Strain engineering provides the ability to control the ground states and associated phase transition in the epitaxial films. However, the systematic study of intrinsic characters and their strain dependency in transition-metal nitrides remains challenging due to the difficulty in fabricating the stoichiometric and high-quality films. Here we report the observation of electronic state transition in highly crystalline antiferromagnetic CrN films with strain and reduced dimensionality. Shrinking the film thickness to a critical value of ~ 30 unit cells, a profound conductivity reduction accompanied by unexpected volume expansion is observed in CrN films. The electrical conductivity is observed surprisingly when the CrN layer as thin as single unit cell thick, which is far below the critical thickness of most metallic films. We found that the metallicity of an ultrathin CrN film recovers from an insulating behavior upon the removal of as-grown strain by fabrication of first-ever freestanding nitride films. Both first-principles calculations and linear dichroism measurements reveal that the strain-mediated orbital splitting effectively customizes the relatively small bandgap at the Fermi level, leading to exotic phase transition in CrN. The ability to achieve highly conductive nitride ultrathin films by harness strain-controlling over competing phases can be used for utilizing their exceptional characteristics.
Ni doping Ti0.5Zr0.25Hf0.25Co1−xNixSb (x=0–0.05) half-Heusler compounds have been fabricated by combining high-frequency induction melting with spark plasma sintering technique, and their thermoelectric transport properties have been investigated in the temperature range of 300–900K. With the increase of Ni doping content, the electrical conductivity increases significantly, and withal the Seebeck coefficient of all doped samples improve to some extent compared with the undoped Ti0.5Zr0.25Hf0.25CoSb compound. These lead to a great improvement in the power factor, and the highest power factor of 1.63×10−3Wm−1K−1 is obtained at 715K for Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound. Furthermore, thermal conductivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds decrease remarkably due to Zr and Hf substitutions on Ti site and Ni doping on Co site. Compared with ternary TiCoSb compound, the thermal conductivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb compound decreases 415%–430% at room temperature, and compared with undoped Ti0.5Zr0.25Hf0.25CoSb compound, the thermal conductivity of Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb decreases 34% at 300K and 21% at 900K, respectively. A maximum dimensionless figure of merit ZT of 0.51 has been achieved for Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound at 813K.
Dedicated control of oxygen vacancies is an important route to functionalizing complex oxide films. It is well-known that tensile strain significantly lowers the oxygen vacancy formation energy, whereas compressive strain plays a minor role. Thus, atomic reconstruction by extracting oxygen from a compressive-strained film is challenging. Here we report an unexpected LaCoO2.5 phase with a zigzag-like oxygen vacancy ordering through annealing a compressive-strained LaCoO3 in vacuum. The synergetic tilt and distortion of CoO5 square pyramids with large La and Co shifts are quantified using scanning transmission electron microscopy. The large in-plane expansion of CoO5 square pyramids weaken the crystal field splitting and facilitated the ordered high-spin state of Co2+, which produces an insulating ferromagnetic state with a Curie temperature of ~284 K and a saturation magnetization of ~0.25 μB/Co. These results demonstrate that extracting targeted oxygen from a compressive-strained oxide provides an opportunity for creating unexpected crystal structures and novel functionalities.
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