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Organic materials have attracted attention for thermoelectric materials reusing low-temperature waste heat. For the thermoelectric performance enhancement of organic materials, the introduction of inorganic nanowires is effective due to the percolation effect. In this study, we synthesized Cu

We propose the methodology for thermoelectric power factor enhancement using nanoscale thermal management. The thermally managed composite is composed of a high electrical conductivity (σ) material...

It is expected to develop the measurement system to obtain physical/chemical information with nanoscale space resolution related to the non-thermal equilibrium phenomena. In this study, we developed controlled temperature-gradient kelvin force microscopy (T-KFM) to measure the temperature difference (ΔT)-induced vacuum level variation under non-thermal equilibrium. Therein, the biggest issue, difficulty in applying the large ΔT in narrow space (∼100 μm), was solved by introducing “heating and cooling systems” in T-KFM; one sample side is heated using a ceramic heater and the other side is cooled using liquid nitrogen. Using T-KFM, the space distribution of ΔT-induced vacuum level variation was well observed on the scale of hundreds of nanometers in a polycrystalline ZnO film with nanostructures. The obtained image of the ΔT-induced vacuum level variation can reflect a distribution of the thermal properties such as the thermal resistance and thermoelectromotive force. This pronounced technique for obtaining surface potential under T-gradient helps us to comprehend the non-thermal equilibrium phenomena.

We have investigated the intrinsic thermoelectric properties of epitaxial β-FeSi2 thin films and the impact of phosphorus (P) doping. Epitaxial β-FeSi2 thin films with single phase were grown on Si(111) substrates by two different techniques in an ultrahigh-vacuum molecular beam epitaxy (MBE) system: solid-phase epitaxy (SPE), where iron silicide films formed by codeposition of Fe and Si at room temperature were recrystallized by annealing at 530°C to form epitaxial β-FeSi2 thin films on Si(111) substrates, and MBE of β-FeSi2 thin films on epitaxial β-FeSi2 templates formed on Si(111) by reactive deposition epitaxy (RDE) at 530°C (RDE + MBE). Epitaxial SPE thin films based on codeposition had a flatter surface and more abrupt β-FeSi2/Si(111) interface than epitaxial RDE + MBE thin films. We investigated the intrinsic thermoelectric properties of the epitaxial β-FeSi2 thin films on Si(111), revealing lower thermal conductivity and higher electrical conductivity compared with bulk β-FeSi2. We also investigated the impact of doping on the Seebeck coefficient of bulk and thin-film β-FeSi2. A route to enhance the thermoelectric performance of β-FeSi2 is proposed, based on (1) fabrication of thin-film structures for high electrical conductivity and low thermal conductivity, and (2) proper choice of doping for high Seebeck coefficient.

We present a carrier-doped Si nanoarchitecture for thermoelectric material, consisting of a stacked structure of carrier-doped Si layer/Si nanocrystals (NCs) with oriented crystal. The NCs and carrier-doped Si layers act as phonon scattering centers and carrier transport layers, respectively. The NCs were covered with ultrathin SiO2 films. Solid-phase epitaxy (SPE) of the Si layers on the amorphous ultrathin SiO2 films was achieved using nanowindows in the ultrathin SiO2 films. By such integration of the ultrathin SiO2 film technique for epitaxial growth of NCs and the SPE method, we fabricated a Ga-doped Si nanoarchitecture and achieved carrier doping of 1018 cm−3 to 1019 cm−3. The thermal conductivity was reduced to a value similar to that of amorphous Si. The thermal resistance per stacking layer in the nanoarchitecture was 7 to 10 times higher than that of connected Si NCs, which exhibited thermal conductivity 200 times smaller than that of bulk Si. This large thermal resistance in the nanoarchitecture may result from precipitation of Ga atoms at the ultrathin SiO2 film interfaces. These Ga atoms played two roles: as dopants for electrical conductivity enhancement and as phonon scatters for thermal conductivity reduction. This nanoarchitecture demonstrates the possibility of achieving high electrical conductivity and low thermal conductivity.

Thin film thermoelectric materials have drawn much attention for realizing one-chip stand-alone power sources of internet of things devices. Here, we fabricate two types of the nanostructured Si films with high crystallinity: Si films containing β-FeSi2 nanodots with wider nanodot size distribution of ~5-120 nm and Si films containing α-FeSi2 nanodots with narrow size distribution of ~5-20 nm. The thermal conductivity of these films is lower than those of Si-silicide nanocomposite bulks. Interestingly, Si films containing β-FeSi2 nanodots shows about two times lower thermal conductivity than Si films containing α-FeSi2 nanodots. This is because the widely-size-distributed β-FeSi2 nanodots can effectively work as phonon scattering centers due to hierarchical architectures. These films also exhibited high power factor due to small amount of point defects and single crystalline epitaxial interfaces, despite iron silicide phase of nanodots. These detailed investigations will open a road for realizing the high-performance thin film thermoelectric materials.

High crystallinity Si films containing silicide nanodots (NDs) were epitaxially grown on Si substrates at high temperature (∼750 °C), where the silicide phase of NDs (metallic α-FeSi2 or semiconductor β-FeSi2) was selectable by tuning the Fe deposition amount. The high crystallinity high-temperature-grown Si films with NDs exhibited lower thermal conductivity (5.4 W m−1 K−1) due to the phonon scattering at the ultrasmall ND interfaces than bulk Si-silicide nanocomposites that have ever been reported. In this ND system with extremely low thermal conductivity, due to the less point defects and high quality ND interface, the thermoelectric power factor (∼28 μW cm−1 K−2) was observed to be the same as the high value of Si films without NDs at room temperature, which is the highest value among Si-silicide bulk nanocomposites ever reported. The simultaneous achievement of a high power factor and low thermal conductivity in the high quality ND system will provide the key for design of high thermoelectric performance of Si-based nanostructured films.

The high electrical and drastically-low thermal conductivities, a vital goal for high performance thermoelectric (TE) materials, are achieved in Si-based nanoarchitecture composed of Si channel layers and epitaxial Ge nanodots (NDs) with ultrahigh areal density (~1012 cm−2). In this nanoarchitecture, the ultrasmall NDs and Si channel layers play roles of phonon scattering sources and electrical conduction channels, respectively. Electron conductivity in n-type nanoacrhitecture shows high values comparable to those of epitaxial Si films despite the existence of epitaxial NDs. This is because Ge NDs mainly scattered not electrons but phonons selectively, which could be attributed to the small conduction band offset at the epitaxially-grown Si/Ge interface and high transmission probability through stacking faults. These results demonstrate an independent control of thermal and electrical conduction for phonon-glass electron-crystal TE materials by nanostructure designing and the energetic and structural interface control.

The core-shell nanostructure of epitaxial Fe3O4 nanocrystals over Ge nuclei showed a large Off/On resistance ratio (∼100), which was the largest value in Fe3O4 materials. The nanocrystals with an average diameter of ∼20 nm were grown epitaxially on Si substrates, whose areal density was high (∼1011 cm−2), and each nanocrystal was isolated from each other. The electrical measurement of the individual isolated nanocrystals by conductive-atomic force microscopy showed the bipolar-type resistive switching in local voltage-current curves, depending on the Fe-O composition. It was also revealed that activation sites for resistive switching were the Fe3O4/Ge interfaces, where electric-field-induced compositional variation caused large resistive changes. This demonstrated the possibility of developing resistance random access memory devices based on ubiquitous materials.

Epitaxial growth method for multilayered structures of ultrasmall β-FeSi2 nanodots (NDs)/Si was developed as a Si-based material for thermoelectric or optical devices by applying our ultrathin SiO2 film technique. In this technique, strain-relaxed β-FeSi2 NDs were epitaxially grown with high density. For the formation of multilayered structures, Si growth on these β-FeSi2 NDs was carefully investigated. Si grew epitaxially on the NDs in three-dimension because of the lattice mismatch strain with the underlying NDs. As a result of three-dimensional Si growth, thicker Si (>20 monolayer) was needed to completely cover the NDs. The authors demonstrated that strain-relaxed β-FeSi2 NDs and the Si covering are two important factors for the formation of multilayered structures of β-FeSi2 NDs/Si.

Si-based epitaxial β-FeSi2 thin films are attractive as materials for on-chip thermoelectric power generators. We investigated the structure, crystallinity, and thermoelectric properties of β-FeSi2 thin films epitaxially grown on Si(111) substrates by using three different techniques: conventional reactive deposition epitaxy followed by molecular beam epitaxy (RDE+MBE), solid phase epitaxy (SPE) based on codeposition of Fe and Si presented previously, and SPE followed by MBE (SPE+MBE) presented newly by this work. Their epitaxial growth temperatures were fixed at 530 °C for comparison. RDE+MBE thin films exhibited high crystalline quality, but rough surfaces and rugged β-FeSi2/Si(111) interfaces. On the other hand, SPE thin films showed flat surfaces and abrupt β-FeSi2/Si(111) interfaces but low crystallinity. We found that SPE+MBE thin films realized crystallinity higher than SPE thin films, and also had flatter surfaces and sharper interfaces than RDE+MBE thin films. In SPE+MBE thin film growth, due to the initial SPE process with low temperature codeposition, thermal interdiffusion of Fe and Si was suppressed, resulting in the surface flatness and abrupt interface. Second high temperature MBE process improved the crystallinity. We also investigated thermoelectric properties of these β-FeSi2 thin films. Structural factors affecting the thermoelectric properties of RDE+MBE, SPE, and SPE+MBE thin films were investigated.