Chromium iodide monolayers, which have different magnetic properties in comparison to the bulk chromium iodide, have been shown to form skyrmionic states in applied electromagnetic fields or in Janus-layer devices. In this work, we demonstrate that spin-canted solutions can be induced into monolayer chromium iodide by select substitution of iodide atoms with isovalent impurities. Several concentrations and spatial configurations of halide substitutional defects are selected to probe the coupling between the local defect-induced geometric distortions and orientation of chromium magnetic moments. This work provides atomic-level insight into how atomically precise strain-engineering can be used to create and control complex magnetic patterns in chromium iodide layers and lays out the foundation for investigating the field- and geometric-dependent magnetic properties in similar two-dimensional materials.
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