Direct Structural Identification and Quantification of the Split-Vacancy Configuration for Implanted Sn in Diamond.

We demonstrate formation of the ideal split-vacancy configuration of the Sn-vacancy center upon implantation into natural diamond. Using ß^{-} emission channeling following low fluence ^{121}Sn implantation (2×10^{12} atoms/cm^{2}, 60 keV) at the ISOLDE facility at CERN, we directly identified and quantified the atomic configurations of the Sn-related centers. Our data show that the split-vacancy configuration is formed immediately upon implantation with a surprisingly high efficiency of ≈40%. Upon thermal annealing at 920 °C ≈30% of Sn is found in the ideal bond-center position. Photoluminescence revealed the characteristic SnV^{-} line at 621 nm, with an extraordinarily narrow ensemble linewidth (2.3 nm) of near-perfect Lorentzian shape. These findings further establish the SnV^{-} center as a promising candidate for single photon emission applications, since, in addition to exceptional optical properties, it also shows a remarkably simple structural formation mechanism.

Local inhomogeneous state in multiferroic SmCrO3.

Rare-earth orthochromites with distorted perovskite structure (e.g. RCrO3, R = Sm, Gd) have been under strong debate with respect to the origin of their ferroelectric order. Of particular interest is the question of whether such orthochromites are, in fact, magnetically driven improper ferroelectrics, as many rare-earth manganites or orthoferrites. Here we show, by studying at the atomic scale the rare-earth SmCrO3 system that a distortion of the Sm local environment emerges within the paramagnetic phase, near room temperature. Our Electric Field Gradient measurements combined with first-principles calculations show that the emergent phase cannot be simply ascribed to the Pna21 structure as reported for GdCrO3 or SmCrO3. Instead a local inhomogeneous state, where regular non-polar and polar distorted environments coexist, develops at low temperatures.

Studying electronic properties in GaN without electrical contacts using γ-γ vs e--γ Perturbed Angular Correlations.

The potential use of combined e--γ vs γ-γ Perturbed Angular Correlations (PAC) experiments as a possible alternative to study electronic properties of materials and/or samples where Hall effect measurements are difficult to perform due to low-quality ohmic contacts is here demonstrated using Si- and Zn-doped GaN samples as a showcase example. To do so, the lattice site of implanted 181Hf/181Ta and the recombination of Ta ionized and excited electronic states were studied as a function of temperature and sample doping in GaN. By combining the γ-γ and e--γ PAC results with Density Functional Theory simulations, it was possible to assign a single stable site with a double-donor character for Ta in GaN. A metastable charge state was also identified at particular temperatures using e--γ PAC. A thermally activated process was observed for the electronic recombination at high temperatures with activation energies of 15(2) meV and 12(1) meV for the Si- and Zn-doped samples, respectively, and attributed to Si shallow donors present in both samples. A reduced number of available electrons was observed in the Zn-doped sample due to donor compensation by the Zn acceptors. At low temperatures, it is suggested that the recombination process occurs via Variable Range Hopping. The doping characteristics of both samples were successfully distinguished.

Lattice Location of Mg in GaN: A Fresh Look at Doping Limitations.

Radioactive ^{27}Mg (t_{1/2}=9.5 min) was implanted into GaN of different doping types at CERN's ISOLDE facility and its lattice site determined via ß^{-} emission channeling. Following implantations between room temperature and 800 °C, the majority of ^{27}Mg occupies the substitutional Ga sites; however, below 350 °C significant fractions were also found on interstitial positions ∼0.6 Å from ideal octahedral sites. The interstitial fraction of Mg was correlated with the GaN doping character, being highest (up to 31%) in samples doped p type with 2×10^{19} cm^{-3} stable Mg during epilayer growth, and lowest in Si-doped n-GaN, thus giving direct evidence for the amphoteric character of Mg. Implanting above 350 °C converts interstitial ^{27}Mg to substitutional Ga sites, which allows estimating the activation energy for migration of interstitial Mg as between 1.3 and 2.0 eV.

Hyperfine local probe study of alkaline-earth manganites SrMnO3 and BaMnO3.

We report perturbed angular correlation measurements with (111m)Cd/(111)Cd and (111)In/(111)Cd probes, at the ISOLDE-CERN facility, in the manganite compounds BaMnO3, with the 6H and 15R polymorphs, and SrMnO3, with the 4H polymorph. The electric field gradient (EFG) is measured, and found approximately constant in a large temperature range for all the compounds. The EFG is also calculated from first principles with density functional theory, and compared with experimental results by considering diluted substitutional Cd impurities. Based on the results, we assign as sites for the probes the Ba (for BaMnO3-6H, 15R) and Sr (for SrMnO3-4H) sites, apart from fractions of undetermined origin in the case of BaMnO3-6H. We predict the hyperfine parameters in the recently synthesized multiferroic manganite Sr(0.5)Ba(0.5)MnO3, and its variation with the structure and electric polarization, which is found to be very small.

Paramagnetism and antiferromagnetic interactions in single-phase Fe-implanted ZnO.

As the intrinsic origin of the high-temperature ferromagnetism often observed in wide-gap dilute magnetic semiconductors becomes increasingly debated, there is a growing need for comprehensive studies on the single-phase region of the phase diagram of these materials. Here we report on the magnetic and structural properties of Fe-doped ZnO prepared by ion implantation of ZnO single crystals. A detailed structural characterization shows that the Fe impurities substitute for Zn in ZnO in a wurtzite Zn(1-x)Fe(x)O phase which is coherent with the ZnO host. In addition, the density of beam-induced defects is progressively decreased by thermal annealing up to 900 ° C, from highly disordered after implantation to highly crystalline upon subsequent annealing. Based on a detailed analysis of the magnetometry data, we demonstrate that isolated Fe impurities occupying Zn-substitutional sites behave as localized paramagnetic moments down to 2 K, irrespective of the Fe concentration and the density of beam-induced defects. With increasing local concentration of Zn-substitutional Fe, strong nearest-cation-neighbor antiferromagnetic interactions favor the antiparallel alignment of the Fe moments.

Jahn-Teller distortion relaxation across the LaMnO3+Δ phase diagram.

The evolution of the local Jahn-Teller distortion across the LaMnO3+Δ phase diagram was obtained using the perturbed angular correlation local probe technique. We found that upon doping, the local distortion decreases continuously with increasing doping and that no fully Jahn-Teller distorted Mn(3+)O6 octahedra are observed within the orthorhombic insulating phase. A local single-phase scenario is established for the orbital disordered orthorhombic crystallographic structure. We also show that the continuous weakening of the Jahn-Teller distortions is not limited to a single-phase environment and occurs in a similar manner within an undistorted rhombohedric matrix upon lowering the temperature.

A versatile apparatus for on-line emission channeling experiments.

The concept and functionality of an apparatus dedicated to emission channeling experiments using short-lived isotopes on-line at ISOLDE∕CERN is described. The setup is assembled in two functional blocks - (a) base stand including beam collimation, implantation and measurement chamber, cryogenic extension, and vacuum control system and (b) Panmure goniometer extension including maneuvering cradle and sample heating furnace. This setup allows for in situ implantation and sample analysis in the as-implanted state and upon cooling down to 50 K and during annealing up to 1200 K. The functionality of the setup will be illustrated with the example of establishing the lattice location of (56)Mn probes implanted into GaAs.

Tunning pore filling of anodic alumina templates by accurate control of the bottom barrier layer thickness.

The role of the alumina barrier layer thickness (δ(b)) on the growth of Ni nanowires (NWs) in porous anodic alumina (PAA) has been revealed. By varying the final anodization voltage to form dendrites at the bottom of the nanoporous structure, we are able to optimize δ(b) (in the 2-16 nm range), allowing us to obtain a Ni pore filling percentage (f(p)) of almost 100% for δ(b) = 10 nm. However, deviations from this optimal δ(b)-value led to a strong decrease of f(p). Moreover, an increase of the electrodeposition efficiency (EE) and NW homogeneity was also verified for δ(b) up to 10 nm. Such increase in nominal δ(b) leads to a consistent growth rate in all pores and consequently a complete and uniform nanopore filling. On the other hand, the decrease in electrodeposition efficiency visible for δ(b) > 10 nm is related with hydrogen evolution and dielectric breakdown of the insulator layer due to the required high deposition voltages. Non-uniform NW growth is then visible, with the consequent decrease in f(p). The control of the pore filling and length homogeneity of the fabricated 1D metallic nanostructures, combined with the ability to adjust the pore dimensions of PAA, can bring novel approaches for the fabrication of nano-objects and thus exciting new applications.

Rapid synthesis of ordered manganite nanotubes by microwave irradiation in alumina templates.

Highly ordered La2/3Ca1/3MnO3 nanotube arrays were successfully synthesized by a simple and rapid process, combining nanoporous alumina template-assisted synthesis with microwave irradiation. The method offers a quick hands-on route to produce manganite bulk sample and nanotube arrays at relative low-temperatures. We obtain thin wall nanotubes of uniform diameter of 80 nm. The growth mechanism of nanotubes is briefly discussed. Magnetic measurements indicate that the ferromagnetic transition temperature T(c) of the nanotubes is depleted with respect to its bulk counterpart possibly due to the geometric confinement imposed by the thin wall of the nanotubes.

Transition metal impurities on the bond-centered site in germanium.

We report on the lattice location of ion implanted Fe, Cu, and Ag impurities in germanium from a combined approach of emission channeling experiments and ab initio total energy calculations. Following common expectation, a fraction of these transition metals (TMs) was found on the substitutional Ge position. Less expected is the observation of a second fraction on the sixfold coordinated bond-centered site. Ab initio calculated heats of formation suggest this is the result of the trapping of a vacancy by a substitutional TM impurity, spontaneously forming an impurity-vacancy complex in the split-vacancy configuration. We also present an approach to displace the TM impurities from the electrically active substitutional site to the bond-centered site.

New phase transition in the Pr1-xCaxMnO3 system: evidence for electrical polarization in charge ordered manganites.

In this Letter a detailed study of the electric field gradient (EFG) across the Pr(1-x)Ca(x)MnO(3) phase diagram and its temperature dependence is given. Clearly, distinct EFG behavior for samples outside or inside the charge order (CO) region are observed. The EFG temperature dependence evidences a new phase transition occurring over the broad CO region of the phase diagram. This transition is discontinuous and occurs at temperatures between the charge ordering and the Néel temperatures. The prominent features observed in the EFG are associated with polar atomic vibrations which eventually lead to a spontaneous local electric polarization below CO transition.

Direct evidence for As as a Zn-site impurity in ZnO.

Arsenic has been reported in the literature as one of the few p-type dopants in the technologically promising II-VI semiconductor ZnO. However, there is an ongoing debate whether the p-type character is due to As simply replacing O atoms or to the formation of more complicated defect complexes, possibly involving As on Zn sites. We have determined the lattice location of implanted As in ZnO by means of conversion-electron emission channeling from radioactive (73)As. In contrast to what one might expect from its nature as a group V element, we find that As does not occupy substitutional O sites but in its large majority substitutional Zn sites. Arsenic in ZnO (and probably also in GaN) is thus an interesting example for an impurity in a semiconductor where the major impurity lattice site is determined by atomic size and electronegativity rather than its position in the periodic system.

Feasibility of a novel design of high resolution parallax-free Compton enhanced PET scanner dedicated to brain research.

A novel concept for a positron emission tomography (PET) camera module is proposed, which provides full 3D reconstruction with high resolution over the total detector volume, free of parallax errors. The key components are a matrix of long scintillator crystals and hybrid photon detectors (HPDs) with matched segmentation and integrated readout electronics. The HPDs read out the two ends of the scintillator package. Both excellent spatial (x, y, z) and energy resolution are obtained. The concept allows enhancing the detection efficiency by reconstructing a significant fraction of events which underwent Compton scattering in the crystals. The proof of concept will first be demonstrated with yttrium orthoaluminate perovskite (YAP):Ce crystals, but the final design will rely on other scintillators more adequate for PET applications (e.g. LSO:Ce or LaBr3:Ce). A promising application of the proposed camera module, which is currently under development, is a high resolution 3D brain PET camera with an axial field-of-view of approximately 15 cm dedicated to brain research. The design philosophy and performance predictions based on analytical calculations and Monte Carlo simulations are presented. Image correction and reconstruction tools required to operate this transmissionless device in a research environment are also discussed. Better or similar performance parameters were obtained compared to other known designs at lower fabrication cost. The axial geometrical concept also seems to be promising for applications such as positron emission mammography.