High-Throughput Prediction of Two-Dimensional Rare Earth Magnets

The development of next-generation microelectronics, signal processing, and data storage technologies demands the discovery of novel materials with advanced electronic and magnetic functionalities that can be seamlessly miniaturized and integrated with silicon. 4f-electron systems hold great promise in addressing this challenge due to the rich array of complex emergent phases, such as strong permanent magnetism, however the current hard magnet materials are difficult to incorporate with standard semiconductor substrates. To address this gap, we conducted a high-throughput search that integrates density functional theory (DFT) and many-body perturbation theory (MBPT) to identify and predict new two-dimensional (2D) 4f-magnets. Here, we identify 295 rare-earth compounds from across the lanthanide series of elements that exhibit a spectrum of crystal structures, electronic properties, and magnetic instabilities. In particular, we find a variety of predicted magnetic ordering vectors that cover ferromagnetic, antiferromagnetic, and competing magnetic phases. Moreover, a significant number of compounds exhibit small interlayer binding energies, suggesting many of the identified compounds can be readily exfoliated to the monolayer. Our work highlights the untapped promise of 4f compounds, opening new avenues for their application in the evolving landscape of 2D materials for cutting-edge technologies.