Evidence of Universal Temperature Scaling in Self-Heated Percolating Networks.

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.

Fractal Lévy Heat Transport in Nanoparticle Embedded Semiconductor Alloys.

Materials with embedded nanoparticles are of considerable interest for thermoelectric applications. Here, we experimentally characterize the effect of nanoparticles on the recently discovered Lévy phonon transport in semiconductor alloys. The fractal space dimension α ≈ 1.55 of quasiballistic (superdiffusive) heat conduction in (ErAs)x:InGaAlAs is virtually independent of the Er content 0.001 < x < 0.1 but instead controlled by alloy scattering of the host matrix. The increased nanoparticle concentration does reduce the diffusive recovery length by an order of magnitude. The bulk conductivity drops by 3-fold, in close agreement with a Callaway model. Our results may provide helpful hints toward engineering superdiffusive heat transport similar to what has been achieved with light in Lévy glasses.

Enhanced thermoelectric properties in bulk nanowire heterostructure-based nanocomposites through minority carrier blocking.

To design superior thermoelectric materials the minority carrier blocking effect in which the unwanted bipolar transport is prevented by the interfacial energy barriers in the heterogeneous nanostructures has been theoretically proposed recently. The theory predicts an enhanced power factor and a reduced bipolar thermal conductivity for materials with a relatively low doping level, which could lead to an improvement in the thermoelectric figure of merit (ZT). Here we show the first experimental demonstration of the minority carrier blocking in lead telluride-silver telluride (PbTe-Ag2Te) nanowire heterostructure-based nanocomposites. The nanocomposites are made by sintering PbTe-Ag2Te nanowire heterostructures produced in a highly scalable solution-phase synthesis. Compared with Ag2Te nanowire-based nanocomposite produced in similar method, the PbTe-Ag2Te nanocomposite containing ∼5 atomic % PbTe exhibits enhanced Seebeck coefficient, reduced thermal conductivity, and ∼40% improved ZT, which can be well explained by the theoretical modeling based on the Boltzmann transport equations when energy barriers for both electrons and holes at the heterostructure interfaces are considered in the calculations. For this p-type PbTe-Ag2Te nanocomposite, the barriers for electrons, that is, minority carriers, are primarily responsible for the ZT enhancement. By extending this approach to other nanostructured systems, it represents a key step toward low-cost solution-processable nanomaterials without heavy doping level for high-performance thermoelectric energy harvesting.

Composition modulation of Ag2Te nanowires for tunable electrical and thermal properties.

In this article, we demonstrated that composition modulation of Ag2Te nanowires can be achieved during the self-templated transformation of Te nanowires into Ag2Te nanowires during solution phase synthesis, which provides a mean to tune the carrier density of the Ag2Te nanowires. Both nearly stoichiometric and Ag-rich nanowires have been synthesized, which give rise to p-type and n-type Ag2Te nanocomposites after hot press, respectively. The electrical and thermal properties of the two kinds of samples have been measured. Theoretical modeling based on the near-equilibrium Boltzmann transport equations has been used to understand the experimental results. We found that ZT of the heavily doped n-type sample reaches 0.55 at 400 K, which is the highest ZT value reported for Ag2Te at the same temperature mainly due to the reduced thermal conductivity by the nanostructures. Theoretical analysis on the carrier transport shows that the power factor is also very well optimized in the doped Ag2Te sample considering the reduced carrier mobility by the nanostructures.