Insights into the Interfacial Contact and Charge Transport of Gas- Sensing Liquid Metal Marbles

Understanding the interfacial contacts between liquid metals and substrate materials is becoming increasingly important for the fast-rising liquid metal-enabled technologies. However, for such technologies, probing the contact behavior and interfacial charge transport has remained challenging due to the deformable nature of liquid metals and the presence of the surface oxide layer. Here, we encapsulate eutectic gallium indium (EGaIn) micro-/nanodroplets with tungsten trioxide (WO3) nanoparticles to form a WO3/EGaIn liquid metal marble network, in which the interfacial contact of the intrinsically semiconducting WO3 governs the charge transport. We investigate the interfacial structures and charge transport characteristics under different contact conditions and various gaseous environments. The results suggest that establishing a WO3/EGaIn heterostructure leads to near-ohmic contact behaviors and also the emergence of localized surface plasmon resonance. Density functional theory calculations of the WO3/EGaIn interface support the experiments by revealing atomistic attractions between EGaIn alloy and the O atoms from WO3, resulting in a Fermi level shift. We also show that the efficient interfacial charge transport of the liquid metal marble network results in an enhanced gas-sensing response. This work paves the way for the possibility of studying other liquid metal/semiconductor contacts for applications in soft electronics and optics.