Prediction of room-temperature two-dimensional $\pi$-electron half-metallic ferrimagnets

TL;DR

This paper proposes a new organic two-dimensional material with room-temperature ferrimagnetism and half-metallicity, combining density functional theory and Hubbard models to explore its electronic and magnetic properties for spintronics.

Contribution

It introduces a novel design of organic 2D ferrimagnetic half-metals with large exchange couplings and topological features, advancing spintronics materials.

Findings

System is half-metallic with ferrimagnetic order and zero net magnetic moment.

Large intermolecular exchange couplings (~50 meV) ensure room temperature stability.

Spin-orbit coupling induces a topological gap with quantized Hall conductance.

Abstract

We propose a strategy to obtain conducting organic materials with fully spin-polarized Fermi surface, lying at a singular flat band, with antiferromagnetically coupled magnetic moments that reside in pi-orbitals of nanographenes. We consider a honeycomb crystal whose unit cell combines two different molecules with S=1/2: an Aza-3-Triangulene, a molecule with orbital degeneracy, and a 2-Triangulene. The analyzed system is half-metallic with a ferrimagnetic order, presenting a zero net total magnetic moment per unit cell. We combine density functional theory calculations with a Hubbard model Hamiltonian to compute the magnetic interactions, the bands, the intrinsic Anomalous Hall effect, and the collective spin excitations. We obtain very large intermolecular exchange couplings, in the range of 50 meV, which ensures room temperature stability. When the magnetization is off-plane, intrinsic spin orbit coupling in graphene opens up a topological gap that, despite being very small, leads to a quantized Hall conductance in the tens of mK range. Above 1 Kelvin, the system will behave like a half-metal with fully compensated magnetic moments, thereby combining two characteristics that make it ideal for spintronics applications.