Two-Dimensional Bipolar Magnetic Semiconductor with High Curie Temperature and Electrically Controllable Spin Polarization Realized in Exfoliated Cr(pyrazine)$_2$ Monolayer

TL;DR

This paper proposes a new 2D magnetic semiconductor material, Cr(pyz)$_2$ monolayer, with high Curie temperature and electrically controllable spin polarization, promising for nanospintronics applications.

Contribution

It introduces a feasible exfoliation method for a novel 2D magnetic semiconductor with room temperature ferrimagnetism and tunable spin polarization, based on first principles calculations.

Findings

Exfoliation energy of 0.27 J/m$^2$ confirms feasibility.

Cr(pyz)$_2$ monolayer exhibits room temperature ferrimagnetism with T$_C$ of 342 K.

Electrical doping induces half-metallic conduction with controllable spin polarization.

Abstract

Exploring two-dimensional (2D) magnetic semiconductors with room temperature magnetic ordering and electrically controllable spin polarization is a highly desirable but challenging task for nanospintronics. Here, through first principles calculations, we propose to realize such a material by exfoliating the recently synthesized organometallic layered crystal Li$_{0.7}$[Cr(pyz)$_2$]Cl$_{0.7}$0.25$\cdot$(THF) (pyz = pyrazine, THF = tetrahydrofuran) [Science 370, 587 (2020)]. The feasibility of exfoliation is confirmed by the rather low exfoliation energy of 0.27 J/m$^2$, even smaller than that of graphite. In exfoliated Cr(pyz)$_2$ monolayer, each pyrazine ring grabs one electron from the Cr atom to become a radical anion, then a strong $d$-$p$ direct exchange magnetic interaction emerges between Cr cations and pyrazine radicals, resulting in room temperature ferrimagnetism with a Curie temperature of 342 K. Moreover, Cr(pyz)$_2$ monolayer is revealed to be an intrinsic bipolar magnetic semiconductor where electrical doping can induce half-metallic conduction with controllable spin-polarization direction.