Anisotropic Spin Fluctuations Induced by Spin‐Orbit Coupling in a Misfit Layer Compound (LaSe)_1.14(NbSe₂)

Abstract Spin‐orbit coupling (SOC) has significant effects on the superconductivity and magnetism of transition metal dichalcogenides (TMDs) at the 2D limit. Although 2D TMD samples possess many exotic properties different from those of bulk samples, experimental characterization in this field is still limited, especially for magnetism. Recent studies have revealed that bulk misfit layer compounds (MLCs) with (LaSe)_1.14(NbSe₂)_{n = 1,2} exhibit an Ising superconductivity similar to that of heavily electron‐doped NbSe₂ monolayers. This offers an opportunity to study the effect of SOC on the magnetism of 2D TMDs. Here, the possible SOC effect in (LaSe)_1.14(NbSe₂) is investigated by measuring nuclear magnetic resonance (NMR) and electrical transport. It is found that the LaSe layer not only functions as a charge reservoir for transferring electrons into the NbSe₂ layer but also remarkably influences the local electronic environment around the ⁹³Nb nuclei. More importantly, the significant SOC induces both a weak antilocalization (WAL) effect and anisotropic spin fluctuations in noncentrosymmetric NbSe₂ layers. The present work contributes to a deep understanding of the role of the SOC effect in 2D TMDs and supports MCLs as an intriguing platform for exploring exotic physical properties within the 2D limit.