Colossal Magnetoresistance in Ti Lightly Doped Cr₂Se₃ Single Crystals with a Layered Structure

Stoichiometric Cr₂Se₃ single crystals are particular layer-structured antiferromagnets, which possess a noncollinear spin configuration, weak ferromagnetic moments, moderate magnetoresistance (MR ∼14.3%), and poor metallic conductivity below the antiferromagnetic phase transition. Here, we report an interesting >16 000% colossal magnetoresistance (CMR) effect in Ti (1.5 atomic percent) lightly doped Cr₂Se₃ single crystals. Such a CMR is approximately 1143 times larger than that of the stoichiometric Cr₂Se₃ crystals and is rarely observed in layered antiferromagnets and is attributed to the frustrated spin configuration. Moreover, the Ti doping not only dramatically changes the electronic conductivity of the Cr₂Se₃ crystal from a bad metal to a semiconductor with a gap of ∼15 meV but also induces a change in the magnetic anisotropy of the Cr₂Se₃ crystal from strong out-of-plane to weak in-plane. Further, magnetotransport measurements reveal that the low-field MR scales with the square of the reduced magnetization, which is a signature of CMR materials. The layered Ti:Cr₂Se₃ with the CMR effect could be used as two-dimensional (2D) heterostructure building blocks to provide colossal negative MR in spintronic devices.