eprintid: 10192846 rev_number: 9 eprint_status: archive userid: 699 dir: disk0/10/19/28/46 datestamp: 2024-05-30 11:55:56 lastmod: 2024-12-09 15:48:37 status_changed: 2024-05-30 11:55:56 type: article metadata_visibility: show sword_depositor: 699 creators_name: Luo, Bingcheng creators_name: Zhang, Zhesi creators_name: Li, Mengyang creators_name: Li, Huanxin creators_name: Zhang, Zili creators_name: Song, Hongzhou title: Atomic-scale insights into electronic, structural, dielectric, and ferroelectric properties of Ba(Zr, Ti)O₃ perovskites ispublished: pub divisions: UCL divisions: B04 divisions: C05 divisions: F43 keywords: Ferroelectric polarization, Ferroelectric instability, Lattice dynamics, Phonon dispersion, Barium zirconate titanate note: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. abstract: Ba(Zr, Ti)O3 perovskites are promising lead-free piezoelectric and relaxor ferroelectric materials for energy storage and harvest devices, of which the ferroelectric mechanism has long been ambiguous. We theoretically investigated the ferroelectric mechanism from the electronic and atomic scale using first-principles calculation based on density functional theory and density functional perturbation theory. With increasing zirconium content, it is obtained a lattice expansion and a decrease in the ferroelectric polarization in agreement with experiment. An unstable zone-center phonon mode is observed in the polar ferroelectric phase, which tends to stabilizein the nonpolar paraelectric phase, which is associated with the engineering of the relative displacement of the B-site ions that alters the short-range force. The newly formed Ti/Zr (dzx,dyz)-O (2px,2py) π-type bonds are discovered to be the origin of the Ba(Zr, Ti)O3ferroelectric instability and polarization. Local relaxation strains caused by lattice misalignment of the ionic displacements of Ti ions and Zr ions suppress the polarization of Ba(Zr, Ti)O3 by counteracting the off-centering of Ti ions and adjacent Zr ions in certain directions. date: 2024-02 date_type: published publisher: Elsevier official_url: https://doi.org/10.1016/j.mseb.2023.117053 oa_status: green full_text_type: other language: eng primo: open primo_central: open_green verified: verified_manual elements_id: 2266625 doi: 10.1016/j.mseb.2023.117053 lyricists_name: Li, Huanxin lyricists_id: HLIPX63 actors_name: Li, Huanxin actors_id: HLIPX63 actors_role: owner funding_acknowledgements: 52202154 [National Natural Science Foundation of China]; [High-performance Computing Platform of China Agricultural University] full_text_status: public publication: Materials Science and Engineering B: Advanced Functional Solid-state Materials volume: 300 article_number: 117053 pages: 8 issn: 0921-5107 citation: Luo, Bingcheng; Zhang, Zhesi; Li, Mengyang; Li, Huanxin; Zhang, Zili; Song, Hongzhou; (2024) Atomic-scale insights into electronic, structural, dielectric, and ferroelectric properties of Ba(Zr, Ti)O₃ perovskites. Materials Science and Engineering B: Advanced Functional Solid-state Materials , 300 , Article 117053. 10.1016/j.mseb.2023.117053 <https://doi.org/10.1016/j.mseb.2023.117053>. Green open access document_url: https://discovery.ucl.ac.uk/id/eprint/10192846/1/Atomic%20Scale%20Insights.pdf