for developing low-cost technologies for disease diagnostics in resource-poor environments.
A passive technique of increasing entrainment was found by using a small-aspect-ratio elliptic jet. The entrainment ratio of an elliptic jet was several times greater than that of a circular jet or a plane jet. The self-induction of the asymmetric coherent structure caused azimuthal distortions which were responsible for engulfing large amounts of surrounding fluid into the jet. In an elliptic jet, an interesting feature in the initial stability process is that the thickness of the shear layer varies around the nozzle. The data indicated that instability frequency was scaled with the thinnest initial momentum thickness which was associated with the maximum vorticity. Turbulence properties were also examined and were found to be significantly different in the major- and minor-axis planes.
An array of microcantilever beams, coated with a self-assembled monolayer of bistable, redox-controllable [3]rotaxane molecules, undergoes controllable and reversible bending when it is exposed to chemical oxidants and reductants. Conversely, beams that are coated with a redox-active but mechanically inert control compound do not display the same bending. A series of control experiments and rational assessments preclude the influence of heat, photothermal effects, and pH variation as potential mechanisms of beam bending. Along with a simple calculation from a force balance diagram, these observations support the hypothesis that the cumulative nanoscale movements within surface-bound “molecular muscles” can be harnessed to perform larger-scale mechanical work.
An experimental study was conducted to investigate the’ generation process of random small-scale turbulence in an originally laminar mixing layer. The evolutions of the two types of deterministic structures, the spanwise and streamwise vortices, were first clarified in order to determine their roles in the transition process. A scaling rule for the streamwise distance from the trailing edge of the splitter plate to the vortex merging position was found for various velocity ratios. After this streamwise lengthscale was determined, it became clear that the spanwise wavelength of the streamwise vortices doubled after the merging of the spanwise structures which nominally doubled streamwise wavelengths. The most interesting finding was that the random small-scale eddies were produced by the interactions between the merging spanwise structures and the streamwise vortices.
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