No Arabic abstract
We report charge-transfer up to a single electron per interfacial unit cell across non-polar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and tri-layer systems grown using pulsed laser deposition, soft X-ray absorption, dichroism and STEM-EELS are used to probe the cobalt 3d-electron count and provide an element-specific investigation of the magnetic properties. The experiments prove a deterministically-tunable charge transfer process acting in the LaCoO3 within three unit cells of the heterointerface, able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3 / LaCoO3 interfaces, the thickness of an additional break layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in tri-layers provide a trio of sensitive control knobs for the charge transfer process, illustrating the efficacy of O2p-band alignment as a guiding principle for property design in complex oxide heterointerfaces.
Controlling interfacial interactions in magnetic/topological insulator heterostructures is a major challenge for the emergence of novel spin-dependent electronic phenomena. As for any rational design of heterostructures that rely on proximity effects, one should ideally retain the overall properties of each component while tuning interactions at the interface. However, in most inorganic interfaces interactions are too strong, consequently perturbing, and even quenching, both the magnetic moment and the topological surface states at each side of the interface. Here we show that these properties can be preserved by using ligand chemistry to tune the interaction of magnetic ions with the surface states. By depositing Co-based porphyrin and phthalocyanine monolayers on the surface of Bi$_2$Te$_3$ thin films, robust interfaces are formed that preserve undoped topological surface states as well as the pristine magnetic moment of the divalent Co ions. The selected ligands allow us to tune the interfacial hybridization within this weak interaction regime. These results, which are in stark contrast with the observed suppression of the surface state at the first quintuple layer of Bi$_2$Se$_3$ induced by the interaction with Co phthalocyanines, demonstrate the capability of planar metal-organic molecules to span interactions from the strong to the weak limit.
Perovskite stability is of the core importance and difficulty in current research and application of perovskite solar cells. Nevertheless, over the past century, the formability and stability of perovskite still relied on simplified factor based on human knowledge, such as the commonly used tolerance factor t. Combining machine learning (ML) with first-principles density functional calculations, we proposed a strategy to firstly calculate the decomposition energies, considered to be closely related to thermodynamic stability, of 354 kinds halide perovskites, establish the machine learning relationship between decomposition energy and compositional ionic radius and investigate the stabilities of 14,190 halide double perovskites. The ML-predicted results enable us to rediscover a series of stable rare earth metal halide perovskites (up to ~1000 kinds), indicating the generalization of this model and further provide elemental and concentration suggestion for improving the stability of mixed perovskite.
The interfacial behavior of quantum materials leads to emergent phenomena such as two dimensional electron gases, quantum phase transitions, and metastable functional phases. Probes for in situ and real time surface sensitive characterization are critical for active monitoring and control of epitaxial synthesis, and hence the atomic-scale engineering of heterostructures and superlattices. Termination switching, especially as an interfacial process in ternary complex oxides, has been studied using a variety of probes, often ex situ; however, direct observation of this phenomena is lacking. To address this need, we establish in situ and real time reflection high energy electron diffraction and Auger electron spectroscopy for pulsed laser deposition, which provide structural and compositional information of the surface during film deposition. Using this unique capability, we show, for the first time, the direct observation and control of surface termination in complex oxide heterostructures of SrTiO3 and SrRuO3. Density-functional-theory calculations capture the energetics and stability of the observed structures and elucidate their electronic behavior. This demonstration opens up a novel approach to monitor and control the composition of materials at the atomic scale to enable next-generation heterostructures for control over emergent phenomena, as well as electronics, photonics, and energy applications.
In this work we show the presence of a magnetoelectric coupling in silicon-nitride gated Pt/Co/Pt heterostructures using X-ray photoemission electron microscopy (XPEEM). We observe a change in magnetic anisotropy in the form of domain wall nucleation and a change in the rate of domain wall fluctuation as a function of the applied electric field to the sample. We also observe the coexistence of in-plane and out of plane magnetization in Pt/Co/Pt heterostructures in a region around the spin reorientation transition whose formation is attributed to substrate surface roughness comparable to the film thickness; with such domain configuration, we find that the in-plane magnetization is more sensitive to the applied electric field than out of plane magnetization. Although we find an effective magnetoelectric coupling in our system, the presence of charge defects in the silicon nitride membranes hampers a systematic electrostatic control of the magnetization.
Antiferromagnetic thin films typically exhibit a multi-domain state, and control of the antiferromagnetic Neel vector is challenging as antiferromagnetic materials are robust to magnetic perturbations. By relying on anisotropic in-plane strain engineering of epitaxial thin films of the prototypical antiferromagnetic material LaFeO3, uniaxial Neel vector control is demonstrated. Orthorhombic (011)- and (101)-oriented DyScO3, GdScO3 and NdGaO3 substrates are used to engineer different anisotropic in-plane strain states. The anisotropic in-plane strain stabilises structurally monodomain monoclinic LaFeO3 thin films. The uniaxial Neel vector is found along the tensile strained b axis, contrary to bulk LaFeO3 having the Neel vector along the shorter a axis, and no magnetic domains are found. Hence, anisotropic strain engineering is a viable tool for designing unique functional responses, further enabling antiferromagnetic materials for mesoscopic device technology.