High Entropy Oxide Relaxor Ferroelectrics

Sharma, Yogesh; Lee, Min-Cheol; Pitike, Krishna Chaitanya; Mishra, Karuna K.; Zheng, Qiang; Gao, Xiang; Musico, Brianna L.; Mazza, Alessandro R.; Katiyar, Ram S.; Keppens, Veerle; Brahlek, Matthew; Yarotski, Dmitry Anatolievitch; Prasankumar, Rohit Prativadi; Chen, Aiping; Cooper, Valentino R.; Ward, T. Zac

doi:10.1021/acsami.2c00340

Title: High Entropy Oxide Relaxor Ferroelectrics

Journal Article · Mon Feb 28 00:00:00 EST 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.2c00340· OSTI ID:1862117

^[1]; Lee, Min-Cheol ^[2];

^[3]; Mishra, Karuna K. ^[4]; Zheng, Qiang ^[3];

^[3]; Musico, Brianna L. ^[5];

^[3]; Katiyar, Ram S. ^[4]; Keppens, Veerle ^[6];

^[3];

^[2];

^[3];

^[3]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Puerto Rico, San Juan (Puerto Rico). Inst. for Functional Nanomaterials
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)

Relaxor ferroelectrics are important in technological applications due to strong electromechanical response, energy storage capacity, electrocaloric effect, and pyroelectric energy conversion properties. Current efforts to discover and design materials in this class generally rely on substitutional doping as slight changes to local compositional order can significantly affect the Curie temperature, morphotropic phase boundary, and electromechanical responses. In this work, we demonstrate that moving to the strong limit of compositional complexity in an ABO₃ perovskite allows stabilization of relaxor responses that do not rely on a single narrow phase transition region. Entropy-assisted synthesis approaches are utilized to synthesize single-crystal Ba(Ti_0.2Sn_0.2Zr_0.2Hf_0.2Nb_0.2)O₃ [Ba(5B)O] films. The high levels of configurational disorder present in this system are found to influence dielectric relaxation, phase transitions, nanopolar domain formation, and Curie temperature. Temperature-dependent dielectric, Raman spectroscopy, and second-harmonic generation measurements reveal multiple phase transitions, a high Curie temperature of 570 K, and the relaxor ferroelectric nature of Ba(5B)O films. The first-principles theory calculations are used to predict possible combinations of cations to design relaxor ferroelectrics and quantify the relative feasibility of synthesizing these highly disordered single-phase perovskite systems. The ability to stabilize single-phase perovskites with various cations on the B-sites offers possibilities for designing high-performance relaxor ferroelectric materials for piezoelectric, pyroelectric, and electrocaloric applications.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOD

Grant/Contract Number:: AC05-00OR22725; 89233218CNA000001; FA9550-20-1-0064

OSTI ID:: 1862117

Alternate ID(s):: OSTI ID: 1878049; OSTI ID: 1900494

Report Number(s):: LA-UR-21-24954; LA-UR-21-30229

Journal Information:: ACS Applied Materials and Interfaces, Vol. 14, Issue 9; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
high entropy oxides
configurational disorder
relaxor ferroelectrics
dielectrics
thin film epitaxy
perovskite oxides
Material Science

Title: High Entropy Oxide Relaxor Ferroelectrics

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