Research Article First-Principles Calculations to Investigate Structural, Electronic, Optical, and Elastic Properties of Ceria Lemessa Asefa Eressa 1 and Teshome Gerbaba Edossa 2 1 Department of Physics, College of Natural & Computational Sciences, Ambo University, Ambo, Ethiopia 2 Departments of Physics, College of Natural & Computational Sciences, Wachemo University, Hossana, Ethiopia Correspondence should be addressed to Lemessa Asefa Eressa; lemessaphys@gmail.com Received 16 January 2022; Accepted 25 April 2022; Published 3 June 2022 Academic Editor: Raouf El Mallawany Copyright © 2022 Lemessa Asefa Eressa and Teshome Gerbaba Edossa. is is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. e structural, electronic, optical, and elastic properties of Ceria (CeO 2 ) were investigated using local density approximation (LDA), PBE, DFT + U, and PBE0 approximations. In all approximations, the convergence test of total energy with respect to kinetic energy cutoff, k-point, and lattice constant of CeO 2 was performed consequently to increase the accuracy of computations. e O (2p)-Ce (4f) bandgap of CeO 2 calculated using DFT + U (3.0 eV) is consistent with experimentally reported value (3.0–3.33 eV) than with LDA (2.2 eV), PBE (2.5 eV), and PBE0 (4.47 eV). Both LDA and PBE underestimated the bandgap of CeO 2 while the PBE0 overestimated the bandgap of CeO 2 as compared to the experimental value. e optical properties such as the imaginary part of the dielectric function (ε 2 ), extinction coefficient (k), and refractive index (n) of ceria obtained using the three approaches are also consistent with the available theoretical and experimental data. In addition, the maximum peak for absorption coefficient was found at about 13 eV for (LDA and PBE) and around 11 eV for DFT + U calculations. Furthermore, the analyses of optical properties support the electronic properties of ceria. e elastic properties such as bulk modulus, shear modulus, Young’s modulus, Poisson’s ratio, Debye temperature, and Debye sound velocity were computed to investigate the mechanical properties of CeO 2 and compared with the experimental and theoretical results. e result of elastic parameters found confirms that CeO 2 is mechanically stable and has potential for a variety of different electronic applications. 1. Introduction Ceria (CeO 2 ) is a technologically significant oxide material that has a wide range of applications. It is widely used in automotive three-way catalysts (TWCs) to remove NOx and CO [1], in luminescence devices, gas sensors, and high- temperature superconducting tapes [2], as a catalyst in fuel cells [3–5]. Ceria is a highly correlated material, due to the fact of their confined d- and f-orbitals, where Coulomb repulsion energy acts on them on the order of the electronic bandwidth [1, 6]. Only a few researches have been carried out with density functional theories to define the needed properties of CeO 2 . erefore, it is important to investigate the properties of ceria for the advancement of their practical applications with different density functional theories. e local density approximation (LDA) or PBE under- estimates and fails to reproduce the correct electronic properties (bandgap) of CeO 2 due to the f-electron delo- calization associated with the self-interaction problem [7]. However, the electronic structure of CeO 2 is fundamental to understanding the effects of ions, doping, and other prop- erties that are prerequisites to using CeO 2 for different technological applications. Hence, in order to account for the strong on-site Coulomb repulsion among the Ce-4f electrons, a Hubbard parameter U is added (DFT + U approach) so as to get better electronic properties. e objective of this study was to investigate the structural, electronic, optical, and me- chanical properties of CeO 2 using density functional theories. e values obtained were compared with the available the- oretical and experimental data. Hindawi Advances in Condensed Matter Physics Volume 2022, Article ID 3619600, 11 pages https://doi.org/10.1155/2022/3619600