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Main Authors: Yang, Qing-Han, Li, Jia-Wen, Yi, Xin-Wei, Li, Xiang, You, Jing-Yang, Su, Gang, Gu, Bo
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2508.07278
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author Yang, Qing-Han
Li, Jia-Wen
Yi, Xin-Wei
Li, Xiang
You, Jing-Yang
Su, Gang
Gu, Bo
author_facet Yang, Qing-Han
Li, Jia-Wen
Yi, Xin-Wei
Li, Xiang
You, Jing-Yang
Su, Gang
Gu, Bo
contents The development of room-temperature magnetic semiconductors is critical for advancing spintronic technologies, yet van der Waals magnets like CrI3 exhibit intrinsically low Curie temperatures (Tc = 45 K). This study employs first-principles calculations to demonstrate that atom intercalation, particularly lithium (Li), dramatically enhances magnetic exchange couplings in CrI3, achieving near room-temperature ferromagnetism with a predicted Tc of 286 K-aligning with experimental reports of 420 K. The underlying mechanism involves synergistic superexchange and double-exchange interactions: intercalation reduces the |Ep-Ed| energy difference between iodine p-orbitals and chromium d-orbitals, strengthening superexchange pathways, while charge transfer induces valence mixing (e.g., Cr3+ to Cr2+, as confirmed by experimental X-ray photoelectron spectrometry data), promoting double-exchange. Theoretical predictions extend to other intercalants including Cu and Na, with Cu0.25CrI3 and Na0.25CrI3 exhibiting Tc of 267 K and 247 K, respectively, establishing a versatile strategy for designing high-Tc magnetic semiconductors. This work bridges theoretical insights with experimental validation, offering a transferable framework for intercalation-driven material design and accelerating practical spintronic device realization.
format Preprint
id arxiv_https___arxiv_org_abs_2508_07278
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Intercalation-Induced Near Room-Temperature Ferromagnetism in CrI3 via Synergistic Exchange Pathways
Yang, Qing-Han
Li, Jia-Wen
Yi, Xin-Wei
Li, Xiang
You, Jing-Yang
Su, Gang
Gu, Bo
Materials Science
The development of room-temperature magnetic semiconductors is critical for advancing spintronic technologies, yet van der Waals magnets like CrI3 exhibit intrinsically low Curie temperatures (Tc = 45 K). This study employs first-principles calculations to demonstrate that atom intercalation, particularly lithium (Li), dramatically enhances magnetic exchange couplings in CrI3, achieving near room-temperature ferromagnetism with a predicted Tc of 286 K-aligning with experimental reports of 420 K. The underlying mechanism involves synergistic superexchange and double-exchange interactions: intercalation reduces the |Ep-Ed| energy difference between iodine p-orbitals and chromium d-orbitals, strengthening superexchange pathways, while charge transfer induces valence mixing (e.g., Cr3+ to Cr2+, as confirmed by experimental X-ray photoelectron spectrometry data), promoting double-exchange. Theoretical predictions extend to other intercalants including Cu and Na, with Cu0.25CrI3 and Na0.25CrI3 exhibiting Tc of 267 K and 247 K, respectively, establishing a versatile strategy for designing high-Tc magnetic semiconductors. This work bridges theoretical insights with experimental validation, offering a transferable framework for intercalation-driven material design and accelerating practical spintronic device realization.
title Intercalation-Induced Near Room-Temperature Ferromagnetism in CrI3 via Synergistic Exchange Pathways
topic Materials Science
url https://arxiv.org/abs/2508.07278