Influence of Randomness and Localization on RKKY Interactions in Diluted Magnetic Semiconductors

We show that the spatially random distribution of magnetic moments of dopants in diluted magnetic semiconductors can partially localize the itinerant carriers and change the carrier-mediated indirect RKKY interaction. From numerical calculations of the electron states taking into account the interaction with magnetic impurities which are random both in spatial positions and in orientations of magnetic moments, we obtain the electron states and the RKKY interaction as a function of the distance between magnetic dopants L and of the sp - d exchange integral J. With the increase of disorder, the localization of itinerant electrons become stronger and the long-range regular oscillatory behaviour of the RKKY interaction gradually disappears and is replaced by severe fluctuations. The randomness and localization may enhance the RKKY interaction between dopants with short and middle distances and in favour of the ferromagnetism.     

典型磁性材料价电子结构研究面临的机遇与挑战

目前在磁性材料磁有序现象研究中广泛使用的交换作用、超交换作用和双交换作用模型形成于1950年代及其以前,这些模型都涉及材料中的价电子状态,但那时还没有充分的价电子状态实验依据.1970年代以来,有关价电子结构实验结果的报道越来越多,这些实验结果表明传统的磁有序模型需要改进.首先,大量电子谱实验表明,在氧化物中除存在负二价氧离子之外,还存在负一价氧离子,并且负一价氧离子的含量可达30%或更多.这说明以所有氧离子都是负二价离子为基本假设的超交换和双交换作用模型需要改进.其次,一些实验证明,铁、钴、镍自由原子的一部分4s电子在形成铁磁性金属的过程中变成了3d电子,这为探讨金属磁性与电输运性质的关系提供了依据.此外,即使在现代的密度泛函计算中,仍不能给出磁性交换作用能的函数表达式,只能采取各种不同模型进行模拟计算,从而使磁性材料的模拟计算遇到严重困难.寻求一个磁有序能的函数表达式可能是解决这个困难的途径.这些研究表明磁性材料价电子结构研究面临着重大的机遇与挑战.本文首先介绍一些典型的实验例证,然后介绍了基于这些实验结果的一套典型磁性材料的磁有序新模型,随后介绍了基于新模型的磁性材料价电子结构与旧模型的主要区别,最后指出了未来研究工作面临的挑战.     

Ferromagnetism versus superconductivity in ramdom alloys

Magnetic, superconducting narrow-band alloys are studied within a random lattice model. Coulomb repulsion and contact-type attraction of the itinerant electrons, and the indirect exchange between local magnetic moments are taken into account. Averaging the free energy expansion in coherent potential approximation, the Ginzburg-Landau functional is derived with two biquadratically coupled order parameters. Coherent orderings and concentration-dependent critical temperatures are determined. The coefficients of theq ²-terms, i.e. the stiffness and diffusion constants, involve vertex corrections due to impurity scattering. The coexistence criterion resulting from the 4th-order couplings cannot be fulfilled, referring to a first order transition between ferromagnetism and superconductivity. Tetracritical behaviour is found by including the direct exchanges between the localized spins.     

Non-perturbative approaches to magnetism in strongly correlated electron systems

The microscopic basis for the stability of itinerant ferromagnetism in correlated electron systems is examined. To this end several routes to ferromagnetism are explored, using both rigorous methods valid in arbitrary spatial dimensions, as well as Quantum Monte Carlo investigations in the limit of infinite dimensions (dynamical mean-field theory). In particular we discuss the qualitative and quantitative importance of (i) the direct Heisenberg exchange coupling, (ii) band degeneracy plus Hund's rule coupling, and (iii) a high spectral density near the band edges caused by an appropriate lattice structure and/or kinetic energy of the electrons. We furnish evidence of the stability of itinerant ferromagnetism in the pure Hubbard model for appropriate lattices at electronic densities not too close to half-filling and large enough U. Already a weak direct exchange interaction, as well as band degeneracy, is found to reduce the critical value of U above which ferromagnetism becomes stable considerably. Using similar numerical techniques the Hubbard model with an easy axis is studied to explain metamagnetism in strongly anisotropic antiferromagnets from a unifying microscopic point of view.     

In situ photoemission study of the room temperature ferromagnet ZnGeP2:Mn

The chemical states of the ZnGeP(2):Mn interface which shows ferromagnetism above room temperature have been studied by photoemission spectroscopy. Mn deposition on the ZnGeP2 substrate heated to 400 degrees C induced Mn substitution for Zn and then the formation of metallic Mn-Ge-P compounds. Depth profile studies have shown that Mn 3d electrons changed their character from itinerant to localized along the depth, and in the deep region, dilute divalent Mn species (<5% Mn) was observed with a coexisting metallic Fermi edge of non-Mn 3d character. The possibility of hole doping through Mn substitution for Ge and/or Zn vacancy is discussed.     

Electron spin resonance of proton-irradiated graphite

In the case of colossal magnetoresistance in the perovskite manganites, "double exchange" mediated by the itinerant spins is believed to play a key role in the ferromagnetism. In contrast, the conventional "Heisenberg" interaction, i.e., direct (unmediated) interaction between the localized spins produced by the proton irradiation, is identified as the origin of proton irradiation-induced ferromagnetism in graphite.     

Theory of Coexistence of Charge-Ordering and Antiferromagnetic Phases in R0.5A0.5Mn03

Based on a model Hamiltonian with the nearest-neighbor Coulomb interaction of the itinerant e_g electrons, we investigated the possibility of the coexistence of the charge-ordering phase and the antiferromagnetic phase for the manganites R_i-xA_xMn0₃ with the doping of x = 0.5. Three different types of the magnetic configurations (CEtype antiferromagnetism, simple antiferromagnetism, and ferromagnetism) have been compared by numerical calculation under the mean-field approximation. We found that the charge-ordering phase may coexist with the CEtype antiferromagnetic phase if the nearest-neighbor Coulomb interaction exceeding a certain critical value.     

Intrinsic impurity-band Stoner ferromagnetism in C60Hn

We identify Stoner ferromagnetism in fcc C60H(n) (n=odd) by using a local density approximation in the framework of the density functional theory. Hydrogen chemisorption on fullerenes creates quasilocalized π electrons on the fullerene surface, overlapping of their wave functions giving rise to a narrow half filled impurity band in the fcc C60H(n). The Stoner-type ferromagnetic exchange between the itinerant electrons leads to spin-split impurity bands. The magnetic moment per C60H(n) molecule is 1 μ(B) (for n=odd) or 0 (for n=even, including zero), only one of the hydrogens contributing to the spin-split states. Direct overlapping of the quasilocalized π-electron orbitals is essential for the ferromagnetism.     

Phase diagram of the disordered RKKY model in dilute magnetic semiconductors

We consider ferromagnetism in spatially randomly located magnetic moments, as in a diluted magnetic semiconductor, coupled via the carrier-mediated indirect exchange RKKY interaction. We obtain, via Monte Carlo calculations, the magnetic phase diagram as a function of the impurity moment density n(i) and the relative carrier concentration n(c)/n(i). As evidenced by the diverging correlation length and magnetic susceptibility, the boundary between ferromagnetic and nonferromagnetic phases constitutes a line of zero temperature critical points which can be viewed as a magnetic percolation transition. In the dilute limit, we find that bulk ferromagnetism vanishes for n(c)/n(i) >0.1. We also incorporate the local antiferromagnetic direct superexchange interaction between nearest neighbor impurities and examine the impact of a damping factor in the RKKY range function.     

Ferromagnetism in magnetically doped III-V semiconductors.

The origin of ferromagnetism in semimagnetic III-V materials is discussed. The indirect exchange interaction caused by virtual electron excitations from magnetic impurity acceptor levels to the valence band can explain ferromagnetism in GaAs(Mn) in both degenerate and nondegenerate samples. Formation of ferromagnetic clusters and the percolation picture of phase transition describes well all available experimental data and allows us to predict the Mn-composition dependence of transition temperature in wurtzite (Ga,In,Al)N epitaxial layers.     

Magnetic pair making and breaking effect of Ru in La0.7Sr0.3Mn0.9Ru0.1O3 and La0.5Sr0.5Co0.9Ru0.1O3

The substitutional effect of Ru on the magnetic and transport properties of double exchange ferromagnets, La_0.7Sr_0.3MnO₃ and La_0.5Sr_0.5CoO₃ has been investigated. It is found that substitution of 10% Ru at the Mn site of La_0.7Sr_0.3MnO₃ decreases the Curie temperature by 20 K than that of the parent compound. However, a large decrease in the Curie temperature, ΔT_c80 K and the system undergoes a transition from metallic state to insulating state is observed when 10% Ru is doped in La_0.5Sr_0.5CoO₃. The marginal effect of Ru in the Mn–O–Mn sublattice in comparison to the Co–O–Co sublattice could be due to the magnetic exchange interaction between Mn and Ru by virtue of the fact that Ru exhibits variable valence states, Ru⁺⁴/Ru⁺⁵. The e_g and t_2g parentage of Ru⁺⁵ is similar to Mn⁺⁴ and therefore, Ru⁺⁵ ion appears to participate in the double exchange mediated ferromagnetic (FM) interaction. On the other hand, Ruthenium (IV) ion disrupts an intermediate spin state of cobalt (Co⁺³: t_2g⁵e_g¹), forcing a double exchange FM state to anti-FM state.     

Effect of impurity ions configurations on the magnetic properties of Mn-doped ZnO

The magnetic and electronic properties of Mn-doped ZnO are studied by first-principles calculations. It is found that the exchange interaction between Mn ions depends on the Mn-Mn distribution configuration and distance. We also found that the ferromagnetism can be existed when the Mn-Mn distance is large and Mn ions are distributed uniformly, and the long ranged ferromagnetism is explained by the interaction between Mn and O atoms. Thus, it is possible to tune ferromagnetism in Mn-doped ZnO semiconductors by controlling the doping position in ZnO lattice.     

Evidence of a critical Mn-Mn distance for the onset of ferromagnetism in NiAs type compounds

Recently, the technique of spin wave resonance has been used to measure the exchange coupling constants as a function of composition in several solid solutions of MnSb. From an examination of the results we show that in those alloys in which the linear chains of magnetic atoms are not disturbed, the exchange coupling constants become positive leading to ferromagnetic coupling when the distance between Mn atoms becomes equal to 2.83 Å or more. This experimental value of the Mn-Mn distance for the onset of ferromagnetism is equal to the critical distance derived by Forrer after examining a large number of materials which owe their ferromagnetism predominantly to the direct exchange interaction.     

Anisotropic ferromagnetism in substituted zinc oxide

Room-temperature ferromagnetism is observed in (110) oriented ZnO films made from targets containing 5 at. % of Sc, Ti, V, Fe, Co, or Ni, but not Cr, Mn, or Cu ions. There are large moments, 2.6 micro(B) and 0.5 micro(B)/dopant atom for Co- and Ti-containing oxides, respectively. There is also a moment of 0.3 micro(B)/Sc. Magnetization is very anisotropic, with variations of up to a factor of 3 depending on the orientation of the applied field relative to the substrate. Results are interpreted in terms of a spin-split donor impurity-band model, which can account for ferromagnetism in insulating or conducting high-k oxides with concentrations of magnetic ions that lie far below the percolation threshold. Magnetic moments are associated with two-electron defects in the films as well as unpaired electrons of the 3d ions.     

Role of Ti 3d carriers in mediating the ferromagnetism of Co∶TiO2 anatase thin films

We study the surface and bulk electronic structure of the room-temperature ferromagnet Co∶TiO(2) anatase films using soft- and hard-x-ray photoemission spectroscopy with probe sensitivities of ～1 and ～10 nm, respectively. We obtain direct evidence of metallic Ti(3+) states in the bulk, which get suppressed to give a surface semiconductor, thus indicating the difference in electronic structure between surface and bulk. X-ray absorption and resonant photoemission spectroscopy reveal Ti(3+) electrons at the Fermi level (E(F)) and high-spin Co(2+) electrons occurring away from E(F). The results show the importance of the charge neutrality condition: Co(2+)+V(O)(2-)+2Ti(4+)?Co(2+)+2Ti(3+) (V(O) is oxygen vacancy), which gives rise to the elusive Ti 3d carriers mediating ferromagnetism via the Co 3d-O 2p-Ti 3d exchange interaction pathway of the occupied orbitals.     

基于XPS与XAS的稀磁半导体GaMnN电子结构研究

采用基于同步辐射技术的X射线光电子能谱(XPS)与X射线吸收谱(XAS)测试由金属有机化学气相沉积(MOCVD)技术制备的不同Mn掺杂浓度的稀磁半导体GaMnN薄膜的电子结构,探究Mn掺杂浓度对磁性原子Mn周围的局域环境和电子态等方面的影响,并阐述材料铁磁性变化的机理. XPS和XAS图谱分析表明：Mn²⁺和Mn³⁺共存于薄膜样品内,样品D中Mn²⁺占比高达70%-80%,N空位随Mn掺杂浓度增加而增多且N空位能够使空穴浓度降低,导致Mn 3d和N 2p轨道间的相互交换作用减小,从而减弱体系铁磁性.此外,Mn不同的掺杂浓度会影响GaMnN薄膜p-d耦合杂化能力的强弱,当掺Mn 1.8%时具有较强的p-d耦合杂化能力.     

Layer-heterogeneous magnetic states in metallic nanosystems

The formation of layer-heterogeneous periodic magnetic states in metallic systems is explained in terms of the dependence of the energy of itinerant electrons on the magnetic ordering of localized spins. The interaction of the local magnetic moments with conduction electrons with a certain spin projection is described by a set of spin-dependent δ-function potentials. A matrix method is developed permitting one to calculate the energy spectrum and the density of states of itinerant electrons in the presence of a layered magnetic heterogeneity. This method is used to explain oscillations of the interlayer exchange interaction in metallic magnetic superlattices and the stabilization of spin-density wave structures in transition metals and alloys.     

Phase diagram of a model for diluted magnetic semiconductors beyond mean-field approximations

A lattice spin-fermion model for diluted magnetic semiconductors (DMS) is investigated numerically, improving on previously used mean-field approximations. Curie temperatures are obtained varying the Mn spin x and hole n densities, and the impurity-hole exchange J in units of the hop-ping t. Optimal values are found in the subtle intermediate regime between itinerant and localized carriers. At intermediate and large J/t, a "clustered" state is observed above the Curie temperature and ferromagnetism is suppressed. Formal analogies between DMS and manganites are discussed.     

Spin-orbit coupling enhancement of 3d ions in metals

The interactions between localised 3d and itinerant electrons due to the Coulomb and exchange potential are shown to be responsible for the increase in magnitude of ionic spin-orbit coupling.     

Magnetocaloric and magnetic properties of La_2NiMnO_6 double perovskite

The magnetic effect and the magnetocaloric effect in La_2NiMnO_6(LNMO) double perovskite are studied using the Monte Carlo simulations.The magnetizations,specific heat values,and magnetic entropies are obtained for different exchange interactions and external magnetic fields.The adiabatic temperature is obtained.The transition temperature is deduced.The relative cooling power is established with a fixed value of exchange interaction.According to the master curve behaviors for the temperature dependence of △S_m~(max) predicted for different maximum fields,in this work it is confirmed that the paramagnetic-ferromagnetic phase transition observed for our sample is of a second order.The near room-temperature interaction and the superexchange interaction between Ni and Mn are shown to be due to the ferromagnetism of LNMO.