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.
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.
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.
The structural, surface, and optical properties of phase-pure κ-(AlxGa1−x)2O3 thin films on c-sapphire and STO(111):Nb substrates as well as on MgO(111) and κ-Ga2O3 templates are reported as a function of alloy composition for x < 0.4. The thin films were grown by tin-assisted pulsed laser deposition (PLD). For the variation of the Al-content, we utilized radially segmented PLD targets that enable the deposition of a thin film material library by discrete composition screening. Growth on κ-Ga2O3 (001) thin film templates enhanced the phase pure growth window remarkably up to x = 0.65. The crystallization of the κ-phase was verified by X-ray diffraction 2θ-ω-scans for all samples. Both in- and out-of-plane lattice constants in dependence on the Al-content follow a linear relationship according to Vegard’s law over the complete composition range. Atomic force microscope measurements confirm smooth surfaces (Rq ≈ 1.4 nm) for all investigated Al-contents. Furthermore, bandgap tuning from 4.9 eV to 5.8 eV is demonstrated and a linear increase in the bandgap with increasing Al-content was observed.
High-quality (InxGa1−x)2O3 thin films in the orthorhombic κ-phase were grown by pulsed-laser deposition (PLD) on c-sapphire substrates as well as PLD-grown κ-Ga2O3 thin film templates. We varied the In-content 0 ≤ x ≤ 0.38 of the layers using a single, elliptically segmented, and tin-doped (In0.4Ga0.6)2O3/Ga2O3 target, employing the vertical continuous composition spread (VCCS) PLD-technique. A stoichiometric transfer of In and Ga from the target to the thin films has been confirmed, suggesting that the formation of volatile Ga2O and In2O suboxides is not a limiting factor in the tin-assisted growth mode. For all x, the thin films crystallized predominantly in the κ-modification as demonstrated by XRD 2θ-ω scans. However, for x > 0.28, phase separation of the cubic bixbyite and the κ-phase occurred. The κ-Ga2O3 template increased the crystalline quality of the κ-(InxGa1−x)2O3 thin film layers remarkably. Epitaxial, but relaxed growth with three in-plane rotational domains has been found for all thin films by XRD ϕ-scans or reciprocal space map measurements. Smooth surface morphologies (Rq < 3 nm) for all phase pure thin films were evidenced by atomic force microscopy measurements, making them suitable for multilayer heterostructures. The composition-dependent in- and out-of plane lattice constants follow a linear behavior according to Vegard’s law. A linear relationship can also be confirmed for the optical bandgaps that demonstrate the feasibility of bandgap engineering in the energy range of 4.1–4.9 eV. The results suggest κ-(InxGa1−x)2O3 as a promising material for heterostructure device applications or photodetectors.
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