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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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Giant Orbital Anisotropy with Strong Spin–Orbit Coupling Established at the Pseudomorphic Interface of the Co/Pd Superlattice

Orbital anisotropy at interfaces in magnetic heterostructures has been key to pioneering spin–orbit-related phenomena. However, modulating the interface’s electronic structure to make it abnormally asymmetric has been challenging because of lack of appropriate methods. Here, the authors report that low-energy proton irradiation achieves a strong level of inversion asymmetry and unusual strain at interfaces in [Co/Pd] superlattices through nondestructive, selective removal of oxygen from Co3O4/Pd superlattices during irradiation. Structural investigations corroborate that progressive reduction of Co3O4into Co establishes pseudomorphic growth with sharp interfaces and atypically large tensile stress. The normal component of orbital to spin magnetic moment at the interface is the largest among those observed in layered Co systems, which is associated with giant orbital anisotropy theoretically confirmed, and resulting very large interfacial magnetic anisotropy is observed. All results attribute not only to giant orbital anisotropy but to enhanced interfacial spin–orbit coupling owing to the pseudomorphic nature at the interface. They are strongly supported by the observation of reversal of polarity of temperature-dependent Anomalous Hall signal, a signature of Berry phase. This work suggests that establishing both giant orbital anisotropy and strong spin–orbit coupling at the interface is key to exploring spintronic devices with new functionalities.

42 ENGINEERING↗

Dc and microwave characteristics of a high current double interface GaAs/InGaAs/AlGaAs pseudomorphic modulation-doped field-effect transistor

Extremely large current double interface GaAs/In(0.15)Ga(0.85)As/Al(0.15)Ga(0.85)As pseudomorphic modulation-doped field-effect transistors (MODFET's) grown by molecular beam epitaxy were achieved. The 1-micron gate devices studied have peak current levels (430 mA/mm at 300 K and 483mA/mm at 77 K) roughly one and a half to two times that found in single interface pseudomorphic MODFET's. These devices also retain high transconductances over a broad range of gate voltage, peaking at 312 mS/mm at 300 K and 362 mS/mm at 77 K. Excellent microwave performance is also obtained with a maximum frequency of oscillation (f-max) of 37 GHz and a current gain cut-off frequency of as high as 23 GHz at 300 K. An output power level of 14 dBm (1 dB gain compression) was obtained at 6 GHz for a 290-micron gate width. This double interface single quantum well MODFET may be of great importance in millimeter wave power amplifiers.

Henderson, T.↗

Strain-graded quantum dots with spectrally pure, stable and polarized emission

Structural deformation modifies the bandgap, exciton fine structure and phonon energy of semiconductors, providing an additional knob to control their optical properties. The impact can be exploited in colloidal semiconductor quantum dots (QDs), wherein structural stresses can be imposed in three dimensions while defect formation is suppressed by controlling surface growth kinetics. Yet, the control over the structural deformation of QDs free from optically active defects has not been reached. Here, we demonstrate strain-graded CdSe-ZnSe core-shell QDs with compositionally abrupt interface by the coherent pseudomorphic heteroepitaxy. Resulting QDs tolerate mutual elastic deformation of varying magnitudes at the interface with high structural fidelity, allowing for spectrally stable and pure emission of photons at accelerated rates with near unity luminescence efficiency. We capitalize on the asymmetric strain effect together with the quantum confinement effect to expand emission envelope of QDs spanning the entire visible region and exemplify their use in photonic applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Characterization of graded interface In(x)Ga(1-x)As/In(0.52)Al(0.48)As (x between 0.53 and 0.70) structures grown by molecular-beam epitaxy

Modulation-doped In(x)Ga(1-x)As/In(0.52)Al(0.48)As/InP structures were grown by molecular-beam epitaxy with x values between 53 and 70 percent. For pseudomorphic cases, graded instead of abrupt interfaces were used. Hall mobility and persistent photoconductivity measurements as a function of temperature were used to characterize samples with different structural parameters. Consistent trends in the variation of mobilities and two-dimensional carrier concentration, n(2D), under light and dark conditions have been observed and discussed in terms of applicable scattering mechanisms. The Hall mobilities are comparable to the best results obtained to date but with significantly higher n(2D) concentration.

Peng, C. K.↗

Heterostructure engineering for wurtzite LaN

Wurtzite LaN (wz-LaN) is a semiconducting nitride with favorable piezoelectric and ferroelectric properties, making it promising for applications in electronics. Here, we use first-principles density functional theory with a hybrid functional to investigate several features that are key for its use in heterostructures. First, for the purposes of growing wz-LaN on a substrate or designing a heterostructure, we show that it can be lattice-matched with a number of cubic materials along their [111] axes. We also evaluate the bound charge at such interfaces, taking into account both the polarization discontinuity and the piezoelectric polarization due to pseudomorphic strain. Second, we investigate band alignments and assess the results for interfaces with zincblende-, rocksalt-, and perovskite-structure compounds, along with chemically similar wurtzite and rocksalt nitrides. Our results provide guidance for the development of electronic devices based on wz-LaN.

36 MATERIALS SCIENCE↗

Structure-Related Electronic and Magnetic Properties in Ultrathin Epitaxial Ni x Fe 3–x O 4 Films on MgO(001)

Off-stoichiometric Ni x Fe 3–x O 4 ultrathin films (x < 2.1) with varying Ni content x and thickness 16 (±2) nm were grown on MgO(001) by reactive molecular beam epitaxy. Synchrotron-based high-resolution X-ray diffraction measurements reveal vertical compressive strain for all films, resulting from a lateral pseudomorphic adaption of the film to the substrate lattice without any strain relaxation. Complete crystallinity with smooth interfaces and surfaces is obtained independent of the Ni content x. For x < 1 an expected successive conversion from Fe 3 O 4 to NiFe 2 O 4 is observed, whereas local transformation into NiO structures is observed for films with Ni content x > 1. However, angle-resolved hard X-ray photoelectron spectroscopy measurements indicate homogeneous cationic distributions without strictly separated phases independent of the Ni content, while X-ray absorption spectroscopy shows that also for x > 1, not all Fe 2+ cations are substituted by Ni 2+ cations. The ferrimagnetic behavior, as observed by superconducting quantum interference device magnetometry, is characterized by decreasing saturation magnetization due to the formation of antiferromagnetic NiO parts.

36 MATERIALS SCIENCE↗

Diagenetic Crystal Growth in the Murray Formation, Gale Crater, Mars

The Pahrump region (Gale Crater, Mars) marks a critical transition between sedimentary environments dominated by alluvial-to-fluvial materials associated with the Gale crater rim, and depositional environments fundamentally linked to the crater's central mound, Mount Sharp. At Pahrump, the Murray formation consists of an approximately 14-meter thick succession dominated by massive to finely laminated mudstone with occasional interbeds of cross-bedded sandstone, and is best interpreted as a dominantly lacustrine environment containing tongues of prograding fluvial material. Murray formation mudstones contain abundant evidence for early diagenetic mineral precipitation and its subsequent removal by later diagenetic processes. Lenticular mineral growth is particularly common within lacustrine mudstone deposits at the Pahrump locality. High-resolution MAHLI images taken by the Curiosity rover permit detailed morphological and spatial analysis of these features. Millimeter-scale lenticular features occur in massive to well-laminated mudstone lithologies and are interpreted as pseudomorphs after calcium sulfate. The distribution and orientation of lenticular features suggests deposition at or near the sediment-water (or sediment-air) interface. Retention of chemical signals similar to host rock suggests that original precipitation was likely poikilotopic, incorporating substantial amounts of the primary matrix. Although poikilotopic crystal growth is common in burial environments, it also occurs during early diagenetic crystal growth within unlithified sediment where high rates of crystal growth are common. Loss of original calcium sulfate mineralogy suggests dissolution by mildly acidic, later-diagenetic fluids. As with lenticular voids observed at Meridiani by the Opportunity Rover, these features indicate that calcium sulfate deposition may have been widespread on early Mars; dissolution of depositional and early diagenetic minerals is a likely source for both calcium and sulfate ion-enrichment in burial fluids that precipitated in ubiquitous late-stage hydrofracture veins

Kah, L. C.↗

Role of structural defects in mediating disordering processes at irradiated epitaxial Fe 3 O 4 / Cr 2 O 3 interfaces

Disordering processes in oxide materials are complicated by the presence of interfaces, which can serve as either point defect sinks or accumulation sites; the response depends on factors such as interfacial structure, chemistry, and termination. Here, we have characterized the disordering of epitaxial Fe 3 O 4 (111) / Cr 2 O 3 (0001) thin film heterostructures after 400 keV Ar 2+ radiation at room temperature. The density of misfit dislocations in both the Fe 3 O 4 overlayer and Cr 2 O 3 buffer layer is varied by changing the thickness of Cr 2 O 3 to be pseudomorphically strained to the Al 2 O 3 (0001) substrate (5 nm thick) or partially relaxed (20 nm thick), as confirmed by Bragg filtering analysis of scanning transmission electron microscopy images. In both cases, irradiation leads to damage accumulation on the Fe 3 O 4 side of the heterointerface, as shown by Rutherford backscattering spectrometry measurements in the channeling geometry. However, the interface with more misfit dislocations exhibits disordering at a faster rate than the less-defective interface. Likewise, layer-resolved electron energy loss spectroscopy reveals interfacial reduction of Fe after irradiation at the more defective interface. Intermixing of Cr across the interface is observed by atom probe tomography, which is likely facilitated by the generation of Cr interstitials in Cr 2 O 3 under irradiation.

36 MATERIALS SCIENCE↗

Morphological and crystallographic controls in the replacement of calcite and aragonite by cerussite and otavite

Mineral replacement reactions are essential solid-fluid interactions in natural and industrial processes including metasomatism, diagenesis, and metamorphism, and sequestration of metal toxins from polluted water. In this paper, we explore the morphological evolution of aragonite and calcite (polymorphs of CaCO 3 ) during their replacement by cerussite (PbCO 3 , an isomorph of aragonite) and otavite (CdCO 3 , an isomorph of calcite) in acidic aqueous solutions (with initial pH 3 to 4). Observations using scanning electron and synchrotron-based transmission X-ray microscopies reveal the formation of pseudomorphic shells (~5 to 10 µm thick) of cerussite and otavite when Pb 2+ is reacted with either calcite or aragonite and when Cd 2+ is reacted with aragonite. The formation of pore space at the substrate-precipitate interface and within the precipitate is found to be key in promoting chemical exchange between the dissolving phase and the solution. In contrast, minimal reactivity is observed when Cd 2+ is reacted with calcite. These results demonstrate that the lack of substrate-precipitate epitaxy (either because of inconsistent symmetries or due to large lattice constant mismatch) is a critical factor that enables replacement of primary CaCO 3 minerals by Pb- or Cd-bearing secondary minerals while the presence of epitaxial relationships inhibit those reactions. When calcite and aragonite coexist, the replacement of aragonite by cerussite and otavite occurs preferentially over calcite. We postulate that the relative reactivity of calcite and aragonite to Pb 2+ and Cd 2+ can be determined by interplay between morphological and crystallographic properties of CaCO 3 materials as well as solution chemistry. Our results demonstrate that coupled dissolution-precipitation processes of carbonate minerals play an important role in controlling mobility and bioavailability of lead and cadmium in environments where acidic metal-contaminated water interacts with carbonate-rich rocks and soils.

58 GEOSCIENCES↗

Integrated Cryogenic Satellite Communications Cross-Link Receiver Experiment

An experiment has been devised which will validate, in space, a miniature, high-performance receiver. The receiver blends three complementary technologies; high temperature superconductivity (HTS), pseudomorphic high electron mobility transistor (PHEMT) monolithic microwave integrated circuits (MMIC), and a miniature pulse tube cryogenic cooler. Specifically, an HTS band pass filter, InP MMIC low noise amplifier, HTS-sapphire resonator stabilized local oscillator (LO), and a miniature pulse tube cooler will be integrated into a complete 20 GHz receiver downconverter. This cooled downconverter will be interfaced with customized signal processing electronics and integrated onto the space shuttle's 'HitchHiker' carrier. A pseudorandom data sequence will be transmitted to the receiver, which is in low Earth orbit (LEO), via the Advanced Communication Technology Satellite (ACTS) on a 20 GHz carrier. The modulation format is QPSK and the data rate is 2.048 Mbps. The bit error rate (BER) will be measured in situ. The receiver is also equipped with a radiometer mode so that experiment success is not totally contingent upon the BER measurement. In this mode, the receiver uses the Earth and deep space as a hot and cold calibration source, respectively. The experiment closely simulates an actual cross-link scenario. Since the receiver performance depends on channel conditions, its true characteristics would be masked in a terrestrial measurement by atmospheric absorption and background radiation. Furthermore, the receiver's performance depends on its physical temperature, which is a sensitive function of platform environment, thermal design, and cryocooler performance. This empirical data is important for building confidence in the technology.

Romanofsky, R. R.↗

Strain-Mediated Sn Incorporation and Segregation in Compositionally Graded Ge 1– x Sn x Epilayers Grown by MBE at Different Temperatures

We investigated the process of Sn incorporation and surface segregation for compositionally graded Ge 1–x Sn x epilayers grown on high-quality Ge (001) substrates. Here, the growth resulted in pseudomorphic GeSn layers with a ~6% maximal Sn fraction at a constant substrate temperature. The maximal fraction of Sn was increased to 9.0% when the growth temperature was continuously lowered while increasing the Sn flux. The analysis of surface droplets and SIMS profiles of elemental composition give evidence of Sn rejection during the growth, potentially associated with a critical energy of elastic strain. The intentional reduction of the coherent strain by decreasing the Sn flux near the sample surface has been shown to trap a higher fraction of Sn in the Ge 1–x Sn x layer and lower surface segregation. Our results demonstrate that strain relief by misfit dislocations in the compositionally graded layer is inhibited, which leads to Sn segregation. Specifically, the compressive strain in the graded Ge 1–x Sn x epilayer is effectively “zero” near the interface with the Ge substrate and increases up to about –1.5 × 10 –2 near the surface. Thus, although the nucleation of a dislocation may reduce the compressive strain for the top region of the epilayer, it is not beneficial for the bottom region.

42 ENGINEERING↗

Epitaxial (Al x Ga 1-x-y In y ) 2 O 3 Alloys Lattice Matched to Monoclinic Ga 2 O 3 Substrates

We have epitaxially stabilized a series of monoclinic (Al x Ga 1-x-y In y ) 2 O 3 alloys by careful choice of molecular beam epitaxy growth conditions, which balance alloy growth with suboxide desorption. The films are pseudomorphic to (010) β-Ga 2 O 3 substrates at thicknesses up to 150 nm with compositions ranging from (Al 0.01 Ga 0.83 In 0.16 ) 2 O 3 to (Al 0.24 Ga 0.75 In 0.03 ) 2 O 3 . The absorption edge shifts from approximately 4.62-5.14 eV with coincidently increasing Al and decreasing In mole fractions. J-V measurements reveal an increase in resistivity over four orders of magnitude with a maximum value of 4.2 x 10 5 Ω-cm for (Al 0.17 Ga 0.76 In 0.07 ) 2 O 3 , which has nearly identical lattice parameters (both in-plane and out-of-plane) to the underlying β-Ga 2 O 3 . Scanning transmission electron microscopy of this sample reveals a mostly uniform and single crystalline film, though we identify areas of non-uniform In incorporation and some γ-phase inclusions. This work demonstrates the feasibility of thick layers lattice-matched to β-Ga 2 O 3 with increased bandgap compared to phase-separation limited (Al,Ga) 2 O 3 . These alloys can enable higher bandgap epitaxial dielectrics and high sheet charge density transistors by increasing the conduction band offset with respect to β-Ga 2 O 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗