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Liquid metals have long been treated as Newtonian liquids, but several researchers have recently indicated that some metals may shear thin. While apparent shear thinning can be caused by surface oxidation, the reports of shear-thinning metals were investigated using cup and bob type rheometers, which are expected to only be weakly impacted by the surface contamination effects. We show here that even small amounts of oxide on the surface of liquid metals can cause dramatic changes to the measured viscosity of the sample. Using a Searle-type rotational rheometer, we measured the viscosity of eutectic gallium indium and tin in a low-oxygen environment. When either metal is slightly oxidized, the measured viscosity increases by orders of magnitude and the liquid displays erroneous shear-thinning behavior. When the oxide is removed via an active flux, the measured viscosity is Newtonian. The results outlined here provide insight into the difficulties of measuring the viscosity of easily oxidized liquids and confirm that liquid metals are likely best described as Newtonian liquids at all measured shear rates.

This work establishes that static contact angles for gallium-based liquid metals have no utility despite the continued and common use of such angles in the literature. In the presence of oxygen, these metals rapidly form a thin (∼1-3 nm) surface oxide "skin" that adheres to many surfaces and mechanically impedes its flow. This property is problematic for contact angle measurements, which presume the ability of liquids to flow freely to adopt shapes that minimize the interfacial energy. We show here that advancing angles for a metal are always high (>140°)-even on substrates to which it adheres-because the solid native oxide must rupture in tension to advance the contact line. The advancing angle for the metal depends subtly on the substrate surface chemistry but does not vary strongly with hydrophobicity of the substrate. During receding measurements, the metal droplet initially sags as the liquid withdraws from the "sac" formed by the skin and thus the contact area with the substrate initially increases despite its volumetric recession. The oxide pins at the perimeter of the deflated "sac" on all the surfaces are tested, except for certain rough surfaces. With additional withdrawal of the liquid metal, the pinned angle gets smaller until eventually the oxide "sac" collapses. Thus, static contact angles can be manipulated mechanically from 0° to >140° due to hysteresis and are therefore uninformative. We also provide recommendations and best practices for wetting experiments, which may find use in applications that use these alloys such as soft electronics, composites, and microfluidics.

Liquid metals adhere to most surfaces despite their high surface tension due to the presence of a native gallium oxide layer. The ability to change the shape of functional fluids within a three-dimensional (3D) printed part with respect to time is a type of four-dimensional printing, yet surface adhesion limits the ability to pump liquid metals in and out of cavities and channels without leaving residue. Rough surfaces prevent adhesion, but most methods to roughen surfaces are difficult or impossible to apply on the interior of parts. Here, we show that silica particles suspended in an appropriate solvent can be injected inside cavities to coat the walls. This technique creates a transparent, nanoscopically rough (10-100 nm scale) coating that prevents adhesion of liquid metals on various 3D printed plastics and commercial polymers. Liquid metals roll and even bounce off treated surfaces (the latter occurs even when dropped from heights as high as 70 cm). Moreover, the coating can be removed locally by laser ablation to create selective wetting regions for metal patterning on the exterior of plastics. To demonstrate the utility of the coating, liquid metals were dynamically actuated inside a 3D printed channel or chamber without pinning the oxide, thereby demonstrating electrical circuits that can be reconfigured repeatably.

The focus of this chapter is to review the literature on flexible and stretchable electronics fabricated using gallium-based liquid metal alloys. Over the past few decades, gallium-based liquid metal alloys have gathered growing interest due to their application in various soft electronic applications as conductive yet fluidic metals that can be patterned at room temperature. Gallium-based liquid metal alloys have a melting point at or near room temperature and offer a low toxicity as opposed to the conventional liquid metal – mercury, in addition to having negligible vapor pressure and low viscosity. The surface of these metals reacts rapidly with oxygen in air to form a thin surface oxide ‘skin’ that allows these liquids to be deposited in several useful stable shapes despite the destabilizing effects of a large surface tension and gravity. There are several methods to pattern these liquid metals – traditionally using lithography-based subtractive approaches, and unconventionally using 3D printing and other additive techniques. Gallium-based liquid metal alloys have been used for fabricating various electronic structures such as ultrastretchable and self-healing wires, interconnects, and stretchable antennas. Integrating these components, many electronic components have been built such as optical and soft memory devices, reconfigurable circuits, soft diodes, microfluidic pumps, soft strain sensors, capacitors, and circuit boards.

Materials used in wearable and implantable electronic devices should match the mechanical properties of biological tissues, which are inherently soft and deformable. In comparison to conventional rigid electronics, soft bioelectronics can provide accurate and real-time monitoring of physiological signals, improve comfort, and enable altogether new modalities for sensing. This article highlights recent progress, identifies technical challenges, and offers possible solutions for the emerging field of stretchable bioelectronics. We organize the content into three topical categories: (1) biological integration of soft electronic materials, (2) materials and mechanics, and (3) soft robotics. Finally, we conclude this article with a discussion on the outlook of the field and future challenges. Published version

Based on parallel-plate waveguides (PWWGs), we have developed both passive and active terahertz (THz) sensors, filters, splitters, and switches. We utilize the PPWG since it has excellent waveguiding properties with a simple geometry that allows for incorporation of unique electromagnetic functionalities. A few passive devices are discussed while the focus remains on active devices. The active control is enabled by our innovation to incorporate liquid metals, which can be relocated by application of a small electrical voltage (< 4V), as part of the waveguide geometry itself. The device geometry directly affects the device performance (e.g., frequency band of operation, channel output power). Therefore, by moving the liquid metal, the geometry is reconfigured which results in altering the device function. To show the practicality of these devices to be used for THz wireless communications, we demonstrate the ability of these devices to support a 1 Gb/s data stream on a THz carrier wave and show that this signal can be successfully switched with high modulation depths of ±40 dB. These results show the strong promise of these components to form important signal processing building blocks in the future infrastructure of THz wireless communications.

This work reports a simple approach to form, study, and utilize rough coatings that prevent the adhesion of gallium-based liquid metal alloys. Typically, liquids with large interfacial tension do not wet nonreactive surfaces, regardless of surface topography. However, these alloys form a surface oxide "skin" that adheres to many substrates, even those with low surface energy. This work reports a simple approach to render closed channels and surfaces, including soft materials, to be "oxide-phobic" via spray-coating (NeverWet, which is commercially available and inexpensive). Surface spectroscopic techniques and metrology tools elucidate the coatings to comprise silica nanoparticles grafted with silicones that exhibit dual length scales of roughness. Although prior work shows the importance of surface roughness in preventing adhesion, the present work confirms that both hydrophobic and hydrophilic rough surfaces prevent oxide adhesion. Furthermore, the coating enables reversible actuation through submillimeter closed channels to form a reconfigurable antenna in the gigahertz range without the need for corrosive acids or bases that remove the oxide. In addition, the coating enables open surface patterning of conductive traces of liquid metal. This shows it is possible to actuate liquid metals in air without leaving neither metal nor oxide residue on surfaces to enable reconfigurable electronics, microfluidics, and soft electrodes.

Many applications of terahertz (THz) technology require the ability to actively manipulate a free space THz beam. Yet, although there have been many reports on the development of devices for THz signal processing, few of these include the possibility of electrical control of the functionality, and novel ideas are needed for active and reconfigurable THz devices. Here, we introduce a new approach, based on the integration of electrically actuated liquid metal components in THz waveguides. This versatile platform offers many possibilities for control of THz spectral content, wave fron"ts, polarization, and power flow. We demonstrate two illustrative examples: the first active power-splitting switch, and the first channel add–drop filter. We show that both of these devices can be used to electrically switch THz communication signals while preserving the information in a high bit-rate-modulated data stream., Although there are many reports on the development of devices for terahertz signal processing, the possibility of electrical control of the functionality remains elusive. Here, the authors use electrically actuated liquid metal components incorporated into terahertz waveguides for controlling power flow and for frequency filtering.

Liquid metal-based reconfigurable antennas typically must be flushed with an electrolyte to remove the nanometer-thick oxide skin of EGaln that adheres the walls of the microchannels. The EGaln residue prevents repeatable actuation, but the presence of electrolyte introduces other challenges owing to its often corrosive and electrically conductive nature. To overcome this issue, we present a technique for enabling reversible infusion and withdrawal of EGaln into acrylic micro-channels and wide planar cavities by coating the surfaces with a silica-particle based superhydrophobic coating. The coating prevents adhesion of the liquid metal to the acrylic media and allows it to be reconfigured multiple times without the typical flushing process.

Stretchable fibers dissipate energy via the sequential fracturing of a metallic core held together by an elastomeric shell., Tough, biological materials (e.g., collagen or titin) protect tissues from irreversible damage caused by external loads. Mimicking these protective properties is important in packaging and in emerging applications such as durable electronic skins and soft robotics. This paper reports the formation of tough, metamaterial-like core-shell fibers that maintain stress at the fracture strength of a metal throughout the strain of an elastomer. The shell experiences localized strain enhancements that cause the higher modulus core to fracture repeatedly, increasing the energy dissipated during extension. Normally, fractures are catastrophic. However, in this architecture, the fractures are localized to the core. In addition to dissipating energy, the metallic core provides electrical conductivity and enables repair of the fractured core for repeated use. The fibers are 2.5 times tougher than titin and hold more than 15,000 times their own weight for a period 100 times longer than a hollow elastomeric fiber.

Liquid metal co-injected with electrolyte through a microfluidic flow-focusing orifice forms droplets with diameters and production frequencies controlled in real time by voltage. Applying voltage to the liquid metal controls the interfacial tension via a combination of electrochemistry and electrocapillarity. This simple and effective method can instantaneously tune the size of the microdroplets, which has applications in composites, catalysts, and microsystems.

We characterize the THz properties of liquid metals in conductive fluids. These results will inform the design of future reconfigurable THz signal processing components based on liquid metals incorporated into waveguides.

Electrowetting uses voltage to manipulate small volumes of fluid for applications including lab-on-a-chip and optical devices. To avoid electrochemical reactions, a dielectric often separates the fluid from the electrode, which has the undesired effect of adding processing steps while increasing the voltage necessary for electrowetting. We present a new method to dramatically reduce the complexity of electrode and dielectric fabrication while enabling multiple performance advances. This method relies on a self-oxidizing paint-on liquid-metal electrode that can be fabricated in minutes on rigid, rough, or even elastic substrates, enabling low operation voltages (

We utilize electronically reconfigurable liquid metals to dynamically modify the coupling between two THz waveguides, to realize an active tunable filter with channel add-drop functionality.

Herein, elastomeric fibers that have shape memory properties due to the presence of a gallium core that can undergo phase transition from solid to liquid in response to mild heating are described. The gallium is injected into the core of a hollow fiber formed by melt processing. This approach provides a straightforward method to create shape memory properties from any hollow elastic fiber. Solidifying the core changes the effective fiber modulus from 4 to 1253 MPa. This increase in stiffness can preserve the fiber in a deformed shape. The elastic energy stored in the polymer shell during deformation drives the fiber to relax back to its original geometry upon melting the solid gallium core, allowing for shape memory. Although waxes are used previously for this purpose, the use of gallium is compelling because of its metallic electrical and thermal conductivity. In addition, the use of a rigid metallic core provides perfect fixity of the shape memory fiber. Notably, the use of gallium—with a melting point above room temperature but below body temperature—allows the user to melt and deform local regions of the fiber by hand and thereby tune the effective modulus and shape of the fiber., Herein, soft and ultrastretchable elastic shape memory fibers with electrical conductivity are demonstrated fabricated by injecting liquid metal, gallium, into the elastic and hollow fibers. The ability to change the core of the fiber from liquid to solid allows an enormous modulus change and thus, excellent shape memory effects.

Liquid metals based on gallium, such as eutectic gallium indium (EGaIn) and Galinstan, have been integrated as static components in microfluidic systems for a wide range of applications including soft electrodes, pumps, and stretchable electronics. However, there is also a possibility to continuously pump liquid metal into microchannels to create shape reconfigurable metallic structures. Enabling this concept necessitates a simple method to control dynamically the path the metal takes through branched microchannels with multiple outlets. This paper demonstrates a novel method for controlling the directional flow of EGaIn liquid metal in complex microfluidic networks by simply applying a low voltage to the metal. According to the polarity of the voltage applied between the inlet and an outlet, two distinct mechanisms can occur. The voltage can lower the interfacial tension of the metal via electrocapillarity to facilitate the flow of the metal towards outlets containing counter electrodes. Alternatively, the voltage can drive surface oxidation of the metal to form a mechanical impediment that redirects the movement of the metal towards alternative pathways. Thus, the method can be employed like a 'valve' to direct the pathway chosen by the metal without mechanical moving parts. The paper elucidates the operating mechanisms of this valving system and demonstrates proof-of-concept control over the flow of liquid metal towards single or multiple directions simultaneously. This method provides a simple route to direct the flow of liquid metal for applications in microfluidics, optics, electronics, and microelectromechanical systems.

This work characterizes the behavior of a eutectic alloy of gallium and indium (75% Ga, 25% In, by weight, ‘EGaIn’) in response to electric fields. The metal is a liquid at room temperature (M.P., 15.5 °C) and exhibits low toxicity. These fluidic metals may be injected into microfluidic systems, fibers, and capillary networks to form soft electronic devices that are soft and compliant. Once injected, the metal remains in its place because of the adhesive nature of its thin native oxide. Preventing the oxide adhesion within microchannels enables reversible actuation of EGaIn. Actuating liquid metals may be useful for soft actuators, reconfigurable optical displays, frequency tunable antennas, and other opto-fluidic technologies. In this work, we utilize low voltages (

Correction for ‘Electrowetting without external voltage using paint-on electrodes’ by Collin B. Eaker et al., Lab Chip, 2017, DOI: 10.1039/c6lc01500j.