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Abstract Ultrasound is a safe, noninvasive diagnostic technique used to measure internal structures such as tissues, organs, and arterial and venous blood flow. Skin‐mounted wearable ultrasound devices can enable long‐term continuous monitoring of patients to provide solutions to critical healthcare needs. However, stretchable ultrasound devices that are composed of ultrasonic transducers embedded in an elastomer matrix are incompatible with existing rigid acoustic matching layers, leading to reduced energy transmission and reduced imaging resolution. Here, a systematic study of soft composites with liquid metal (LM) fillers dispersed in elastomers reveals key strategies to tune the acoustic impedance of soft materials. Experiments supported by theoretical models demonstrate that the increase in acoustic impedance is primarily driven by the increase in density with negligible changes to the speed of sound through the material. By controlling the volume loading and particle size of the LM fillers, a material is created that achieves a high acoustic impedance 4.8 Mrayl, (> 440% increase over the polymer matrix) with low modulus (< 1 MPa) and high stretchability (> 100% strain). When the device is mechanically strained, a small decrease is observed in acoustic impedance (< 15%) with negligible decrease in sound transmittance and impact on attenuation for all droplet sizes. The stretchable acoustic matching layer is then integrated with a wearable ultrasound device and the ability to measure motion is demonstrated using a phantom model as is performed in Doppler ultrasound. 

Abstract Soft, elastically deformable composites with liquid metal (LM) droplets can enable new generations of soft electronics, robotics, and reconfigurable structures. However, techniques to control local composite microstructure, which ultimately governs material properties and performance, is lacking. Here a direct ink writing technique is developed to program the LM microstructure (i.e., shape, orientation, and connectivity) on demand throughout elastomer composites. In contrast to inks with rigid particles that have fixed shape and size, it is shown that emulsion inks with LM fillers enable in situ control of microstructure. This enables filaments, films, and 3D structures with unique LM microstructures that are generated on demand and locked in during printing. This includes smooth and discrete transitions from spherical to needle‐like droplets, curvilinear microstructures, geometrically complex embedded inclusion patterns, and connected LM networks. The printed materials are soft (modulus < 200 kPa), highly deformable (>600 % strain), and can be made locally insulating or electrically conductive using a single ink by controlling the process conditions. These capabilities are demonstrated by embedding elongated LM droplets in a soft heat sink, which rapidly dissipates heat from high‐power LEDs. These programmable microstructures can enable new composite paradigms for emerging technologies that demand mechanical compliance with multifunctional response.