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Transition-metal dichalcogenides (TMDs) are layered compounds that supportmany electronic phases, including various charge density waves,superconducting, and Mott insulating states. Their intercalation with magneticions introduces magnetic sublayers, which strongly influence the couplingbetween host layers, and feature various magnetic states adjustable by externalmeans. Co$_{1/3}$NbS$_2$ hosts a particularly sensitive magnetic subsystem withthe lowest magnetic ordering temperature in the family of magneticallyintercalated TMDs, and the only one where the complete suppression of magneticorder under pressure has been recently suggested. By combining the results ofseveral experimental methods, electronic ab initio calculations, and modeling,we develop insights into the mechanisms of electric transport, magneticordering, and their interaction in this compound. The elastic neutronscattering is used to directly follow the evolution of the antiferromagneticorder parameter with pressure and temperature. Our results unambiguouslydisclose the complete suppression of the observed magnetic order around 1.7GPa. We delve into possible mechanisms of magnetic order suppression underpressure, highlighting the role of magnetic frustrations indicated by magneticsusceptibility measurements and ab-initio calculations. Electronic conductionanisotropy is measured in the wide temperature and pressure range. Here we showthat the transport in directions along and perpendicular to layers responddifferently to the appearance of magnetic ordering or the application of thehydrostatic pressure. We propose the 'spin-valve' mechanism where theintercalated Co ions act as spin-selective electrical transport bridges betweenhost layers. The mechanism applies to various magnetic states and can beextended to other magnetically intercalated TMDs.

Electronic transport and magnetism in the alternating stack of metallic and highly frustrated magnetic layers in Co$_{1/3}$NbS$_2$