TY - JOUR
T1 - Accurate first-principles evaluation of structural, electronic, optical and photocatalytic properties of BaHfO3 and SrHfO3 perovskites
AU - Ahmed, Shahbaz
AU - Zulfiqar, Waqas
AU - Javed, Farrukh
AU - Arshad, Hurriya
AU - Abbas, Ghulam
AU - Laref, Amel
AU - Alay-e-Abbas, Syed Muhammad
N1 - Funding Information:
The authors are grateful to the Higher Education Commission of Pakistan for financial support under the National Research Program for Universities Grant no. 7107/Punjab/NRPU/R&D/HEC/2017 . S. M. A. A. thank the Knut and Alice Wallenberg Foundation , and Kempestiftelserna for financial support. This research project was supported by a grant from the “Research Centre of Female Scientific and Medical Colleges”, Deanship of Scientific Research, King Saud University . The computations were enabled by resources provided by the Swedish National Infrastructure for Computing (SNIC) at HPC2N and NSC partially funded by the Swedish Research Council through Grant agreement no. 2018-05973 .
Publisher Copyright:
© 2021 The Authors
PY - 2022/2/5
Y1 - 2022/2/5
N2 - A reliable first-principles account of experimentally observed physical properties of perovskite oxides is crucial for realizing their employment in electronic and optical devices. In this context, SCAN meta-GGA functional of DFT offers good approximation for the exchange-correlation energy; facilitating accurate determination of structural and energetic properties. However, SCAN is unable to reproduce electronic and optical properties of wide bad gap materials. In the present study, we report systematic DFT calculations to show that structural, energetic, electronic and optical properties of hafnium based BaHfO
3 and SrHfO
3 perovskite oxides can be accurately determined through a combine application of SCAN and Tran-Blaha modified Becke-Johnson (TB-mBJ) meta-GGAs. The structural and energetic properties computed using SCAN functional for both BaHfO
3 and SrHfO
3 are found to be in good agreement with experimental data; achieving a level of accuracy comparable to computationally expansive hybrid DFT calculations. On the other hand, TB-mBJ calculated band gaps computed using the SCAN optimized lattice parameters provide better agreement with experimental data at a low computational cost. The optical properties, band edge potentials and effective masses of the charge carriers in BaHfO
3 and SrHfO
3 are also computed to examine the combined application of SCAN and TB-mBJ meta-GGAs in predicting the photocatalytic performance of these wide band gap materials. Our results clearly show that the combination of the two meta-GGAs provide a computationally economical route for evaluating the photocatalytic performance of alkaline-earth metal hafnates.
AB - A reliable first-principles account of experimentally observed physical properties of perovskite oxides is crucial for realizing their employment in electronic and optical devices. In this context, SCAN meta-GGA functional of DFT offers good approximation for the exchange-correlation energy; facilitating accurate determination of structural and energetic properties. However, SCAN is unable to reproduce electronic and optical properties of wide bad gap materials. In the present study, we report systematic DFT calculations to show that structural, energetic, electronic and optical properties of hafnium based BaHfO
3 and SrHfO
3 perovskite oxides can be accurately determined through a combine application of SCAN and Tran-Blaha modified Becke-Johnson (TB-mBJ) meta-GGAs. The structural and energetic properties computed using SCAN functional for both BaHfO
3 and SrHfO
3 are found to be in good agreement with experimental data; achieving a level of accuracy comparable to computationally expansive hybrid DFT calculations. On the other hand, TB-mBJ calculated band gaps computed using the SCAN optimized lattice parameters provide better agreement with experimental data at a low computational cost. The optical properties, band edge potentials and effective masses of the charge carriers in BaHfO
3 and SrHfO
3 are also computed to examine the combined application of SCAN and TB-mBJ meta-GGAs in predicting the photocatalytic performance of these wide band gap materials. Our results clearly show that the combination of the two meta-GGAs provide a computationally economical route for evaluating the photocatalytic performance of alkaline-earth metal hafnates.
KW - Density functional theory
KW - Electronic properties
KW - Optical properties
KW - Perovskite oxides
KW - Photocatalysis
UR - http://www.scopus.com/inward/record.url?scp=85115975628&partnerID=8YFLogxK
U2 - 10.1016/j.jallcom.2021.162071
DO - 10.1016/j.jallcom.2021.162071
M3 - Article
SN - 0925-8388
VL - 892
JO - Journal of alloys and Compounds
JF - Journal of alloys and Compounds
IS - 5
M1 - 162071
ER -