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Register a new userOrigin of ferromagnetic response in diluted magnetic semiconductors and oxides
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Tomasz Dietl
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This paper reviews the present understanding of the origin of ferromagnetic response of diluted magnetic semiconductors and diluted magnetic oxides as well as in some nominally magnetically undoped materials. It is argued that these systems can be grouped into four classes. To the first belong composite materials in which precipitations of a known ferromagnetic, ferrimagnetic or antiferromagnetic compound account for magnetic characteristics at high temperatures. The second class forms alloys showing chemical nano-scale phase separation into the regions with small and large concentrations of the magnetic constituent. To the third class belong (Ga,Mn)As, heavily doped p-(Zn,Mn)Te, and related semiconductors. In these solid solutions the theory built on p-d Zeners model of hole-mediated ferromagnetism and on either the Kohn-Luttinger kp theory or the multi-orbital tight-binding approach describes qualitatively, and often quantitatively many relevant properties. Finally, in a number of carrier-doped DMS and DMO a competition between long-range ferromagnetic and short-range antiferromagnetic interactions and/or the proximity of the localisation boundary lead to an electronic nano-scale phase separation.
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The author reviews the present understanding of the hole-mediated ferromagnetism in magnetically doped semiconductors and oxides as well as the origin of high temperature ferromagnetism in materials containing no valence band holes. It is argued that in these systems spinodal decomposition into regions with a large and a small concentration of magnetic component takes place. This self-organized assembling of magnetic nanocrystals can be controlled by co-doping and growth conditions. Functionalities of these multicomponent systems are described together with prospects for their applications in spintronics, nanoelectronics, photonics, plasmonics, and thermoelectrics.
We have studied the magnetic-field and concentration dependences of the magnetizations of the hole and Mn subsystems in diluted ferromagnetic semiconductor Ga_{1-x}Mn_xAs. A mean-field approximation to the hole-mediated interaction is used, in which the hole concentration p(x) is parametrized in terms of a fitting (of the hole effective mass and hole/local moment coupling) to experimental data on the Tc critical temperature. The dependence of the magnetizations with x, for a given temperature, presents a sharply peaked structure, with maxima increasing with applied magnetic field, which indicates that application to diluted-magnetic-semiconductor devices would require quality-control of the Mn-doping composition. We also compare various experimental data for Tc(x) and p(x) on different Ga_{1-x}Mn_xAs samples and stress the need of further detailed experimental work to assure that the experimental measurements are reproducible.
With their broad range of magnetic, electronic and structural properties, transition metal perovskite oxides ABO3 have long served as a platform for testing condensed matter theories. In particular, their insulating character - found in most compounds - is often ascribed to dynamical electronic correlations through the celebrated Mott-Hubbard mechanism where gaping arises from a uniform, symmetry-preserving electron repulsion mechanism. However, structural distortions are ubiquitous in perovskites and their relevance with respect to dynamical correlations in producing this rich array of properties remains an open question. Here, we address the origin of band gap opening in the whole family of 3d perovskite oxides. We show that a single-determinant mean-field approach such as density functional theory (DFT) successfully describes the structural, magnetic and electronic properties of the whole series, at low and high temperatures. We find that insulation occurs via energy-lowering crystal symmetry reduction (octahedral rotations, Jahn-Teller and bond disproportionation effects), as well as intrinsic electronic instabilities, all lifting orbital degeneracies. Our work therefore suggests that whereas ABO3 oxides may be complicated, they are not necessarily strongly correlated. It also opens the way towards systematic investigations of doping and defect physics in perovskites, essential for the full realization of oxide-based electronics.
Spin splitting of photoelectrons in p-type and electrons in n-type III-V Mn-based diluted magnetic semiconductors is studied theoretically. It is demonstrated that the unusual sign and magnitude of the apparent s-d exchange integral reported for GaAs:Mn arises from exchange interactions between electrons and holes bound to Mn acceptors. This interaction dominates over the coupling between electrons and Mn spins, so far regarded as the main source of spin-dependent phenomena. A reduced magnitude of the apparent s-d exchange integral found in n-type materials is explained by the presence of repulsive Coulomb potentials at ionized Mn acceptors and a bottleneck effect.
Chemical pressure is an effective method to tune physical properties, particularly for diluted magnetic semiconductors (DMS) of which ferromagnetic ordering is mediated by charge carriers. Via substitution of smaller Ca for larger Sr, we introduce chemical pressure on (Sr,Na)(Cd,Mn)2As2 to fabricate a new DMS material (Ca,Na)(Cd,Mn)2As2. Carriers and spins are introduced by substitutions of (Ca,Na) and (Cd,Mn) respectively. The unit cell volume reduces by 6.2% after complete substitution of Ca for Sr, suggesting a subsistent chemical pressure. Importantly the local geometry of [Cd/MnAs4] tetrahedron is optimized via chemical compression that increases the Mn-As hybridization leading to enhanced ferromagnetic interactions. As a result, the maximum Curie temperature (TC) is increased by about 50% while the the maximum saturation moment increases by over 100% from (Sr,Na)(Cd,Mn)2As2 to (Ca,Na)(Cd,Mn)2As2. The chemical pressure estimated from the equation of state is equal to an external physical pressure of 3.6 GPa.
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