We present a detailed investigation of the magnetic and magnetotransport properties of thin films of ferromagnetic Ga1-xMnxAs synthesized using ion implantation and pulsed-laser melting (II-PLM). The field and temperature-dependent magnetization, magnetic anisotropy, temperature-dependent resistivity, magnetoresistance, and Hall effect of II-PLM Ga1-xMnxAs films have all of the characteristic signatures of the strong p-d interaction of holes and Mn ions observed in the dilute hole-mediated ferromagnetic phase. The ferromagnetic and electrical transport properties of II-PLM films correspond to the peak substitutional Mn concentration meaning that the non-uniform Mn depth distribution is unimportant in determining the film properties. Good quantitative agreement is found with films grown by low temperature molecular beam epitaxy (LT-MBE) and having the similar substitutional Mn_Ga composition. Additionally, we demonstrate that II-PLM Ga1-xMnxAs films are free from interstitial Mn_I because of the high temperature processing. At high Mn implantation doses the kinetics of solute redistribution during solidification alone determine the maximum resulting Mn_Ga concentration. Uniaxial anisotropy between in-plane [-110]and [110] directions is present in II-PLM Ga1-xMnxAs giving evidence for this being an intrinsic property of the carrier-mediated ferromagnetic phase.
We have studied the evolution of the magnetic, electronic, and structural properties of annealed epilayers of Ga1-xMnxAs grown by low temperature molecular beam epitaxy. Annealing at the optimal temperature of 250 C for less than 2 hours significantly enhances the conductivity and ferromagnetism, but continuing the annealing for longer times suppresses both. These data indicate that such annealing induces the defects in Ga1-xMnxAs to evolve through at least two different processes, and they point to a complex interplay between the different defects and ferromagnetism in this material.
We have investigated the effect of partial isovalent anion substitution in Ga1-xMnxAs on electrical transport and ferromagnetism. Substitution of only 2.4% of As by P induces a metal-insulator transition at a constant Mn doping of x=0.046 while the replacement of 0.4 % As with N results in the crossover from metal to insulator for x=0.037. This remarkable behavior is consistent with a scenario in which holes located within an impurity band are scattered by alloy disorder in the anion sublattice. The shorter mean free path of holes, which mediate ferromagnetism, reduces the Curie temperature TC…
We have investigated the transport and magnetization characteristics of Ga1-xMnxAs intentionally compensated with shallow Te donors. Using ion implantation followed by pulsed-laser melting, we vary the Te compensation and drive the system through a metal-insulator transition (MIT). This MIT is associated with enhanced low-temperature magnetization and an evolution from concave to convex temperature-dependent magnetization.
We have synthesized Ga1-xMnxAs1-yPy and Ga1-xMnxP1-yNy by the combination of ion implantation and pulsed-laser melting. We find that the incorporation of isovalent impurities with smaller atomic radii leads to a realignment of the magnetic easy axis in Ga1-xMnxP1-yNy/GaP and Ga1-xMnxAs1-yPy/GaAs thin films from in-plane to out-of-plane. This tensile-strain-induced magnetic anisotropy is reminiscent of that observed in Ga1-xMnxAs grown on larger lattice constant (In,Ga)As buffer layers indicating that the role of strain in determining magnetic anisotropy is fundamental to III-Mn-V materials. In…
Ferromagnetic properties of In1-xMnxAs thin films were investigated. Room temperature ferromagnetic order was observed in nominally single-phase films with x = 0.01-0.10. Magnetization measurements indicated that these In1-xMnxAs samples had a Curie temperature of 333 K. The Curie temperature was independent of Mn concentration. The temperature dependent magnetization along with the magnitude of the saturation magnetization and microstructural data indicate that the source of the high-temperature ferromagnetism in single-phase films is not attributable to MnAs nanoprecipitates. The high transi…
We present the systematic study of the resonant tunneling spectroscopy on a series of ferromagnetic-semiconductor Ga1-xMnxAs with the Mn content x from ~0.01 to 3.2%. The Fermi level of Ga1-xMnxAs exists in the band gap in the whole x region. The Fermi level is closest to the valence band (VB) at x=1.0% corresponding to the onset of ferromagnetism near the metal-insulator transition (MIT), but it moves away from the VB as x increasing or decreasing from 1.0%. This anomalous behavior of the Fermi level indicates that the ferromagnetism and MIT emerge in the Mn-derived impurity band.
We report the magnetic and transport properties of Ga1-xMnxP synthesized via ion implantation followed by pulsed laser melting over a range of x, namely 0.018 to 0.042. Like Ga1-xMnxAs, Ga1-xMnxP displays a monotonic increase of the ferromagnetic Curie temperature with x associated with the hole-mediated ferromagnetic phase while thermal annealing above 300 C leads to a quenching of ferromagnetism that is accompanied by a reduction of the substitutional fraction of Mn. However, contrary to observations in Ga1-xMnxAs, Ga1-xMnxP is non-metallic over the entire composition range. At the lower tem…
High- and low-field magneto-transport measurements, as well as SQUID measurements of magnetization, were carried out on Ga1-xMnxAs epilayers grown by low temperature molecular beam epitaxy, and subsequently annealed under various conditions. We observe a large enhancement of ferromagnetism when the samples are annealed at an optimal temperature, typically about 280 0C. Such optimal annealing leads to an increase of Curie temperature, accompanied by an increase of both the conductivity and the saturation magnetization. A decrease of the coercive field and of magnetoresistivity is also observed …
We demonstrate two patterning techniques based on hydrogen passivation of Ga1-xMnxAs to produce isolated ferromagnetically active regions embedded uniformly in a paramagnetic, insulating host. The first method consists of selective hydrogenation of Ga1-xMnxAs by lithographic masking. Magnetotransport measurements of Hall-bars made in this manner display the characteristic properties of the hole-mediated ferromagnetic phase, which result from good pattern isolation. Arrays of Ga1-xMnxAs dots as small as 250 nm across have been realized by this process. The second process consists of blanket hyd…
Ion implantation of Mn combined with pulsed laser melting is employed to obtain two representative compounds of dilute ferromagnetic semiconductors (DFSs): Ga1-xMnxAs and In1-xMnxAs. In contrast to films deposited by the widely used molecular beam epitaxy, neither Mn interstitials nor As antisites are present in samples prepared by the method employed here. Under these conditions the influence of localization on the hole-mediated ferromagnetism is examined in two DFSs with a differing strength of p-d coupling. On the insulating side of the transition, ferromagnetic signatures persist to higher…
In1-xMnxAs diluted magnetic semiconductor (DMS) thin films have been grown using metalorganic vapor phase epitaxy (MOVPE). Tricarbonyl(methylcyclopentadienyl)manganese was used as the Mn source. Nominally single-phase, epitaxial films were achieved with Mn content as high as x=0.14 using growth temperatures Tg>475 C. For lower growth temperatures and higher Mn concentrations, nanometer scale MnAs precipitates were detected within the In1-xMnxAs matrix. Magnetic properties of the films were investigated using a superconducting quantum interference device (SQUID) magnetometer. Room-temperature f…
Unexpected ferromagnetism has been observed in carbon doped ZnO films grown by pulsed laser deposition [Phys. Rev. Lett. 99, 127201 (2007)]. In this letter, we introduce carbon into ZnO films by ion implantation. Room temperature ferromagnetism has been observed. Our analysis demonstrates that (1) C-doped ferromagnetic ZnO can be achieved by an alternative method, i.e. ion implantation, and (2) the chemical involvement of carbon in the ferromagnetism is indirectly proven.
The microstructure of (In,Mn)As thin films grown using metalorganic vapor phase epitaxy (MOVPE) was investigated to determine the origin of room temperature ferromagnetism in these films. Transmission electron microscopy (TEM) based techniques were used to investigate phase purity and compositional homogeneity. Microanalysis of an In1-xMnxAs film with x = 0.01 and a Curie temperature of 330 K exhibited a homogeneous distribution of Mn. High Mn concentration films with x = 0.20 exhibited MnAs precipitates within the (In,Mn)As matrix. The analysis indicates that room temperature ferromagnetic, s…
We employ Faraday and Kerr effect spectroscopy in the infrared range to investigate the electronic structure of Ga1-xMnxAs near the Fermi energy. The band structure of this archetypical dilute-moment ferromagnetic semiconductor has been a matter of controversy, fueled partly by previous measurements of the unpolarized infrared absorption and their phenomenological impurity-band interpretation. The infrared magneto-optical effects we study arise directly from the spin-splitting of the carrier bands and their chiral asymmetry due to spin-orbit coupling. Unlike the unpolarized absorption, they ar…
The electronic structure of a prototype dilute magnetic semiconductor (DMS), Ga1-xMnxAs, is studied by magnetic circular dichroism (MCD) spectroscopy. We prove that the optical transitions originated from impurity bands cause the strong positive MCD background. The MCD signal due to the E0 transition from the valence band to the conduction band is negative indicating that the p-d exchange interactions between the p-carriers and d-spin is antiferromagnetic. The negative E0 MCD signal also indicates that the hole-doping of the valence band is not so large as previously assumed. The impurity band…
The structural and magnetic properties of V doped ZnO are presented. V ions were introduced into hydrothermal ZnO single crystals by ion implantation with fluences of 1.2*10^16 to 6*10^16 cm^-2. Post-implantation annealing was performed in high vacuum from 823 K to 1023 K. The ZnO host material still partly remains in a crystalline state after irradiation, and is partly recovered by annealing. The V ions show a thermal mobility as revealed by depth profile Auger electron spectroscopy. Synchrotron radiation x-ray diffraction revealed no secondary phase formation which indicates the substitution…
Ferromagnetic InMnAs has been prepared by Mn ion implantation and pulsed laser annealing. The InMnAs layer reveals a saturated magnetization of 2.6 mu_B/Mn at 5 K and a perpendicular magnetic anisotropy. The Curie temperature is determined to be 46 K, which is higher than those in previous reports with similar Mn concentrations. Ferromagnetism is further evidenced by the large magnetic circular dichroism.
In the last decade, transition-metal-doped ZnO has been intensively investigated as a route to room-temperature diluted magnetic semiconductors (DMSs). However, the origin for the reported ferromagnetism in ZnO-based DMS remains questionable. Possible options are diluted magnetic semiconductors, spinodal decomposition, or secondary phases. In order to clarify this question, we have performed a thorough characterization of the structural and magnetic properties of Co- and Ni-implanted ZnO single crystals. Our measurements reveal that Co or Ni nanocrystals (NCs) are the major contribution of the…
In the present work, we have prepared Mn-doped Ge using different annealing approaches after Mn ion implantation, and obtained samples with hole concentrations ranging from 10^18 to 2.1x10^20 cm^-3, the latter being the highest reported so far. Based on the magnetotransport properties of Mn doped Ge, we argue that the hole concentration is a decisive parameter in establishing carrier-mediated ferromagnetism in magnetic Ge.
We report the fabrication of Ge:Mn ferromagnetic semiconductors by Mn-ion implantation into Ge followed by pulsed laser annealing. Benefiting from the short time annealing, the hole concentration in Mn-implanted Ge has been increased by two orders of magnitude from 10$^{18}$ to over 10$^{20}$ cm$^{-3}$. Likely due to the high hole concentration, we observe that the longitudinal and Hall resistances exhibit the same hysteresis as the magnetization, which is usually considered as a sign of carrier-mediated ferromagnetism.
Ferromagnetic ordering is reported in the post-annealed samples of Co doped n-GaN formed by Co+ implantation. A maximum Curie temperature ~ 250K is recorded for the sample with 8 atomic percent Co. Particle induced x-ray emission-channeling study confirmed the substitutional Co in Ga lattice site. Local atomic arrangement around magnetic impurities is also analyzed using Raman study. A disordered model with carrier mediated coupling of localized magnetic moments is made responsible for the observed ferromagnetic ordering.
Heavily-alloyed, 100 nm Ga1-xMnxAs (x>0.1) films are obtained via low temperature molecular beam epitaxy utilizing a combinatorial technique which allows systematic control of excess arsenic during growth. Reproducible, optimized electronic, magnetic and structural properties are found in a narrow range of stoichiometric growth conditions. The Curie temperature of stoichiometric material is 150-165 K and independent of x within a large window of growth conditions while substitutional Mn content increases linearly, contradicting the prediction of the Zener Model of hole-mediated ferromagnetism.
We have prepared the dilute magnetic semiconductor (DMS) InMnAs with different Mn concentrations by ion implantation and pulsed laser melting. The Curie temperature of the In1-xMnxAs epilayer depends on the Mn concentration x, reaching 82 K for x=0.105. The substitution of Mn ions at the Indium sites induces a compressive strain perpendicular to the InMnAs layer and a tensile strain along the in-plane direction. This gives rise to a large perpendicular magnetic anisotropy, which is often needed for the demonstration of electrical control of magnetization and for spin-transfer-torque induced ma…
We review pitfalls in recent efforts to make a conventional semiconductor, namely ZnO, ferromagnetic by means of doping with transition metal ions. Since the solubility of those elements is rather low, formation of secondary phases and the creation of defects upon low temperature processing can lead to unwanted magnetic effects. Among others, ion implantation is a method of doping, which is highly suited for the investigation of those effects. By focussing mainly on Fe, Co or Ni implanted ZnO single crystals we show that there are manifold sources for ferromagnetism in this material which can …
We report the structural and magnetic properties of ZnO single crystals implanted at 623 K with up to 10 at. % of Ni. As revealed by X-ray diffraction, crystalline fcc-Ni nanoparticles were formed inside ZnO. The magnetic behavior (magnetization with field reversal and with different temperature protocol) of all samples is well explained by a magnetic Ni-nanoparticle system. Although the formation of Ni:ZnO based diluted magnetic semiconductor cannot be ruled out, the major contribution to the magnetic properties stems from crystalline nanoparticles synthesized under these implantation conditi…
We report on structural, magnetic and electronic properties of Co-implanted TiO2 rutile single crystals for different implantation doses. Strong ferromagnetism at room temperature and above is observed in TiO2 rutile plates after cobalt ion implantation, with magnetic parameters depending on the cobalt implantation dose. While the structural data indicate the presence of metallic cobalt clusters, the multiplet structure of the Co L3 edge in the XAS spectra gives clear evidence for a substitutional Co 2+ state. The detailed analysis of the structural and magnetic properties indicates that there…
We have studied the structural, magnetic and electronic properties of Co-implanted ZnO (0001) films grown on Al2O3 (1120) substrates for different implantation doses and over a wide temperature range. Strong room temperature ferromagnetism is observed with magnetic parameters depending on the cobalt implantation dose. A detailed analysis of the structural and magnetic properties indicates that there are two magnetic phases in Co-implanted ZnO films. One is a ferromagnetic phase due to the formation of long range ferromagnetic ordering between implanted magnetic cobalt ions in the ZnO layer, th…
We have synthesized ferromagnetic InMnP, a member of III-Mn-V ferromagnetic semiconductor family, by Mn ion implantation and pulsed laser annealing. Clear ferromagnetic hysteresis loops and a perpendicular magnetic anisotropy are observed up to a Curie temperature of 42 K. Large values of negative magnetoresistance and magnetic circular dichroism as well as anomalous Hall effect are further evidences of a ferromagnetic order in InMnP. An effort is made to understand the transport mechanism in InMnP using the theoretical models. We find that the valence band of InP does not merge with the impur…
Nowadays ferromagnetism is often found in potential diluted magnetic semiconductor systems. However, many authors argue that the observed ferromagnetism stems from ferromagnetic precipitates or spinodal decomposition rather than from carrier mediated magnetic impurities, as required for a diluted magnetic semiconductor. In the present paper we answer this question for Fe-implanted ZnO single crystals comprehensively. Different implantation fluences and temperatures and post-implantation annealing temperatures have been chosen in order to evaluate the structural and magnetic properties over a w…
The discovery of ferromagnetism in Mn doped GaAs [1] has ignited interest in the development of semiconductor technologies based on electron spin and has led to several proof-of-concept spintronic devices [2-4]. A major hurdle for realistic applications of (Ga,Mn)As, or other dilute magnetic semiconductors, remains their below room-temperature ferromagnetic transition temperature. Enhancing ferromagnetism in semiconductors requires understanding the mechanisms for interaction between magnetic dopants, such as Mn, and identifying the circumstances in which ferromagnetic interactions are maximiz…
For the prototype diluted ferromagnetic semiconductor (Ga,Mn)As, there is a fundamental concern about the electronic states near the Fermi level, i.e., whether the Fermi level resides in a well-separated impurity band derived from Mn doping (impurity-band model) or in the valence band that is already merged with the Mn-derived impurity band (valence-band model). We investigate this question by carefully shifting the Fermi level by means of carrier compensation. We use helium-ion implantation, a standard industry technology, to precisely compensate the hole doping of GaAs-based diluted ferromag…
Ion implantation of Mn ions into hole-doped GaP has been used to induce ferromagnetic behavior above room temperature for optimized Mn concentrations near 3 at.%. The magnetism is suppressed when the Mn dose is increased or decreased away from the 3 at.% value, or when n-type GaP substrates are used. At low temperatures the saturated moment is on the order of one Bohr magneton, and the spin wave stiffness inferred from the Bloch-law T^3/2 dependence of the magnetization provides an estimate Tc = 385K of the Curie temperature that exceeds the experimental value, Tc = 270K. The presence of ferro…
Room-temperature ferromagnetism has been induced within ZnO single crystals by implant-doping with Fe ions. For an implantation temperature of 620 K and an ion fluence of 4x10^16 cm^-2, very tiny Fe particles, formed inside the host matrix, are responsible for the ferromagnetic properties. They were identified using synchrotron X-ray diffraction and Moessbauer spectroscopy. On the other hand, Fe ions implanted at a temperature of 253 K and an ion fluence of 4x10^15 cm^-2 are incorporated into the host matrix and develop a room temperature diluted magnetic semiconductor (DMS).
We report on the formation of the dilute $Pd_{1-x}Fe_x$ compositions with tunable magnetic properties under an ion-beam implantation of epitaxial Pd thin films. Binary $Pd_{1-x}Fe_x$ alloys with a mean iron content $x$ of $0.025$, $0.035$ or $0.075$ were obtained by the implantation of $40 keV$ $Fe^+$ ions into the palladium films on MgO (001) substrate to the doses of $0.5\cdot10^{16}, 1.0\cdot10^{16}$ and $3.0\cdot10^{16}$ $ions/cm^2$, respectively. Structural and magnetic studies have shown that iron atoms occupy regular fcc-lattice Pd-sites without the formation of any secondary crystallog…
