Nature Communications, DOI:10.1038/s41467-026-74019-7 (2026)
Jiamin Chen, Jiahao Chen, Cong Wang*, Yi Zhang, Minglai Li, Yanping Li, Jiejun Wu, Tongjun Yu, Wei Ji*, and Lun Dai*
Abstract:
The research about two-dimensional van der Waals magnetic materials has advanced the 22 breakthroughs in ultrathin magnetic devices. We experimentally demonstrate that single-crystal 23 N-face AlN polar substrate can program layer-number-parity-dependent magnetic multistates and 24 their evolution sequence in few-layer CrI3. In odd-layer samples, as 5L-CrI3/AlN, when μ0H 25 sweeps from 3 to −3 T, the reflective magnetic circular dichroism signal evolves through distinct 26 magnetic multistates (+5 → –1 → +1 → –5), where +1 corresponds to the moment of a spin-up 27 monolayer. Thereby, we vertically program novel magnetic ground states and their evolution 28 sequence via a simplified heterointerface. Our first-principles calculations attribute this effect to 29 interfacial hole doping: it globally reconfigures the magnetic ground state of odd-layer CrI3 to a 30 novel ferrimagnetic order, and spatially differentiates the interlayer exchange and magnetic 31 anisotropy between the surface/interfacial and interior layers. Our work advances the practical 32 integration and design of two-dimensional magnetic devices with tailored functionalities.
