Swarm-intelligent predictions of high-TC polymorphs in monolayer CrI3 above 77 K

doi:10.1088/1674-1056/addbcb

Abstract Monolayer CrI$_{3}$, crystalizing in the $P\bar{3}$1$m$ space group, is a prototypical two-dimensional (2D) material for observing intrinsic ferromagnetic order. However, its relatively low Curie temperature ($T_{\rm C}$) of 45 K severely limits its practical applications, highlighting the need to explore novel metastable polymorphs with enhanced magnetic properties. In this study, we employ a global crystal structure search technique combined with first-principles calculations to systematically investigate new monolayer CrI$_{3}$ phases. Our structural predictions identify two novel polymorphs with C_m and $P2/m$ space groups, both of which are dynamically stable and exhibit significantly higher $T_{\rm C}$ values of 145 K and 81 K, respectively. Electronic property calculations show that the C_m phase is a half-metal, while the $P2/m$ phase is semiconducting with a bandgap of 0.14 eV. Monte Carlo simulations attribute these enhanced $T_{\rm C}$ values to a notable increase in exchange interactions. These findings expand the known phase space of CrI$_{3}$ and provide a promising pathway for designing high-temperature 2D ferromagnets for next-generation spintronic applications.

Keywords: chromium triiodide 2D magnets structure prediction first-principles calculations monolayer structure

Received: 25 March 2025
Revised: 13 May 2025
Accepted manuscript online: 22 May 2025

PACS:	71.15.Mb	(Density functional theory, local density approximation, gradient and other corrections)
	71.20.-b	(Electron density of states and band structure of crystalline solids)
	63.20.dk	(First-principles theory)
	75.50.Pp	(Magnetic semiconductors)

Fund: Project supported by the National Key Research and Development Program of China (Grant No. 2023YFA1610000), the National Natural Science Foundation of China (Grant Nos. 12304036 and 12304265), the Basic and Applied Basic Research Foundation of Guangdong Province, China (Grant No. 2023A1515010071), and the Fundamental Research Funds for the Central Universities to Sun Yat-sen University (Grant No. 23xkjc016).

Corresponding Authors: Yanan Wang, Yunwei Zhang
E-mail: wangyanan@sslab.org.cn;zhangyunw@mail.sysu.edu.cn

Cite this article:

Ying Luo(罗颖), Shuangyi Xu(许双旖), Yanan Wang(王亚南), and Yunwei Zhang(张云蔚) Swarm-intelligent predictions of high-T_C polymorphs in monolayer CrI₃ above 77 K 2025 Chin. Phys. B 34 117105

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Swarm-intelligent predictions of high-TC polymorphs in monolayer CrI3 above 77 K

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Swarm-intelligent predictions of high-T_C polymorphs in monolayer CrI₃ above 77 K