Charting new regions of Cobalt's chemical space with maximally large magnetic anisotropy: A computational high-throughput study

TL;DR

This study uses high-throughput computational methods to explore cobalt(II) complexes, discovering new compounds with record-breaking magnetic anisotropy that challenge traditional coordination paradigms.

Contribution

It introduces a large-scale computational screening of Co(II) complexes, revealing new structures with high magnetic anisotropy beyond known paradigms.

Findings

Over 100 compounds show high magnetic anisotropy.

Record-breaking anisotropy achieved with coordination numbers four or higher.

Expands understanding of chemical space for designing single-molecule magnets.

Abstract

Magnetic anisotropy slows down magnetic relaxation and plays a prominent role in the design of permanent magnets. Coordination compounds of Co(II) in particular exhibit large magnetic anisotropy in the presence of low-coordination environments and have been used as single-molecule magnet prototypes. However, only a limited sampling of Cobalt's vast chemical space has been performed, potentially obscuring alternative chemical routes toward large magnetic anisotropy. Here we perform a computational high-throughput exploration of Co(II)'s chemical space in search of new single-molecule magnets. We automatically assemble a diverse set of about 15000 novel complexes of Co(II) and fully characterize them with multi-reference ab initio methods. More than 100 compounds exhibit magnetic anisotropy comparable to or larger than leading known compounds. The analysis of these results shows that compounds with record-breaking magnetic anisotropy can also be achieved with coordination four or higher, going beyond the established paradigm of two-coordinated linear complexes.