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The presence of inclusions, twinning, and low-angle grain boundaries, demanded to exist by the third law of thermodynamics, drive the behavior of quantum materials. Identification and quantification of these structural complexities often requires destructive techniques. X-ray micro-computed tomography (µCT) uses high-energy X-rays to non-destructively generate 3D representations of a material with micron/nanometer precision, taking advantage of various contrast mechanisms to enable the quantification of the types and number of inhomogeneities. We present case studies of µCT informing materials design of electronic and quantum materials, and the benefits to characterizing inclusions, twinning, and low-angle grain boundaries as well as optimizing crystal growth processes. We discuss recent improvements in µCT instrumentation that enable elemental analysis and orientation to be obtained on crystalline samples. The benefits of µCT as a non-destructive tool to analyze bulk samples should encourage the community to adapt this technology into everyday use for quantum materials discovery.

 

Entropic stabilization has evolved into a strategy to create new oxide materials and realize novel functional properties engineered through the alloy composition. Achieving an atomistic understanding of these properties to enable their design, however, has been challenging due to the local compositional and structural disorder that underlies their fundamental structure-property relationships. Here, we combine high-throughput atomistic calculations and linear regression algorithms to investigate the role of local configurational and structural disorder on the thermodynamics of vacancy formation in (MgCoNiCuZn)O-based entropy-stabilized oxides (ESOs) and their influence on the electrical properties. We find that the cation-vacancy formation energies decrease with increasing local tensile strain caused by the deviation of the bond lengths in ESOs from the equilibrium bond length in the binary oxides. The oxygen-vacancy formation strongly depends on structural distortions associated with the local configuration of chemical species. Vacancies in ESOs exhibit deep thermodynamic transition levels that inhibit electrical conduction. By applying the charge-neutrality condition, we determine that the equilibrium concentrations of both oxygen and cation vacancies increase with increasing Cu mole fraction. Our results demonstrate that tuning the local chemistry and associated structural distortions by varying alloy composition acts an engineering principle that enables controlled defect formation in multi-component alloys.

 

Rutile compounds have exotic functional properties that can be applied for various electronic applications; however, the limited availability of epitaxial substrates has restricted the study of rutile thin films to a limited range of lattice parameters. Here, rutile GeO 2 is demonstrated as a new rutile substrate with lattice parameters of [Formula: see text] and [Formula: see text]. Rutile GeO 2 single crystals up to 4 mm in size are grown by the flux method. X-ray diffraction reveals high crystallinity with a rocking curve having a full width half-maximum of 0.0572°. After mechanical polishing, a surface roughness of less than 0.1 nm was obtained, and reflection high-energy electron diffraction shows a crystalline surface. Finally, epitaxial growth of (110)-oriented TiO 2 thin films on GeO 2 substrates was demonstrated using molecular beam epitaxy. Templated by rutile GeO 2 substrates, our findings open the possibility of stabilizing new rutile thin films and strain states for the tuning of physical properties. 

Abstract Compelling evidence suggests distinct correlated electron behavior may exist only in clean 2D materials such as 1T-TaS 2 . Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers disrupts correlation-driven quantum behavior. Here we demonstrate a route to realizing fragile 2D quantum states through endotaxial polytype engineering of van der Waals materials. The true isolation of 2D charge density waves (CDWs) between metallic layers stabilizes commensurate long-range order and lifts the coupling between neighboring CDW layers to restore mirror symmetries via interlayer CDW twinning. The twinned-commensurate charge density wave (tC-CDW) reported herein has a single metal–insulator phase transition at ~350 K as measured structurally and electronically. Fast in-situ transmission electron microscopy and scanned nanobeam diffraction map the formation of tC-CDWs. This work introduces endotaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication. 

Magnetoactive soft materials, typically composed of magnetic particles dispersed in a soft polymer matrix, are finding many applications in soft robotics due to their reversible and remote shape transformations under magnetic fields. To achieve complex shape transformations, anisotropic, and heterogeneous magnetization profiles must be programmed in the material. However, once programmed and assembled, magnetic soft actuators cannot be easily reconfigured, repurposed, or repaired, which limits their application, their durability, and versatility in their design. Here, magnetoactive soft composites are developed from squid‐derived biopolymers and NdFeB microparticles with tunable ferromagnetic and thermomechanical properties. By leveraging reversible crosslinking nanostructures in the biopolymer matrix, a healing‐assisted assembly process is developed that allows for on‐demand reconfiguration and magnetic reprogramming of magnetoactive composites. This concept in multi‐material modular actuators is demonstrated with programmable deformation modes, self‐healing properties to recover their function after mechanical damage, and shape‐memory behavior to lock in their preferred configuration and un‐actuated catch states. These dynamic magnetic soft composites can enable the modular design and assembly of new types of magnetic actuators, not only eliminating device vulnerabilities through healing and repair but also by providing adaptive mechanisms to reconfigure their function on demand.

 

Non‐collinear antiferromagnets (AFMs) are an exciting new platform for studying intrinsic spin Hall effects (SHEs), phenomena that arise from the materials’ band structure, Berry phase curvature, and linear response to an external electric field. In contrast to conventional SHE materials, symmetry analysis of non‐collinear antiferromagnets does not forbid non‐zero longitudinal and out‐of‐plane spin currents with polarization and predicts an anisotropy with current orientation to the magnetic lattice. Here, multi‐component out‐of‐plane spin Hall conductivities are reported in L1₂‐ordered antiferromagnetic PtMn₃thin films that are uniquely generated in the non‐collinear state. The maximum spin torque efficiencies (ξ  =J_S /J_e ≈ 0.3) are significantly larger than in Pt (ξ  ≈  0.1). Additionally, the spin Hall conductivities in the non‐collinear state exhibit the predicted orientation‐dependent anisotropy, opening the possibility for new devices with selectable spin polarization. This work demonstrates symmetry control through the magnetic lattice as a pathway to tailored functionality in magnetoelectronic systems.

 

BAs is a III–V semiconductor with ultra-high thermal conductivity, but many of its electronic properties are unknown. This work applies predictive atomistic calculations to investigate the properties of BAs heterostructures, such as strain effects on band alignments and carrier mobility, considering BAs as both a thin film and a substrate for lattice-matched materials. The results show that isotropic biaxial in-plane strain decreases the band gap independent of sign or direction. In addition, 1% biaxial tensile strain increases the in-plane electron and hole mobilities at 300 K by >60% compared to the unstrained values due to a reduction of the electron effective mass and of hole interband scattering. Moreover, BAs is shown to be nearly lattice-matched with InGaN and ZnSnN₂, two important optoelectronic semiconductors with tunable band gaps by alloying and cation disorder, respectively. The results predict type-II band alignments and determine the absolute band offsets of these two materials with BAs. The combination of the ultra-high thermal conductivity and intrinsic p-type character of BAs, with its high electron and hole mobilities that can be further increased by tensile strain, as well as the lattice-match and the type-II band alignment with intrinsically n-type InGaN and ZnSnN₂demonstrate the potential of BAs heterostructures for electronic and optoelectronic devices.