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DOE OSTI2021

A dissolution model of alite coupling surface topography and ions transport under different hydrodynamics conditions at microscale

Portland cement is the most produced material in the world. The hydration process of cement consists of a group of complex chemical reactions. In order to investigate the mechanism of cement hydration, it is vital to study the hydration of each phase separately. An integrated model is proposed in this paper to simulate the dissolution of alite under different hydrodynamic conditions at microscale, coupling Kinetic Monte Carlo model (KMC), Lattice Boltzmann method (LBM) and diffusion boundary layer (DBL). The dissolution of alite is initialised with KMC. Two Multiple-relaxation-time (MRT) LB models are used to simulate the fluid flow and transport of ions, respectively. For solid-liquid interface, DBL is adapted to calculate the concentration gradient and dissolution flux. The model is validated with experiment from literature. The simulation results show good agreements with the results published in the literature.

36 MATERIALS SCIENCE↗

DOE OSTI2020

On the hydrogenation of Poly-Si passivating contacts by Al 2 O 3 and SiN x thin films

Doped polycrystalline silicon (poly-Si), when coupled with a thin SiO 2 interlayer, is of large interest for crystalline silicon ( c -Si) solar cells due to its outstanding passivating contact properties. To reach high levels of surface passivation, it is pivotal to hydrogenate the poly-Si and the underlying c -Si/SiO 2 interface. This can be done by capping the poly-Si with a hydrogen-containing dielectric layer such as Al 2 O 3 or SiN x , followed by a thermal anneal. On the basis of recent research, this work addresses several aspects of such hydrogenation by dielectric materials, including the effect of the annealing ambient, the thermal stability and reversibility of hydrogenation, the poly-Si doping level and c -Si surface texture. Additionally, the implementation of hydrogenation of poly-Si by dielectric materials in solar cells is discussed.

14 SOLAR ENERGY↗

DOE OSTI2021

Towards replacing physical testing of granular materials with a Topology-based Model

In the study of packed granular materials, the performance of a sample (e.g., the detonation of a high-energy explosive) often correlates to measurements of a fluid flowing through it. The “effective surface area,” the surface area accessible to the airflow, is typically measured using a permeametry apparatus that relates the flow conductance to the permeable surface area via the Carman-Kozeny equation. This equation allows calculating the flow rate of a fluid flowing through the granules packed in the sample for a given pressure drop. However, Carman-Kozeny makes inherent assumptions about tunnel shapes and flow paths that may not accurately hold in situations where the particles possess a wide distribution in shapes, sizes, and aspect ratios, as is true with many powdered systems of technological and commercial interest. To address this challenge, we replicate these measurements virtually on micro-CT images of the powdered material, introducing a new Pore Network Model based on the skeleton of the Morse-Smale complex. Pores are identified as basins of the complex, their incidence encodes adjacency, and the conductivity of the capillary between them is computed from the cross-section at their interface. We build and solve a resistive network to compute an approximate laminar fluid flow through the pore structure. Here, we provide two means of estimating flow-permeable surface area: (i) by direct computation of conductivity, and (ii) by identifying dead-ends in the flow coupled with isosurface extraction and the application of the Carman-Kozeny equation, with the aim of establishing consistency over a range of particle shapes, sizes, porosity levels, and void distribution patterns.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Variable Daily Autocorrelation Functions of High-Frequency Seismic Data on Mars

Abstract High-frequency seismic data on Mars are dominated by wind-generated lander vibrations, which are radiated partially to the subsurface. Autocorrelation functions (ACFs) of seismic data on Mars filtered between 1 and 5 Hz show clear phases at ∼1.3, ∼2.6, and ∼3.9 s. Daily temporal changes of their arrival times (dt/t) correlate well with the daily changes of ground temperature, with ∼5% daily variation and ∼50 min apparent phase delay. The following two mechanisms could explain the observations: (1) the interference of two predominant spectral peaks at ∼3.3 and ∼4.1 Hz, assumed to be both lander resonance modes, generate the apparent arrivals in the ACFs; (2) the interference of the lander vibration and its reflection from an interface ∼200 m below the lander generate the 3.3 Hz spectral peak and ∼1.3 s arrival in the ACFs. The driving mechanism of the resolved dt/t that most likely explains the ∼50 min delay is thermoelastic strain at a near-surface layer, affecting the lander–ground coupling and subsurface structures. The two outlined mechanisms suggest, respectively, up to ∼10% changes in ground stiffness at 1–5 Hz and ∼15% velocity changes in the top ∼20 m layer. These are upper bound values considering also other possible contributions. The presented methodology and results contribute to analysis of ACFs with limited data and the understanding of subsurface materials on Mars.

Geochemistry & Geophysics↗

DOE OSTI2024

Structure and Dynamics of Aqueous Electrolytes at Quartz (001) and (101) Surfaces

Here, understanding and describing reactivity at mineral-water interfaces such as ion adsorption, the kinetics of dissolution, or surface charge development depends on our ability to improve the accuracy of electrical double layer (EDL) models. While molecular dynamics (MD) simulations are routinely used to investigate the structure and energetics of adsorbed ions comprising the EDL, less attention is paid to their self-diffusion dynamics, which can uniquely inform on coupling to interfacial reactions. Here we use MD to investigate both the organization and diffusion dynamics of water and electrolyte ions (NaCl, KCl, CaCl 2 ) at hydroxylated quartz (001) and (101) surfaces, a comparison which allowed us to assess surface structural effects of corrugation and silanol density. We found that inner- versus outer-sphere complex formation depends on cation size and charge but not necessarily hydration energies. Participation of surface silanols in the hydration spheres of Na + and K + generally indicated their preference for inner-sphere complexation, but this depends strongly on the orientation of the surface considered through its influence over the organization and dynamics of adsorbed water layers. In particular, surface orientation substantially affects the diffusive behavior of the near-surface water. Na + was found to decrease the mobility of water in the first layer, consistent with an increasing frequency of hydrolysis implied by faster quartz dissolution rates observed in experiments via the well known salt effect. Our results are also in good agreement with the observed dissolution rate of quartz vs. surface adsorption strength measure by Dove and Nix. This study sets the stage for a forthcoming paper examining how the dynamics at quartz/electrolyte interfaces are influenced by externally applied electric fields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Vibronic Relaxation Pathways in Molecular Spin Qubit Na 9 [Ho(W 5 O 18 ) 2 ]·35H 2 O under Pressure

In order to explore how spectral sparsity and vibronic decoherence pathways can be controlled in a model qubit system with atomic clock transitions, we combined diamond anvil cell techniques with synchrotron-based far infrared spectroscopy and first-principles calculations to reveal the vibrational response of Na 9 [Ho(W 5 O 18 ) 2 ]·35H 2 O under compression. Because the hole in the phonon density of states acts to reduce the overlap between the phonons and f manifold excitations in this system, we postulated that pressure might move the HoO 4 rocking, bending, and asymmetric stretching modes that couple with the M J = ±5, ±2, and ±7 levels out of resonance, reducing their interactions and minimizing decoherence processes, while a potentially beneficial strategy for some molecular qubits, pressure slightly hardens the phonons in Na 9 [Ho(W 5 O 18 ) 2 ]·35H 2 O and systematically fills in the transparency window in the phonon response. The net result is that the vibrational spectrum becomes less sparse and the overlap with the various M J levels of the Ho 3+ ion actually increases. These findings suggest that negative pressure, achieved using chemical means or elongational strain, could further open the transparency window in this rare earth-containing spin qubit system, thus paving the way for the use of device surfaces and interface elongational/compressive strains to better manage decoherence pathways.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Advances and perspectives on mass transfer and enzymatic hydrolysis in the enzyme-mediated lignocellulosic biorefinery: A review

We report enzymatic hydrolysis is a critical process for the cellulase-mediated lignocellulosic biorefinery to produce sugar syrups that can be converted into a whole range of biofuels and biochemicals. Such a process operating at high-solid loadings (i.e., scarcely any free water or roughly ≥ 15% solids, w/w) is considered more economically feasible, as it can generate a high sugar concentration at low operation and capital costs. However, this approach remains restricted and incurs “high-solid effects”, ultimately causing the lower hydrolysis yields with increasing solid loadings. The lack of available water leads to a highly viscous system with impaired mixing that exhibits strong transfer resistance and reaction limitation imposed on enzyme action. Evidently, high-solid enzymatic hydrolysis involves multi-scale mass transfer and multi-phase enzyme reaction, and thus requires a synergistic perspective of transfer and biotransformation to assess the interactions among water, biomass components, and cellulase enzymes. Porous particle characteristics of biomass and its interface properties determine the water form and distribution state surrounding the particles, which are summarized in this review aiming to identify the water-driven multi-scale/multi-phase bioprocesses. Further aided by the cognition of rheological behavior of biomass slurry, solute transfer theories, and enzyme kinetics, the coupling effects of flow-transfer-reaction are revealed under high-solid conditions. Based on the above basic features, this review lucidly explains the causes of high-solid hydrolysis hindrances, highlights the mismatched issues between transfer and reaction, and more importantly, presents the advanced strategies for transfer and reaction enhancements from the viewpoint of process optimization, reactor design, as well as enzyme/auxiliary additive customization.

45 multi-scale, multi-phase, enzymatic reaction↗

DOE OSTI2025

Binding and Translocation of Substrate Allosterically Promotes Functional Interactions Within the AlkB–AlkG Electron Transfer Complex

The alkane monooxygenase AlkB and rubredoxin AlkG form an electron transfer complex that hydroxylates terminal alkanes to produce alcohols. The recent cryoEM study of Fontimonas thermophila AlkB-AlkG complex revealed its architecture, including a dodecane (D12) substrate at the active site. However, FtAlkBG molecular mechanism of action of remains unknown. Here, in this study, we examined its dynamics and interactions by multiscale computations, including molecular dynamics simulations, elastic network models, and QM/MM of the oxygen activation mechanism at the AlkB catalytic site. D12 maintained stable interactions within the catalytic site during two MD runs, coordinated by hydrophobic residues L263-L264, I267, I133. A third extended run revealed that D12 could translocate to a membrane-exposed site near S49/F46 along a hydrophobic channel gated by I54. During this translocation, D12 was temporarily stabilized at intermediate sites IS1 (lined by I27/L30-G31/G50/L53-I54/P59/S124/A127-V128) and IS2 (I33-G34/L37/L45-F46/S49) before nearly exiting the protein, and diffused back to the active site, assisted by L30. Substrate binding and translocation across those intermediate sites affects the coupling between the iron centers in AlkBG, and interfacial interactions between AlkB-AlkG. The channel was further connected to the cytosol, near two surface-exposed arginines, potentially allowing for O 2 passage. The allosteric effects between D12 putative entry site, catalytic site and AlkB-AlkG interface were analyzed by ENM-based methods which confirmed the cooperative perturbation-responses and strongly correlated movements of residues belonging to those distal regions. Our study provides new mechanistic insights into key sites and their interactions that could be targeted for developing AlkB-variants with desirable alkane conversion functions.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Sensitivity analysis of thermal contact conductance modeling to inform MiniFuel irradiation capsule designs

The MiniFuel irradiation platform has been developed by Oak Ridge National Laboratory as a flexible, high-throughput separate effects testing capability within the High Flux Isotope Reactor (HFIR). Finite element thermal models are relied upon to design MiniFuel experiments to achieve a specific time-averaged irradiation temperature for experimental objectives. A previous study identified that uncertainty in the component heat generation rates and thermal contact conductance (TCC) model are the most significant contributors to predicted fuel temperature variance. To address both sources of uncertainty, this work performs sensitivity analysis on the TCC model to identify high-impact, high-uncertainty parameters that contribute to fuel temperature variance. The TCC model is analyzed in increasing detail, first using a standalone Python code, then again after coupling Python to the BISON fuel performance code. Furthermore, the parameters with the largest contributions to fuel temperature variance which can be reduced through design changes are identified as the initial subcapsule gas pressure, contact pressure between the fuel and dish, and the effective surface roughness of the interface. A set of design recommendations for future capsule designs has been established and applied to reduce the previously quantified average fuel temperature uncertainty ranges of ± 40 °C in the HFIR vertical experiment facilities (VXF) and ± 80 °C in the removable beryllium (RB) reflector to approximately ± 32 °C and ± 53 °C, respectively. This equates to a 21 % and 33 % reduction in the uncertainty range of the average fuel temperature for VXF and RB, respectively.

BISON↗

DOE OSTI2021

A Review of Lattice-Boltzmann Models Coupled with Geochemical Modeling Applied for Simulation of Advanced Waterflooding and Enhanced Oil Recovery Processes

To maintain economic profit and improve the oil production efficiency after the primary and secondary production phase, advanced waterflooding techniques such as low salinity waterflooding in carbonate reservoirs have been investigated in numerical simulations, laboratory experiments, and field pilot tests. Multiple underlying mechanisms have been proposed based on these studies, and they are still under debate. Various numerical modeling approaches are introduced, but there exists a lack of a pore-scale comprehensive modeling scheme to fully understand the processes. Lattice-Boltzmann method (LBM) is a type of numerical fluid flow modeling technique that shows capabilities and flexibilities in modeling pore-scale fluid flow to integrate physical–chemical processes within complex structures. The intrinsic feature of LBM makes it a promising framework for simulating advanced waterflooding due to its flexibility, accuracy, and parallel efficiency. LBM works either by itself for solving reactive transport problems or by coupling with a third-party reaction solver. This review mainly introduces the LBM fluid flow and reactive transport capabilities and the concept and modeling approaches to simulate advanced waterflooding techniques. Meanwhile, an evaluation of the coupled LBM models for enhanced oil recovery (EOR) simulations is discussed with future research challenges and directions concluded.

02 PETROLEUM↗

DOE OSTI2024

Subsurface Redox Interactions Regulate Ebullitive Methane Flux in Heterogeneous Mississippi River Deltaic Wetland

Abstract As interfaces connecting terrestrial and ocean ecosystems, coastal wetlands develop temporally and spatially complex redox conditions, which drive uncertainties in greenhouse gas emission as well as the total carbon budget of the coastal ecosystem. To evaluate the role of complex redox reactions in methane emission from coastal wetlands, a coupled reactive‐transport model was configured to represent subsurface biogeochemical cycles of carbon, nitrogen, and sulfur, along with production and transport of multiple gas species through diffusion and ebullition. This model study was conducted at multiple sites along a salinity gradient in the Barataria Basin at the Mississippi River Deltaic Plain. Over a freshwater to saline gradient, simulated total flux of methane was primarily controlled by its subsurface production and consumption, which were determined by redox reactions directly (e.g., methanogenesis, methanotrophy) and indirectly (e.g., competition with sulfate reduction) under aerobic and/or anaerobic conditions. At fine spatiotemporal scales, surface methane fluxes were also strongly dependent on transport processes, with episodic ebullitive fluxes leading to higher spatial and temporal variability compared to the gradient‐driven diffusion flux. Ebullitive methane fluxes were determined by methane fraction in total ebullitive gas and the frequency of ebullitive events, both of which varied with subsurface methane concentrations and other gas species. Although ebullition thresholds are constrained by local physical factors, this study indicates that redox interactions not only determine gas composition in ebullitive fluxes but can also regulate ebullition frequency through gas production.

03 NATURAL GAS↗

DOE OSTI2021

All-epitaxial long-range surface plasmon polariton structures with integrated active materials

We demonstrate all-epitaxial structures capable of supporting short- and long-range surface plasmon polariton (SRSPP and LRSPP) modes in the long-wave infrared region of the electromagnetic spectrum. The SRSPP and LRSPP modes are bound to the interfaces of a buried heavily doped (n ++ ) semiconductor layer and surrounding quantum-engineered type-II superlattice (T2SL) materials. The surrounding T2SLs are designed to allow optical transitions across the frequency dispersion of the SPP modes. We map the SPP dispersion in our structure using grating-coupled angle- and polarization-dependent reflection and photoluminescence spectroscopy. The epitaxial structures are analytically described using a simplified three-layer system (T2SL/n ++ /T2SL) and modeled using rigorous coupled wave analysis with excellent agreement to our experimental results. The presented structures offer the potential to serve as long-range interconnects or waveguides in all-epitaxial plasmonic/optoelectronic systems operating in the long-wave infrared.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Correlated nanoelectronics and the second quantum revolution

The growing field of correlated nanoelectronics exists at the intersection of two established fields: correlated oxide electronics and semiconductor nanoelectronics. The development of quantum technologies that exploit quantum coherence and entanglement for the purposes of computation, simulation, and sensing will require complex material properties to be controlled at nanoscale dimensions. Heterostructures and nanostructures formed at the interface between LaAlO 3 and SrTiO 3 exhibit striking behavior that arises from the ability to program the conductive behavior at extreme nanoscale dimensions. The active electronic layer, SrTiO 3 , exhibits a wide range of gate-tunable phenomena such as ferroelectricity, ferroelasticity, magnetism, superconductivity, and spin–orbit coupling, all of which can be controlled at the nanoscale using two reversible methods: conductive atomic force microscope lithography and ultra-low-voltage electron beam lithography. Mesoscopic devices such as single-electron transistors and quasi-one-dimensional electron waveguides can be “sketched” using these techniques, and the properties of these devices differ significantly from those created from traditional semiconductors, such as Si or GaAs. The strongly correlated nature of the SrTiO 3 system is evident from superconducting behavior as well as a state in which electrons are paired outside the superconducting state. A highly exotic phase was discovered in which a degenerate quantum liquid is formed from bound states of n = 2, 3, 4, … electrons. Further development of correlated nanoelectronics based on the LaAlO 3 /SrTiO 3 system can potentially lead to a general platform for quantum simulation as well as a pathway for the development of highly entangled states of multiple photons.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Full-sky Models of Galactic Microwave Emission and Polarization at Subarcminute Scales for the Python Sky Model

Polarized foreground emission from the Galaxy is one of the biggest challenges facing current and upcoming cosmic microwave background (CMB) polarization experiments. We develop new models of polarized Galactic dust and synchrotron emission at CMB frequencies that draw on the latest observational constraints; that employ the “polarization fraction tensor” framework to couple intensity and polarization in a physically motivated way; and that allow for stochastic realizations of small-scale structure at subarcminute angular scales currently unconstrained by full-sky data. We implement these models into the publicly available Python Sky Model (PySM) software and additionally provide PySM interfaces to select models of dust and CO emission from the literature. We characterize the behavior of each model by quantitatively comparing it to observational constraints in both maps and power spectra, demonstrating an overall improvement over previous PySM models. Finally, we synthesize models of the various Galactic foreground components into a coherent suite of three plausible microwave skies that span a range of astrophysical complexity allowed by current data. Author contributions to this paper can be found at the end of this work.

Group, The Pan-Experiment Galactic Science↗

DOE OSTI2021

A Structural Basis for Inhibition of the Complement Initiator Protease C1r by Lyme Disease Spirochetes

Abstract Complement evasion is a hallmark of extracellular microbial pathogens such as Borrelia burgdorferi, the causative agent of Lyme disease. Lyme disease spirochetes express nearly a dozen outer surface lipoproteins that bind complement components and interfere with their native activities. Among these, BBK32 is unique in its selective inhibition of the classical pathway. BBK32 blocks activation of this pathway by selectively binding and inhibiting the C1r serine protease of the first component of complement, C1. To understand the structural basis for BBK32-mediated C1r inhibition, we performed crystallography and size-exclusion chromatography–coupled small angle X-ray scattering experiments, which revealed a molecular model of BBK32-C in complex with activated human C1r. Structure-guided site-directed mutagenesis was combined with surface plasmon resonance binding experiments and assays of complement function to validate the predicted molecular interface. Analysis of the structures shows that BBK32 inhibits activated forms of C1r by occluding substrate interaction subsites (i.e., S1 and S1’) and reveals a surprising role for C1r B loop–interacting residues for full inhibitory activity of BBK32. The studies reported in this article provide for the first time (to our knowledge) a structural basis for classical pathway–specific inhibition by a human pathogen.

Garrigues, Ryan J. (ORCID:0000000259233250)↗

DOE OSTI2024

Collaborative Research Proposal: Time Resolved Optical Emissions Spectroscopy and Laser Induced Fluorescence Spectroscopy of Nanosecond Pulsed Discharges in a Gas-Liquid Water Film Reactor

Electrical discharge plasma formed in contact with liquid water is of interest for a wide range of applications in chemical, biomedical, agricultural, electrical, and materials science and engineering. Such plasma reactors are of very timely importance since they also have significant disinfection capability by inactivating bacteria, viruses and other pathogens. Many types of plasma sources including those driven by AC, DC, RF, microwave, and pulsed electrical power supplies coupled to a wide range of different electrode configurations and reactor designs have been developed and explored which contact the plasma with liquid water. Recent roadmaps have recommended that further work is needed to develop our understanding of the fundamental chemical and physical process which occur at the interface of non-thermal plasma with liquid water solutions in order to advance this large diversity of applications which ultimately depend upon efficient production of key reactive chemical species. There is a wide range of interacting factors that affect the chemical reactions that occur in the plasma, in the liquid phase, and at the interface. These factors ultimately govern the key reactive chemical species formed and used in the various applications and they include a) the reactor design and input parameters, b) the discharge and transport processes, c) the plasma properties, and d) the resulting chemical reactions. For pulsed discharges, the power supply design and output parameters control the applied voltage, frequency, rise time, and width (duration) of the applied pulses. The reactor design involves specification of the gas-liquid contacting methods, electrode gap distance, reactor volume and shape, and gas and liquid flow rates achievable. The gas and liquid compositions as well as the liquid properties such as pH and conductivity are also of key importance in determination of the resulting chemical reactions. In addition, the important plasma properties include plasma gas temperature, electron density, electron energy (distribution), and size of the plasma channels which are all affected by the discharge and transport properties. Many studies have focused on specific aspects of these various processes. Of particular important and relevance to the proposed work is the utilization of nanosecond pulses to generate plasma in gas-liquid systems, liquid bubbles, underwater, and in gases. Recent advances in nanosecond pulses provide significant advantages in utilization with liquid water. For example, fast rise time and short pulses are less sensitive to water conductivity, such short pulses may provide advantages in fast temporal quenching of the plasma, and fundamental analysis of pulse properties, including pulse shape and width, may be facilitated by investigation of single filamentary fast pulses. Many studies have also dealt with the role of the gas composition on formation of reactive oxygen species (ROS) (i.e., hydroxyl radicals – ·OH, hydrogen peroxide – H 2 O 2 , various atomic oxygen species, ozone-O 3 , hydroperoxyl radicals HO 2 ·) and reactive nitrogen species (RNS) (i.e., nitrogen oxides – NO, NO 2 , N 2 O - collectively termed NO X , nitrite-NO 2 - , nitrate-NO 3 - , peroxynitrite-ONOO - ). The hydroxyl radical is the critical species in many chemical oxidation reactions for chemical degradation of toxic compounds in water and gases and for synthesis of some compounds. The mixture of various nitrogen oxide species is important for many biochemical and biological processes involved in biomedical and agricultural applications including disinfection and fertilizer production. The present proposal focuses on determination of the effects of time resolved electron density and hydroxyl radicals on plasma chemical reactions through collaboration with the Princeton Collaborative Low Temperature Plasma Research Facility (PCRF) at the Princeton Plasma Physics Laboratory (PPPL). In order to further investigate the role of the plasma generated electrons and hydroxyl radicals on the overall formation of the key species including hydrogen peroxide, hydroxyl radicals, and nitrogen oxides, the proposed work, thus seeks to determine high resolution time resolved electron density by optical emissions spectroscopy and time resolved hydroxyl radicals using laser induced fluorescence in the nanosecond discharge reactor. The combination of data on electron density and hydroxyl radical concentration will be utilized in the present work to more fully characterize the chemical reaction processes in this system and to advance the design, development, and operation of such chemical reactors for a wide range of applications.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Thin-film lithium niobate on diamond as a platform for efficient spin-phonon coupling

Negatively charged silicon vacancy (SiV − ) centers in diamond are leading candidates for solid-state quantum memory that can be controlled using electromagnetic or acoustic waves. The latter are particularly promising due to the strong strain response of SiV − , enabling large spin-phonon interaction strengths. Indeed, coherent spin control via surface acoustic waves (SAWs) has been demonstrated and is essential for developing on-chip phononic quantum networks. However, the absence of piezoelectricity in diamond requires an interface with a piezoelectric material for efficient transduction and delivery of acoustic waves to spins in diamonds. Here, we demonstrate a heterogeneously integrated phononic platform that combines thin-film lithium niobate with diamond to enable acoustic control of single SiV − spins. Additionally, leveraging large SAW-induced strain at the location of SiV − , we achieve coherent acoustic control of an electron spin with more than twofold improvement in Rabi frequency compared to state-of-the-art devices based on aluminum nitride on diamond. Furthermore, this work represents a crucial step towards realizing phonon-based quantum information processing systems.

Optically detected magnetic resonance↗

DOE OSTI2021

Redox-stable symmetrical solid oxide fuel cells with exceptionally high performance enabled by electrode/electrolyte diffuse interface

Here, in this study, we report a high performance and redox-stable symmetrical solid oxide fuel cell (SOFC) based on (Ba 0.5 Sr 0.5 ) (Mo 0.1 Fe 0.9 )O 3-δ (BSMF) electrode and La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3-δ (LSGM) electrolyte. BSMF is able to operate both as anode and cathode. Excellent electrocatalytic activity has been achieved on BSMF towards hydrogen oxidation and oxygen reduction. Due to its closely matched lattice parameter to LSGM electrolyte, a unique diffuse interface is formed between BSMF and LSGM. Compared to a clean interface, e.g. BSMF/gadolinium doped ceria interface, this diffuse interface promotes the performance of BSMF electrode 1–1.8 times in 600–800 °C. Polarization resistance of the BSMF/LSGM specimen is as low as 0.047 and 0.007 Ωcm 2 in humidified H 2 and in air at 800 °C, respectively. On the BSMF/LSGM/BSMF symmetrical cell, a maximum power density of 2.28 W/cm 2 is achieved at 800 °C, the highest among with redox-stable ceramic electrodes to the best of our knowledge. Redox stability of this cell is confirmed. The role of anode and cathode is reversed back and forth in different operation modes. No apparent degradation is observed through 4 cycles within a 110 h operation period. These findings demonstrate that (Ba 0.5 Sr 0.5 ) (M o0.1 Fe 0.9 )O 3-δ coupled with LSGM electrolyte is an excellent choice to build a high performance, redox-stable SOFC.

25 ENERGY STORAGE↗