Ferroelectronics Lab

Understanding and utilizing non-volatile properties of materials

New Publication! “Chemically-Disordered Transparent Conductive Perovskites With High Crystalline Fidelity”

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Abstract: This manuscript presents a working model linking chemical disorder and transport properties in correlated-electron perovskites with high-entropy formulations and a framework to actively design them. This work demonstrates this new learning in epitaxial Srx(Ti,Cr,Nb,Mo,W)O3 thin films that exhibit exceptional crystalline fidelity despite a diverse chemical formulation where most B-site species are highly misfit with respect to valence and radius. X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy confirm a unique combination of chemical disorder and structural perfection in thin and thick epitaxial layers. This combination produces an optical transparency window that surpasses that of the constituent end-members in the UV and IR, while maintaining relatively low electrical resistivity. This work addresses the computational challenges of modeling such systems and investigate short-range ordering using cluster expansion. These results showcase that unusual d-metal combinations access an expanded property design space that is predictable using end-member characteristics and their interactions– though unavailable to them– thus offering performance advances in optical, high-frequency, spintronic, and quantum devices.

Read more at Advanced Science

New Publication! ” Local structure maturation in high entropy oxide (Mg,Co,Ni,Cu,Zn)1-x(Cr,Mn)xO thin films”

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Abstract: High entropy oxides (HEOs) have garnered much interest due to their available high degree of tunability. Here, we study the local structure of (MgNiCuCoZn)0.167(MnCr)0.083O, a composition based on the parent HEO (MgNiCuCoZn)0.2O. We synthesized a series of thin films via pulsed laser deposition at incremental oxygen partial pressures. X-ray diffraction shows lattice parameters to decrease with increased pO2 pressures until the onset of phase separation. X-ray absorption fine structure shows that specific atomic species in the composition dictate the global structure of the material as Cr, Co, and Mn shift to energetically favorable coordination with increasing pressure. Transmission electron microscopy analysis on a lower-pressure sample exhibits a rock salt structure, but the higher-pressure sample reveals reflections reminiscent of the spinel structure. In all, these findings give a more complete picture of how (MgNiCuCoZn)0.167(MnCr)0.083O forms with varying initial conditions and advances fundamental knowledge of cation behavior in high entropy oxides.

Full text available at The Journal of the American Ceramic Society

New Publication! “Perspective: Entropy-Stabilized Oxide Memristors”

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Abstract: A memristor array has emerged as a potential computing hardware for artificial intelligence (AI). It has an inherent memory effect that allows information storage in the form of easily programmable electrical conductance, making it suitable for efficient data processing without shuttling of data between the processor and memory. To realize its full potential for AI applications, fine-tuning of internal device dynamics is required to implement a network system that employs dynamic functions. Here, we provide a perspective on multicationic entropy-stabilized oxides as a widely tunable materials system for memristor applications. We highlight the potential for efficient data processing in machine learning tasks enabled by the implementation of “task specific” neural networks that derive from this material tunability.

Full text available from Applied Physics Letters

New Publication! “Investigation of the Influence of Growth Conditions on the Local Structure in High Entropy Oxides Using S/TEM”

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Abstract: Recently, the chemically disordered multi-cation oxide class of materials called High Entropy Oxides (HEOs) has been widely explored due to their tunable functional properties because of their higher configurational entropy and to understand their fundamental phase formation. These HEOs have shown potential applications as thermoelectrics, ionic conductors, electrocaloric materials, etc. Since these systems have multiple aliovalent cations in a single lattice, it necessitates the understanding of elemental distribution and structure of these novel oxides. This would help us understand how the HEOs navigate the configurational space and enable us to establish a correlation between structure and property. In this study, we are investigating the influence of oxygen partial pressure during pulsed laser deposition on the structure, and chemical environment on the HEO thin films. (Mg0.2Ni0.2Co0.2Cu0.2Zn0.2)O, commonly known as ‘J14’, is the prototype HEO that has been widely studied. We are currently exploring the seven component HEO system with the composition: (Mg0.167Ni0.167Co0.167Cu0.167Zn0.167(Cr, Mn)0.167)O, referred to as ‘J14MnCr’. The goal of this study is to understand the influence of addition of Cr and Mn to J14 on the structure and how the growth conditions modulate the structure and tune magnetic properties. Due to the presence of seven cations with some cations that can adapt multiple valences, it is necessary to probe the structural nuances and chemical environment in these systems. In this study, Scanning/Transmission Electron Microscope is used to characterize the HEOs as S/TEM allows us to probe the structure, composition, and valence variation at nanoscale regime.

We have probed the J14MnCr thin film grown at 5mTorr and 50mTorr oxygen partial pressure. We have observed from Selected Area Electron Diffraction (SAED) and dark field TEM experiments that there is a change in the crystal structure in the films grown at 5mTorr vs. 50mTorr. At 50mTorr, the SAED reveals the formation of rock salt structure with additional secondary phase. The increase in oxygen partial pressure during synthesis has led to the nucleation of a new phase with a different structure which is speculated to influence the magnetic property. We have further performed STEM experiments and will be implementing unsupervised machine learning to detect the local structural variation. STEM-EELS experiments have also been performed to investigate the local changes in structure and to correlate it to changes in the valences of the cations and chemical environment. These S/TEM experiments enable us to understand the influence of processing conditions on microstructures and chemical environment, informing us about the structural nuances at the nanoscale and allowing us to tune the structure for desired properties.

Full text available from Microscopy and Microanalysis

New publication! “Efficient Data Processing Using Tunable Entropy-Stabilized Oxide Memristors“

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Abstract: Memristive devices are of potential use in a range of computing applications. However, many of these devices are based on amorphous materials, where systematic control of the switching dynamics is challenging. Here we report tunable and stable memristors based on an entropy-stabilized oxide. We use single-crystalline (Mg,Co,Ni,Cu,Zn)O films grown on an epitaxial bottom electrode. By adjusting the magnesium composition (XMg = 0.11–0.27) of the entropy-stabilized oxide films, a range of internal time constants (159–278 ns) for the switching process can be obtained. We use the memristors to create a reservoir computing network that classifies time-series input data and show that the reservoir computing system, which has tunable reservoirs, offers better classification accuracy and energy efficiency than previous reservoir system implementations.

Full text available from Nature Electronics

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Our research is at the intersection of multiple disciplines, drawing on principles and methodologies from materials science, chemistry, physics, and electrical engineering. Our mission is to pioneer … Read More

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Ferroelectronics Lab
Address: 2030 H.H. Dow

T: (734) 763-6914
E: jtheron@umich.edu