TY - JOUR
T1 - Searching for New Ferroelectric Materials Using High-Throughput Databases
T2 - An Experimental Perspective on BiAlO3and BiInO3
AU - Acharya, Megha
AU - Mack, Stephanie
AU - Fernandez, Abel
AU - Kim, Jieun
AU - Wang, Huaiyu
AU - Eriguchi, Kazutaka
AU - Meyers, Derek
AU - Gopalan, Venkatraman
AU - Neaton, Jeffrey
AU - Martin, Lane W.
N1 - Funding Information:
This work was funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract DE-AC02-05-CH11231 (Materials Project program KC23MP) for the discovery of novel functional materials, the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award DE-SC-0012375 for the study of ferroic materials, and the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract DE-AC02-05CH11231 within the Electronic Materials Program (KC1201) for the study of electronic/optical properties of materials. A.F. acknowledges support from the National Science Foundation under Grant OISE-1545907. J.K. acknowledges partial support from the Kwanjeong Educational Foundation and the National Science Foundation under Grant DMR-1708615. Computational resources used at the Molecular Foundry were supported by the Office of Science, Office of Basic Energy Sciences, of the US DOE under Contract DE-AC02-05CH11231. Additional computational resources were provided by NERSC. The authors acknowledge the technical support and scientific insights of Prof. Oscar Dubon.
Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/9/8
Y1 - 2020/9/8
N2 - Recent advances in high-throughput computational workflows are expanding the realm of materials for a range of applications. Here, we report the experimental evaluation of two such predicted candidate ferroelectric perovskite oxides: BiAlO3 and BiInO3. Attempts were made to synthesize polar BiAlO3 and BiInO3 using pulsed-laser deposition. Despite exploring a wide range of temperatures, pressures, substrates, laser fluences, and so on, attempts to grow BiAlO3 with this approach resulted in no perovskite phase and decomposition to Bi2O3 and Bi24Al2O40. Various orientations of BiInO3 films were synthesized on multiple substrates, with the best crystallinity demonstrated for (200)-oriented films on MgO (001). Density-functional theory predicts two energetically competitive ground-state structures for BiInO3: Pnma (nonpolar) and Pna21 (polar). BiInO3 films were studied by using X-ray diffraction and second-harmonic generation (SHG) and found to exhibit the nonpolar Pnma structure. Temperature-dependent SHG and dielectric measurements revealed no transition to the polar structure. Optical transmission-absorption studies suggest a direct bandgap of ∼4.5 eV for BiInO3. Our study underscores the need for additional descriptors for synthesizability in assessing the potential of ferroelectric candidate materials identified from high-throughput materials databases.
AB - Recent advances in high-throughput computational workflows are expanding the realm of materials for a range of applications. Here, we report the experimental evaluation of two such predicted candidate ferroelectric perovskite oxides: BiAlO3 and BiInO3. Attempts were made to synthesize polar BiAlO3 and BiInO3 using pulsed-laser deposition. Despite exploring a wide range of temperatures, pressures, substrates, laser fluences, and so on, attempts to grow BiAlO3 with this approach resulted in no perovskite phase and decomposition to Bi2O3 and Bi24Al2O40. Various orientations of BiInO3 films were synthesized on multiple substrates, with the best crystallinity demonstrated for (200)-oriented films on MgO (001). Density-functional theory predicts two energetically competitive ground-state structures for BiInO3: Pnma (nonpolar) and Pna21 (polar). BiInO3 films were studied by using X-ray diffraction and second-harmonic generation (SHG) and found to exhibit the nonpolar Pnma structure. Temperature-dependent SHG and dielectric measurements revealed no transition to the polar structure. Optical transmission-absorption studies suggest a direct bandgap of ∼4.5 eV for BiInO3. Our study underscores the need for additional descriptors for synthesizability in assessing the potential of ferroelectric candidate materials identified from high-throughput materials databases.
UR - http://www.scopus.com/inward/record.url?scp=85092025695&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85092025695&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.0c01770
DO - 10.1021/acs.chemmater.0c01770
M3 - Article
AN - SCOPUS:85092025695
SN - 0897-4756
VL - 32
SP - 7274
EP - 7283
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 17
ER -