Achieving Product Control in Furfural Hydrogenation Using Intermetallic Catalysts
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Ward, Charles J.↗
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Controlling Catalyst–Semiconductor Contacts: Interfacial Charge Separation in p-InP Photocathodes
Charge-carrier-selective interfaces between electrocatalyst particles and semiconductor light absorbers are critical for solar photochemistry but controlling their properties is challenging. Using thin films and nanoparticle arrays of Pt hydrogen-evolution catalysts on p-InP (a high-performance photocathode material), along with macroscopic and nanoscopic electrical and chemical analysis, we show how hydrogen alloying, the pinch-off effect for nanoscale contacts, and the formation of a native surface oxides all play different roles in creating charge-carrier-selective junctions. As a result, the new insights can be broadly applied to photocathodes, photoanodes, and overall water-splitting systems to control charge-carrier selectivity and improve performance.
14 SOLAR ENERGY↗
Active Reaction Control of Cu Redox State Based on Real-Time Feedback from In Situ Synchrotron Measurements
Abstract not provided
Rakita, Yevgeny↗
Spatial Control Of Functional Properties Via Octahedral Modulations In Complex Oxide Superlattices
The design of distortions and rotations of the corner-connected BO6 octahedra across interfaces has emerged as an exciting platform to control electronic or ferroic behavior in ABO3 perovskite heterostructures. Here, we investigate isovalent manganite superlattices, [(La0.7Sr0.3MnO3)n/(Eu0.7Sr0.3MnO3)n]×m, as a route to spatial control over electronic bandwidth and ferromagnetism through the creation of octahedral superstructures. Electron energy loss spectroscopy confirms a uniform Mn valence state throughout the superlattices. In contrast, the presence of modulations of the MnO6 octahedral rotations along the growth direction commensurate with the superlattice period is revealed by scanning transmission electron microscopy and x-ray diffraction. We show that the Curie temperatures of the constituent materials can be systematically engineered via the octahedral superstructures leading to a modulated magnetization in samples where the superlattice period is larger than the interfacial octahedral coupling length scale, while a single magnetic transition is observed in the short period superlattices.
Environmental Molecular Sciences Laboratory↗
Controlled synthesis of highly-branched plasmonic gold nanoparticles through peptoid engineering
Inspired by peptide- and protein-controlled formation of hierarchical inorganic nanostructures in nature, herein we report the design of sequence-defined peptoids for biomimetic synthesis of flower-like gold nanosuperstruc-tures. We demonstrate that the peptoid-induced morphosyn-thesis of gold nanoflowers is sequence-dependent. By varying the hydrophobicity, number of carboxylate and amino groups, and side-chain positions of peptoids, we develop a rule of thumb for designing peptoids that yield gold nanoflowers. Through a combination of hyperspectral UV-Vis absorption micro-spectroscopy (H-UVVIS-AMS) and three-photon photoemission electron microscopy (TP-PEEM), we measured the plasmonic properties of individual nanoflowers. Whereas H-UVVIS-AMS experiments revealed well-defined plasmon resonances centered at ~528 nm, TP-PEEM measurements showed an unprecedented plasmonic enhancement as high as 105 for a single nanoflower. A com-bination of the unique plasmonic property and the high sta-bility endows the peptoid-engineered nanoflowers with po-tential applications in chemical and biological imaging. FY, YC, HJ and C-LC acknowledge support by the Materials Synthesis and Simulation Across Scales (MS3) Initiative, through the Laboratory Directed Research & Development (LDRD) fund at Pacific Northwest National Laboratory (PNNL). FY was also partially supported by fellowships from Shandong Provincial Education Association for International Exchanges. YG was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. PZE acknowledges support from the Laboratory Directed Research and Development Program through a Linus Pauling Fellowship at PNNL. PNNL is multi-program national laboratory operated for the Department of Energy by Battelle under Contracts No. DE-AC05-76RL01830. The authors are most grateful to Alan Joly and Wayne Hess (PNNL) for their support with the PEEM measurements and several useful discussions.
Yan, Feng↗
Emergent properties at oxide interfaces controlled by ferroelectric polarization
Abstract Ferroelectric materials are characterized by the spontaneous polarization switchable by the applied fields, which can act as a “gate” to control various properties of ferroelectric/insulator interfaces. Here we review the recent studies on the modulation of oxide hetero-/homo-interfaces by ferroelectric polarization. We discuss the potential applications of recently developed four-dimensional scanning transmission electron microscopy and how it can provide insights into the fundamental understanding of ferroelectric polarization-induced phenomena and stimulate future computational studies. Finally, we give the outlook for the potentials, the challenges, and the opportunities for the contribution of materials computation to future progress in the area.
Chemistry↗
Controlling the polarization and vortex charge of attosecond high-harmonic beams via simultaneous spin–orbit momentum conservation
Optical interactions are governed by both spin and angular momentum conservation laws, which serve as a tool for controlling light–matter interactions or elucidating electron dynamics and structure of complex systems. Here, we uncover a form of simultaneous spin and orbital angular momentum conservation and show, theoretically and experimentally, that this phenomenon allows for unprecedented control over the divergence and polarization of extreme-ultraviolet vortex beams. High harmonics with spin and orbital angular momenta are produced, opening a novel regime of angular momentum conservation that allows for manipulation of the polarization of attosecond pulses—from linear to circular—and for the generation of circularly polarized vortices with tailored orbital angular momentum, including harmonic vortices with the same topological charge as the driving laser beam. As a result, our work paves the way to ultrafast studies of chiral systems using high-harmonic beams with designer spin and orbital angular momentum.
High-harmonic generation↗
Accessing conjugated polymers with precisely controlled heterobisfunctional chain ends via post-polymerization modification of the OTf group and controlled Pd(0)/t-Bu 3 P-catalyzed Suzuki cross-coupling polymerization
In this study, a general strategy toward the synthesis of well-defined conjugated polymers with controlled heterobisfunctional chain ends via combination of controlled Pd(0)/t-Bu 3 P Suzuki cross-coupling polymerization with the post-polymerization modification of the triflate (OTf) group was disclosed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Controllable transformation between 3D and 2D perovskites through cation exchange
The transformation between 3D and 2D perovskites can be controlled through the post-synthesis introduction of foreign cations.
Chemistry↗
Optimal control of orientation and entanglement for two dipole–dipole coupled quantum planar rotors
Optimal control simulations are performed for orientation and entanglement of two dipole–dipole coupled identical quantum rotors.
Chemistry↗
Tunable assembly of biomimetic peptoids as templates to control nanostructure catalytic activity
Tunable peptoid assembly directs the control over structure and function of Pd nanomaterial catalysts.
Merrill, Nicholas A.↗
Controlling 3-D Morphology of Ni-Fe-Based Nanocatalysts for Oxygen Evolution Reaction
Controlling the 3-D morphology of nanocatalysts is one of the underexplored but important approaches for improving the sluggish kinetics of the oxygen evolution reaction (OER) in water electrolysis. This work reports a scalable, oil-based method based on thermal decomposition of organometallic complexes to yield highly uniform Ni–Fe-based nanocatalysts with a well-defined morphology (i.e. Ni–Fe core–shell, Ni/Fe alloy, and Fe–Ni core–shell). Transmission electron microscopy reveals their morphology and composition to be NiOx–FeOx/NiOx core-mixed shell, NiOx/FeOx alloy, and FeOx–NiOx core–shell. X-ray techniques resolve the electronic structures of the bulk and are supported by electron energy loss spectroscopy analysis of individual nanoparticles. These results suggest that the crystal structure of Ni is most likely to contain α-Ni(OH)2 and that the chemical environment of Fe is variable, depending on the morphology of the nanoparticle. The Ni diffusion from the amorphous Ni-based core to the iron oxide shell makes the NiOx–NiOx/FeOx core-mixed shell structure the most active and the most stable nanocatalyst, which outperforms the comparison NiOx/FeOx alloy nanoparticles expected to be active for the OER. This study suggests that the chemical environment of the mixed NiOx/FeOx alloy composition is important to achieve high electrocatalytic activity for the OER and that the 3-D morphology plays a key role in the optimization of the electrocatalytic activity and stability of the nanocatalyst for the OER.
Nanocatalysts↗
Carrier density control in Cu 2 HgGeTe 4 and discovery of Hg 2 GeTe 4 via phase boundary mapping
Phase boundary mapping in Cu 2 HgGeTe 4 allows discovery of Hg 2 GeTe 4 and further enables carrier density control over 4 orders of magnitude.
Ortiz, Brenden R.↗
Steric control of dioxygen activation pathways for Mn II complexes supported by pentadentate, amide-containing ligands
Steric control of dioxygen activation is demonstrated through O 2 titration and isotopic labeling experiments for two Mn( ii ) complexes.
Parham, Joshua D.↗
Control of focusing forces and emittances in plasma-based accelerators using near-hollow plasma channels
A near-hollow plasma channel, where the plasma density in the channel is much less than the plasma density in the walls, is proposed to provide independent control over the focusing and accelerating forces in a plasma accelerator. In this geometry the low density in the channel contributes to the focusing forces, while the accelerating fields are determined by the high density in the channel walls. The channel also provides guiding for intense laser pulses used for wakefield excitation. Both electron and positron beams can be accelerated in a nearly symmetric fashion. Near-hollow plasma channels can effectively mitigate emittance growth due to Coulomb scattering for high-energy physics applications.
43 PARTICLE ACCELERATORS↗
High carrier mobility in orientation-controlled large-grain (≥50 μm) Ge directly formed on flexible plastic by nucleation-controlled gold-induced-crystallization
High-carrier-mobility semiconductors on flexible-plastic are essential to realize flexible electronics. For this purpose, electrical properties of orientation-controlled large-grain Ge crystals on flexible-plastic directly formed by nucleation-controlled gold-induced-crystallization (GIC) are examined, and compared with those obtained by aluminum-induced-crystallization (AIC). The Ge crystals show p-type conductions. Here, hole concentrations are 2.2 × 10{sup 17} and 5.8 × 10{sup 20} cm{sup −3} for GIC-Ge and AIC-Ge, respectively, which are explained on the basis of the solubility of Au and Al in Ge. Thanks to the low hole concentration, GIC-Ge shows high hole mobility (160 cm{sup 2} V{sup −1} s{sup −1}) compared with AIC-Ge (37 cm{sup 2} V{sup −1} s{sup −1}). These demonstrate significant advantage of GIC to realize high-performance flexible-electronics.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Near-infrared spectroscopy for divertor plasma diagnosis and control in DIII-D tokamak
New near infrared (NIR) spectroscopic measurements performed in the DIII-D tokamak divertor plasma suggest new viable diagnostic applications: divertor recycling and low-Z impurity flux measurements, a spectral survey for divertor Thomson scattering (DTS) diagnostic, and T{sub e} monitoring for divertor detachment control. A commercial 0.3 m spectrometer coupled to an imaging lens via optical fiber and a InGaAs 1024 pixel array detector enabled deuterium and impurity emission measurements in the range 800–2300 nm. The first full NIR survey identified D, He, B, Li, C, N, O, Ne lines and provided plasma T{sub e}, n{sub e} estimates from deuterium Paschen and Brackett series intensity and Stark line broadening analysis. The range 1.000–1.060 mm was surveyed in high-density and neon seeded divertor plasmas for spectral background emission studies for λ = 1.064 μm laser-based DTS development. The ratio of adjacent deuterium Paschen-α and Brackett Br9 lines in recombining divertor plasmas is studied for divertor T{sub e} monitoring aimed at divertor detachment real-time feedback control.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
A new apparatus design for high temperature (up to 950 °C) quasi-elastic neutron scattering in a controlled gaseous environment
A design for a sample cell system suitable for high temperature Quasi-Elastic Neutron Scattering (QENS) experiments is presented. The apparatus was developed at the Spallation Neutron Source in Oak Ridge National Lab where it is currently in use. The design provides a special sample cell environment under controlled humid or dry gas flow over a wide range of temperature up to 950 °C. Using such a cell, chemical, dynamical, and physical changes can be studied in situ under various operating conditions. While the cell combined with portable automated gas environment system is especially useful for in situ studies of microscopic dynamics under operational conditions that are similar to those of solid oxide fuel cells, it can additionally be used to study a wide variety of materials, such as high temperature proton conductors. The cell can also be used in many different neutron experiments when a suitable sample holder material is selected. The sample cell system has recently been used to reveal fast dynamic processes in quasi-elastic neutron scattering experiments, which standard probes (such as electrochemical impedance spectroscopy) could not detect. In this work, we outline the design of the sample cell system and present results demonstrating its abilities in high temperature QENS experiments.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗