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Here, we present results of a computational study of electronic, magnetic, and structural properties of FeVTaAl and FeCrZrAl, quaternary Heusler alloys that have been recently reported to exhibit spin-gapless semiconducting behavior. Our calculations indicate that these materials may crystallize in regular Heusler cubic structure, which has a significantly lower energy than the inverted Heusler cubic phase. Both FeVTaAl and FeCrZrAl exhibit ferromagnetic alignment, with an integer magnetic moment per unit cell at equilibrium lattice constant. Band structure analysis reveals that while both FeVTaAl and FeCrZrAl indeed exhibit nearly spin-gapless semiconducting electronic structure at their optimal lattice parameters, FeVTaAl is a 100% spin-polarized semimetal, while FeCrZrAl is a magnetic semiconductor. Our calculations indicate that expansion of the unit cell volume retains 100% spin-polarization of both compounds. In particular, both FeVTaAl and FeCrZrAl are 100% spin-polarized magnetic semiconductors at the largest considered lattice constant. At the same time, at smaller lattice parameters, both compounds exhibit a more complex electronic structure, somewhat resembling half-metallic properties. Thus, both of these alloys may be potentially useful for practical applications in spin-based electronics, but their electronic structure is very sensitive to the external pressure. We hope that these results will stimulate experimental efforts to synthesize these materials. 

Here, we present results of combined experimental and computations study of V2CoAl, a Heusler alloy that exhibits nearly perfect spin-polarization. Our calculations indicate that this material maintains a high degree of spin-polarization (over 90%) in the wide range of lattice parameters, except at the largest considered unit cell volume. The magnetic alignment of V2CoAl is ferrimagnetic, due to the antialignment of the magnetic moments of vanadium atoms in their two sublattices. The calculated total magnetic moment per formula unit is nearly integer at the optimal lattice parameter and at the smaller volumes of the unit cell, but it deviated from the integer values as the unit cell expands. This is consistent with the calculated variation in the degree of spin polarization with lattice constant. The expected ferrimagnetic behavior has been observed in the arc-melted V2CoAl sample, with a Curie temperature of about 80 K. However, the saturation magnetization is significantly smaller than the theoretical prediction of ∼2 μB/f.u., most likely due to the observed B2-type atomic disorder. The samples exhibit metallic electron transport across the measurement range of 2 K to 300 K. 

Spin-gapless semiconductor (SGS) is a new class of material that has been studied recently for potential applications in spintronics. This material behaves as an insulator for one spin channel, and as a gapless semiconductor for the opposite spin. In this work, we present results of a computational study of two quaternary Heusler alloys, MnCrNbAl and MnCrTaAl that have been recently reported to exhibit spin-gapless semiconducting electronic structure. In particular, using density functional calculations we analyze the effect of external pressure on electronic and magnetic properties of these compounds. It is shown that while these two alloys exhibit nearly SGS behavior at optimal lattice constants and at negative pressure (expansion), they are half-metals at equilibrium, and magnetic semiconductors at larger lattice constant. At the same time, reduction of the unit cell volume has a detrimental effect on electronic properties of these materials, by modifying the exchange splitting of their electronic structure and ultimately destroying their half-metallic/semiconducting behavior. Thus, our results indicate that both MnCrNbAl and MnCrTaAl may be attractive for practical device applications in spin-based electronics, but a potential compression of the unit cell volume (e.g. in thin-film applications) should be avoided. 

Half-metallic Heusler compounds have been extensively studied in the recent years, both experimentally and theoretically, for potential applications in spin-based electronics. Here, we present the results of a combined theoretical and experimental study of the quaternary Heusler compound NiFeMnAl. Our calculations indicate that this material is half-metallic in the ground state and maintains its half-metallic electronic structure under a considerable range of external hydrostatic pressure and biaxial strain. NiFeMnAl crystallizes in the regular cubic Heusler structure, and exhibits ferromagnetic alignment. The practical feasibility of the proposed system is confirmed in the experimental section of this work. More specifically, a bulk ingot of NiFeMnAl was synthesized in A2 type disordered cubic structure using arc melting. It shows a high Curie temperature of about 468 K and a saturation magnetization of 2.3 μ_B⁄(f.u). The measured magnetization value is smaller than the one calculated for the ordered structure. This discrepancy is likely due to the A2 type atomic disorder, as demonstrated by our calculations. We hope that the presented results may be useful for researchers working on practical applications of spin-based electronics. 

We present computational results on electronic, magnetic, and structural properties of CoVMnSb, a quaternary Heusler alloy. Our calculations indicate that this material may crystallize in two energetically close structural phases: inverted and regular cubic. The inverted cubic phase is the ground state, with ferrimagnetic alignment, and around 80% spin polarization. Despite having a relatively large bandgap in the minority-spin channel close to the Fermi level, this phase does not undergo a half-metallic transition under pressure. This is explained by the “pinning” of the Fermi level at the minority-spin states at the Γ point. At the same time, the regular cubic phase is half-metallic and retains its perfect spin polarization under a wide range of mechanical strain. Transition to a regular cubic phase may be attained by applying uniform pressure (but not biaxial strain). In practice, this pressure may be realized by an atomic substitution of non-magnetic atoms (Sb) with another non-magnetic atom (Si) of a smaller radius. Our calculations indicate that 25% substitution of Sb with Si results in a half-metallic regular cubic phase being the ground state. In addition, CoVMnSb0.5Si0.5 retains its half-metallic properties under a considerable range of mechanical pressure, as well as exhibits thermodynamic stability, thus making this alloy attractive for potential spintronic applications. We hope that the presented results will stimulate experimental efforts to synthesize this compound.