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At least 1,189 records · Page 66
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Quantum state reduction: Generalized bipartitions from algebras of observables

Reduced density matrices are a powerful tool in the analysis of entanglement structure, approximate or coarse-grained dynamics, decoherence, and the emergence of classicality. It is straightforward to produce a reduced density matrix with the partial-trace map by tracing out part of the quantum state, but in many natural situations this reduction may not be achievable. We investigate the general problem of identifying how the quantum state is reduced given a restriction on the observables. For example, in an experimental setting, the set of observables that can actually be measured is usually modest (compared to the set of all possible observables) and their resolution is limited. In such situations, the appropriate state-reduction map can be defined via a generalized bipartition, which is associated with the structure of irreducible representations of the algebra generated by the restricted set of observables. One of our main technical results is a general, not inherently numeric, algorithm for finding irreducible representations of matrix algebras. In our work, we demonstrate the viability of this approach with two examples of limited-resolution observables. The definition of quantum state reductions can also be extended beyond algebras of observables. To accomplish this task we introduce a more flexible notion of bipartition, the partial bipartition, which describes coarse grainings preserving information about a limited set (not necessarily algebra) of observables. We describe a variational method to choose the coarse grainings most compatible with a specified Hamiltonian, which exhibit emergent classicality in the reduced state space. We apply this construction to the concrete example of the one-dimensional Ising model. Our results have relevance for quantum information, bulk reconstruction in holography, and quantum gravity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Experimental study of ECH pre-ionization on J-TEXT

An experimental study on electron cyclotron heating (ECH) pre-ionization has been conducted on J-TEXT in support of the joint experiment research for ITER plasma initiation. In this experiment, ECH power was injected to the vessel before the application of loop voltage ionize the neutral gas and form the initial plasma or so-called pre-plasma. The impact of several significant factors, such as magnetic field configuration, pre-fill gas pressure, ECH toroidal injection angle and ECH power on the evolution of pre-plasma are systematically studied, aiming to identify shared features, clarify their potential relationship and optimize the discharge parameters to generate a rather high pre-plasma density. By separating ECH power from the inductive start-up, the effect of pre-plasma on tokamak start-up can be observed. A dynamic magnetic configuration facilitates the transition of pre-plasma to tokamak plasma. To assess the influence of pre-plasma density on tokamak start-up, two kinds of magnetic field configurations are examined. While the effect of different pre-plasma densities on tokamak start-up is negligible, a significant difference is observed between pure ohmic start-up and start-up with pre-ionization. The studies presented here show evolutionary trends and threshold values needed to optimize ECH pre-ionization and also a feasible way to improve pre-plasma density and a configuration to stabilize pre-plasma for transition. Eventually, these results may contribute to multi-machine research and physics analysis that can assist ITER with its optimal preparation for first plasma operation.

ECH↗
DOE OSTI2023

Energy management systems for forecasted demand error compensation using hybrid energy storage system in nanogrid

This paper proposes an energy management system (EMS) for nanogrids to balance the power supply and forecasted demand in consideration of forecasting errors arising from high instantaneous demand. The proposed EMS employs a power-balancing optimization process for forecasted demand and a reference power modulation strategy for forecasting errors. This power-balancing optimization utilizes nanogrid sources, such as photovoltaics, fuel cells, and batteries, to meet forecasted demand and a supercapacitor charging process to overcome issues with a low energy density. The proposed reference power modulation strategy is utilized to allocate power from a hybrid energy storage system consisting of a battery and supercapacitor in order to compensate for forecasting errors. In addition, this proposed strategy considers battery and supercapacitor constraints such as the power changing rate and total power limitations. Further, the power-balancing optimization process also operates at faster sampling rate than the reference power modulation process in order to improve the computational efficiency. The performance of the proposed EMS is evaluated using real data obtained from the Korea Electric Power Exchange.

25 ENERGY STORAGE↗
DOE OSTI2021

Stopping-power enhancement from discrete particle-wake correlations in high-energy-density plasmas

Three-dimensional (3D) simulations of electron beams propagating in high-energy-density plasmas using the quasistatic Particle-in-Cell (PIC) code QuickPIC demonstrate a significant increase in stopping power when beam electrons mutually interact via their wakes. Each beam electron excites a plasma wave wake of wavelength ~ 2 π c / ω p e , where c is the speed of light and ω p e is the background plasma frequency. Here we show that a discrete collection of electrons undergoes a beam-plasma-like instability caused by mutual particle-wake interactions that causes electrons to bunch in the beam, even for beam densities n b for which fluid theory breaks down. This bunching enhances the beam's stopping power, which we call “correlated stopping,” and the effect increases with the “correlation number” N b ≡ n b ( c / ω p e ) 3 . For example, a beam of monoenergetic 9.7 MeV electrons with N b = 1 / 8 , in a cold background plasma with n e = 10 26 cm – 3 (450 g cm – 3 DT), has a stopping power of 2.28 ± 0.04 times the single-electron value, which increases to 1220 ± 5 for N b = 64 . The beam also experiences transverse filamentation, which eventually limits the stopping enhancement.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Process and feedstock driven microstructure for laser powder bed fusion of 316L stainless steel

Here in the pursuit of improving additively manufactured (AM) component quality and reliability, fine-tuning critical process parameters such as laser power and scan speed is a great first step toward limiting defect formation and optimizing the microstructure. However, the synergistic effects between these process parameters, layer thickness, and feedstock attributes (e.g. powder size distribution) on part characteristics such as microstructure, density, hardness, and surface roughness are not as well-studied. In this work, we investigate 316L stainless steel density cubes built via laser powder bed fusion (L-PBF), emphasizing the significant microstructural changes that occur due to altering the volumetric energy density (VED) via laser power, scan speed, and layer thickness changes, coupled with different starting powder size distributions. This study demonstrates that there is not one ideal process set and powder size distribution for each machine. Instead, there are several combinations or feedstock/process parameter ‘recipes’ to achieve similar goals. This study also establishes that for equivalent VEDs, changing powder size can significantly alter part density, GND density, and hardness. Through proper parameter and feedstock control, part attributes such as density, grain size, texture, dislocation density, hardness, and surface roughness can be customized, thereby creating multiple high-performance regions in the AM process space.

316L stainless steel↗
DOE OSTI2022

Large-Area (Ag,Cu)(In,Ga)Se 2 Thin-Film Solar Cells with Increased Bandgap and Reduced Voltage Losses Realized with Bulk Defect Reduction and Front-Grading of the Absorber Bandgap

The 1.24 eV bandgap, 18.8% power conversion efficiency Ag-alloyed chalcopyrite (Ag,Cu)(In,Ga)Se 2 (ACIGS) solar cells are characterized to relate voltage and efficiency improvements to electro-optical (EO) characteristics. Shockley-Read-Hall recombination center defect density, identified and characterized through deep level transient spectroscopy and time-resolved photoluminescence (TRPL), is reduced through potassium and copper treatment optimization. Concomitantly, longer minority carrier lifetimes are achieved, which increases open-circuit voltage (V OC ). Near-conduction band defects associated in earlier studies with light-induced current instability are also mitigated. Analysis of charge-carrier dynamics after single- and two-photon excitation is used to separate recombination at the front interface and in the absorber bulk. From TRPL decay simulations, the authors estimate ranges of key solar cell material characteristics: bulk carrier lifetime T bulk = 110-210 ns, charge-carrier mobility u = 110-160 cm 2 V -1 s -1 , and front interface recombination velocity S front = 700-1050 cm s -1 . This lowest-reported S front for ACIGS absorbers originates from the notched conduction band grading, which also makes the impact of the back interface recombination negligible. It is suggested in the results that solar cell performance enhancements can be made most readily with two distinct strategies: improving device architecture and reducing semiconductor defect densities. Using these approaches, power conversion efficiency in large-area solar cells is improved by 1.1% absolute.

14 SOLAR ENERGY↗
DOE OSTI2025

Legacy Metallic Fuel U(Pu)Zr Data Qualification

The Metallic Fuels Irradiation and Physics Database (FIPD) is an organized collection of legacy metallic fuel U(Pu)Zr data, measurements, and reactor conditions from the Experimental Breeder Reactor II (EBR-II) and the Fast Flux Test Facility (FFTF). The database provides a wealth of information and is easily accessed and utilized by the U.S. nuclear industry and the Nuclear Regulatory Commission (NRC). The database contains three categories of data. The first category covers fuel pin fabrication specifications, including fuel slug diameter and length, cladding diameter, smeared density, etc. The second consists of operational conditions, which include axial distributions of power, temperature, fluence, burnup, isotopic density, etc. The third category contains post-irradiation examination (PIE) results, largely collected at facilities now part of the Idaho National Laboratory (INL), formerly part of Argonne National Laboratory -West (ANL-W) and at the Alpha-Gamma Hot Cell Facility (AGHCF) at Argonne National Laboratory, comprising fission gas release and chemistry analysis, profilometry measurements, neutron radiography data, etc. All these data have been organized and preserved in FIPD.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Amine-Assisted Ligand-Exchange Method to Enhance Photovoltaic Parameters in FAPbI3 Nanocrystal Solar Cells

Perovskite colloidal nanocrystals (PeNCs) have exceptional optoelectronic properties and phase stability, making them promising for photovoltaic applications. However, insulating ligands on PeNC surfaces limit the current density and reduce the power conversion efficiency (PCE) in PeNC solar cells (SCs). This study introduces an amine-assisted ligand-exchange (ALE) strategy using 3-phenyl-1-propylamine (3P1P) to effectively remove long ligands from PeNC films. ALE reduced long-chain ligand density without increasing the number of defect states and therefore reduced the exciton-binding energy of FAPbI3 NC films. These changes facilitated exciton dissociation and charge transport in FAPbI3 PeNC SCs. The facilitation of exciton dissociation was due to the increased magnetic dipole interaction between excitons after the ALE process. The use of ALE achieved FAPbI3 PeNC SCs that had an improved short-circuit current density of 17.98 mA/cm2 and a PCE of 15.56% with improved stability after the treatment and negligible hysteresis. This work provides new insight into engineering PeNC films.

amines↗
DOE OSTI2023

The physics basis to integrate an MHD stable, high-power hybrid scenario to a cool divertor for steady-state reactor operation

Abstract Coupling a high-performance core to a low heat flux divertor is a crucial step for ITER and a Fusion Pilot Plant or DEMO. Experiments in DIII-D recently expanded the steady-state hybrid scenario to high density and divertor impurity injection to study the feasibility of a radiating mantle solution. This work presents the physics basis for trade-offs between density, current drive and stability to tearing modes (TMs) at high β. EC power is crucial to tailor the plasma profiles into a passively stable state, and to eject impurities from the core. Off-axis EC depositions decrease the heating efficiency, but calculated electron heat transport coefficients show that this effect is partially mitigated by improved confinement inside the EC deposition. Additionally, the reduction in pressure is recovered by increasing the density. This favourable scaling of confinement with density was observed in high power plasmas for years, and this work provides a comprehensive explanation. ELITE predictions indicate that a path in peeling-ballooning stability opens up for certain conditions of density, power, q 95 and shaping, allowing the edge pressure to continue increasing without encountering a limit. In the core, calculated anomalous fast-ion diffusion coefficients are consistent with density fluctuation measurements in the toroidicity-induced Alfvén eigenmode range, showing that smaller fast-ion losses contribute to the enhanced confinement at high density. The edge integration study shows that divertor heat loads can be reduced with Ne and Ar injection, but this eventually triggers a cascade of n = 1, 2, 3 core TMs. We can now show that impurity radiation in the core is small and it is not the cause for the drop in confinement at high Ar and Ne injection rates. The overlap between the core TMs is consistent with the loss of pressure as estimated by the Belt model for the coupled rational surfaces. Optimization of these trade-offs has achieved plasmas with sustained H 98y2 = 1.7, f GW = 0.7 and ∼85% mantle radiation. The scenario and its variations at higher density and on- vs off-axis EC heating has been studied as a candidate for an integrated solution for several reactor designs, such as ITER, ARC, and the ARIES-ACT1 case, showing promising results in terms of fusion power and gain.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

The discovery of a radio galaxy of at least 5 Mpc

Context. Giant radio galaxies (GRGs, or colloquially ‘giants’) are the Universe’s largest structures generated by individual galaxies. They comprise synchrotron-radiating active galactic nucleus ejecta and attain cosmological (megaparsec-scale) lengths. However, the main mechanisms that drive their exceptional growth remain poorly understood. Aims. To deduce the main mechanisms that drive a phenomenon, it is usually instructive to study extreme examples. If there exist host galaxy characteristics that are an important cause for GRG growth, then the hosts of the largest GRGs are likely to possess them. Similarly, if there exist particular large-scale environments that are highly conducive to GRG growth, then the largest GRGs are likely to reside in them. For these reasons, we aim to perform a case study of the largest GRG available. Methods. We reprocessed the LOFAR Two-Metre Sky Survey DR2 by subtracting compact sources and performing multi-scale CLEAN de-convolutions at 60" and 90" resolution. The resulting images constitute the most sensitive survey yet for radio galaxy lobes, whose diffuse nature and steep synchrotron spectra have allowed them to evade previous detection attempts at higher resolution and shorter wavelengths. We visually searched these images for GRGs. Results. We have discovered Alcyoneus, a low-excitation radio galaxy with a projected proper length l p = 4.99 ± 0.04 Mpc. Both its jets and lobes are detected at very high significance, and the SDSS-based identification of the host, at spectroscopic redshift z spec = 0.24674 ± 6 × 10 -5 , is unambiguous. The total luminosity density at ν = 144 MHz is L ν = 8 ± 1 × 10 25 W Hz -1 , which is below average, though near median (percentile 45 ± 3%) for GRGs. The host is an elliptical galaxy with a stellar mass M* = 2.4 ± 0.4 × 10 11 M ⊙ and a super-massive black hole mass M• = 4 ± 2 × 10 8 M ⊙ , both of which tend towards the lower end of their respective GRG distributions (percentiles 25 ± 9% and 23 ± 11%). The host resides in a filament of the Cosmic Web. Through a new Bayesian model for radio galaxy lobes in three dimensions, we estimate the pressures in the megaparsec-cubed-scale northern and southern lobes to be P min,1 = 4.8 ± 0.3 × 10 -16 Pa and P min,2 = 4.9 ± 0.6 × 10 -16 Pa, respectively. The corresponding magnetic field strengths are B min,1 = 46 ± 1 pT and B min,2 = 46 ± 3 pT. Conclusions. We have discovered what is in projection the largest known structure made by a single galaxy – a GRG with a projected proper length l p = 4.99 ± 0.04 Mpc. The true proper length is at least l min = 5.04 ± 0.05 Mpc. Beyond geometry, Alcyoneus and its host are suspiciously ordinary: the total low-frequency luminosity density, stellar mass, and super-massive black hole mass are all lower than, though similar to, those of the medial GRG. Thus, very massive galaxies or central black holes are not necessary to grow large giants, and, if the observed state is representative of the source over its lifetime, neither is high radio power. A low-density environment remains a possible explanation. The source resides in a filament of the Cosmic Web, with which it might have significant thermodynamic interaction. The pressures in the lobes are the lowest hitherto found, and Alcyoneus therefore represents the most promising radio galaxy yet to probe the warm–hot inter-galactic medium.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Coupled neutronic-thermal-hydraulic simulations of the European SFR core

Within the European SFR (Sodium-cooled Fast Reactor) - Safety Measures Assessment and Research Tools (ESFR-SMART) project, steady-state coupled simulation of the ESFR core has been performed using several core analysis packages, with the objective of quantifying the coupling effect. Focus is on the fuel Doppler effect and coolant expansion effect. Standalone neutronics calculations in TRACE/PARCS (PSI), DYN3D (HZDR) and WIMS (Jacobs) showed superb agreement with the reference Serpent power distribution (root mean square - rms discrepancies of 1.3%, 1.5% and 0.7% respectively). Results for COUNTHER (CIEMAT) were also in reasonable agreement, but with a somewhat higher discrepancy of 3.7%. Temperature distributions from thermal-hydraulic calculations were also compared and are found to be in good agreement. The effect of Doppler and coolant density feedback on core power distribution was predicted by TRACE/PARCS, DYN3D and WIMS to be between 0.4% and 0.8% rms difference in assembly powers. Reactivity coefficients for perturbations in the inlet temperature, flow rate and core power were shown to be negative for these three codes, with values of roughly -0.5 pcm/C. degree, -0.3 pcm/C. degree and -3.5 pcm/C. degree respectively. A preliminary investigation of differential thermal expansion effects indicates that this may have a significant effect on core power distribution of a few %, greater than anticipated a priori and may warrant inclusion in coupled core analysis to ensure the accurate calculation of power distributions. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2023

Study on divertor detachment and pedestal characteristics in the DIII-D upper closed divertor

Abstract Experiments performed in DIII-D demonstrate that higher plasma current and heating power combined with impurity seeding facilitate the achievement of divertor detachment with a higher pedestal pressure and higher plasma performance in H-mode plasmas with a baffled closed divertor compared with an open divertor. Dedicated experiments were carried out to study the impact of power, plasma current and impurity seeding on divertor detachment with ion B × ∇ B directed into the divertor favorable for the L–H transition. With a factor of three variation in heating power and with only D 2 puffing, no significant difference in the separatrix density at detachment onset was found. The higher heating power leads to higher impurity concentration and wider scrape-off layer (SOL) width, and reduces the detachment onset density to one similar to that in lower-power plasmas. Higher current requires higher pedestal and line-averaged densities to achieve divertor detachment; however, the increase in separatrix density at increasing plasma current is found to be less pronounced. Initial calculations found that both power scan and plasma current scan datasets are qualitatively consistent with theory after considering the change in impurity concentration and heat flux width. This also motivates the future extensive study of transport and divertor impurity behavior in order to have a quantitative comparison between experiment and theory. Compared with an open divertor, a closed divertor facilitates detachment onset at ∼40% lower line-averaged plasma density. Additional N 2 seeding facilitates the achievement of detachment at a lower separatrix density and thus a higher pedestal temperature, which is beneficial for advanced tokamak scenarios. Higher heating power requires a higher N 2 puffing rate to achieve the same degree of detachment, while a higher N 2 puffing rate leads to lower detachment onset line-averaged density, both of which agree with theory. In contrast to the narrower pedestal in an open divertor approaching detachment, the pedestal density width in a closed divertor increases with density. The density gradient increases with line-averaged density at higher plasma current, but remains nearly unchanged at lower plasma current. In particular, compared with discharges with low power, at high heating power the pedestal density gradient is much weaker, while the SOL density is significantly higher and wider. At the same plasma current, both pedestal pressure gradient and temperature gradient decrease linearly with the line-averaged density but remain similar across different heating powers. Even with different plasma current and heating power, the normalized pressure gradient remains identical. As a result, achievement of divertor detachment with a higher pedestal pressure and higher plasma performance is shown in a closed divertor, which is important for improving core–edge integration as one of the critical issues for future tokamak fusion reactors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Density limits as disruption forecasters for spherical tokamaks

Fusion power output from spherical tokamaks would benefit from increased confined plasma density, but there exists a limit on the density before confinement is lost and the plasma current is disrupted. This density limit has long been characterized by a simple, global Greenwald limit proportional to the plasma current and inversely proportional to the cross sectional area of the plasma. It is shown that in the database of discharges from the National Spherical Tokamak Experiment (NSTX) and Mega Ampere Spherical Tokamak (MAST) spherical tokamaks, the likelihood of disruption does increase above the Greenwald limit, and especially in the plasma current rampdown phase. The physics of the density limit has been recently theoretically explored through local criteria. Several of these are tested using the disruption event characterization and forecasting (DECAF TM ) code for their potential effectiveness as disruption warning signals. For a limited set of NSTX discharges, a local island power balance criteria was found to be less reliable, presently, than the Greenwald limit. For this work, an empirical critical edge line density and a boundary turbulent transport limit were both tested for MAST-U, which has an electron density profile measurement with high spatial resolution in the outer part of the plasma. Both were found to have similar dependencies on key plasma parameters. In a limited set of MAST-U discharges that appear to disrupt due to rising density at values under the Greenwald limit, crossing of the boundary turbulent transport limit occurred close to the time of disruption. Finally, these limits were evaluated for their potential use in real-time, and it was found that with the necessary real-time inputs and with refinement through further testing, these limits could be implemented in a real-time disruption forecasting system.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Self-consistent core-pedestal ITER scenario modeling

The purpose of these integrated ITER simulations is to identify dependencies that can impact the performance of ITER. The dependence of fusion power production, temperature and density pedestals, and core profiles on varying magnetic-q, edge density fueling strength, neoclassical transport, magnetic field strength, and alpha heating, are examined. It is noted that ion modes usually dominate the interior, while electron modes dominate the barrier. The electron mode without flow shear is substantially stronger. The q increase tends to cause more kinetic ballooning modes at the edge and the q decrease means that the peeling is getting worse, but the ballooning is getting better. The large edge q tends to provide hollow density while small edge q gives normal density profile. This is consistent with the observation that the density of particles is inversely proportional to the density of the plasma current. The rise in the source of the edge particle increases the density of the edge and the reaction rate close to the edge increases temperature fluxes, resulting in weak pedestal barriers. When neoclassical transport is turned off or the strength of B-field is increased, the pronounced edge barriers are identified. In addition, a distinct effect on the magnetohydrodynamic (MHD) modes is observed due to the increased B-field. The interesting aspect is that the barrier collapses about q = 2 as the stability of MHD has decreased to replace the barrier with a continuous slope but with roughly the same fusion power. This would actually be good for a reactor. The slope of the H-mode pedestal is found to be reduced due to the alpha heating. It is expected that the problem of edge-localized modes causing damage to the first wall will be eased. The effects of circular, elongated, and general geometry on plasma profiles are also compared and contrasted. The circular geometry has a hollow density profile and no edge or internal thermal transport barrier (ETB or ITB). However, both ETBs and ITBs can be found in the elongated geometry. In general geometry, there is a weaker ETB, comparable ITBs, but a higher edge particle transport barrier than in elongated geometry. Higher density near the edge, on the other hand, causes more wall erosion, so elongated geometry might be the best option.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Methanol tolerance of atomically dispersed single metal site catalysts: mechanistic understanding and high-performance direct methanol fuel cells

Proton-exchange membrane fuel cells (PEMFCs) and direct methanol fuel cells (DMFCs) are promising power sources from portable electronic devices to vehicles. The high-cost issue of these low-temperature fuel cells can be primarily addressed by using platinum-group metal (PGM)-free oxygen reduction reaction (ORR) catalysts, in particular atomically dispersed metal–nitrogen–carbon (M–N–C, M = Fe, Co, Mn). Furthermore, a significant advantage of M–N–C catalysts is their superior methanol tolerance over Pt, which can mitigate the methanol cross-over effect and offer great potential of using a higher concentration of methanol in DMFCs. In this work, we investigated the ORR catalytic properties of M–N–C catalysts in methanol-containing acidic electrolytes via experiments and density functional theory (DFT) calculations. FeN 4 sites demonstrated the highest methanol tolerance ability when compared to metal-free pyridinic N, CoN 4 , and MnN 4 active sites. The methanol adsorption on MN 4 sites is even strengthened when electrode potentials are applied during the ORR. The negative influence of methanol adsorption becomes significant for methanol concentrations higher than 2.0 M. However, the methanol adsorption does not affect the 4e - ORR pathway or chemically destroy the FeN 4 sites. The understanding of the methanol-induced ORR activity loss guides the design of promising M–N–C cathode catalyst in DMFCs. Accordingly, we developed a dual-metal site Fe/Co–N–C catalyst through a combined chemical-doping and adsorption strategy. Instead of generating a possible synergistic effect, the introduced Co atoms in the first doping step act as “scissors” for Zn removal in metal–organic frameworks (MOFs), which is crucial for modifying the porosity of the catalyst and providing more defects for stabilizing the active FeN 4 sites generated in the second adsorption step. The Fe/Co–N–C catalyst significantly improved the ORR catalytic activity and delivered remarkably enhanced peak power densities (i.e., 502 and 135 mW cm -2 ) under H 2 –air and methanol–air conditions, respectively, representing the best performance for both types of fuel cells. Notably, the fundamental understanding of methanol tolerance, along with the encouraging DMFC performance, will open an avenue for the potential application of atomically dispersed M–N–C catalysts in other direct alcohol or ammonia fuel cells.

25 ENERGY STORAGE↗
DOE OSTI2023

Accurate prediction of global-density-dependent range-separation parameters based on machine learning

In this work, we develop an accurate and efficient XGBoost machine learning model for predicting the global-density-dependent range-separation parameter, ωGDD, for long-range corrected functional (LRC)-ωPBE. This ωGDDML model has been built using a wide range of systems (11 466 complexes, ten different elements, and up to 139 heavy atoms) with fingerprints for the local atomic environment and histograms of distances for the long-range atomic correlation for mapping the quantum mechanical range-separation values. The promising performance on the testing set with 7046 complexes shows a mean absolute error of 0.001 117 a0−1 and only five systems (0.07%) with an absolute error larger than 0.01 a0−1, which indicates the good transferability of our ωGDDML model. In addition, the only required input to obtain ωGDDML is the Cartesian coordinates without electronic structure calculations, thereby enabling rapid predictions. LRC-ωPBE(ωGDDML) is used to predict polarizabilities for a series of oligomers, where polarizabilities are sensitive to the asymptotic density decay and are crucial in a variety of applications, including the calculations of dispersion corrections and refractive index, and surpasses the performance of all other popular density functionals except for the non-tuned LRC-ωPBE. Finally, LRC-ωPBE (ωGDDML) combined with (extended) symmetry-adapted perturbation theory is used in calculating noncovalent interactions to further show that the traditional ab initio system-specific tuning procedure can be bypassed. The present study not only provides an accurate and efficient way to determine the range-separation parameter for LRC-ωPBE but also shows the synergistic benefits of fusing the power of physically inspired density functional LRC-ωPBE and the data-driven ωGDDML model.

Chemistry↗