Direct Probing of Cross-Plane Thermal Properties of Atomic Layer Deposition Al2O3/ZnO Superlattice Films with an Improved Figure of Merit and Their Cross-Plane Thermoelectric Generating Performance.

There is a recent interest in semiconducting superlattice films because their low dimensionality can increase the thermal power and phonon scattering at the interface in superlattice films. However, experimental studies in all cross-plane thermoelectric (TE) properties, including thermal conductivity, Seebeck coefficient, and electrical conductivity, have not been performed from these semiconducting superlattice films because of substantial difficulties in the direct measurement of the Seebeck coefficient and electrical conductivity. Unlike the conventional measurement method, we present a technique using a structure of sandwiched superlattice films between two embedded heaters as the heating source, and electrodes with two Cu plates, which directly enables the investigation of the Seebeck coefficient and electrical conductivity across the Al2O3/ZnO superlattice films, prepared by the atomic layer deposition method. Used in combination with the promising cross-plane four-point probe 3-ω method, our measurements and analysis demonstrate all cross-plane TE properties of Al2O3/ZnO superlattice films in the temperature range of 80 to 500 K. Our experimental methodology and the obtained results represent a significant advancement in the understanding of phonons and electrical transports in nanostructured materials, especially in semiconducting superlattice films in various temperature ranges.

Control of phonon transport by the formation of the Al2O3 interlayer in Al2O3-ZnO superlattice thin films and their in-plane thermoelectric energy generator performance.

Recently, significant progress has been made in increasing the figure-of-merit (ZT) of various nanostructured materials, including thin-film and quantum dot superlattice structures. Studies have focused on the size reduction and control of the surface or interface of nanostructured materials since these approaches enhance the thermopower and phonon scattering in quantum and superlattice structures. Currently, bismuth-tellurium-based semiconductor materials are widely employed for thermoelectric (TE) devices such as TE energy generators and coolers, in addition to other sensors, for use at temperatures under 400 K. However, new and promising TE materials with enhanced TE performance, including doped zinc oxide (ZnO) multilayer or superlattice thin films, are also required for designing solid-state TE power generating devices with the maximum output power density and for investigating the physics of in-plane TE generators. Herein, we report the growth of Al2O3/ZnO (AO/ZnO) superlattice thin films, which were prepared by atomic layer deposition (ALD), and the evaluation of their electrical and TE properties. All the in-plane TE properties, including the Seebeck coefficient (S), electrical conductivity (σ), and thermal conductivity (κ), of the AO/ZnO superlattice (with a 0.82 nm-thick AO layer) and AO/ZnO films (with a 0.13 nm-thick AO layer) were evaluated in the temperature range 40-300 K, and the measured S, σ, and κ were -62.4 and -17.5 µV K-1, 113 and 847 (Ω cm)-1, and 0.96 and 1.04 W m-1 K-1, respectively, at 300 K. Consequently, the in-plane TE ZT factor of AO/ZnO superlattice films was found to be ∼0.014, which is approximately two times more than that of AO/ZnO films (ZT of ∼0.007) at 300 K. Furthermore, the electrical power generation efficiency of the TE energy generator consisting of four couples of n-AO/ZnO superlattice films and p-Bi0.5Sb1.5Te3 (p-BST) thin-film legs on the substrate was demonstrated. Surprisingly, the output power of the 100 nm-thick n-AO/ZnO superlattice film/p-BST TE energy generator was determined to be ∼1.0 nW at a temperature difference of 80 K, corresponding to a significant improvement of ∼130% and ∼220% compared to the 100 nm-thick AO/ZnO film/p-BST and n-BT/p-BST film generators, respectively, owing to the enhancement of the TE properties, including the power factor of the superlattice film.