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At least 739 records · Page 41

Pyrolyzed Triazine-Based Nanoporous Frameworks Enable Electrochemical CO 2 Reduction in Water

The first study of rational synthesis of triazine-based nanoporous frameworks as electrocatalysts for CO 2 reduction reaction (CO 2 RR) was presented. The resulting optimized framework with rich pyridinic nitrogen-containing sites can selectively reduce CO 2 to CO in water with a high Faradic efficiency of ca. 82% under a moderate overpotential of 560 mV. The key of our success lies in the use of pyridine-based backbones as sacrificial groups inside the triazine framework for in situ generation of CO 2 RR-active pyridinic N-doped sites during the high-temperature ZnCl 2 -promoted polymerization process. We anticipate that this study may facilitate new possibilities for the development of porous organic polymers for electrochemical conversion of CO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast band engineering and transient spin currents in antiferromagnetic oxides

Here, we report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO 3 , we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO 3 . These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.

36 MATERIALS SCIENCE↗

Distance dependent quenching and gamma-ray spectroscopy in tin-loaded polystyrene scintillators

In this study, we report the synthesis and inclusion of rationally designed organotin compounds in polystyrene matrices as a route towards plastic scintillators capable of gamma-ray spectroscopy. Tin loading ratios of up to 15% w/w have been incorporated, resulting in photopeak energy resolution values as low as 10.9% for 662 keV gamma-rays. Scintillator constituents were selected based upon a previously reported distance-dependent quenching mechanism. Data obtained using UV-Vis and photoluminescence measurements are consistent with this phenomenon and are correlated with the steric and electronic properties of the respective organotin complexes. We also report fast scintillation decay behavior that is comparable to the quenched scintillators 0.5% trans-stilbene doped bibenzyl and the commercial plastic scintillator BC-422Q-1%. These observations are discussed in the context of practical considerations such as optical transparency, ease-of-preparation/scale-up, and total scintillator cost.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Manipulating cobalt oxide on N-doped aligned electrospun carbon nanofibers towards instant electrochemical detection of dopamine secreted by living cells

A demand exists for the development of miniaturized biosensors with high sensitivity and a wide dynamic range for rapid detecting dopamine (DA) levels. Here, an electrochemical sensor is created by decorating closely packed cobalt oxide (Co 3 O 4 ) nanograins on nitrogen-doped electrospun carbon nanofibers (NECNFs) via a facile electrodeposition method. The carbon nanofiber matrix provides both a scaffold with ultrahigh surface area for homogeneous dispersion of cobalt oxide nanostructures and facilitates the electrochemical conductivity for the hybrid electrode. The sensing principle is based on the redox reaction between DA and DA quinone that generates electrical signal, which is detectable via differential pulse voltammetry (DPV) and chronoamperometry (CA). Owing to a high electroactive surface area and facilitating electron transfer between electrode surface and the target molecule, the electrical sensing platform exhibits superior sensitivity and selectivity toward DA, with an excellent limit of detection (9 nM) over a wide range of concentrations (0.01 to 100 μM). Moreover, based on its excellent sensing properties and biocompatibility, the sensor has been used for the real-time monitoring exogeneous DA released from pheochromocytoma (PC12) cells. This work demonstrates promise of a novel sensor technology that may render rapid point-of-care testing of DA towards early clinical diagnosis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Defect Clustering and Nano-phase Structure Characterization of Multicomponent Rare Earth-Oxide-Doped Zirconia-Yttria Thermal Barrier Coatings

Advanced thermal barrier coatings (TBCs) have been developed by incorporating multicomponent rare earth oxide dopants into zirconia-based thermal barrier coatings to promote the creation of the thermodynamically stable, immobile oxide defect clusters and/or nanophases within the coating systems. In this paper, the defect clusters, induced by Nd, Gd, and Yb rare earth dopants in the zirconia-yttria thermal barrier coatings, were characterized by high-resolution transmission electron microscopy (TEM). The TEM lattice imaging, selected area diffraction (SAD), and electron energy-loss spectroscopy (EELS) analyses demonstrated that the extensive nanoscale rare earth dopant segregation exists in the plasma-sprayed and electron-physical-vapor-deposited (EB PVD) thermal barrier coatings. The nanoscale concentration heterogeneity and the resulting large lattice distortion promoted the formation of parallel and rotational defective lattice clusters in the coating systems. The presence of the 5-to 100-nm-sized defect clusters and nanophases is believed to be responsible for the significant reduction of thermal conductivity, improved sintering resistance, and long-term high temperature stability of the advanced thermal barrier coating systems.

Zhu, Dongming↗

Tuning the Radius Ratio to Enhance Thermoelectric Properties in the Zintl Compounds AM 2 Sb 2 (A = Ba, Sr; M = Zn, Cd)

Five novel Zintl phase solid solutions in the Ba 1–x Sr x Zn 2–y Cd y Sb 2 (0 ≤ x ≤ 0.13(1); 0 ≤ y ≤ 0.32(2)) system were successfully synthesized by the molten Pb metal-flux method, and the powder X-ray diffraction and single-crystal X-ray diffraction analyses proved that all five title compounds adopted the BaCu 2 S 2 -type phase having the orthorhombic Pnma space group (Z = 4, Pearson code oP20) with five crystallographically independent atomic sites. The previously studied BaCu 2 S 2 -type antimonides demonstrated a limited tolerance for doping in contrast to the CaAl 2 Si 2 -type antimonides. To understand the relatively narrower phase width and limited dopability of the title BaCu 2 S 2 -type phase than the CaAl 2 Si 2 -type phase in the overall Ba 1–x Sr x Zn 2–y Cd y Sb 2 system, the radius ratio of cations and anionic elements r + /r – for two structure types were thoroughly investigated. For the first time, the r + /r – ratio was identified as a critical factor for the phase selectivity: (1) r + /r – > 1 favored the BaCu 2 S 2 -type phase, and (2) r + /r – < 1 favored the CaAl 2 Si 2 -type phase. Further, we also revealed the structural transformation mechanism from the more widely observed CaAl 2 Si 2 -type phase to the title BaCu 2 S 2 -type phase as the relatively larger cationic elements were introduced to the system. A series of DFT calculations using the three hypothetical models indicated that a resonance peak near EF in the density of states curves was descended from the relatively flat band structure at several special symmetry points rationalizing the enhanced Seebeck coefficients of Ba 0.94(1) Sr 0.06 Zn 1.86(3) Cd 0.14 Sb 2 and Ba 0.96(1) Sr 0.04 Zn 1.68(2) Cd 0.32 Sb 2 . Electron localization function analysis rationalized the correlation between the polarity change of anionic Zn/Cd–Sb bonds and the charge carrier mobility on the anionic frameworks. Temperature-dependent thermoelectric properties were studied for the four title compounds, and the results proved that the Sr and Cd doping in the title Ba 1–x Sr x Zn 2–y Cd y Sb 2 system successfully enhanced the ZT values through the increased Seebeck coefficients and the reduced total thermal conductivities.

36 MATERIALS SCIENCE↗

Structural, Magnetic, and Photoluminescence Properties of BiFeO{sub 3}: Er-Doped Nanoparticles Prepared by Sol-Gel Technique

A simple sol-gel technique is used to synthesize zero-dimensional pure and Er-doped BiFeO{sub 3} (BFO) nanoparticles. The effect of Er dopant on morphology, structure, optical, magnetic, and photoluminescence properties of single-phase BFO was studied. X-ray diffraction (XRD) studies reveal that the structural phase transformation is noticed from rhombohedral to orthorhombic with substitution of Er to pure BFO. From scanning electron microscopy (SEM) and transmission electron microscopy (TEM), morphology of the synthesized samples were spherical in shape. Agglomeration and particle size reduced with substitution of Er, particle size is around ∼ 30 nm. Energy-dispersive analysis of X-ray (EDAX) spectra confirms the presence of selective elements in synthesized samples. Fourier transform infrared spectra (FTIR) confirms that all the bonds strongly correspond to BFO. The substitution of Er in BFO nanoparticles also demonstrates a strong reduction in optical band-gap energy compared with pure BFO. Magnetization studies were carried out by using vibrating sample magnetometer (VSM), and the saturation magnetization increases with increasing substitution of Er. A photoluminescence (PL) spectrum reveals that the substitution of Er suppressed the recombination of electron-hole pairs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Oscillatory electrostatic potential on graphene induced by group IV element decoration

The structures and electronic properties of partial C, Si and Ge decorated graphene were investigated by first-principles calculations. The calculations show that the interaction between graphene and the decoration patches is weak and the semiconductor patches act as agents for weak electron doping without much disturbing graphene electronic π-bands. Redistribution of electrons due to the partial decoration causes the electrostatic potential lower in the decorated graphene areas, thus induced an electric field across the boundary between the decorated and non-decorated domains. Such an alternating electric field can change normal stochastic adatom diffusion to biased diffusion, leading to selective mass transport.

36 MATERIALS SCIENCE↗

Application of the van der Pauw method for electrical conductivity measurements at high temperatures using an insulating compressing ring

High quality data on the high temperature electrical properties of ceramics, particularly oxides, is of great value for material selection, design, and modeling for a broad range of emerging applications. Utilizing the mismatch in the coefficient of thermal expansion between two materials, a purely mechanical method for establishing electrical contact in the van der Pauw geometry to measure the bulk resistivity of ceramic disks at high temperatures is presented. Measurements of a reference material, 20 mol. % Gd-doped cerium oxide, are presented up to 1000 °C. The viability of electrical measurements up to a maximum temperature of 1600 °C is also considered. Measurements are performed using multiple techniques and compared to literature values finding excellent agreement. Finally, the approach described in this work enables the van der Pauw method to be applied to many ceramic materials over a wide range of temperatures and environments.

47 OTHER INSTRUMENTATION↗

Conductivity space isotherm behavior in quantum anomalous Hall devices

The quantum Hall effect (QHE) has enhanced accessibility to measure and disseminate electrical units, owed in part to the recently redefined International System of Units in 2019. Graphene remains one of the preferred options to realize the ohm despite the limitations of high magnetic fields to produce a robust QHE. Topological insulators, on the other hand, show promise in providing quantized resistance via the quantum anomalous Hall effect, a phenomenon that removes the need for magnetic fields during operation. To optimize future devices for metrological applications, it is important to gain a better understanding of magnetically doped topological insulators like Cr-doped bismuth antimony telluride. The application of differential conductivity space analyses offers a more sensitive way to analyze the data and distinguish between 2D and 3D transport behaviors. This is particularly important in thin films, where the transition between 2D and 3D behavior can be subtle. The ability to confidently determine the dimensionality of the transport is crucial for selecting appropriate theoretical models for future device optimization. Furthermore, this work identifies variable range hopping as the dominant transport mechanism in the 2D regime using a rigorous statistical analysis (via the Bayes factor). These elements assist in the understanding of microscopic processes that govern charge transport in these materials.

Tran, N. T. M. [National Inst. of Standards and Te↗

Crystal structures and phase transitions in Sr doped Ba{sub 2}InTaO{sub 6} perovskites

The crystal structures of the double perovskites of the type Ba{sub 2−x}Sr{sub x}InTaO{sub 6} have been studied by synchrotron X-ray and neutron powder diffraction methods. The structures are based on ordered array of the tilted InO{sub 6} and TaO{sub 6} octahedra, with the Ba/Sr cations being completely disordered. The structure evolves from cubic to monoclinic Fm3{sup ¯}m→{sup x∼0.6}I4/m→{sup x∼1.2}I2/m→{sup x∼1.6}P2{sub 1}/n. The changes in the symmetry induced by replacing the Ba with Sr have been identified by a symmetry-mode analysis. Variable temperature S-XRD studies of selected examples have shown that heating the samples induces the same sequence of transitions observed in the composition dependent studies. - Graphical abstract: The evolution of the structure of the B-site ordered perovskites has been determined by high resolution powder diffraction. The nature of the transitions are probed by examination of the symmetry-adapted modes. Display Omitted - Highlights: • Synthesis of Ba{sub 2−x}Sr{sub x}InTaO{sub 6} cation ordered perovskites. • Synchrotron X-ray and neutron diffraction structural studies of Ba{sub 2−x}Sr{sub x}InTaO{sub 6}. • Phase transitions in Ba{sub 2−x}Sr{sub x}InTaO{sub 6}. • Symmetry-adapted mode analysis of phase transitions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High performance high-power textured Mn/Cu-doped PIN-PMN-PT ceramics

Piezoelectric ceramics with combinatory soft and hard characteristics are highly desired for high-power applications. However, it remains grand challenge to achieve simultaneous presence of hard (e.g. high coercive field, E c ; high mechanical quality factor, Q m ) and soft (e.g. high piezoelectric constant, d; high electromechanical coupling factor, k) piezoelectric properties in piezoelectric ceramics since the mechanism controlling the hard behavior (pinned domain walls) will significantly reduce the soft behavior. Here, we address this grand challenge and demonstrate <001> textured MnO 2 and CuO co-doped Pb(In 1/2 Nb 1/2 )O 3- Pb(Mg 1/3 Nb 2/3 )O 3- PbTiO 3 (PIN-PMN-PT) ceramics exhibiting ultrahigh combined soft and hard piezoelectric properties (d 33 = 713 pC N –1 , k 31 = 0.52, Q m ≈950, E c = 9.6 kV cm –1 , tan δ = 0.45%). The outstanding electromechanical properties are explained by considering composition/phase selection, crystallographic anisotropy and defect engineering. Phase-field model in conjunction with high resolution electron microscopy and diffraction techniques is utilized to delineate the contributions arising from intrinsic piezoelectric response, domain dynamics, and local structural heterogeneity. Furthermore, these results will have significant impact in the development of high-power transducers and actuators.

36 MATERIALS SCIENCE↗

Heterostructures through Divergent Edge Reconstruction in Nitrogen-Doped Segmented Graphene Nanoribbons

Atomically precise engineering of defined segments within individual graphene nanoribbons (GNRs) represents a key enabling technology for the development of advanced functional device architectures. In this paper, the bottom-up synthesis of chevron GNRs decorated with reactive functional groups derived from 9-methyl-9H-carbazole is reported. Scanning tunneling and non-contact atomic force microscopy reveal that a thermal activation of GNRs induces the rearrangement of the electron-rich carbazole into an electron-deficient phenanthridine. Finally, the selective chemical edge-reconstruction of carbazole-substituted chevron GNRs represents a practical strategy for the controlled fabrication of spatially defined GNR heterostructures from a single molecular precursor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Applications of Nickelate perovskites for neuromorphic computing from electronic structure and Machine Learning

While the limit of Moore's law is presently being reached with current microelectronic technologies, we need to develop new paradigms that overcome this limitation. In that respect, neuromorphic computing is a concept that emulates the neural behavior and response of the human brain, and it has been recognized as a promising alternative approach. In this research project, we will perform multi-fidelity scale bridging to explore the potential use of materials with metal to insulator transition for neuromorphic applications. In particular, rare earth nickelates are promising for such purposes, as the transition in these materials is quite sensitive to a broad set of different external stimuli. Our multi-fidelity approach will bridge the high-fidelity electronic structure calculations with classical potentials. We will bridge dynamical mean field theory with a classical atomistic representation via a deep learning force field. The neural network is trained with energies, charges, and forces obtained by accurate electronic structure theories based on Dynamical Mean Field Theory. The configurational space is generated from known crystal phases, ab initio molecular dynamics with exchange-correlation functionals corrected with the Hubbard model, disordered phases with different concentrations of oxygen vacancies, and nonsymmetrical positions and induced strain by grain interfaces or contact with a substrate. Strategies to train the model with a reduced number of training examples are obtained from active learning methods, and new structures for improving the learning process are generated by using machine learning autoencoders. This classical potential will be validated through a diversity of electronic structure methods and represents an important step to combine the flexibility and accuracy of first-principles with the speed of classical potentials. The generated multi-fidelity surrogate model will be used to understand the role of strain, oxygen vacancies, proton doping, the variation of the crystal phase, substrate effects, vibrational effects as the octahedral rotation, grain boundaries and defect effects on the response of a Metal to Insulator Transition (MIT) in correlated materials. Long time and large-scale simulations will help understand the role of different stimuli to control the hysteresis of the MIT, as it has been experimentally suggested. Selected configurations will be analyzed with higher-level theories to provide an accurate electronic description and to study how the orbitals and charges are rearranged under different conditions.

36 MATERIALS SCIENCE↗

A stabilized large-aperture far-infrared telescope gondola

Description of a recently developed balloon-borne 1-m far-infrared telescope designed to carry out astronomical observations and to map radiation from selected areas of the sky. The telescope optical system consists of a conventional Cassegrain arrangement with an f/2 aluminum primary mirror, spherically figured, which feeds a pyrex secondary mirror to produce an f/13.8 beam at the focal plane with a scale of 15.2 arc sec/mm. Three focal planes are provided. The infrared detectors consist of an array of four gallium-doped germanium bolometers fitted within a two-liter helium dewar. An altitude-azimuth mount design is used for attitude control, with the pointing objectives being achieved in two steps. The azimuth control system is capable of operation in a position mode, in which the sensing element is a servo-driven null magnetometer always pointed north, and in an inertial mode, in which the gyro is uncaged and becomes the azimuth reference. The elevation system also operates in both position and inertial modes. An auxiliary position control, powered by an independent battery and controlled by a separate tone command system, is provided in case of a primary system difficulty.

Hazen, N. L.↗

Integrating Flow Imaging Analysis and Single-Particle ICP-TOFMS for Comprehensive Micro- and Nanoplastic Characterization

Flow imaging analysis (FIA), provides composition-agnostic morphological characterization. These measurements of particle size and shape are valuable to mass-based analysis, such as single particle inductively coupled plasma time-of-flight mass spectrometry (sp-ICP-TOFMS), which provides quantitative data on elements within particles. Using these two methods together enables informed use of geometric assumptions required by sp-ICP-TOFMS, as particle mass is typically converted to a particle diameter using assumed-spherical geometry. To validate this concept, parallel measurements to determine particle diameters were performed by FIA and sp-ICP-TOFMS on four particle suspensions: 300 nm polystyrene Eu-doped nanoparticles, 1 μm Fe-rich beads, 3 μm four element calibration polystyrene beads and 5 μm polystyrene beads. The Fe-particles obtained the highest percent difference from the manufacturer’s nominal diameter, as the mean diameter obtained by FIA was overestimated by 21% and sp-ICP-TOFMS underestimated the mean diameter by 20.7%. Two types of particles were selected to test the effect of varying the particle number concentrations (PNC) on sizing accuracy, and both methods accurately sized each particle population at the PNC expected. Single particle analysis of carbon has continued to be a popular research topic, with direct applications to environmental pollutants in terms of nano- and micro- plastics. Real-world plastic particles were studied, and FIA’s measured circularity values demonstrated that the particles deviated from spherical geometries, therefore sp-ICP-TOFMS data should be interpreted as mass-based rather than size-based. Combining these techniques enables improved interpretation of particle populations and evaluation of particle sizes.

Szakas, Sarah [ORNL] (ORCID:0000000241332197)↗

Thermoelectric Performance and Defect Chemistry in n-Type Zintl KGaSb 4

The rise of high-throughput calculations has accelerated the discovery of promising classes of thermoelectric materials. In prior work, we identified the n-type Zintl pnictides as one such material class. To date, however, a lack of detailed defect calculations and chemical intuition has led the community to investigate p-type Zintls almost exclusively. Here, we investigate the synthesis, thermoelectric properties, and defect structure of the complex Zintl KGaSb 4 . We find that KGaSb 4 is successfully doped n-type with Ba and has the potential for p-type doping with Zn. Our calculations reveal the fundamental defect structure in KGaSb 4 that enables n-type and p-type doping. We find that Ba doped KGaSb4 exhibits high electronic mobility (~50 cm 2 V -1 s -1 ) and near minimum lattice thermal conductivity (<0.5 Wm -1 K -1 ) at 400 °C. Samples doped with 1.5% Ba achieve zT > 0.9 at 400 °C, promising for a previously unstudied material. Here, we also briefly investigate the series of alloys between KGaSb 4 and KAlSb 4 , finding that a full solid solution exists. Altogether our work reinforces motivation for the exploration of n-type Zintl materials, especially in tandem with high-throughput defect calculations to inform selection of effective dopants and systems amenable to n-type transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗