Abstract The accessible exfoliation of layered CrI3 [Nature 546 (2017) 270, Ref. 1] has inspired the upsurge of two-dimensional intrinsic magnetism, which is desirable for next generation of information technology. The underlying magnetic coupling mechanism is still in debate and their magnetic ordering temperature is far less than room temperature, which prohibits their real application. Herein, anion ion(iodine being replaced by bromine) and cation ions(Cr substituted by V/Mn) substitution are conducted using density functional theory, including both electron correlation(U) and spin-orbit coupling(SOC) effect, to provide an intuitive physical picture to understand their electronic and magnetic behavior. Our results indicate that the in-plane parameters, band gap, magnetic moment and magnetic ordering temperature can be tuned linearly via the concentration of bromine. Intriguingly, Both V and Mn substitution would give rise to half metallic character, a promising spintronic candidate. Moreover, V3+(3d2) would give rise to a V dxy–I px–Cr dxy exchange path, which is ferromagnetic, and thus hold great promise to enhance the magnetic ordering temperature (397 K) being above room temperature.

中文翻译：

---

调节三卤化铬单层的电子和磁性

摘要 层状 CrI3 的易剥落 [Nature 546 (2017) 270, Ref. 1]激发了二维内在磁性的热潮，这是下一代信息技术所需要的。底层的磁耦合机制仍在争论中，它们的磁有序温度远低于室温，这阻碍了它们的实际应用。在这里，阴离子（碘被溴取代）和阳离子（Cr 被 V/Mn 取代）取代是使用密度泛函理论进行的，包括电子相关（U）和自旋轨道耦合（SOC）效应，以提供一个直观的物理图片来了解它们的电子和磁性行为。我们的结果表明，面内参数、带隙、磁矩和磁有序温度可​​以通过溴的浓度线性调节。有趣的是，V 和 Mn 的替代都会产生半金属特性，这是一个很有前途的自旋电子候选者。此外，V3+(3d2) 会产生 V dxy-I px-Cr dxy 交换路径，它是铁磁性的，因此很有希望提高高于室温的磁有序温度（397 K）。