An emergence of chiral helimagnetism or ferromagnetism governed by Cr intercalation in a dichalcogenide CrNb3S6

<jats:p>A synthesis of single crystals of chiral dichalcogenides TM3X6 (T: 3d transition metal, M: Nb or Ta, X: S or Se) remains an intriguing issue for the investigation of emergent quantum properties such as chiral helimagnetism. In this study, we investigated a correlation between the quantity of Cr intercalation x and the magnetic property in single crystals of a chromium (Cr) intercalated chiral disulfide CrxNb3S6 in order to optimize the synthesis condition for the intercalation-controlled single crystals. The magnetic properties, including a magnetic transition temperature Tc, take different values depending on the samples. We systematically grew single crystals of CrxNb3S6 with x ranged from 0.89 to 1.03 and found that the amount of the Cr intercalation x is an essential factor in controlling the magnetic properties of the grown crystals. The magnetization anomaly, which appears in the temperature dependence as evidence of the formation of chiral magnetic soliton lattice (CSL), was observed only in a narrow region of x from 0.98 to 1.03. The single crystals with x being 0.98 and 0.99 showed the CSL behavior with the highest Tc of 133 K. These results indicate that the small number of defects on the sites for T ions dramatically affects the quality of the single crystals in the synthesis of TM3S6. We also discuss the importance of synthesizing enantiopure single crystals of chiral dichalcogenides in order to observe chiral physical properties unique to chiral compounds such as magneto-chiral effect and chiral-induced spin selectivity.</jats:p>