Jonathan B. Boreyko

Delayed Frost Growth on Jumping-Drop Superhydrophobic Surfaces

Self-propelled jumping drops are continuously removed from a condensing superhydrophobic surface to enable a micrometric steady-state drop size. Here, we report that subcooled condensate on a chilled superhydrophobic surface are able to repeatedly jump off the surface before heterogeneous ice nucleation occurs. Frost still forms on the superhydrophobic surface due to ice nucleation at neighboring edge defects, which eventually spreads over the entire surface via an interdrop frost wave. The growth of this interdrop frost front is shown to be up to 3 times slower on the superhydrophobic surface compared to a control hydrophobic surface, due to the jumping-drop effect dynamically minimizing the average drop size and surface coverage of the condensate. A simple scaling model is developed to relate the success and speed of interdrop ice bridging to the drop size distribution. While other reports of condensation frosting on superhydrophobic surfaces have focused exclusively on liquid-solid ice nucleation for isolated drops, these findings reveal that the growth of frost is an interdrop phenomenon that is strongly coupled to the wettability and drop size distribution of the surface. A jumping-drop superhydrophobic condenser minimized frost formation relative to a conventional dropwise condenser in two respects: preventing heterogeneous ice nucleation by continuously removing subcooled condensate, and delaying frost growth by limiting the success of interdrop ice bridge formation.

Planar jumping-drop thermal diodes

Phase-change thermal diodes rectify heat transport much more effectively than solid-state ones, but are limited by either the gravitational orientation or one-dimensional configuration. Here, we report a planar phase-change diode scalable to large areas with an orientation-independent diodicity of over 100, in which water/vapor is enclosed by parallel superhydrophobic and superhydrophilic plates. The thermal rectification is enabled by spontaneously jumping dropwise condensate which only occurs when the superhydrophobic surface is colder than the superhydrophilic surface.

Wetting and Dewetting Transitions on Hierarchical Superhydrophobic Surfaces

Many natural superhydrophobic structures have hierarchical two-tier roughness which is empirically known to promote robust superhydrophobicity. We report the wetting and dewetting properties of two-tier roughness as a function of the wettability of the working fluid, where the surface tension of water/ethanol drops is tuned by the mixing ratio, and compare the results to one-tier roughness. When the ethanol concentration of deposited drops is gradually increased on one-tier control samples, the impalement of the microtier-only surface occurs at a lower ethanol concentration compared to the nanotier-only surface. The corresponding two-tier surface exhibits a two-stage wetting transition, first for the impalement of the microscale texture and then for the nanoscale one. The impaled drops are subsequently subjected to vibration-induced dewetting. Drops impaling one-tier surfaces could not be dewetted; neither could drops impaling both tiers of the two-tier roughness. However, on the two-tier surface, drops impaling only the microscale roughness exhibited a full dewetting transition upon vibration. Our work suggests that two-tier roughness is essential for preventing catastrophic, irreversible wetting of superhydrophobic surfaces.

Dynamic defrosting on nanostructured superhydrophobic surfaces.

Water suspended on chilled superhydrophobic surfaces exhibits delayed freezing; however, the interdrop growth of frost through subcooled condensate forming on the surface seems unavoidable in humid environments. It is therefore of great practical importance to determine whether facile defrosting is possible on superhydrophobic surfaces. Here, we report that nanostructured superhydrophobic surfaces promote the growth of frost in a suspended Cassie state, enabling its dynamic removal upon partial melting at low tilt angles (<15°). The dynamic removal of the melting frost occurred in two stages: spontaneous dewetting followed by gravitational mobilization. This dynamic defrosting phenomenon is driven by the low contact angle hysteresis of the defrosted meltwater relative to frost on microstructured superhydrophobic surfaces, which forms in the impaled Wenzel state. Dynamic defrosting on nanostructured superhydrophobic surfaces minimizes the time, heat, and gravitational energy required to remove frost from the surface, and is of interest for a variety of systems in cold and humid environments.

Air-stable droplet interface bilayers on oil-infused surfaces

Significance By suspending a lipid bilayer in an aperture or between water droplets, single-molecule transport through membrane channels can be electrically detected. To date, all suspended bilayers have been confined to fluid reservoirs. This study demonstrates that droplet interface bilayers can be created in an ambient environment using noncoalescing water droplets on an oil-infused surface. Air-stable droplet interface bilayers are easy to manipulate and electrically characterize, and could potentially allow for the biosensing of airborne molecules. Droplet interface bilayers are versatile model membranes useful for synthetic biology and biosensing; however, to date they have always been confined to fluid reservoirs. Here, we demonstrate that when two or more water droplets collide on an oil-infused substrate, they exhibit noncoalescence due to the formation of a thin oil film that gets squeezed between the droplets from the bottom up. We show that when phospholipids are included in the water droplets, a stable droplet interface bilayer forms between the noncoalescing water droplets. As with traditional oil-submerged droplet interface bilayers, we were able to characterize ion channel transport by incorporating peptides into each droplet. Our findings reveal that droplet interface bilayers can function in ambient environments, which could potentially enable biosensing of airborne matter.

Controlling condensation and frost growth with chemical micropatterns

In-plane frost growth on chilled hydrophobic surfaces is an inter-droplet phenomenon, where frozen droplets harvest water from neighboring supercooled liquid droplets to grow ice bridges that propagate across the surface in a chain reaction. To date, no surface has been able to passively prevent the in-plane growth of ice bridges across the population of supercooled condensate. Here, we demonstrate that when the separation between adjacent nucleation sites for supercooled condensate is properly controlled with chemical micropatterns prior to freezing, inter-droplet ice bridging can be slowed and even halted entirely. Since the edge-to-edge separation between adjacent supercooled droplets decreases with growth time, deliberately triggering an early freezing event to minimize the size of nascent condensation was also necessary. These findings reveal that inter-droplet frost growth can be passively suppressed by designing surfaces to spatially control nucleation sites and by temporally controlling the onset of freezing events.

Self-propelled jumping drops on superhydrophobic surfaces

We report a self-propelled jumping phenomenon for coalescing drops on superhydrophobic surfaces. The spontaneous motion is powered by surface energy released upon coalescence. On a horizontal, chilled superhydrophobic surface with an apparent contact angle close to 180°, coalescing drops of water condensate spontaneously jump out of plane, against gravity. In the capillary-inertial regime, the velocity scales as v / r, where is the surface tension, is the density, and r is the drop radius before coalescence. Therefore, smaller drops jump with a higher velocity Fig. 1 , as long as the drop diameter is above 100 m where viscous effects are not dominating. On a heated Leidenfrost surface with liquid drops floating on a vapor layer which resembles superhydrophobicity, the mechanism of the out-of-plane directionality was revealed by releasing two drops from opposing synchronized gates to induce coalescence. The jumping motion resulted from the evolving liquid bridge of the coalescing drops impinging against the substrate Fig. 2 a ; the liquid bridge initiated well above the surface because of the high contact angle of the drops. As a confirmation of the impingement mechanism, when bouncing drops coalesced away from the substrate, no appreciable jumping occurred Fig. 2 b .

Self-propelled sweeping removal of dropwise condensate

Dropwise condensation can be enhanced by superhydrophobic surfaces on which the condensate drops spontaneously jump upon coalescence. However, the self-propelled jumping in prior reports is mostly perpendicular to the substrate. Here, we propose a substrate design with regularly spaced micropillars. Coalescence on the sidewalls of the micropillars leads to self-propelled jumping in a direction nearly orthogonal to the pillars and therefore parallel to the substrate. This in-plane motion in turn produces sweeping removal of multiple neighboring drops. The spontaneous sweeping mechanism may greatly enhance dropwise condensation in a self-sustained manner.

Asymmetric Wettability of Nanostructures Directs Leidenfrost Droplets

Leidenfrost phenomena on nano- and microstructured surfaces are of great importance for increasing control over heat transfer in high power density systems utilizing boiling phenomena. They also provide an elegant means to direct droplet motion in a variety of recently emerging fluidic systems. Here, we report the fabrication and characterization of tilted nanopillar arrays (TNPAs) that exhibit directional Leidenfrost water droplets under dynamic conditions, namely on impact with Weber numbers ≥40 at T ≥ 325 °C. The directionality for these droplets is opposite to the direction previously exhibited by macro- and microscale Leidenfrost ratchets where movement against the tilt of the ratchet was observed. The batch fabrication of the TNPAs was achieved by glancing-angle anisotropic reactive ion etching of a thermally dewet platinum mask, with mean pillar diameters of 100 nm and heights of 200-500 nm. In contrast to previously implemented macro- and microscopic Leidenfrost ratchets, our TNPAs induce no preferential directional movement of Leidenfrost droplets under conditions approaching steady-state film boiling, suggesting that the observed droplet directionality is not a result of the widely accepted mechanism of asymmetric vapor flow. Using high-speed imaging, phase diagrams were constructed for the boiling behavior upon impact for droplets falling onto TNPAs, straight nanopillar arrays, and smooth silicon surfaces. The asymmetric impact and directional trajectory of droplets was exclusive to the TNPAs for impacts corresponding to the transition boiling regime, linking asymmetric surface wettability to preferential directionality of dynamic Leidenfrost droplets on nanostructured surfaces.

On Localized Vapor Pressure Gradients Governing Condensation and Frost Phenomena

Interdroplet vapor pressure gradients are the driving mechanism for several phase-change phenomena such as condensation dry zones, interdroplet ice bridging, dry zones around ice, and frost halos. Despite the fundamental nature of the underlying pressure gradients, the majority of studies on these emerging phenomena have been primarily empirical. Using classical nucleation theory and Becker-Döring embryo formation kinetics, here we calculate the pressure field for all possible modes of condensation and desublimation in order to gain fundamental insight into how pressure gradients govern the behavior of dry zones, condensation frosting, and frost halos. Our findings reveal that in a variety of phase-change systems the thermodynamically favorable mode of nucleation can switch between condensation and desublimation depending upon the temperature and wettability of the surface. The calculated pressure field is used to model the length of a dry zone around liquid or ice droplets over a broad parameter space. The long-standing question of whether the vapor pressure at the interface of growing frost is saturated or supersaturated is resolved by considering the kinetics of interdroplet ice bridging. Finally, on the basis of theoretical calculations, we propose that there exists a new mode of frost halo that is yet to be experimentally observed; a bimodal phase map is developed, demonstrating its dependence on the temperature and wettability of the underlying substrate. We hope that the model and predictions contained herein will assist future efforts to exploit localized vapor pressure gradients for the design of spatially controlled or antifrosting phase-change systems.