The long-standing popularity of thermoelectric materials has contributed to the creation of various thermoelectric devices and stimulated the development of strategies to improve their thermoelectric performance. In this review, we aim to comprehensively summarize the state-of-the-art strategies for the realization of high-performance thermoelectric materials and devices by establishing the links between synthesis, structural characteristics, properties, underlying chemistry and physics, including structural design (point defects, dislocations, interfaces, inclusions, and pores), multidimensional design (quantum dots/wires, nanoparticles, nanowires, nano- or microbelts, few-layered nanosheets, nano- or microplates, thin films, single crystals, and polycrystalline bulks), and advanced device design (thermoelectric modules, miniature generators and coolers, and flexible thermoelectric generators). The outline of each strategy starts with a concise presentation of their fundamentals and carefully selected examples. In the end, we point out the controversies, challenges, and outlooks toward the future development of thermoelectric materials and devices. Overall, this review will serve to help materials scientists, chemists, and physicists, particularly students and young researchers, in selecting suitable strategies for the improvement of thermoelectrics and potentially other relevant energy conversion technologies.

Advanced Thermoelectric Design: From Materials and Structures to Devices

Textiles have been concomitant of human civilization for thousands of years. With the advances in chemistry and materials, integrating textiles with energy harvesters will provide a sustainable, environmentally friendly, pervasive, and wearable energy solution for distributed on-body electronics in the era of Internet of Things. This article comprehensively and thoughtfully reviews research activities regarding the utilization of smart textiles for harvesting energy from renewable energy sources on the human body and its surroundings. Specifically, we start with a brief introduction to contextualize the significance of smart textiles in light of the emerging energy crisis, environmental pollution, and public health. Next, we systematically review smart textiles according to their abilities to harvest biomechanical energy, body heat energy, biochemical energy, solar energy as well as hybrid forms of energy. Finally, we provide a critical analysis of smart textiles and insights into remaining challenges and future directions. With worldwide efforts, innovations in chemistry and materials elaborated in this review will push forward the frontiers of smart textiles, which will soon revolutionize our lives in the era of Internet of Things.

Smart Textiles for Electricity Generation.

The urgent need for ecofriendly, stable, long-lifetime power sources is driving the booming market for miniaturized and integrated electronics, including wearable and medical implantable devices. Flexible thermoelectric materials and devices are receiving increasing attention, due to their capability to convert heat into electricity directly by conformably attaching them onto heat sources. Polymer-based flexible thermoelectric materials are particularly fascinating because of their intrinsic flexibility, affordability, and low toxicity. There are other promising alternatives including inorganic-based flexible thermoelectrics that have high energy-conversion efficiency, large power output, and stability at relatively high temperature. Herein, the state-of-the-art in the development of flexible thermoelectric materials and devices is summarized, including exploring the fundamentals behind the performance of flexible thermoelectric materials and devices by relating materials chemistry and physics to properties. By taking insights from carrier and phonon transport, the limitations of high-performance flexible thermoelectric materials and the underlying mechanisms associated with each optimization strategy are highlighted. Finally, the remaining challenges in flexible thermoelectric materials are discussed in conclusion, and suggestions and a framework to guide future development are provided, which may pave the way for a bright future for flexible thermoelectric devices in the energy market.

Flexible Thermoelectric Materials and Generators: Challenges and Innovations.

The programmable nature of smart textiles makes them an indispensable part of an emerging new technology field. Smart textile-integrated microelectronic systems (STIMES), which combine microelectronics and technology such as artificial intelligence and augmented or virtual reality, have been intensively explored. A vast range of research activities have been reported. Many promising applications in healthcare, the internet of things (IoT), smart city management, robotics, etc., have been demonstrated around the world. A timely overview and comprehensive review of progress of this field in the last five years are provided. Several main aspects are covered: functional materials, major fabrication processes of smart textile components, functional devices, system architectures and heterogeneous integration, wearable applications in human and nonhuman-related areas, and the safety and security of STIMES. The major types of textile-integrated nonconventional functional devices are discussed in detail: sensors, actuators, displays, antennas, energy harvesters and their hybrids, batteries and supercapacitors, circuit boards, and memory devices.

Smart Textile-Integrated Microelectronic Systems for Wearable Applications

Flexible thermoelectric materials and devices

Thermoelectric devices that are flexible and optically transparent hold unique promise for future electronics. However, development of invisible thermoelectric elements is hindered by the lack of p-type transparent thermoelectric materials. Here we present the superior room-temperature thermoelectric performance of p-type transparent copper iodide (CuI) thin films. Large Seebeck coefficients and power factors of the obtained CuI thin films are analysed based on a single-band model. The low-thermal conductivity of the CuI films is attributed to a combined effect of the heavy element iodine and strong phonon scattering. Accordingly, we achieve a large thermoelectric figure of merit of ZT=0.21 at 300 K for the CuI films, which is three orders of magnitude higher compared with state-of-the-art p-type transparent materials. A transparent and flexible CuI-based thermoelectric element is demonstrated. Our findings open a path for multifunctional technologies combing transparent electronics, flexible electronics and thermoelectricity. Flexible thermoelectric devices with high optical transparency may enable new applications; however, the lack of a p-type counterpart has hitherto hindered its development. Yanget al., report a transparent p-type thermoelectric based on polycrystalline copper iodide thin film with record performance.

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Transparent flexible thermoelectric material based on non-toxic earth-abundant p-type copper iodide thin film.

CuI is a p-type transparent conductive semiconductor with unique optoelectronic properties, including wide band gap (3.1 eV), high hole mobility (>40 cm2 V−1 s−1 in bulk) and large room-temperature exciton binding energy (62 meV). The difficulty in epitaxy of CuI is the main obstacle for its application in advanced solid-state electronic devices. Herein, room-temperature heteroepitaxial growth of CuI on various substrates with well-defined in-plane epitaxial relations is realized by reactive sputtering technique. In such heteroepitaxial growth the formation of rotation domains is observed and hereby systematically investigated in accordance with existing theoretical study of domain-epitaxy. The controllable epitaxy of CuI thin films allows for the combination of p-type CuI with suitable n-type semiconductors with the purpose to fabricate epitaxial thin film heterojunctions. Such heterostructures have superior properties to structures without or with weakly ordered in-plane orientation. The obtained epitaxial thin film heterojunction of p-CuI(111)/n-ZnO(00.1) exhibits a high rectification up to 2 × 109 (±2 V), a 100-fold improvement compared to diodes with disordered interfaces. Also a low saturation current density down to 5 × 10−9 Acm−2 is formed. These results prove the great potential of epitaxial CuI as a promising p-type optoelectronic material.

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Room-temperature Domain-epitaxy of Copper Iodide Thin Films for Transparent CuI/ZnO Heterojunctions with High Rectification Ratios Larger than 10 9

High-quality Ga2O3 thin films in the orthorhombic κ-phase are grown by pulsed-laser deposition using a tin containing target on c-sapphire, MgO(111), SrTiO3(111), and yttria-stabilized ZrO2(111) substrates. The structural quality of the layers is studied based on the growth parameters employing X-ray diffraction 2θ-ω scans, rocking curves, ϕ scans, and reciprocal space maps. Our layers exhibit superior crystalline properties in comparison to thin films deposited in the monoclinic β-phase at nominally identical growth parameters. Furthermore, the surface morphology is significantly improved and the root-mean-squared roughness of the layers was as low as ≈0.5 nm, on par with homoepitaxial β-Ga2O3 thin films in the literature. The orthorhombic structure of the thin films was evidenced, and the epitaxial relationships were determined for each kind of the substrate. A tin-enriched surface layer on our thin films measured by depth-resolved photoelectron spectroscopy suggests surfactant-mediated epitaxy as a possible growth mechanism. Thin films in the κ-phase are a promising alternative for β-Ga2O3 layers in electronic and optoelectronic device applications.High-quality Ga2O3 thin films in the orthorhombic κ-phase are grown by pulsed-laser deposition using a tin containing target on c-sapphire, MgO(111), SrTiO3(111), and yttria-stabilized ZrO2(111) substrates. The structural quality of the layers is studied based on the growth parameters employing X-ray diffraction 2θ-ω scans, rocking curves, ϕ scans, and reciprocal space maps. Our layers exhibit superior crystalline properties in comparison to thin films deposited in the monoclinic β-phase at nominally identical growth parameters. Furthermore, the surface morphology is significantly improved and the root-mean-squared roughness of the layers was as low as ≈0.5 nm, on par with homoepitaxial β-Ga2O3 thin films in the literature. The orthorhombic structure of the thin films was evidenced, and the epitaxial relationships were determined for each kind of the substrate. A tin-enriched surface layer on our thin films measured by depth-resolved photoelectron spectroscopy suggests surfactant-mediated epitaxy as a pos...

Tin-assisted heteroepitaxial PLD-growth of κ-Ga2O3 thin films with high crystalline quality

Heteroepitaxial growth of α-, β-, γ- and κ-Ga2O3 phases by metalorganic vapor phase epitaxy

Material properties of orthorhombic κ-phase (InxGa1−x)2O3 thin films grown on a c-plane sapphire substrate by pulsed-laser deposition are reported for an indium content up to x ∼ 0.35. This extended range of miscibility enables band gap engineering between 4.3 and 4.9 eV. The c-lattice constant as well as the bandgap depends linearly on the In content. For x > 0.35, a phase change to the hexagonal InGaO3(ii) and the cubic bixbyite structure occurred. The dielectric function and the refractive index were determined by spectroscopic ellipsometry as a function of the alloy composition. We propose zirconium to induce n-type conductivity and have achieved electrically conducting thin films with a room temperature conductivity of up to 0.1 S/cm for samples with a low In content of about x = 0.01. Temperature-dependent Hall-effect measurements yielded a thermal activation energy of the free electron density of 190 meV. Schottky barrier diodes with rectification ratios up to 106 were investigated by quasi-static capacitance voltage and temperature-dependent current voltage measurements.

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Max Kneiß

Papers

Transparent flexible thermoelectric material based on non-toxic earth-abundant p-type copper iodide thin film.

Room-temperature Domain-epitaxy of Copper Iodide Thin Films for Transparent CuI/ZnO Heterojunctions with High Rectification Ratios Larger than 10 9

Tin-assisted heteroepitaxial PLD-growth of κ-Ga2O3 thin films with high crystalline quality

Heteroepitaxial growth of α-, β-, γ- and κ-Ga2O3 phases by metalorganic vapor phase epitaxy

Structural, optical, and electrical properties of orthorhombic κ -(In x Ga 1-x ) 2 O 3 thin films