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1. Low thermal conductivity in a modular inorganic material with bonding anisotropy and mismatch

Author

Marco Zanella, Jonathan Alaria, Luke M. Daniels, Matthew J. Rosseinsky, Furio Corà, Matthew S. Dyer, Ramzy Daou, Quinn Gibson, Helen Walker, Ben Slater, John B. Claridge, Michael W. Gaultois, Sylvie Hébert, Tianqi Zhao, Univ Liverpool, Dept Chem, Crown St, Liverpool L69 7ZD, Merseyside, England, UCL, Dept Chem, 20 Gordon St,Kings Cross, London WC1H 0AJ, England, ISIS Rutherford Appleton Lab, Didcot OX110QX, Oxon, England, Laboratoire de cristallographie et sciences des matériaux (CRISMAT), École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC), Univ Liverpool, Mat Innovat Factory, Leverhulme Res Ctr Funct Mat Design, 51 Oxford St, Liverpool L7 3NY, Merseyside, England, Univ Liverpool, Oliver Lodge Lab, Dept Phys, Liverpool L69 ZE, Merseyside, England, University of Liverpool, Department of Chemistry [University College of London], University College of London [London] (UCL), Science and Technology Facilities Council (STFC), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Multidisciplinary, Materials science, Condensed matter physics, Phonon, Superlattice, Stacking, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Transverse plane, Thermal conductivity, Molecular vibration, Dispersion (optics), [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], 0210 nano-technology, Anisotropy, ComputingMilieux_MISCELLANEOUS
Abstract

International audience; The thermal conductivity of crystalline materials cannot be arbitrarily low, as the intrinsic limit depends on the phonon dispersion. We used complementary strategies to suppress the contribution of the longitudinal and transverse phonons to heat transport in layered materials that contain different types of intrinsic chemical interfaces. BiOCl and Bi2O2Se encapsulate these design principles for longitudinal and transverse modes, respectively, and the bulk superlattice material Bi4O4SeCl2 combines these effects by ordering both interface types within its unit cell to reach an extremely low thermal conductivity of 0.1 watts per kelvin per meter at room temperature along its stacking direction. This value comes within a factor of four of the thermal conductivity of air. We demonstrated that chemical control of the spatial arrangement of distinct interfaces can synergically modify vibrational modes to minimize thermal conductivity.

Published
2021
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2. Discovery of a Low Thermal Conductivity Oxide Guided by Probe Structure Prediction and Machine Learning

Author

Christopher Collins, Michael Moran, Matthew S. Dyer, George R. Darling, Olivier Perez, Charlene Delacotte, Gyorgyi Glodan, Quinn Gibson, Richard Feetham, Michael J. Pitcher, Denis Pelloquin, Marco Zanella, Jonathan Alaria, Luke M. Daniels, Matthew J. Rosseinsky, John B. Claridge, Michael W. Gaultois, Troy D. Manning, Claire A. Murray, University of Liverpool, DIAMOND Light source, University of Manchester [Manchester], Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Department of Chemistry University of Liverpool, Univ Liverpool, Dept Chem, Crown St, Liverpool L69 7ZD, Merseyside, England, Conditions Extrêmes et Matériaux : Haute Température et Irradiation (CEMHTI), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université d'Orléans (UO), École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC), and University of Liverpool - Department of Chemistry

Subjects
Materials science, Oxide, Structure (category theory), 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, Machine learning, computer.software_genre, 010402 general chemistry, Heat capacity, 01 natural sciences, Catalysis, symbols.namesake, chemistry.chemical_compound, Thermal conductivity, README, [CHIM.CRIS]Chemical Sciences/Cristallography, [CHIM]Chemical Sciences, Aperiodic structure, ComputingMilieux_MISCELLANEOUS, Research Articles, titanium oxides, Titanium, 010405 organic chemistry, business.industry, Experimental data, Oxides, General Chemistry, General Medicine, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, Aperiodic graph, symbols, Transition‐Metal Oxides | Very Important Paper, Artificial intelligence, Metastable compounds, Raman spectroscopy, business, 0210 nano-technology, computer, Research Article
Abstract

We report the aperiodic titanate Ba10Y6Ti4O27 with a room‐temperature thermal conductivity that equals the lowest reported for an oxide. The structure is characterised by discontinuous occupancy modulation of each of the sites and can be considered as a quasicrystal. The resulting localisation of lattice vibrations suppresses phonon transport of heat. This new lead material for low‐thermal‐conductivity oxides is metastable and located within a quaternary phase field that has been previously explored. Its isolation thus requires a precisely defined synthetic protocol. The necessary narrowing of the search space for experimental investigation was achieved by evaluation of titanate crystal chemistry, prediction of unexplored structural motifs that would favour synthetically accessible new compositions, and assessment of their properties with machine‐learning models., Ba10Y6Ti4O27 has a complex aperiodic structure with the lowest thermal conductivity of any first‐transition‐series oxide. It is metastable, which makes it challenging to identify. Experimental exploration was focused sufficiently by structure prediction and property‐targeted machine learning to enable the isolation of this material (see picture), whose structural motifs provide new insight into the control of heat transport.

Published
2021
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3. One site, two cations, three environments: s2 and s0 electronic configurations generate Pb-free relaxor behaviour in a perovskite oxide

Author

Marco Zanella, William J. Thomas, Jonathan Alaria, Luke M. Daniels, Jacinthe Gamon, Thomas A. Whittle, Philippa M. Shepley, Matthew J. Rosseinsky, Anton Goetzee-Barral, Quinn Gibson, T. Wesley Surta, Matthew A. Wright, Yang Li, John B. Claridge, Andrew J. Bell, Hongjun Niu, Department of Chemistry University of Liverpool, University of Liverpool, School of Physics and Astronomy [Leeds], University of Leeds, School of Chemical and Process Engineering, Department of Physics - University of Liverpool, and We thank the EPSRC (EP/R011753 and EP/R010293) for funding this research. J.G. and Q.D.G. acknowledge support through EP/N004884. We thank the STFC for access to Polaris (Xpress proposal 1890309) and Dr. Ron Smith for collecting the data and performing absorption corrections. We thank Argonne National Laboratory for access to the 11BM beamline (Rapid Access proposal 65125) and to Dr. Saul Lapidus and Dr. Lynn Ribaud for collecting the data

Subjects
010302 applied physics, Phase boundary, Oxide, 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Biochemistry, Piezoelectricity, Ferroelectricity, Catalysis, Article, chemistry.chemical_compound, Colloid and Surface Chemistry, chemistry, Chemical physics, Local symmetry, 0103 physical sciences, Electron configuration, 0210 nano-technology, Solid solution, Perovskite (structure)
Abstract

The piezoelectric devices widespread in society use noncentrosymmetric Pb-based oxides because of their outstanding functional properties. The highest figures of merit reported are for perovskites based on the parent Pb(Mg1/3Nb2/3)O3 (PMN), which is a relaxor: a centrosymmetric material with local symmetry breaking that enables functional properties, which resemble those of a noncentrosymmetric material. We present the Pb-free relaxor (K1/2Bi1/2)(Mg1/3Nb2/3)O3 (KBMN), where the thermal and (di)electric behavior emerges from the discrete structural roles of the s0 K+ and s2 Bi3+ cations occupying the same A site in the perovskite structure, as revealed by diffraction methods. This opens a distinctive route to Pb-free piezoelectrics based on relaxor parents, which we demonstrate in a solid solution of KBMN with the Pb-free ferroelectric (K1/2Bi1/2)TiO3, where the structure and function evolve together, revealing a morphotropic phase boundary, as seen in PMN-derived systems. The detailed multiple-length-scale understanding of the functional behavior of KBMN suggests that precise chemical manipulation of the more diverse local displacements in the Pb-free relaxor will enhance performance.

Published
2021
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4. Na2Fe2OS2, a new earth abundant oxysulphide cathode material for Na-ion batteries

Author

Laurence J. Hardwick, Tim D. Veal, Arnaud J. Perez, Leanne A. H. Jones, Rhun E. Morris, Chiu C. Tang, Matthew J. Rosseinsky, John B. Claridge, Marco Zanella, Luke M. Daniels, Jacinthe Gamon, Matthew S. Dyer, Department of Chemistry, University of Liverpool, Stephenson Institute for Renewable Energy, Oliver Lodge Laboratory, Diamond Light Source Ltd, and We thank EPSRC for funding under EP/N004884. We thank Diamond Light Source for access to beamlines I11 and I18, Dr Sarah Day, Prof. Alan Chadwick and Dr Giannantonio Cibin for assistance on the beamlines. We thank STFC for access to Polaris (Xpress proposal 1990220) and Dr Ron Smith for running the measurements. XPS data collection was performed at the EPSRC National Facility for XPS (‘HarwellXPS’), operated by Cardiff University and UCL, under contract No. PR16195. Dr Mark Isaacs is greatly acknowledged for his support during the measurement. MJR thanks the Royal Society for the award of a Research Professor position. We acknowledge Dr Konstantin Luzyanin, Mr Stephen Moss and Mrs Jean Ellis (University of Liverpool) for ICP-OES and CHNS measurements, and Dr Quinn Gibson and Dr Wesley Surta for helpful discussions.

Subjects
Materials science, Extended X-ray absorption fine structure, Renewable Energy, Sustainability and the Environment, Rietveld refinement, 02 engineering and technology, General Chemistry, Crystal structure, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 7. Clean energy, 01 natural sciences, Energy storage, 0104 chemical sciences, Amorphous solid, Ion, Chemical engineering, Phase (matter), General Materials Science, 0210 nano-technology
Abstract

International audience; Multiple anion materials are of particular interest for the discovery of new crystal structures and offer an original way to modulate physical properties, including energy storage materials with enhanced performances. Through careful synthesis optimization, a new Na2Fe2OS2 phase was prepared by two different routes: high temperature solid-state synthesis and simple mechanochemical synthesis. The long-range and local structure of Na2Fe2OS2 was studied by Rietveld refinement of neutron and X-ray diffraction data combined with EXAFS data refinement. The phase comprises an amorphous and a crystalline part which has an anti-K2NiF4 structure, corresponding to the n = 1 member of the homologous anti-Ruddlesden–Popper [AX][ABX3]n series. Its electrochemical properties as a cathode material were studied in Na half cells and Na-ion full cells, revealing that the material becomes fully amorphous upon initial desodiation to Na0.5Fe2OS2, but maintains a reversible capacity of 135 mA h g−1 in full cells where up to 1.2 Na+ can be reversibly extracted and reinserted when compensating for the Na lost in SEI formation. The stability of the pristine material and its structural evolution upon charging are discussed, paving the way for further optimization of this material. Being composed exclusively of earth-abundant elements and stable under dry air, Na2Fe2OS2 perfectly illustrates the great opportunity of multiple anion chemistry to explore new structure types and develop better energy storage systems.

Published
2020
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5. Computationally guided discovery of the sulfide Li3AlS3 in the Li–Al–S phase field: structure and lithium conductivity

Author

Matthew S. Dyer, John B. Claridge, Michael W. Gaultois, T. Wesley Surta, Frédéric Blanc, Matthew J. Rosseinsky, Paul M. Sharp, Christopher Collins, Luke M. Daniels, Jacinthe Gamon, Benjamin B. Duff, Department of Chemistry University of Liverpool, University of Liverpool, and Stephenson Institute for Renewable Energy

Subjects
chemistry.chemical_classification, Materials science, Field (physics), Sulfide, General Chemical Engineering, chemistry.chemical_element, 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, Conductivity, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Article, 0104 chemical sciences, chemistry, Phase (matter), Materials Chemistry, Fast ion conductor, Physical chemistry, Lithium, 0210 nano-technology
Abstract

International audience; With the goal of finding new lithium solid electrolytes by a combined computational–experimental method, the exploration of the Li–Al–O–S phase field resulted in the discovery of a new sulfide Li3AlS3. The structure of the new phase was determined through an approach combining synchrotron X-ray and neutron diffraction with 6Li and 27Al magic-angle spinning nuclear magnetic resonance spectroscopy and revealed to be a highly ordered cationic polyhedral network within a sulfide anion hcp-type sublattice. The originality of the structure relies on the presence of Al2S6 repeating dimer units consisting of two edge-shared Al tetrahedra. We find that, in this structure type consisting of alternating tetrahedral layers with Li-only polyhedra layers, the formation of these dimers is constrained by the Al/S ratio of 1/3. Moreover, by comparing this structure to similar phases such as Li5AlS4 and Li4.4Al0.2Ge0.3S4 ((Al + Ge)/S = 1/4), we discovered that the AlS4 dimers not only influence atomic displacements and Li polyhedral distortions but also determine the overall Li polyhedral arrangement within the hcp lattice, leading to the presence of highly ordered vacancies in both the tetrahedral and Li-only layer. AC impedance measurements revealed a low lithium mobility, which is strongly impacted by the presence of ordered vacancies. Finally, a composition–structure–property relationship understanding was developed to explain the extent of lithium mobility in this structure type.

Published
2019
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6. Iron and Porphyrin Metal–Organic Frameworks: Insight into Structural Diversity, Stability, and Porosity

Author

Christelle Goutaudier, Dominique Luneau, John E. Warren, Thomas Devic, Brian Abeykoon, Matthew J. Rosseinsky, Jade Clarisse, Guillaume Pilet, Farid Nouar, Jean-Marc Greneche, Alexandra Fateeva, Frédéric Guégan, Reconnaissance Ionique et Chimie de Coordination (RICC), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Multimatériaux et Interfaces (LMI), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], 010405 organic chemistry, Inorganic chemistry, Free base, General Chemistry, 010402 general chemistry, Condensed Matter Physics, Crystal engineering, 01 natural sciences, Porphyrin, Chloride, 0104 chemical sciences, chemistry.chemical_compound, Crystallography, Paddle wheel, chemistry, Octahedron, Oxidation state, medicine, General Materials Science, Metal-organic framework, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS, medicine.drug
Abstract

Reaction of iron(IIII)chloride with the free base tetrakis(4-carboxyphenyl)porphyrin (H2TCPP) in the presence of different bases leads to the formation of a series of iron/porphyrin metal–organic frameworks. Such a crystal engineering approach led to the obtaining of four structures presenting three different topologies and inorganic secondary building units. Depending on the synthesis conditions, isolated FeIII octahedra, diiron(II) paddle wheel dimers, or extended [FeIII(OH)O4]n chains could be obtained in a controlled manner. The influence of the synthetic conditions on the final structure and the oxidation state of iron is discussed. Stability of the porous solids towards air and water is studied, and their intrinsic porosity is assessed.

Published
2015
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7. SrHf0.67Ti0.33O3 high-k films deposited on Si by pulsed laser deposition

Author

Simon Romani, John Bacsa, Zhongling Xu, Paul R. Chalker, S. R. C. McMitchell, Lei Yan, C. Grygiel, Joanna H. Clark, Matthew J. Rosseinsky, Hongjun Niu, Robert G. Palgrave, Matthew R. Suchomel, University of Liverpool, Advanced Photon Source [ANL] (APS), and Argonne National Laboratory [Lemont] (ANL)-University of Chicago-US Department of Energy

Subjects
Permittivity, Band gap, 02 engineering and technology, Dielectric, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 01 natural sciences, Pulsed laser deposition, [SPI.MAT]Engineering Sciences [physics]/Materials, Optics, X-ray photoelectron spectroscopy, 0103 physical sciences, [PHYS.HEXP]Physics [physics]/High Energy Physics - Experiment [hep-ex], [CHIM.CRIS]Chemical Sciences/Cristallography, General Materials Science, Thin film, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS, High-κ dielectric, 010302 applied physics, business.industry, Chemistry, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Optoelectronics, [PHYS.COND.CM-SCE]Physics [physics]/Condensed Matter [cond-mat]/Strongly Correlated Electrons [cond-mat.str-el], 0210 nano-technology, business, Current density
Abstract

The large band gap (3.58 eV) and dielectric properties (e r =50) of bulk SrHf0.67Ti0.33O3 (SHTO) make it a promising high-k material. SHTO films were deposited on p-type (100) Si single crystal substrates by pulsed laser deposition. The composition, structure, thickness, and roughness of the SHTO films have been studied using X-ray Photoelectron Spectroscopy, X-ray reflectivity, transmission electron microscopy, and atomic force microscopy. The capacitance–voltage and leakage current density characteristics of the films have been evaluated. For a post-annealed SHTO film with a thickness of 25 nm, the relatively high permittivity of 35 was achieved with the low leakage current density of 4.96×10−4 A/cm2 at −2 V bias voltage.

Published
2011
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8. A-Site Order Control in Mixed Conductor NdBaCo 2 O 5+δ Films through Manipulation of Growth Kinetics

Author

Hongjun Niu, Lei Yan, Paul R. Chalker, D. Giap, Zhongling Xu, S. R. C. McMitchell, Matthew J. Rosseinsky, John Bacsa, C. Grygiel, and University of Liverpool

Subjects
Reflection high-energy electron diffraction, Materials science, Growth kinetics, General Chemical Engineering, Kinetics, Analytical chemistry, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 01 natural sciences, Pulsed laser deposition, [SPI.MAT]Engineering Sciences [physics]/Materials, Order control, 0103 physical sciences, Materials Chemistry, [PHYS.HEXP]Physics [physics]/High Energy Physics - Experiment [hep-ex], [CHIM.CRIS]Chemical Sciences/Cristallography, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS, 010302 applied physics, Supersaturation, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, A-site, Crystallography, Mixed conductor, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [PHYS.COND.CM-SCE]Physics [physics]/Condensed Matter [cond-mat]/Strongly Correlated Electrons [cond-mat.str-el], 0210 nano-technology
Abstract

NdBaCo2O5+δ films have been grown on (001)-SrTiO3 substrates using pulsed laser deposition with RHEED to access both A-site ordered and A-site disordered films grown in a layer-by-layer manner. Ionic diffusion kinetics are shown to be key parameter for A-site order, attained by control of growth kinetics, mobility, and supersaturation.

Published
2010
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9. High permittivity SrHf0.5Ti0.5O3 films grown by pulsed laser deposition

Author

Joanna H. Clark, Lei Yan, Matthew R. Suchomel, Clara Grygiel, Matthew Werner, S. R. C. McMitchell, Paul R. Chalker, Matthew J. Rosseinsky, Hongjun Niu, John Bacsa, University of Liverpool, Advanced Photon Source [ANL] (APS), and Argonne National Laboratory [Lemont] (ANL)-University of Chicago-US Department of Energy

Subjects
Permittivity, Materials science, Physics and Astronomy (miscellaneous), Silicon, Band gap, chemistry.chemical_element, 02 engineering and technology, Substrate (electronics), Dielectric, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 01 natural sciences, 7. Clean energy, Pulsed laser deposition, [SPI.MAT]Engineering Sciences [physics]/Materials, Electric field, 0103 physical sciences, [PHYS.HEXP]Physics [physics]/High Energy Physics - Experiment [hep-ex], [CHIM.CRIS]Chemical Sciences/Cristallography, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], ComputingMilieux_MISCELLANEOUS, 010302 applied physics, business.industry, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Optoelectronics, [PHYS.COND.CM-SCE]Physics [physics]/Condensed Matter [cond-mat]/Strongly Correlated Electrons [cond-mat.str-el], 0210 nano-technology, business, Current density
Abstract

High permittivity SrHf0.5Ti0.5O3 films (k=62.8) have been deposited on (001) Nb–SrTiO3 single crystal conducting substrates by pulsed laser deposition. The SrHf0.5Ti0.5O3 films grow epitaxially with atomically smooth surfaces (root mean square roughness 4.8 A) and a c-axis orientation parallel to the substrate. The measured band gap of SrHf0.5Ti0.5O3 is 3.47 eV compared with 3.15 eV in SrTiO3. Under an applied electric field of 600 kV/cm, the leakage current density of the SrHf0.5Ti0.5O3 films is 4.63×10−4 A/cm2. These attractive dielectric properties and enhanced band gap values make SrHf0.5Ti0.5O3 a promising candidate for high-k dielectric applications in silicon-based integrated circuits.

Published
2009
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