The content presents a comprehensive investigation of the magnetically ordered states in the transition metal dichalcogenide compounds Cr1/3NbS2 and Mn1/3NbS2 using nuclear magnetic resonance (NMR) techniques.
For Cr1/3NbS2, the 53Cr NMR data clearly identifies the compound as a textbook case of a chiral monoaxial helimagnet. The 53Cr NMR spectra show the signatures of the chiral soliton lattice (CSL), chiral conical phase (CCP), and forced ferromagnetic (FFM) phases as a function of applied magnetic field. The extracted conical angle θ(H) agrees well with mean-field theory predictions. The transition from the chiral helimagnetic (CHM) to paramagnetic phase is found to be of first-order.
The 55Mn NMR results for Mn1/3NbS2 are more complex due to higher structural disorder, but still confirm the presence of a CHM phase. The 55Mn spectra exhibit multiple broad components attributed to different local magnetic environments, likely arising from partial occupancy of the Mn 2b Wyckoff site. Despite the disorder, the analysis of spin-echo oscillations reveals the same type of interplay between quadrupolar and magnetic interactions as in the Cr compound, supporting the chiral conical model.
The DFT calculations provide further insights, predicting the EFG and hyperfine parameters in good agreement with the experimental observations. Overall, the study establishes that both Cr1/3NbS2 and Mn1/3NbS2 are chiral helical magnets, with the Cr compound representing a textbook case and the Mn compound exhibiting more complex magnetic behavior due to structural disorder.
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