Machine learning (ML)-assisted surface tension and oscillation-induced elastic modulus studies of oxide-coated liquid metal (LM) alloys.

Pendant drops of oxide-coated high-surface tension fluids frequently produce perturbed shapes that impede interfacial studies. Eutectic gallium indium or Galinstan are high-surface tension fluids coated with a ∼5 nm gallium oxide (Ga2O3) film and falls under this fluid classification, also known as liquid metals (LMs). The recent emergence of LM-based applications often cannot proceed without analyzing interfacial energetics in different environments. While numerous techniques are available in the literature for interfacial studies- pendant droplet-based analyses are the simplest. However, the perturbed shape of the pendant drops due to the presence of surface oxide has been ignored frequently as a source of error. Also, exploratory investigations of surface oxide leveraging oscillatory pendant droplets have remained untapped. We address both challenges and present two contributing novelties- (a) by utilizing the machine learning (ML) technique, we predict the approximate surface tension value of perturbed pendant droplets, (ii) by leveraging the oscillation-induced bubble tensiometry method, we study the dynamic elastic modulus of the oxide-coated LM droplets. We have created our dataset from LM's pendant drop shape parameters and trained different models for comparison. We have achieved >99% accuracy with all models and added versatility to work with other fluids. The best-performing model was leveraged further to predict the approximate values of the nonaxisymmetric LM droplets. Then, we analyzed LM's elastic and viscous moduli in air, harnessing oscillation-induced pendant droplets, which provides complementary opportunities for interfacial studies alternative to expensive rheometers. We believe it will enable more fundamental studies of the oxide layer on LM, leveraging both symmetric and perturbed droplets. Our study broadens the materials science horizon, where researchers from ML and artificial intelligence domains can work synergistically to solve more complex problems related to surface science, interfacial studies, and other studies relevant to LM-based systems.

Reactive etching of gallium oxide on eutectic gallium indium (eGaIn) with chlorosilane vapor to induce differential wetting.

Differentially wettable surfaces are well sought after in energy, water, health care, separation science, self-cleaning, biology, and other lab-on-chip applications-however, most demonstrations of realizing differential wettability demand complex processes. Herein, we chemically etch gallium oxide (Ga2O3) from in-plane patterns (2D) of eutectic gallium indium (eGaIn) to demonstrate a differentially wettable interface using chlorosilane vapor. We produce 2D patterns of eGaIn on bare glass slides in native air using cotton swabs as paint brushes. Exposing the entire system to chlorosilane vapor induces chemical etching of the oxide layer, which recovers the high-surface energy of eGaIn, to produce nano-to-mm droplets on the pre-patterned area. We rinse the entire system with deionized (DI) water to achieve differentially wettable surfaces. Measurements of contact angles using a goniometer confirmed hydrophobic and hydrophilic interfaces. Scanning electron microscopy (SEM) images confirmed the distribution and energy dispersive spectra (EDS) exhibited the elemental compositions of the micro-to-nano droplets after silanization (silane treatment). Also, we demonstrated two proofs of concept, i.e., open-ended microfluidics and differential wettability on curved interfaces, to demonstrate the advanced applications of the current work. This straightforward approach using two soft materials (silane and eGaIn) to achieve differential wettability on laboratory-grade glass slides and other surfaces has future implications for nature-inspired self-cleaning surfaces in nanotechnologies, bioinspired and biomimetic open-channel microfluidics, coatings, and fluid-structure interactions.

Vacuum filling of complex microchannels with liquid metal.

This paper describes the utilization of vacuum to fill complex microchannels with liquid metal. Microchannels filled with liquid metal are useful as conductors for soft and stretchable electronics, as well as for microfluidic components such as electrodes, antennas, pumps, or heaters. Liquid metals are often injected manually into the inlet of a microchannel using a syringe. Injection can only occur if displaced air in the channels has a pathway to escape, which is usually accomplished using outlets. The positive pressure (relative to atmosphere) needed to inject fluids can also cause leaks or delamination of the channels during injection. Here we show a simple and hands-free method to fill microchannels with liquid metal that addresses these issues. The process begins by covering a single inlet with liquid metal. Placing the entire structure in a vacuum chamber removes the air from the channels and the surrounding elastomer. Restoring atmospheric pressure in the chamber creates a positive pressure differential that pushes the metal into the channels. Experiments and a simple model of the filling process both suggest that the elastomeric channel walls absorb residual air displaced by the metal as it fills the channels. Thus, the metal can fill dead-ends with features as small as several microns and branched structures within seconds without the need for any outlets. The method can also fill completely serpentine microchannels up to a few meters in length. The ability to fill dense and complex geometries with liquid metal in this manner may enable broader application of liquid metals in electronic and microfluidic applications.

A Method to Manipulate Surface Tension of a Liquid Metal via Surface Oxidation and Reduction.

Controlling interfacial tension is an effective method for manipulating the shape, position, and flow of fluids at sub-millimeter length scales, where interfacial tension is a dominant force. A variety of methods exist for controlling the interfacial tension of aqueous and organic liquids on this scale; however, these techniques have limited utility for liquid metals due to their large interfacial tension. Liquid metals can form soft, stretchable, and shape-reconfigurable components in electronic and electromagnetic devices. Although it is possible to manipulate these fluids via mechanical methods (e.g., pumping), electrical methods are easier to miniaturize, control, and implement. However, most electrical techniques have their own constraints: electrowetting-on-dielectric requires large (kV) potentials for modest actuation, electrocapillarity can affect relatively small changes in the interfacial tension, and continuous electrowetting is limited to plugs of the liquid metal in capillaries. Here, we present a method for actuating gallium and gallium-based liquid metal alloys via an electrochemical surface reaction. Controlling the electrochemical potential on the surface of the liquid metal in electrolyte rapidly and reversibly changes the interfacial tension by over two orders of magnitude ( Ì´500 mN/m to near zero). Furthermore, this method requires only a very modest potential (< 1 V) applied relative to a counter electrode. The resulting change in tension is due primarily to the electrochemical deposition of a surface oxide layer, which acts as a surfactant; removal of the oxide increases the interfacial tension, and vice versa. This technique can be applied in a wide variety of electrolytes and is independent of the substrate on which it rests.