A detailed study of depth-resolved magnetization and microstructure of Fe16N2 thin films on MgO (001) and MgAl2O4 (001) substrates and Fe and Cr seed layers is presented. Two aspects of the magnetic properties of Fe16N2 thin films are discussed. First, magnetization enhancement at the interface is observed. Strain and nitrogen deficiency are discussed as possible interfacial mechanisms contributing to this enhancement. Second, the perpendicularly magnetized component (PMC) is identified in Fe16N2 thin films. Correlation with microstructural observations suggests that the PMC is associated with V-shaped grains that are not fully confined within the continuous Fe16N2 layer.

“Magic-sized” nanocrystals (MSNCs) grow in discrete jumps between a series of specific sizes. Consequently, MSNCs have been explored as an alternative route to uniform semiconductor particles, potentially with atomic precision. However, because the growth mechanism has been poorly understood, the best strategies to control MSNC syntheses and obtain desired sizes are unknown. Experiments have found that common parameters such as growth time and temperature have limited utility. Here, we theoretically and experimentally investigate reactant supersaturation as a tool to control MSNC growth. We compare direct synthesis of CdSe MSNCs with ripening of isolated MSNCs or their mixtures. Surprisingly, we find that MSNCs readily synchronize to the same growth trajectory, even starting from distinct initial conditions, explaining the robustness of MSNC growth. Further, by understanding the synchronization mechanism, we demonstrate methods to control the final MSNC size. These results deepen our knowledge of MSNCs and indicate strategies to tailor their growth.

Gamma alumina (γ-Al2O3) is widely used as a catalyst and catalytic support due to its high specific surface area and porosity. However, synthesis of γ-Al2O3 nanocrystals is often a complicated process requiring high temperatures or additional post-synthetic steps. Here, we report a single-step synthesis of size-controlled and monodisperse, facetted γ-Al2O3 nanocrystals in an inductively coupled nonthermal plasma reactor using trimethylaluminum and oxygen as precursors. Under optimized conditions, we observed phase-pure, cuboctahedral γ-Al2O3 nanocrystals with defined surface facets. Nuclear magnetic resonance studies revealed that nanocrystal surfaces are populated with AlO6, AlO5 and AlO4 units with clusters of hydroxyl groups. Nanocrystal size tuning was achieved by varying the total reactor pressure yielding particles as small as 3.5 nm, below the predicted thermodynamic stability limit for γ-Al2O3.

Magnetic doping of topological quantum materials provides an attractive route for studying the effects of time-reversal symmetry breaking. Thus motivated, we explore the introduction of the transition metal Mn into thin films of the Dirac semimetal Cd3As2 during growth by molecular beam epitaxy. Scanning transmission electron microscopy measurements show the formation of a Mn-rich phase at the top surface of Mn-doped Cd3As2 thin films grown using both uniform doping and delta doping. This suggests that Mn acts as a surfactant during epitaxial growth of Cd3As2, resulting in phase separation. Magnetometry measurements of such samples indicate a ferromagnetic phase with out-of-plane magnetic anisotropy. Electrical magneto-transport measurements of these films as a function of temperature, magnetic field, and chemical potential reveal a lower carrier density and higher electron mobility compared to pristine Cd3As2 films grown under similar conditions. This suggests that the surfactant effect might also serve to getter impurities. We observe robust quantum transport (Shubnikov-de Haas oscillations and an incipient integer quantum Hall effect) in very thin (7 nm) Cd3As2 films despite being in direct contact with a structurally disordered surface ferromagnetic overlayer.

Carbon combustion synthesis of oxides was applied for quick and energy efficient production of multiferroic composite of cobalt ferrite and barium titanate to form Janus-like particles matrix structure. The exothermic oxidation of carbon nanoparticles with an average size of 5 nm and a specific surface area of 110 m(2)/g generates a self-propagating thermal wave with peak temperature of up to 1000 degrees C. The thermal front rapidly propagates through the mixture of solid reactants (magnetic-CoFe2O4 and ferroelectric-BaTiO3) and results in localized hot-spot sintering of magneto-electric phases to form a nanocomposite structure. Carbon is not incorporated in the product and is emitted as a gaseous CO2. Existence of discrete CoFe2O4 and BaTiO3 phases in the composites nanostructures was confirmed using X-ray powder diffraction along with SEM and TEM analysis. We estimated the activation energy for the combustion synthesis of Janus-like particles to be 112 +/- 3.3 kJ/mol, indicating that the barium titanate and cobalt ferrite presence decrease the activation energy barrier of carbon oxidation and facilitate the ignition process of the combustion synthesis. We observe that the as-synthesized samples show magnetoelectric coupling on multiferroic cobalt ferrite-barium titanate ceramic composites.

Magic-sized semiconductor nanocrystals (MSNCs) grow via discrete jumps between specific sizes. Despite their potential to offer atomically precise structures, their use has been limited by poor stability and trap-dominated photoluminescence. Recently, CdSe MSNCs have been grown to larger sizes. We exploit such particles and demonstrate a method to grow shells on CdSe MSNC cores via high-temperature synthesis. Thin CdS shells lead to dramatic improvements in the emissive properties of the MSNCs, narrowing their fluorescence line widths, enhancing photoluminescence quantum yields, and eliminating trap emission. Although thicker CdS shells lead to decreased performance, CdxZn1-xS alloyed shells maintain efficient and narrow emission lines. These alloyed core/shell crystallites exhibit a tetrahedral shape, in agreement with a recent model for MSNC growth. Our results indicate that MSNCs can compete with other state-of-the-art semiconductor nanocrystals. Furthermore, these core/shell structures will allow further study of MSNCs and their potential for atomically precise growth.

Magic-sized semiconductor nanocrystals (MSNCs) grow via discrete jumps between specific sizes. Despite their potential to offer atomically precise structures, their use has been limited by poor stability and trap-dominated photoluminescence. Recently, syntheses have been reported that produce CdSe MSNCs over a larger size series. We exploit such particles and demonstrate a method to grow shells on CdSe MSNC cores. Thin CdS shells lead to dramatic improvements in the emissive properties of the MSNCs, narrowing their fluorescence linewidths, enhancing photoluminescence quantum yields, and eliminating trap emission. While thicker CdS shells lead to decreased performance, CdxZn1-xS alloyed shells maintain efficient and narrow fluorescence lines. These alloyed core/shell crystallites also exhibit a tetrahedral shape, in agreement with a recent model for MSNC growth. Our results indicate that MSNCs can compete with other state-of-the-art semiconductor nanocrystals. Furthermore, these core/shell structures will allow further study of MSNCs and their potential for atomically precise growth.

We report spin-to-charge and charge-to-spin conversion at room temperature in heterostructure devices that interface an archetypal Dirac semimetal, Cd3As2, with a metallic ferromagnet, Ni0.80Fe0.20 (permalloy). The spin-charge interconversion is detected by both spin torque ferromagnetic resonance and ferromagnetic resonance driven spin pumping. Analysis of the symmetric and anti-symmetric components of the mixing voltage in spin torque ferromagnetic resonance and the frequency and power dependence of the spin pumping signal show that the behavior of these processes is consistent with previously reported spin-charge interconversion mechanisms in heavy metals, topological insulators, and Weyl semimetals. We find that the efficiency of spin-charge interconversion in Cd3As2/permalloy bilayers can be comparable to that in heavy metals. We discuss the underlying mechanisms by comparing our results with first principles calculations.

We studied the spin-to-charge and charge-to-spin conversion at room temperature in sputtered WTe2−x (x = 0.8) (t)/Co20Fe60B20(6 nm) heterostructures. Spin pumping measurements were used to characterize the spin-to-charge efficiency, and the spin efficiency was calculated to be larger than ∼0.035. Second harmonic Hall measurements were carried out to estimate the charge-to-spin conversion ratio. We found that the system exhibits a large field-like torque (spin torque efficiency ∼0.1) and small damping-like torque (spin torque efficiency ∼0.001) compared to those reported for heavy metals. High-resolution transmission electron microscopy images show that the WTe2−x layer is amorphous, which may enhance the spin swapping effect by inducing large interfacial spin–orbit scattering, thus contributing to a large field-like torque.

Semiconductor materials with independently controlled electrical and thermal properties have a unique promise for energy-related applications from thermoelectrics and thermophotovoltaics. Here, using nonthermal plasma synthesized, direct-contact zinc oxide (ZnO) nanocrystal (NC) networks infilled with amorphous Al2O3, and amorphous ZnO-Al2O3 mixture, it is shown that such independent control of electrical and thermal properties is achievable. In this study, in addition to our early reports on control of the electrical properties in these two-phase nanocomposites by tailoring the contact radius between NCs, we demonstrate that the infill composition has a significant impact on the overall thermal conductivity of the NC network and can be used for thermal control. It is also shown that in these heterogeneous systems, the phonons are the dominant heat carriers, and the NC-NC contact radius has a negligible effect on thermal transport. The work suggests that this paradigm of independently controlling the electrical and thermal properties of NC-based materials through tuning the NC-NC contact radius and infill composition can be exploited even further by varying NC and infill materials with potential applications ranging from solar cells and light emitting diodes to solid-state energy converters.

The authors produce plasmonic ZnO-TiN nanocomposite films by depositing plasma-synthesized ZnO nanocrystals onto a substrate and then by infilling the nanocrystal network's pores with TiN via remote plasma-enhanced atomic layer deposition (PEALD). This ZnO-TiN nanocomposite exhibits a plasmonic resonance that is blueshifted compared to planar titanium nitride thin films. The authors study the effects of PEALD conditions and the ZnO film thickness on the plasmonic response of these nanocomposites and exploit the optimized film in a device that generates photocurrent at zero bias.

Molybdenum disulfide (MoS2) is being studied for a wide range of applications including lithium-ion batteries and hydrogen evolution reaction catalysts. In this paper, we present a single-step nonthermal plasma-enhanced chemical vapor deposition (PECVD) process for the production of two-dimensional MoS2. This method provides an alternative route to established CVD and plasma synthesis routes. The approach presented here synthesizes films in only a few minutes using elemental sulfur (S8) and molybdenum pentachloride (MoCl5) as precursors. Deposition utilizes a nonthermal inductively coupled plasma reactor and temperatures around 500 °C. Film growth characteristics and nucleation are studied as a function of precursor concentrations, argon flow rate, plasma power, and deposition time. Few-layer two-dimensional (MoS2) films were formed at low precursor concentrations. Films with nanoparticle-like features were formed when the precursor concentration was high. Noncontinuous nonstoichiometric films were found at low plasma power, while high plasma power led to continuous films with good stoichiometry. The vacancies and defects in these films may provide active sites for hydrogen evolution.

Strain-free ${\mathrm{Fe}}_{16}{\mathrm{N}}_{2}$ thin films were obtained on MgO (001) single-crystal substrates with Cr seed layers. X-ray diffraction and transmission electron microscopy confirmed that the film is textured in all three spatial directions with crystallographic orientation determined by epitaxial constraints from the substrate. Average grain size was estimated to be in the range of tens of nanometers. Ten pieces of 40-nm-thick ${\mathrm{Fe}}_{16}{\mathrm{N}}_{2}$ thin-film samples were stacked together for half-polarized neutron diffraction study at room temperature. A total of six reflections were usable, from which the magnetic structure of ${\mathrm{Fe}}_{16}{\mathrm{N}}_{2}$ was determined and compared to existing models. Contrary to most electronic structure calculations, the present results suggest that the magnetic moment of Fe atoms at the $8h$ site is large and larger than that of the $4d$ site. Our results support the giant magnetization of ${\mathrm{Fe}}_{16}{\mathrm{N}}_{2}$.

Silicon quantum dots (Si QDs) are attractive, nontoxic luminophores for luminescent solar concentrators (LSCs). Here, we produced Si QD/poly(methyl methacrylate) (PMMA) films on glass by doctor-blading polymer solutions and achieved films with low light scattering at an order of magnitude higher Si QD weight fraction than has been achieved previously in the bulk. We suggest that the fast solidification rate of films as compared to slow bulk polymerization is an enabling factor in avoiding large agglomerates within the nanocomposites. Scanning electron microscopy confirmed that ∼100 nm or larger QD agglomerates exist in light-scattering films, and photoluminescence intensity measurements show that light scattering, if present, significantly reduces waveguiding efficiencies for LSCs. Nonscattering films fabricated in this work exhibit high ultraviolet absorption (>80%) paired with high visible transmission (>87%) and minimal visible haze (∼1%), making them well suited for semitransparent coatings for LSCs realized as solar harvesting windows.

Interests in alkaline-earth stannate perovskites have increased dramatically in recent years as future materials for oxide electronics. Wider band gaps (~ 3-4 eV) and high electron mobility at roomtemperature (60-180 cmVs) make them ideal for applications in power electronics and high frequency devices [1,2]. While majority of the works have focused on BaSnO3 (BSO), recent reports on strain engineering in SrSnO3 (SSO) have expanded the boundary of research in stannates [3]. Compared to BSO, SSO has a smaller lattice mismatch with most of commercial perovskite substrates. Additionally, SSO can be grown strained on BSO and their favorable band alignment allows for the realization of modulation doping in stannate heterostructures. Here, SSO/BSO heterostructures were grown for modulation doping of BSO via La-doped-SrSnO3 (LSSO) and elemental quantification of the system was performed using STEM-EELS.

Journal Article Simultaneous Multi-Region Background Subtraction for EELS Spectra Get access Jacob T Held, Jacob T Held Department of Chemical Engineering & Materials Science, University of Minnesota, Minneapolis, MN, USA Corresponding author: heldx123@umn.edu Search for other works by this author on: Oxford Academic Google Scholar Hwanhui Yun, Hwanhui Yun Department of Chemical Engineering & Materials Science, University of Minnesota, Minneapolis, MN, USA Search for other works by this author on: Oxford Academic Google Scholar K Andre Mkhoyan K Andre Mkhoyan Department of Chemical Engineering & Materials Science, University of Minnesota, Minneapolis, MN, USA Search for other works by this author on: Oxford Academic Google Scholar Microscopy and Microanalysis, Volume 25, Issue S2, 1 August 2019, Pages 650–651, https://doi.org/10.1017/S1431927619003982 Published: 01 August 2019

Separating electrons from their source atoms in La-doped BaSnO3, the first perovskite oxide semiconductor to be discovered with high room-temperature electron mobility, remains a subject of great interest for achieving high-mobility electron gas in two dimensions. So far, the vast majority of work in perovskite oxides has focused on heterostructures involving SrTiO3 as an active layer. Here we report the demonstration of modulation doping in BaSnO3 as the high room-temperature mobility host without the use of SrTiO3. Significantly, we show the use of angle-resolved hard X-ray photoelectron spectroscopy (HAXPES) as a nondestructive approach to not only determine the location of electrons at the buried interface but also to quantify the width of electron distribution in BaSnO3. The transport results are in good agreement with the results of self-consistent solution to one-dimensional Poisson and Schrödinger equations. Finally, we discuss viable routes to engineer two-dimensional electron gas density through band-offset engineering.

We present a multi-region extension of power law background subtraction for core-level EEL spectra to improve the robustness of background removal. This method takes advantage of the post-edge shape of core-loss EEL edges to enable simultaneous fitting of pre- and post-edge background regions. This method also produces simultaneous and consistent background removal from multiple edges in a single EEL spectrum. The stability of this method with respect to the fitting energy window and the EELS signal to noise ratio is also discussed.

Core-loss electron energy loss spectroscopy (EELS) is a powerful tool for characterizing elemental composition and electronic structure. When paired with scanning transmission electron microscopy (STEM), two-dimensional spectrum images of EEL spectra can be produced at atomic resolution, enabling the detection of single dopant atoms [1] and local electronic structure [2]. However, only under special circumstances are the EEL edges collected from a single point of a spectrum image representative of a pure material due to plural-scattering, substrates, oxidation, and variation in sample structure.