Self-stacked 1T-1H layers in 6R-NbSeTe and the emergence of charge and magnetic correlations due to ligand disorder

The emergence of correlated phenomena arising from the combination of 1T and 1H van der Waals layers is the focus of intense research. Here, we synthesize a novel self-stacked 6R phase in NbSeTe, showing a perfect alternating 1T and 1H layers that grow coherently along the c-direction, as revealed by scanning transmission electron microscopy. Angle resolved photoemission spectroscopy shows a mixed contribution of the trigonal and octahedral Nb bands to the Fermi level. Diffuse scattering reveals temperature-independent short-range charge fluctuations with propagation vector qCO=(0.25,0), derived from the condensation of a longitudinal mode in the 1T layer. We observe that ligand disorder quenches the formation of a charge density wave. Magnetization measurements suggest the presence of an inhomogeneous, short-range magnetic order, further supported by the absence of a clear phase transition in the specific heat. These experimental analyses in combination with ab initio calculations indicate that the ground state of 6R-NbSeTe is described by a statistical distribution of short-range charge-modulated and spin-correlated regions driven by ligand disorder. Our results devise a route to synthesize 1T-1H self-stacked bulk heterostructures to study emergent phases of matter.