Local moment formation and magnetic coupling of Mn guest atoms in Bi$_2$Se$_3$: a low-temperature ferromagnetic resonance study (1707.00975v1)

Abstract: We compare the magnetic and electronic configuration of single Mn atoms in molecular beam epitaxy (MBE) grown Bi$_2$Se$_3$ thin films, focusing on electron paramagnetic (ferromagnetic) resonance (EPR and FMR, respectively) and superconducting quantum interference device (SQUID) techniques. X-ray diffraction (XRD) and electron backscatter diffraction (EBSD) reveal the expected increase of disorder with increasing concentration of magnetic guest atoms, however, Kikuchi patterns show that disorder consists majorly of mum-scale 60deg twin domains in the hexagonal Bi$_2$Se$_3$ structure, which are promoted by the presence of single unclustered Mn impurities. Ferromagnetism below T$_C$ ~ (5.4 +/- 0.3) K can be well described by critical scaling laws M(T) ~ (1-T/T$_C$)$^\beta$ with a critical exponent $\beta$ = (0.34 +/- 0.2)), suggesting 3D Heisenberg class magnetism instead of e.g. 2D-type coupling between Mn-spins in van der Waals gap sites. From EPR hyperfine structure data we determine a Mn$^{2+}$ (d$^5$, S = 5/2) electronic configuration with a g-factor of 2.002 for -1/2 --> +1/2 transitions. In addition, from the strong dependence of the low temperature FMR fields and linewidth on the field strength and orientation with respect to the Bi$_2$Se$_3$ (0001) plane, we derive magnetic anisotropy energies of up to K1 = -3720 erg/cm3 in MBE-grown Mn-doped Bi$_2$Se$_3$, reflecting the first order magneto-crystalline anisotropy of an in-plane magnetic easy plane in a hexagonal (0001) crystal symmetry. Across the ferromagnetic-paramagnetic transition the FMR intensity is suppressed and resonance fields converge the paramagnetic limit of a Mn$^{2+}$ (d$^5$, S = 5/2).