Robust Intrinsic Ferromagnetism and Half Semiconductivity in Stable Two-Dimensional Single-Layer Chromium Trihalides

Abstract

Two-dimensional (2D) intrinsic ferromagnetic (FM) semiconductors are crucial to develop low-dimensional spintronic devices. Using density functional theory, we show that single-layer chromium trihalides (SLCTs) (CrX${}_3$,X=F, Cl, Br and I) constitute a series of stable 2D intrinsic FM semiconductors. A free-standing SLCT can be easily exfoliated from the bulk crystal, due to a low cleavage energy and a high in-plane stiffness. Electronic structure calculations using the HSE06 functional indicate that both bulk and single-layer CrX${}_3$ are half semiconductors with indirect gaps and their valence bands and conduction bands are fully spin-polarized in the same spin direction. The energy gaps and absorption edges of CrBr${}_3$ and CrI${}_3$ are found to be in the visible frequency range, which implies possible opt-electronic applications. Furthermore, SLCTs are found to possess a large magnetic moment of 3${\mu }_B$ per formula unit and a sizable magnetic anisotropy energy. The magnetic exchange constants of SLCTs are then extracted using the Heisenberg spin Hamiltonian and the microscopic origins of the various exchange interactions are analyzed. A competition between a near 90${}^{\circ }$ FM superexchange and a direct antiferromagnetic (AFM) exchange results in a FM nearest-neighbour exchange interaction. The next and third nearest-neighbour exchange interactions are found to be FM and AFM respectively and this can be understood by the angle-dependent extended Cr-X-X-Cr superexchange interaction. Moreover, the Curie temperatures of SLCTs are also predicted using Monte Carlo simulations and the values can further increase by applying a biaxial tensile strain. The unique combination of robust intrinsic ferromagnetism, half semiconductivity and large magnetic anisotropy energies renders the SLCTs as promising candidates for next-generation semiconductor spintronic applications.

12 pages, 14 figures. published in J. Mater. Chem. C

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