High‐Spin Defect Clustering and Emergent Magnetism in TiS ₂

Defect‐induced magnetism in layered transition metal dichalcogenides (TMDCs) has recently emerged as a promising strategy for tailoring their electronic and magnetic properties. In this work, we investigate the origin of paramagnetism in titanium disulfide (TiS 2 ) and propose that Ti adatoms may act as the primary source of local magnetization. Atomically resolved scanning tunneling microscopy (STM) images allowed for the estimation of point defect concentration in the surface of bulk TiS 2 , revealing a significant population of Ti adatoms. Magnetic characterization using superconducting quantum interference device (SQUID) magnetometry confirmed the presence of paramagnetism, with a surprisingly effective spin state of 4. This indicates a cooperative clustering effect, in which Ti adatoms couple to form high‐spin structures. Density functional theory (DFT) calculations indicate that Ti adatoms generate localized magnetic moments, consistent with their role as the source of the magnetization detected in SQUID measurements. Our comprehensive STM, SQUID, and DFT analysis highlights structural and magnetic properties that enable defect engineering in TiS 2 as an effective route to introduce controlled magnetism, expanding the possibilities for the use of two‐dimensional magnetic systems in spintronics.