Transistors, sensors, and transparent conductors based on randomly assembled nanowire networks rely on multi-component percolation for unique and distinctive applications in flexible electronics, biochemical sensing, and solar cells. While conduction models for 1-D and 1-D/2-D networks have been developed, typically assuming linear electronic transport and self-heating, the model has not been validated by direct high-resolution characterization of coupled electronic pathways and thermal response. In this letter, we show the occurrence of nonlinear “super-Joule” self-heating at the transport bottlenecks in networks of silver nanowires and silver nanowire/single layer graphene hybrid using high resolution thermoreflectance (TR) imaging. TR images at the microscopic self-heating hotspots within nanowire network and nanowire/graphene hybrid network devices with submicron spatial resolution are used to infer electrical current pathways. The results encourage a fundamental reevaluation of transport models for network-based percolating conductors.

During routine operation, electrically percolating nanocomposites are subjected to high voltages, leading to spatially heterogeneous current distribution. The heterogeneity implies localized self-heating that may (self-consistently) reroute the percolation pathways and even irreversibly damage the material. In the absence of experiments that can spatially resolve the current distribution and a nonlinear percolation model suitable to interpret them, one relies on empirical rules and safety factors to engineer these materials. In this paper, we use ultrahigh resolution thermo-reflectance imaging, coupled with a new imaging processing technique, to map the spatial distribution ΔT(x, y; I) and histogram f(ΔT) of temperature rise due to self-heating in two types of 2D networks (percolating and copercolating). Remarkably, we find that the self-heating can be described by a simple two-parameter Weibull distribution, even under voltages high enough to reconfigure the percolation pathways. Given the generality of the phenomenological argument supporting the distribution, other percolating networks are likely to show similar stress distribution in response to sufficiently large stimuli. Furthermore, the spatial evolution of the self-heating of network was investigated by analyzing the spatial distribution and spatial correlation, respectively. An estimation of degree of hotspot clustering reveals a mechanism analogous to crystallization physics. The results should encourage nonlinear generalization of percolation models necessary for predictive engineering of nanocomposite materials.

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Abstract:Although transparent conductive oxides such as indium tin oxide (ITO) are widely employed as transparent conducting electrodes (TCEs) for applications such as touch screens and displays, new nanostructured TCEs are of interest for future applications, including emerging transparent and flexible electronics. A number of twodimensional networks of nanostructured elements have been reported, including metallic nanowire networks consisting of silver nanowires, metallic carbon nanotubes (mCNTs), copper nanowires or gold nanowires, and metallic mesh structures. In these single-component systems, it has generally been difficult to achieve sheet resistances that are comparable to ITO at a given broadband optical transparency. A relatively new third category of TCEs consisting of networks of 1D-1D and 1D-2D nanocomposites (such as silver nanowires and CNTs, silver nanowires and polycrystalline graphene, silver nanowires and reduced graphene oxide) have demonstrated TCE performance comparable to, or better than, ITO. In such hybrid networks, copercolation between the two components can lead to relatively low sheet resistances at nanowire densities corresponding to high optical transmittance. This review provides an overview of reported hybrid networks, including a comparison of the performance regimes achievable with those of ITO and single-component nanostructured networks. The performance is compared to that expected from bulk thin films and analyzed in terms of the copercolation model. In addition, performance characteristics relevant for flexible and transparent applications are discussed. The new TCEs are promising, but significant work must be done to ensure earth abundance, stability, and reliability so that they can eventually replace traditional ITO-based transparent conductors.

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