Recent heat capacity and low field magnetic susceptibility measurements revealed unusual magnetic phenomena occurring in Er 1-x R x Al 2 systems (where R = Dy, Tb) in the vicinity of a "magic" concentration of x = 0.25. Empirically, the reasons for such behavior were attributed to different shapes of the 4f charge densities of the R 3+ ions, which are represented by the opposite signs of the second order Stevens' factors. Here we show that by using both the signs and magnitudes of the second order Stevens' factors, magnetic transitions can be predicted in a broader range of pseudo binary R 1-x R' x Al 2 alloys where R and R' are rare earth metals that have opposite signs of second orderStevens' factors. The predictions have been verified using Tm 1-x Tb x Al 2 system as model 2 using x-ray diffraction, magnetic susceptibility and heat capacity measurements. First principles calculations have also been performed in order to explore the behavior of the density of states near the Fermi level.PACS No's: 75.50.Cc, 75.10.Dg, 71.20.Lp, 71.20.Eh.
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IntroductionThe fundamental magnetic properties of the RAl 2 compounds, where R is a rare earth element, have continuously attracted attention of researchers for more than forty years. 1,2,3,4,5 Specifically the isostructural RAl 2 compounds are well known for interesting properties including crystalline electric field effects 5 and low temperature ferromagnetism 4,5 that can be controlled by varying the rare earth component. Recent research results suggest that despite of broad experimental and theoretical investigations that have been already performed using these relatively simple MgCu 2 -type Laves phases, some fascinating and new phenomena in the RAl 2 compounds are yet to be discovered.Most of the earlier studies explored the properties of the pure binary RAl 2 compounds.Since the 4f charge densities of the R atoms are significantly different from one another, unusual behaviors may be observed when the R atoms in the RAl 2 alloys are partially replaced by a different R' atom to form pseudo binary R 1-x R' x Al 2 compounds. Such replacements have resulted in important discoveries such as zero net magnetic moment in annealing was not necessary. To check the phase purity and identify the crystal structure of the samples, room temperature x-ray powder diffraction (XRD) was performed on a PANAnalytical powder diffractometer employing monochromatic Cu K α1 radiation.Temperature dependent XRD measurements were performed on a Rigaku TTRAX rotating anode powder diffractometer employing Mo Kα radiation. 18 The diffractometer was equipped with a continuous flow 4 He cryostat controlling the temperature of a sample, which was prepared and mounted on a copper sample holder as described in The lattice parameter for pure TmAl 2 (7.7757 Å) was taken from the report of Harris et al. 21 As shown in the inset of Fig. 1, the lattice parameters depend linearly on the Tb concentration (x). Assuming that Vegard's law holds (which is reasonable considering that the structure is cubic and that ...