Albina Y Borisevich

Oak Ridge National Laboratory | ORNL · Materials Science and Technology Division

The functionalities and diverse metastable phases of multiferroic BiFeO3 (BFO) thin films depend on the misfit strain. Although mixed phase-induced strain relaxation in multiphase BFO thin films is well known, it is unclear whether a single-crystalline BFO thin film can accommodate misfit strain without the involvement of its polymorphs. Thus, unde...

High nickel content layered oxide LiNi0.8Mn0.1Co0.1O2 (NMC811) is a promising cathode material with a high theoretical capacity of 200 mAh g-1 for use in high energy density lithium-ion batteries. However, its surface can easily get passivated by LiOH and Li2CO3 due to its surface residual Li2O being reacting with ambient moisture and CO2. Herein,...

High‐capacity metal oxide conversion anodes for lithium‐ion batteries (LIBs) are primarily limited by their poor reversibility and cycling stability. In this study, a promising approach has been developed to improve the electrochemical performance of a MoO2 anode by direct fluorination of the prelithiated MoO2. The fluorinated anode contains a mixt...

In this Letter, we used fluorescence microscopy to image the reversible transformation of individual CsPbCl3 nanocrystals to CsPbBr3, which enables us to quantify heterogeneity in reactivity among hundreds of nanocrystals prepared within the same batch. We observed a wide distribution of waiting times for individual nanocrystals to react as has bee...

Ultrathin epitaxial films of ferromagnetic insulators (FMIs) with Curie temperatures near room temperature are critically needed for use in dissipationless quantum computation and spintronic devices. However, such materials are extremely rare. Here, a room‐temperature FMI is achieved in ultrathin La0.9Ba0.1MnO3 films grown on SrTiO3 substrates via...

We introduce novel communication strategies in synchronous distributed Deep Learning consisting of decentralized gradient reduction orchestration and computational graph-aware grouping of gradient tensors. These new techniques produce an optimal overlap between computation and communication and result in near-linear scaling (0.93) of distributed tr...

A central problem of solid polymer electrolytes is their inability to achieve robust mechanical strength with fast ionic conductivities required for commercialization of lithium metal batteries (LMBs). At present, state‐of‐the‐art offers superiority of one at the expense of the other. Here, this dilemma has been solved by fabricating mechanically r...

A STEM-based Path Towards Atomic-scale Silicon-based Devices - Volume 25 Supplement - Bethany M. Hudak, Stephen Jesse, Jiaming Song, Albina Borisevich, Paul C. Snijders, Sergei V. Kalinin, Andrew R. Lupini

Tracing Oxygen Transport Pathways with In-Situ STEM and Theory - Volume 25 Supplement - Axiel Yaël Birenbaum, Valentino R. Cooper, Albina Borisevich

Functional oxide superlattices offer new and exciting possibilities for the exploration of emergent properties at the nanoscale. While the behavior of La1−xSrxFeO3 films has been extensively investigated at low temperatures, few studies have been carried out at high temperatures, particularly for LaFeO3/SrFeO3 superlattice systems. Here, we investi...

Solar cells made up of lead-halide perovskites have shown a remarkable increase in power conversion efficiency; however, they are plagued with instability issues that combined with the toxicity of lead have led to a search for new semiconductors made up of heavy and non-toxic metals such as bismuth. Here, we report on a new, inorganic, double perov...

Deep learning has demonstrated superb efficacy in processing imaging data, yet its suitability in solving challenging inverse problems in scientific imaging has not been fully explored. Of immense interest is the determination of local material properties from atomically-resolved imaging, such as electron microscopy, where such information is encod...

Three trimethylsilyl based malonate esters, bis(trimethylsilyl) 2-methyl-2-fluoromalonate (BTMSMFM), bis(trimethylsilyl) 2-ethyl-2-fluoromalonate (BTMSEFM) and bis(trimethylsilyl) 2-propyl-2-fluoromalonate (BTMSPFM), have been used as additives in 1.0 M LiPF6/ethylene carbonate (EC)-dimethyl carbonate (DMC)-diethyl carbonate (DEC) (1-1-1, by v) bas...

The authors report the epitaxial growth and the dielectric properties of relaxor ferroelectric 0.5Ba(Zr0.2Ti0.8)O3–0.5(Ba0.7Ca0.3)TiO3 thin films with atomically flat surface on GdScO3 single crystal substrates. The authors studied the effects of growth conditions, such as the substrate temperature and the oxygen pressure on the structure of the th...

To evaluate the role of planar defects in lead-halide perovskites — cheap, versatile semiconducting materials — it is critical to examine their structure, including defects, at the atomic scale and develop a detailed understanding of their impact on electronic properties. In this study, we combine post-synthesis nanocrystal fusion, aberration-corre...

Lead-halide perovskite nanocrystals (PNCs) have attracted much attention in recent years due to their outstanding optical properties. We report here a new chemical route for triggering post-synthetic growth of CsPbBr3 PNCs at room temperature via intentional depletion of stabilizing ligands, resulting in an immediate fusion growth of the as-synthes...

We study the nonlinear optical response in a strained thin film ferroelectric oxide BaTiO3 using piezoelectric Pb(Mg1/3Nb2/3)O3-PbTiO3 (001) as a variable strain substrate and La-doped SrTiO3 as a conductive buffer layer. The rotation-anisotropic second harmonic intensity profile shows hysteretic modulation corresponding to the strain variation fro...

Ripples and impurity atoms are universally present in 2D materials, limiting carrier mobility, creating pseudo-magnetic fields, or affecting the electronic and magnetic properties. Scanning transmission electron microscopy (STEM) generally provides picometer-level precision in the determination of the location of atoms or atomic 'columns' in the in...

Atomic-Scale Identification of Planar Defects in Cesium Lead Bromide Perovskite Nanocrystals - Volume 24 Supplement - Arashdeep Singh Thind, Guangfu Luo, Jordan A. Hachtel, Mariia Goriacheva, Sung Beom Cho, Albina Borisevich, Juan Carlos Idrobo, Yangchuan Xing, Rohan Mishra

Towards the Mechanism of Oxygen Vacancy Formation & Ordering via Tracking of Beam-Induced Dynamics and Density Functional Theory - Volume 24 Supplement - Axiel Yael Birenbaum, Liang Qiao, Valentino R. Cooper, Albina Borisevich

Rapid Atomic-Resolution Image Analysis: Towards Near-Instant Feedback - Volume 24 Supplement - Oleg S. Ovchinnikov, Andrew O’Hara, Sergei V. Kalinin, Stephen Jesse, Albina Y. Borisevich, Sokrates T. Pantelides

Deep Convolutional Neural Network Approach as a Universal Tool for Determination of Local 3D Structure from ABF STEM Images of Perovskitesy - Volume 24 Supplement - Nouamane Laanait, Albina Y. Borisevich

Towards Atomic-Scale Fabrication in Silicon - Volume 24 Supplement - Bethany M. Hudak, Stephen Jesse, Jiaming Song, Albina Borisevich, Paul C. Snijders, Sergei V. Kalinin, Andrew R. Lupini

Atomic Manipulation on a Scanning Transmission Electron Microscope Platform using Real-Time Image Processing and Feedback - Volume 24 Supplement - Ondrej Dyck, Songkil Kim, Albina Borisevich, Bethany M. Hudak, Andrew R. Lupini, Sergei V. Kalinin, Stephen Jesse

The Si-compatibility of perovskite heterostructures offers the intriguing possibility of producing oxide-based quantum well (QW) optoelectronic devices for use in Si photonics. While the SrTiO3/LaAlO3 (STO/LAO) system has been studied extensively in the hopes of using the interfacial 2-dimensional electron gas in Si-integrated electronics, the pote...

Single and few-layers MoS 2 were uniformly grown on the surface of chemically reduced graphene oxide (r-GO), via a facile liquid phase approach. The method is based on a simple functionalization of r-GO with oleyl amine which seems to affect significantly the MoS 2 way of growth. Scanning-transmission-electron microscopy (STEM) analysis revealed th...

Single and few-layers MoS 2 were uniformly grown on the surface of chemically reduced graphene oxide (r-GO), via a facile liquid phase approach. The method is based on a simple functionalization of r-GO with oleyl amine which seems to affect significantly the MoS 2 way of growth. Scanning-transmission-electron microscopy (STEM) analysis revealed th...

The equilibrium position of atoms in a unit cell is directly connected to crystal functionalities, e.g., ferroelectricity, ferromagnetism, and piezoelectricity. The artificial tuning of the energy landscape can involve repositioning atoms as well as manipulating the functionalities of perovskites (ABO3), which are good model systems to test this le...

Dielectric relaxation in ABO3 perovskite oxides can result from many different charge carrier-related phenomena. Despite a strong understanding of dielectric relaxations, a detailed investigation of the relationship between the content of oxygen vacancies (VO) and dielectric relaxation has not been performed in perovskite oxide films. In this work,...

Semiconductor fabrication is a mainstay of modern civilization, enabling the myriad applications and technologies that underpin everyday life. However, while sub-10 nanometer devices are already entering the mainstream, the end of the Moore's Law roadmap still lacks tools capable of bulk semiconductor fabrication on sub-nanometer and atomic levels,...

We develop an algorithm for feature extraction based on structural similarity and demonstrate its application for atom and pattern finding in high-resolution electron and scanning probe microscopy images. The use of the combined local identifiers formed from an image subset and appended Fourier, or other transform, allows tuning selectivity to spec...

Semiconductor fabrication is a mainstay of modern civilization, enabling the myriad applications and technologies that underpin everyday life. However, while sub-10 nanometer devices are already entering the mainstream, the end of the Moore's Law roadmap still lacks tools capable of bulk semiconductor fabrication on sub-nanometer and atomic levels,...

Modulation and δ-doping strategies, in which atomically thin layers of charged dopants are precisely deposited within a heterostructure, have played enabling roles in the discovery of new physical behavior in electronic materials. Here, we demonstrate a purely structural “δ-doping” strategy in complex oxide heterostructures, in which atomically thi...

The recent discovery of “polar metals” with ferroelectriclike displacements offers the promise of designing ferroelectrics with tunable energy gaps by inducing controlled metal-insulator transitions. Here we employ first-principles calculations to design a metallic polar superlattice from nonpolar metal components and show that controlled intermixi...

Twenty-one distinct AlxCoCrFeNi alloys were rapidly prepared by laser alloying an equiatomic CoCrFeNi substrate with Al powder to create an alloy library ranging x=0.15-1.32. Variations in crystal structure, microstructure and mechanical properties were investigated using X-ray diffraction, scanning electron microscopy, scanning transmission electr...

Twenty-one distinct AlxCoCrFeNi alloys were rapidly prepared by laser alloying an equiatomic CoCrFeNi substrate with Al powder to create an alloy library ranging x=0.15-1.32. Variations in crystal structure, microstructure and mechanical properties were investigated using X-ray diffraction, scanning electron microscopy, scanning transmission electr...

Strong electronic correlations, interfaces, defects and disorder each individually challenge theoretical methods for predictions of materials properties. These challenges are all simultaneously present in complex transition metal-oxide interfaces and superlattices, which are known to exhibit unique and unusual properties caused by multiple coupled...

Controlling functionalities, such as magnetism or ferroelectricity, by means of oxygen vacancies (VO) is a key issue for the future development of transition-metal oxides. Progress in this field is currently addressed through VO variations and their impact on mainly one order parameter. Here we reveal a mechanism for tuning both magnetism and ferro...

We report on the fabrication of epitaxial La0.5Y0.5AlO3 ultrathin films on (001) LaAlO3 substrates. Structural characterizations by scanning transmission electron microscopy and X-ray diffraction confirm the high quality of the film with AlO6 octahedral tilt pattern. Unlike either of the nonpolar parent compound, LaAlO3 and YAlO3, second harmonic g...

New developments in manufacturing and automation, from three-dimensional printing to the Internet of things, signify dramatic changes in our society. The push toward quantum materials is driving device fabrication toward atomic precision. Recent results suggest that scanning transmission electron microscopy (STEM) with sub-angstrom scale beams coul...

Controlling functionalities, such as magnetism or ferroelectricity, by means of oxygen vacancies (VO) is a key issue for the future development of transition metal oxides. Progress in this field is currently addressed through VO variations and their impact on mainly one order parameter. Here we reveal a new mechanism for tuning both magnetism and f...

Single crystals of the van-der-Waals layered ferrielectric material CuInP2S6 spontaneously phase separate when synthesized with Cu deficiency. Here we identify a route to form and tune intralayer heterostructures between the corresponding ferrielectric (CuInP2S6) and paraelectric (In4/3P2S6 ) phases through control of chemical phase-separation. We...

Structural defects often dominate the electronic- and thermal-transport properties of thermoelectric (TE) materials and are thus a central ingredient for improving their performance. However, understanding the relationship between TE performance and the disordered atomic defects that are generally inherent in nanostructured alloys remains a challen...

Acquisition and Fast Analysis of Multi-Dimensional STEM Data - Volume 23 Issue S1 - Andrew R. Lupini, Albina Y. Borisevich, Juan Carlos Idrobo

Investigating Ionic Transport Anisotropy in Oxygen Deficient Lanthanum Cobaltites via STEM and First Principles Theory - Volume 23 Issue S1 - Axiel Yaël Birenbaum, Liang Qiao, Michael D. Biegalski, Valentino R. Cooper, Albina Y. Borisevich

Identifying Novel Polar Distortion Modes in Engineered Magnetic Oxide Superlattices - Volume 23 Issue S1 - Saurabh Ghosh, Amber Choquette, Steve May, Mark P. Oxley, Andrew R. Lupini, Sokrates T. Pantelides, Albina Y. Borisevich

Vacancy dynamics and ordering underpin the electrochemical functionality of complex oxides and strongly couple to their physical properties. In the field of the epitaxial thin films, where connection between chemistry and film properties can be most clearly revealed, the effects related to oxygen vacancies are attracting increasing attention. In th...

Thin films of magnetic garnet materials, e.g. yttrium iron garnet (Y3Fe5O12, YIG), are useful for a variety of applications including microwave integrated circuits and spintronics. Substitution of rare earth ions, such as cerium, is known to enhance the magneto-optic Kerr effect (MOKE) as compared to pure YIG. Thin films of Ce0.75Y2.25Fe5O12 (Ce:YI...

Octahedral tilt behavior is increasingly recognized as an important contributing factor to the physical behavior of perovskite oxide materials and especially their interfaces, necessitating the development of high-resolution methods of tilt mapping. There are currently two major approaches for quantitative imaging of tilts in scanning transmission...

A wealth of fascinating phenomena have been discovered at the BiFeO3 domain walls, examples such as domain wall conductivity, photovoltaic effects and magnetoelectric coupling. Thus, the ability to precisely control the domain structures and accurately study of their switching behaviors is critical to realize the next generation of novel devices ba...

For epitaxial films, a critical thickness (tc) can create a phenomenological interface between a strained bottom layer and a relaxed top layer. Here, we present an experimental report of how the tc in BiFeO3 thin films acts as a boundary to determine the crystalline phase, ferroelectricity, and piezoelectricity in 60 nm thick BiFeO3/SrRuO3/SrTiO3 s...

Rethink electron microscopy to build quantum materials from scratch, urge Sergei V. Kalinin, Albina Borisevich and Stephen Jesse.

Supported gold (Au) nanocatalysts hold great promise for heterogeneous catalysis; however, their practical application is greatly hampered by poor thermodynamic stability. Herein, a general synthetic strategy is reported where discrete metal nanoparticles are made resistant to sintering, preserving their catalytic activities in high-temperature oxi...

The availability of atomically resolved imaging modalities enables an unprecedented view into the local structural states of materials, which manifest themselves by deviations from the fundamental assumptions of periodicity and symmetry. Consequently, approaches that aim to extract these local structural states from atomic imaging data with minimal...

The identity of active species in supported gold catalysts for low temperature carbon monoxide oxidation remains an unsettled debate. With large amounts of experimental evidence supporting theories of either gold nanoparticles or sub-nm gold species being active, it was recently proposed that a size-dependent activity hierarchy should exist. Here w...

Supplementary Figures 1-8, Supplementary Tables 1-5, Supplementary Notes 1-2 and Supplementary References

The highly energetic electron beam (e-beam) in a scanning transmission electron microscope (STEM) can induce local changes in the state of matter, ranging from knock-on and atomic movement, to amorphization/crystallization, and to localized chemical/electrochemical reactions. To date, fundamental studies of e-beam induced phenomena and practical ap...

We experimentally investigate the structural, magnetic and electrical transport properties of La$_{0.67}$Sr$_{0.33}$MnO$_{3}$ based magnetic tunnel junctions with a SrSnO$_3$ barrier. Our results show that despite the large number of defects in the strontium stannate barrier, due to the large lattice mismatch, the observed tunnel magnetoresistance...

We experimentally investigate the structural, magnetic and electrical transport properties of La$_{0.67}$Sr$_{0.33}$MnO$_{3}$ based magnetic tunnel junctions with a SrSnO$_3$ barrier. Our results show that despite the large number of defects in the strontium stannate barrier, due to the large lattice mismatch, the observed tunnel magnetoresistance...

The surfaces of transition-metal oxides with the perovskite structure are fertile grounds for the discovery of novel electronic and magnetic phenomena. In this article, we combine scanning transmission electron microscopy (STEM) with density functional theory (DFT) calculations to obtain the electronic and magnetic properties of the (001) surface o...

div class="title"> Tracking BO 6 Coupling in Perovskite Superlattices to Engineer Magnetic Interface Behavior - Volume 22 Issue S3 - Qian He, Saurabh Ghosh, Eun Ju Moon, Steven J. May, Andrew R. Lupini, Sokrates T. Pantelides, Albina Y. Borisevich

div class="title">Using Multivariate Analysis of Scanning-Rochigram Data to Reveal Material Functionality - Volume 22 Issue S3 - Stephen Jesse, Miaofang Chi, Albina Y. Borisevich, Alex Belianinov, Sergei V. Kalinin, Eirik Endeve, Richard K. Archibald, Christopher T. Symons, Andrew R. Lupini

div class="title">Fast Aberration Measurement in Multi-Dimensional STEM - Volume 22 Issue S3 - Andrew R. Lupini, Miaofang Chi, Sergei V. Kalinin, Albina Y. Borisevich, Juan Carlos Idrobo, Stephen Jesse

div class="title"> Growth and In Situ Characterization of Oxide Epitaxial Heterostructures with Atomic Plane Precision - Volume 22 Issue S3 - Q. He, S. Jesse, A.R. Lupini, M. Fuentes-Cabrera, B.G. Sumpter, A. Akbashev, M. Falmbigl, J. Spanier, S. V. Kalinin, A.Y. Borisevich

div class="title">Big, deep, and smart data from atomically resolved images: exploring the origins of materials functionality - Volume 22 Issue S3 - S.V. Kalinin, R. Vasudevan, A. Borisevich, A. Belianinov, R.K. Archibald, C. Symons, E. Lingerfelt, B. Sumpter, L. Vlcek, S. Jesse

div class="title">Distortion Correction in Scanning Transmission Electron Microcopy with Controllable Scanning Pathways - Volume 22 Issue S3 - Xiahan Sang, Andrew R. Lupini, Raymond R. Unocic, Tricia L. Meyer, Thomas Z. Ward, Ho Nyung Lee, Eirik Endeve, Richard K. Archibald, Albina Y. Borisevich, Sergei V. Kalinin, Stephen Jesse

div class="title">Local Crystallography for Quantitative Analysis of Atomically Resolved Images - Volume 22 Issue S3 - Alex Belianinov, Qian He, Mikhail Kravchenko, Stephen Jesse, Albina Borisevich, Sergei V. Kalinin

Scanning transmission electron microscopy (STEM) has emerged as one of the foremost techniques to analyze materials at atomic resolution. However, two practical difficulties inherent to STEM imaging are: radiation damage imparted by the electron beam, which can potentially damage or otherwise modify the specimen and slow-scan image acquisition, whi...

Electron microscopy is undergoing a transition; from the model of producing only a few micrographs, through the current state where many images and spectra can be digitally recorded, to a new mode where very large volumes of data (movies, ptychographic and multi-dimensional series) can be rapidly obtained. Here, we discuss the application of so-cal...

Enabling memristive, neuromorphic, and quantum based computing as well as efficient mainstream energy storage and conversion technologies requires next generation of materials customized at the atomic scale. This requires full control of atomic arrangement and bonding in three dimensions. The last two decades witnessed substantial industrial, acade...