Unraveling the nature of carrier mediated ferromagnetism in diluted magnetic semiconductors

After more than a decade of intensive research in the field of diluted magnetic semiconductors (DMS), the nature and origin of ferromagnetism, especially in III-V compounds is still controversial. Many questions and open issues are under intensive debates. Why after so many years of investigations Mn doped GaAs remains the candidate with the highest Curie temperature among the broad family of III-V materials doped with transition metal (TM) impurities ? How can one understand that these temperatures are almost two orders of magnitude larger than that of hole doped (Zn,Mn)Te or (Cd,Mn)Se? Is there any intrinsic limitation or is there any hope to reach in the dilute regime room temperature ferromagnetism? How can one explain the proximity of (Ga,Mn)As to the metal-insulator transition and the change from Ruderman-Kittel-Kasuya-Yosida (RKKY) couplings in II-VI compounds to double exchange type in (Ga,Mn)N? In spite of the great success of density functional theory based studies to provide accurately the critical temperatures in various compounds, till very lately a theory that provides a coherent picture and understanding of the underlying physics was still missing. Recently, within a minimal model it has been possible to show that among the physical parameters, the key one is the position of the TM acceptor level. By tuning the value of that parameter, one is able to explain quantitatively both magnetic and transport properties in a broad family of DMS. We will see that this minimal model explains in particular the RKKY nature of the exchange in (Zn,Mn)Te/(Cd,Mn)Te and the double exchange type in (Ga,Mn)N and simultaneously the reason why (Ga,Mn)As exhibits the highest critical temperature among both II-VI and III-V DMS.Comment: 6 figures. To appear in Comptes Rendus de l'Acad\'emie des Sciences (2015

Why RKKY exchange integrals are inappropriate to describe ferromagnetism in diluted magnetic semiconductors

We calculate Curie temperatures and study the stability of ferromagnetism in diluted magnetic materials, taking as a model for the exchange between magnetic impurities a damped Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction and a shor t range term representing the effects of superexchange. To properly include effects of spin and thermal fluctuations as well as geometric disorder, we solve the effective Heisenberg Hamiltonian by means of a recently developed semi-analytical approach. This approach, ``self-consistent local Random Phase Approximation (SC-L RPA)'', is explained. We show that previous mean-field treatments, which have been widely used in the literature, largely overestimate both the Curie temperatures and the stability of ferromagnetism as a function of carrier density. The discr epancy when compared to the current approach was that effects of frustration in RKKY oscillations had been strongly underestimated by such simple mea n-field theories. We argue that the use, as is frequent, of a weakly-disordered RKKY exchange to model ferromagnetism in diluted III-V systems is inconsistent with the observation of ferromagnetism over a wide region of itinerant carrier densities. This may be puzzling when compared to the apparent success of calculations based on {\it ab-initio} estimates of the coupling; we propose a resolution to this issue by taking RKKY-like interactions between resonant states close to the Fermi level.Comment: Accepted for publication in Physical Review B. 22 pages, 7 figure

Optical conductivity of Mn doped GaAs

We study the optical conductivity in the III-V diluted magnetic semiconductor GaMnAs and compare our calculations to available experimental data. Our model study is able to reproduce both qualitatively and quantitatively the observed measurements. We show that compensation (low carrier density) leads, in agreement to the observed measurements to a red shift of the broad peak located at approximately 200 meV for the optimally annealed sample. The non perturbative treatment appears to be essential, otherwise a blueshift and an incorrect amplitude would be obtained. By calculating the Drude weight (order parameter) we establish the metal-insulator phase diagram. We indeed find that Mn doped GaAs is close to the metal-insulator transition and that for 5$$ and 7$$ doped samples, 20$$ of the carriers only are delocalized. We have found that the optical mass is approximately 2 m$_{e}$. We have also interesting results for overdoped samples which could be experimentally realized by Zn codoping.Comment: the manuscript has been extended, new figures are include

Spontaneous magnetization in presence of nanoscale inhomogeneities in diluted magnetic systems

The presence of nanoscale inhomogeneities has been experimentally evidenced in several diluted magnetic systems, which in turn often leads to interesting physical phenomena. However, a proper theoretical understanding of the underlying physics is lacking in most of the cases. Here we present a detailed and comprehensive theoretical study of the effects of nanoscale inhomogeneities on the temperature dependent spontaneous magnetization in diluted magnetic systems, which is found to exhibit an unusual and unconventional behavior. The effects of impurity clustering on the magnetization response have hardly been studied until now. We show that nanosized clusters of magnetic impurities can lead to drastic effects on the magnetization compared to that of homogeneously diluted compounds. The anomalous nature of the magnetization curves strongly depends on the relative concentration of the inhomogeneities as well as the effective range of the exchange interactions. In addition we also provide a systematic discussion of the nature of the distributions of the local magnetization.Comment: 18 pages, 9 figures, 4 new references added and Text modified to match the published versio

Nanoscale inhomogeneities: A new path toward high Curie temperature ferromagnetism in diluted materials

Room temperature ferromagnetism has been one of the most sought after topics in today's emerging field of spintronics. It is strongly believed that defect- and inhomogeneity- free sample growth should be the optimal route for achieving room-temperature ferromagnetism and huge efforts are made in order to grow samples as "clean" as possible. However, until now, in the dilute regime it has been difficult to obtain Curie temperatures larger than that measured in well annealed samples of (Ga,Mn)As ($\sim$190 K for 12% doping). In the present work, we propose an innovative path to room-temperature ferromagnetism in diluted magnetic semiconductors. We theoretically show that even a very small concentration of nanoscale inhomogeneities can lead to a tremendous boost of the critical temperatures: up to a 1600% increase compared to the homogeneous case. In addition to a very detailed analysis, we also give a plausible explanation for the wide variation of the critical temperatures observed in (Ga,Mn)N and provide a better understanding of the likely origin of very high Curie temperatures measured occasionally in some cases. The colossal increase of the ordering temperatures by nanoscale cluster inclusions should open up a new direction toward the synthesis of materials relevant for spintronic functionalities.Comment: 16 pages, 4 figures, New references added and Text revised to match the accepted versio

Reconsidering the possibility of room temperature ferromagnetism in Mn doped Zirconium oxide

The possibility to induce long range ferromagnetic order by doping oxides with transition metal ions has become a very exciting challenge in the last decade. Theoretically, it has been claimed that Mn doped ZrO$_2$ could be a very promising spintronic candidate and that high critical temperatures could be already achieved even for a low Mn concentration. Some experiments have reported room temperature ferromagnetism (RT-FM) whilst some others only paramagnetism. When observed, the nature of RT-FM appears to be controversial and not clearly understood. In this study, we propose to clarify and shed light on some of theses existing issues. A detailed study of the critical temperatures and low energy magnetic excitations in Mn doped ZrO$_2$ is performed. We show that the Curie temperatures were largely overestimated previously, due to the inadequate treatment of both thermal and transverse fluctuations, and disorder. It appears that the Mn-Mn couplings can not explain the observed RT-FM. We argue, that this can be attributed to the interaction between large moments induced in the vicinity of the manganese. This is similar to the non-magnetic defect induced ferromagnetism reported in oxides, semiconductors and graphene/graphite.Comment: 13 pages, 7 figures, to appear in EP

Dynamical properties of a three-dimensional diluted Heisenberg model

We study the magnetic excitation spectrum in three-dimensional diluted ferromagnetic nearest-neighbor systems down to the percolation threshold. The disorder effects resulting from the dilution are handled accurately within self-consistent local random phase approximation approach. The calculations are performed using relatively large systems containing typically 20 000 localized spins, a systematic average over many configurations of disorder is performed. We analyze in details the change in the magnon spectrum and magnon density of states as we increase the dilution. The zone of stability of the well-defined magnon modes is shown to shrink drastically as we approach the percolation threshold. We also calculate the spin stiffness which appears to vanish at the percolation threshold exactly. A comparison with available data, based on a different theoretical approach, is also provided. We hope that this study will motivate new experimental studies based on inelastic neutron-scattering measurements.Comment: 5 pages, 5 figure