Fig. 8

Interpretation of single-crystal magnetization experiments. a Single-crystal magnetization experiment (blue curve) measured at T = 0.03 K and a sweep rate of 0.1 T s−1 for a magnetic field oriented along the in-plane easy axis (y-axis in Fig. 6), superimposed on the theoretical equilibrium magnetization (orange curve) computed for the same temperature and field direction; b Energy levels as function of magnetic field (Zeeman spectrum) computed using the model presented in the text. The magenta (green) arrows connecting a and b associate the steep (smooth) raise of the theoretical (experimental) magnetization with slow/quasi-forbidden (fast/allowed) transition mechanisms occurring at level crossing between the two ground states (involving excited states) encircled in magenta (green). c Magnification of the low-field region of the Zeeman spectrum, highlighting degeneracy points (level crossings) of states between which faster 1-flip and 2-flip tunneling transitions are allowed (green circles and hexagons), and also highlighting 3-flip or higher-flip processes that are essentially forbidden (magenta circles). Some of the allowed phonon emission processes are also indicated with dashed green arrows; d High-field region of the Zeeman spectrum, where the four onion states antiferromagnetically coupled to Cr spin states become isolated from excited states, leading the system’s magnetization to saturate