Colloidal free-standing Cr 3+ -doped In 2 O 3 nanocrystals were synthesized in oleylamine from indium (III) and chromium (III) acetylacetonate precursors. The nanocrystals were treated with trioctylphosphine oxide to remove surface-bound dopant ions and ensure internal doping. The lattice resolved transmission electron microscopy images reveal that nanocrystals are faceted and highly crystalline, with no evidence of a secondary phase formation. The average doping concentration estimated with energy dispersive X-ray spectroscopy at the single nanocrystal level agrees with the average doping concentration from the analogous nanocrystal ensemble measurement. Ligand-field electronic absorption spectroscopy suggests that Cr 3+ dopants are preferentially substituted for In 3+ ions in their trigonally distorted octahedral (b) sites in In 2 O 3 nanocrystals. Nanocrystalline films, prepared under mild conditions using colloidal Cr 3+ -doped In 2 O 3 nanocrystals as building blocks, exhibit robust room temperature ferromagnetism. Structural and compositional analyses combined with the ligand-field spectroscopy indicate intrinsic ferromagnetism in this material. The ability to rationally synthesize and manipulate a new form of transition-metal-doped In 2 O 3 nanocrystals opens up new opportunities for spintronics applications and may provide a framework for understanding the origin of ferromagnetism in transparent conducting oxides.
We report the first synthesis and characterization of cobalt- and chromium-doped GaN nanowires (NWs), and compare them to manganese-doped GaN NWs. Samples were synthesized by chemical vapor deposition method, using cobalt(II) chloride and chromium(III) chloride as dopant precursors. For all three impurity dopants hexagonal, triangular, and rectangular NWs were observed. The fraction of NWs having a particular morphology depends on the initial concentration of the dopant precursors. While all three dopant ions have the identical effect on GaN NW growth and faceting, Co and Cr are incorporated at much lower concentrations than Mn. These findings suggest that the doping mechanism involves binding of the transition-metal intermediates to specific NW facets, inhibiting their growth and causing a change in the NW morphology. We discuss the doping concentrations of Mn, Co, and Cr in terms of differences in their crystal-field stabilization energies (DeltaCFSE) in their gas-phase intermediates and in substitutionally doped GaN NWs. Using iron(III) chloride and cobalt(II) acetate as dopant precursors we show that the doping concentration dependence on DeltaCFSE allows for the prediction of achievable doping concentrations for different dopant ions in GaN NWs, and for a rational choice of a suitable dopant-ion precursor. This work further demonstrates a general and rational control of GaN NW growth using transition-metal impurities.
Multiferroics, materials that exhibit coupling between spontaneous magnetic and electric dipole ordering, have significant potential for high-density memory storage and the design of complex multistate memory elements. In this work, we have demonstrated the solvent-controlled synthesis of Cr(3+)-doped BaTiO(3) nanocrystals and investigated the effects of size and doping concentration on their structure and phase transformation using X-ray diffraction and Raman spectroscopy. The magnetic properties of these nanocrystals were studied by magnetic susceptibility, magnetic circular dichroism (MCD), and X-ray magnetic circular dichroism (XMCD) measurements. We observed that a decrease in nanocrystal size and an increase in doping concentration favor the stabilization of the paraelectric cubic phase, although the ferroelectric tetragonal phase is partly retained even in ca. 7 nm nanocrystals having the doping concentration of ca. 5%. The chromium(III) doping was determined to be a dominant factor for destabilization of the tetragonal phase. A combination of magnetic and magneto-optical measurements revealed that nanocrystalline films prepared from as-synthesized paramagnetic Cr(3+)-doped BaTiO(3) nanocrystals exhibit robust ferromagnetic ordering (up to ca. 2 μ(B)/Cr(3+)), similarly to magnetically doped transparent conducting oxides. The observed ferromagnetism increases with decreasing constituent nanocrystal size because of an enhancement in the interfacial defect concentration with increasing surface-to-volume ratio. Element-specific XMCD spectra measured by scanning transmission X-ray microscopy (STXM) confirmed with high spatial resolution that magnetic ordering arises from Cr(3+) dopant exchange interactions. The results of this work suggest an approach to the design and preparation of multiferroic perovskite materials that retain the ferroelectric phase and exhibit long-range magnetic ordering by using doped colloidal nanocrystals with optimized composition and size as functional building blocks.
Manganese-doped SnO2 nanocrystals and nanowires with diameters below SnO2 Bohr radius were synthesized by solution methods. X-ray absorption studies reveal that dopant ions are substitutionally incorporated as Mn2+ and Mn3+. Mn2+ is the dominant species at low doping levels, but the fraction of Mn3+ increases with doping concentration. Room-temperature ferromagnetism with the saturation moment of 0.27 μB/Mn is observed for nanocrystalline films containing high fraction of Mn2+ dopant, which is associated with hybridization of Mn2+ d-levels with a donor-impurity band. These results imply the possibility of manipulating magnetic interactions via dopant electronic structure and quantum confinement of the host lattice.
Thin films of niobium nitride are useful for their physical, chemical, and electrical properties. NbN superconducting properties have been utilized in a wide range of applications. Plasma-enhanced atomic layer deposition (PEALD) of NbN with (t-butylimido) tris(diethylamido) niobium(V) and remote H2/N2 plasmas has been investigated. Deposited film properties have been studied as a function of substrate temperature (100–300 °C), plasma power (150–300 W), and H2 flow rate (10–80 sccm). PEALD NbN films were characterized with spectroscopic ellipsometry (thickness, optical properties), four point probe (resistivity), x-ray photoelectron spectroscopy (composition), x-ray reflectivity (density and thickness), x-ray diffraction (crystallinity), and superconductivity measurements. Film composition varied with deposition conditions, but larger cubic NbN crystallites and increased film density at higher substrate temperatures and H2 flow rates lead to room temperature resistivity values as low as 173 μΩ cm and superconductivity critical temperatures as high as 13.7 K.
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