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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Rational Design of Weakly‐Solvating Molecules for Salt‐In‐Pre‐Ionic‐Liquid Electrolytes for Li Metal Batteries

Lithium metal batteries (LMBs) promise step‐changes in energy densities but suffer from poor cycle life due to unstable electrolyte‐lithium interfaces. Conventional carbonate electrolytes exhibit excessive lithium‐ion solvation and low oxidative stability, leading to rapid capacity loss. Herein, we report a rationally designed weakly‐solvating cyclic sulfonamide, 1‐trifluoromethanesulfonyl)amide pyrrolidine (TFMSPyr), which integrates an electron‐withdrawing trifluoromethanesulfonyl functional group at pyrrolidinic‐N. TFMSPyr acts as a pre‐ionic‐liquid solvent that forms intrinsically localized, anion‐dominated solvation, coupling molecular architecture, solvation topology, and transport dynamics. As a result, LiFSI based salt‐in‐pre‐ionic‐liquid (SIPIL) electrolytes exhibit high lithium‐ion transference number, oxidative stability > 5 V versus Li/Li + and anion‐derived solid electrolyte interphases (SEI). Li||Cu cells with SIPIL deliver a first cycle Coulombic efficiency (CE) of ≈ 99% with average CE of 99.2% for 100 cycles, and lithium half‐cells with lithium iron phosphate (LFP) cathode exhibit 82% capacity retention after 400 cycles with CE of 99.98%. In anode‐free full cells, 95% of initial capacity is retained after 63 cycles with an average CE of 99.5%. These results demonstrate that molecular engineering of solvents offers a powerful pathway to stabilize lithium metal interfaces and enable practical Anodeless LMBs.

25 ENERGY STORAGE↗
DOE OSTI2021

Photodissociation and Infrared Spectroscopy of Uranium–Nitrogen Cation Complexes

Laser vaporization of uranium in a pulsed supersonic expansion of nitrogen is used to produce complexes of the form U + (N 2 ) n (n = 1–8). These ions are mass selected in a reflectron time-of-flight spectrometer and studied with visible and UV laser fixed-frequency photodissociation and with tunable infrared laser photodissociation spectroscopy. The dissociation patterns and spectroscopy of U + (N 2 ) n indicate that N 2 ligands are intact molecules and that there is no insertion chemistry resulting in UN + or NUN + . Fixed frequency photodissociation at 532 and 355 nm indicate that the U + –N 2 bond dissociation energy varies little with changing coordination. The photon energy and the number of ligands eliminated allow an estimate of the average U + –N 2 dissociation energy of 12 kcal/mol. Infrared bands are observed for these complexes near the N–N stretch vibration via elimination of N 2 molecules. These resonances are observed to be shifted about 130 cm–1 to the red from the free-N 2 frequency for complexes with n = 3–8. Density functional theory indicates that U + is most stable in the sextet state in these complexes and that N 2 molecules bind in end-on configurations. Furthermore, the fully coordinated complex is predicted to be U + (N 2 ) 8 , which has a cubic structure. The vibrational frequencies predicted by theory are consistently lower than those in the experiment, independent of the isomeric structure or spin state of the complexes. Despite its failure to reproduce the infrared spectra, theory provides an average U + –N 2 dissociation energy of 11.8 ± 0.5 kcal/mol, in good agreement with the value from the experiments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Revisiting the Growth Mechanism of Hierarchical Semiconductor Nanostructures: The Role of Secondary Nucleation in Branch Formation

Although advances in synthesizing hierarchical semiconductor materials, there have been few studies on the fundamental nucleation mechanisms to explain the origins of such complex structures. Resolving these nucleation and growth pathways is very difficult and time consuming, but is critical for developing predictive synthetic capabilities for the synthesis and applications of new materials. In this paper, we use state-of-the-art in-situ liquid phase scanning electron microscopy (SEM) and high-resolution transmission electron microscopy in combination of classical Density Functional Theory (cDFT) to study the nucleation of highly-branched wurtzite ZnO nanostructures via a facile, room temperature aqueous synthesis route. Using a range of precursor concentrations, we systematically vary their hierarchical organization. In situ liquid phase SEM demonstrates that all branches form through secondary nucleation and grow by classical processes. Neither random aggregation nor oriented attachment is observed. cDFT results imply the morphological evolution with increasing [Zn 2+ ] arises from an interplay between rising thermodynamic driving force, which promotes branch number and variability of orientation, and increasing barriers to interfacial transport due to ion correlation forces that alter the anisotropic kinetics of growth. Finally, these findings provide a quantitative picture of branching that sets to rest past controversies and advances efforts to decipher growth mechanisms of hierarchical structures in real solution environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

A New Class of Ionically Conducting Fluorinated Ether Electrolytes with High Electrochemical Stability

Increasing battery energy density is greatly desired for applications such as portable electronics and transportation. However, many next-generation batteries are limited by electrolyte selection because high ionic conductivity and poor electrochemical stability are typically observed in most electrolytes. For example, ether-based electrolytes have high ionic conductivity but are oxidatively unstable above 4 V, which prevents the use of high-voltage cathodes that promise higher energy densities. In contrast, hydrofluoroethers (HFEs) have high oxidative stability but do not dissolve lithium salt. Here, we synthesize a new class of fluorinated ether electrolytes that combine the oxidative stability of HFEs with the ionic conductivity of ethers in a single compound. We show that conductivities of up to 2.7 × 10 –4 S/cm (at 30 °C) can be obtained with oxidative stability up to 5.6 V. The compounds also show higher lithium transference numbers compared to typical ethers. Furthermore, we use nuclear magnetic resonance (NMR) and molecular dynamics (MD) to study their ionic transport behavior and ion solvation environment, respectively. Finally, we demonstrate that this new class of electrolytes can be used with a Ni-rich layered cathode (NMC 811) to obtain over 100 cycles at a C/5 rate. The design of new molecules with high ionic conductivity and high electrochemical stability is a novel approach for the rational design of next-generation batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2003

Cycle Trades for Nuclear Thermal Rocket Propulsion Systems

Nuclear fission has been used as a reliable source for utility power in the United States for decades. Even in the 1940's, long before the United States had a viable space program, the theoretical benefits of nuclear power as applied to space travel were being explored. These benefits include long-life operation and high performance, particularly in the form of vehicle power density, enabling longer-lasting space missions. The configurations for nuclear rocket systems and chemical rocket systems are similar except that a nuclear rocket utilizes a fission reactor as its heat source. This thermal energy can be utilized directly to heat propellants that are then accelerated through a nozzle to generate thrust or it can be used as part of an electricity generation system. The former approach is Nuclear Thermal Propulsion (NTP) and the latter is Nuclear Electric Propulsion (NEP), which is then used to power thruster technologies such as ion thrusters. This paper will explore a number of indirect-NTP engine cycle configurations using assumed performance constraints and requirements, discuss the advantages and disadvantages of each cycle configuration, and present preliminary performance and size results. This paper is intended to lay the groundwork for future efforts in the development of a practical NTP system or a combined NTP/NEP hybrid system.

White, C.↗
DOE OSTI2020

Laser-plasma instabilities in long scale-length plasmas relevant to shock-ignition

We present 2D particle-in-cell simulations of laser-plasma instabilities (LPI) performed using conditions relevant to experiments on the OMEGA and NIF laser facilities. The laser intensity used is 2×10 15 W cm -2 , which allows comparison with previous experiments and simulations investigating shock ignition, though this is a relatively low intensity for the scheme. We find that the large convective gain of the instabilities leads to dynamics that are largely controlled by pump depletion and to scattering or absorption by LPIs predominantly occurring away from the quarter-critical density. The two-plasmon decay (TPD) instability is dominant for OMEGA-type conditions and remains important at the NIF-scale. In both cases, most absorption from TPD occurs near its Landau cutoff density, and we examine its nonlinear dynamics in this region, focusing on the ion-acoustic waves responsible for saturation. For NIF-type conditions, stimulated Raman scattering (SRS) and stimulated Brillouin scattering divert significant fractions of laser energy, and we find that SRS backscatter can occur with high gain at low densities due to kinetic effects. An in-depth analysis of hot-electron production is performed to identify the main sources and their characteristic electron temperature. For both simulations presented, the overall hot-electron temperature lies between 30 and 35 keV. This is relatively low and will likely increase shock pressure; however, the distributions also contain a significant number of high-energy (E k >100 keV) electrons that would likely cause unacceptable preheat. We, therefore, suggest some strategies that may be utilized to minimize this high-energy component. I. INTROD

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

High Energy Aqueous Lithium-Ion Batteries (Final Report)

Lithium-ion batteries (LIBs) are a widely used energy storage device. For decades, researchers have been studying aqueous electrolytes due to their non-flammability and environmental friendless. However, the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) of water greatly limit the voltage window of the aqueous electrolyte. The recent concept of ‘solvent-in-salt’ electrolytes, namely ‘water-in-salt’ electrolytes (WISE) for aqueous batteries and ‘super-concentrated’ electrolytes for non-aqueous batteries, greatly expands the electrochemical window of these battery systems and consequently their energy density. This expansion occurs because the large number of salt aggregates in ‘solvent-in-salt’ electrolytes enables preferential salt decomposition over solvent decomposition to form robust interphase layers on electrodes, thus enhancing their stability in a wide range of operating voltages. However, even when the salt concentration reached 63m, regardless of cost, the cathodic potential of the WISE expanded only to 1.75V with an overall electrochemical stability window of <3.25V. To design the next generation of high energy aqueous LIBs, electrolytes that possess a wider electrochemical stability window and lower cost but still maintain the merit of non-flammability are much needed. In this project, we designed the aqueous LIBs with widened voltage window. We reported a cheap and non-flammable ternary eutectic electrolyte that can form a robust solid electrolyte interface (SEI)so that the cathodic limiting potential can be decreased to <1.5 V for Li 4 Ti 5 O 12 anodes, while maintaining both a high ionic conductivity of >10 -3 S cm –1 and a low viscosity. We demonstrated the super-stable2.5V LiMn 2 O 4 ||Li 4 Ti 5 O 12 pouch cell with mass loading of 2.5 mAh/cm. Further, LiCl-LiBr-Graphite/Li full cells were designed with high energy density. Finally, we use a bi-layer design to enlarge the voltage window of aqueous electrolyte, which can endow the stable cycling of aqueous Lithium metal batteries.

25 ENERGY STORAGE↗
NASA NTRS1972

Electrostatic instability of ring current protons beyond the plasmapause during injection events

The stability of ring current protons with an injection spectrum modeled by an m = 2 mirror distribution function was examined for typical ring current parameters. It was found that the high frequency loss cone mode can be excited at wave numbers K lambda sub Di about = to 0.1 to 0.5, at frequencies omega about = to (0.2 to 0.6) omega sub pi and with growth rates up to gamma/omega about = to 0.03. These waves interact with the main body of the proton distribution and propagate nearly perpendicular to the local magnetic field. Cold particle partial densities tend to reduce the growth rate so that the waves are quenched at or near to the plasmapause boundary. Wave e-folding lengths are comparable to 0.1 R sub e, compared to the value of about 4 R sub e found for ion cyclotron waves at the same plasma conditions.

Coroniti, F. V.↗
DOE OSTI2023

Two-dimensional spin systems in PECVD-grown diamond with tunable density and long coherence for enhanced quantum sensing and simulation

Systems of spins engineered with tunable density and reduced dimensionality enable a number of advancements in quantum sensing and simulation. Defects in diamond, such as nitrogen-vacancy (NV) centers and substitutional nitrogen (P1 centers), are particularly promising solid-state platforms to explore. However, the ability to controllably create coherent, two-dimensional spin systems and characterize their properties, such as density, depth confinement, and coherence, is an outstanding materials challenge. We present a refined approach to engineer dense (≳1 ppm ∙ nm), 2D nitrogen, and NV layers in diamond using delta-doping during plasma-enhanced chemical vapor deposition epitaxial growth. We employ both traditional materials techniques, e.g., secondary ion mass spectrometry, alongside NV spin decoherence-based measurements to characterize the density and dimensionality of the P1 and NV layers. We find P1 densities of 5–10 ppm ∙ nm, NV densities between 1 and 3.5 ppm ∙ nm tuned via electron irradiation dosage, and depth confinement of the spin layer down to 1.6 nm. We also observe high (up to 0.74) ratios of NV to P1 centers and reproducibly long NV coherence times, dominated by dipolar interactions with the engineered P1 and NV spin baths.

36 MATERIALS SCIENCE↗
NASA NTRS1981

Energetic oxygen and sulfur ions in the Jovian magnetosphere

Observations of 1 to 20 MeV/nuc oxygen, sodium, and sulfur ions in the Jovian magnetosphere are reported. Measurements made by the cosmic ray subsystem on Voyager 1 and 2 were used to calculate abundances and energy spectra in the region from 5 to 20 Jovian radii. The phase space density of the oxygen ions calculated from the spectra has a positive radial gradient between 6 and 17 Jovian radii, indicating an inward diffusive flow. The diffusion coefficient upper limit at 9 Jovian radii is approximately 10 to the -5 power/s. This limit, combined with the analysis of Voyager plasma observations by Siscoe et al.1981, implies an upper limit to the mass loading rate near Io of approximately 10 to the 28th power ions/s. The energetic oxygen lifetime is within an order of magnitude of the strong pitch-angle diffusion lifetime in this region, with the largest total number of particles lost between 7.5 and 12.5 Jovian radii. It is shown that the losses are not due to geometric absorption by Io, absorption by dust grains, or energy loss in the plasma of the inner magnetosphere, and it is therefore postulated that the primary loss mechanism is pitch-angle scattering into the loss cone.

Gehrels, N.↗
NASA NTRS1992

Dielectronic recombination as a function of electric field strength

Dielectronic recombination (DR) is the dominant recombination mechanism at coronal temperatures and densities. We present a procedure for calculating DR rate coefficients as a function of electric field strength and apply this method to carbon ions. We focus on the competing effects of enhancement by plasma microfields and rate decrease through collisional excitation and ionization. We find that, in the case of C(3+), a significant rate enhancement results, leading to a reinterpretation of C IV emission-line intensities in the sun and late-type stars. We further consider how macroscopic electric fields, in particular motional electric fields, can affect DR rate coefficients, demonstrating dramatic rate increases for a number of the carbon ions.

Reisenfeld, Daniel B.↗
DOE OSTI2022

Critical role of magnetic moments in heavy-fermion materials: Revisiting mysteries of SmB 6

Heavy-fermion family exhibits fascinating and often puzzling properties due to the presence of open-shell f ions and the complexity of the associated charge, orbital, and spin degrees of freedom. SmB 6 is a prototypical heavy-fermion compound that is electrically insulating but yet it displays quantum oscillations, which are a telltale signature of the metallic state. Adding to the enigma is the possibility that SmB 6 is a topological Kondo insulator. Here, by treating the spin degree of freedom on an equal footing with other degrees of freedom using the parameter-free strongly-constrained and appropriately-normed (SCAN) density functional, we explore the ground-state electronic structure of SmB6. A number of competing magnetic phases lying very closely in energy are found, indicating the key role of spin fluctuations in the material. The computed band structure, crystal-field splittings in the f-electron complex, the heavy effective electron mass at the Fermi energy, and the large specific heat are all in good agreement with the corresponding experimental results. In particular, our predicted FS explains the experimentally observed bulk quantum oscillations as well as the low electrical conductivity of SmB 6 . The topological Kondo state of SmB6 is shown to be robust regardless of its magnetic configuration. The excellent performance of SCAN in heavy-fermion systems is explained in terms of its ability to treat self-interaction errors and symmetry breaking within the framework of the density functional theory. Our study provides a new approach for modeling heavy-fermion materials

36 MATERIALS SCIENCE↗
NASA NTRS2016

Simultaneous Observations of Atmospheric Tides from Combined in Situ and Remote Observations at Mars from the MAVEN Spacecraft

We report the observations of longitudinal variations in the Martian thermosphere associated with nonmigrating tides. Using the Neutral Gas Ion Mass Spectrometer (NGIMS) and the Imaging Ultraviolet Spectrograph (IUVS) on NASA's Mars Atmosphere and Volatile EvolutioN Mission (MAVEN) spacecraft, this study presents the first combined analysis of in situ and remote observations of atmospheric tides at Mars for overlapping volumes, local times, and overlapping date ranges. From the IUVS observations, we determine the altitude and latitudinal variation of the amplitude of the nonmigrating tidal signatures, which is combined with the NGIMS, providing information on the compositional impact of these waves. Both the observations of airglow from IUVS and the CO2 density observations from NGIMS reveal a strong wave number 2 signature in a fixed local time frame. The IUVS observations reveal a strong latitudinal dependence in the amplitude of the wave number 2 signature. Combining this with the accurate CO2 density observations from NGIMS, this would suggest that the CO2 density variation is as high as 27% at 0-10 deg latitude. The IUVS observations reveal little altitudinal dependence in the amplitude of the wave number 2 signature, varying by only 20% from 160 to 200 km. Observations of five different species with NGIMS show that the amplitude of the wave number 2 signature varies in proportion to the inverse of the species scale height, giving rise to variation in composition as a function of longitude. The analysis and discussion here provide a roadmap for further analysis as additional coincident data from these two instruments become available.

atmospheric tides↗
DOE OSTI2025

Structural Evolution of Mixed-Addenda Keggin Polyoxometalate Anions with Atom-by-Atom Substitution

Polyoxometalates (POMs) are molecular metal oxides with distinctive electronic properties that make them promising materials for applications in energy, sensors, and memory devices. One of the most promising methods of tuning the stability, photochromic, redox, and electron-spin properties of POMs is through the substitution of the metal “addenda” atoms that, along with oxygen, constitute their cage-like structures. Because traditional synthesis methods typically produce a distribution of POMs, the isolation and characterization of multimetallic POMs with predetermined stoichiometry remains challenging. The presence of multiple energetically accessible isomers further complicates the experimental characterization and theoretical modeling of multimetallic POMs. Herein, we leverage the distinguishing mass-selection capabilities of ion soft landing to prepare stoichiometrically selected Keggin PMo x W 12-x O 40 3- (x = 0 – 6, 8, 10, and 12) POMs on self-assembled monolayer surfaces free of the solvent molecules and counterions that often confound characterization of complex species at interfaces. The structures of the supported POMs are characterized with atom-by-atom precision using in situ infrared (IR) reflection absorption spectroscopy complemented by detailed density functional theory calculations. Our joint experimental and theoretical results reveal an almost linear shift in the positions of the IR bands towards lower wavenumbers with an increase in the number of lighter molybdenum atoms compared to heavier W atoms in PMoxW 12-x O 40 3- . The theoretical calculations also indicate that numerous isomeric structures may be populated at the experimental conditions and, consequently, contribute to the overall IR spectra. In conclusion, our findings indicate that in addition to the number of substituted addenda atoms and the presence of multiple isomeric structures, interactions with the surface play an important role in determining the IR spectra and structure of supported bimetallic POMs.

Prabhakaran, Venkateshkumar [Pacific Northwest Nat↗
DOE OSTI2024

Structural and optical characterization of dilute Bi-doped GaN nanostructures grown by molecular beam epitaxy

We have carried out detailed studies on the epitaxy and characterization of dilute Bi-doped GaN nanostructures. A comprehensive investigation of Bi-doped GaN nanowires and quasi-film epitaxial growth conditions has been performed. Scanning electron microscopy studies show that lowering the GaBiN growth temperature causes gradual changes in top c-plane nanowire morphology due to the incremental incorporation of foreign Bi atoms. This trend is further substantiated by the secondary ion mass spectroscopy analysis of a multi-layer Bi-doped GaN quasi-film. However, it is also found that the amount of Bi incorporation into the GaN lattice is relatively independent of the N2 flow rate variation under the growth conditions investigated. Furthermore, room-temperature micro-Raman spectra show that there are additional peaks near 530, 650, and 729 cm−1 wave numbers in the Bi-doped GaN samples, which can primarily be attributed to Bi local vibrational modes, indicative of a small amount of Bi incorporation in the GaN lattice. Moreover, phonon calculations with density functional theory indicate that Bi replacing the N sites is the likely origin of the experimentally measured Raman modes. X-ray photoelectron spectroscopy measurements have also been obtained to deduce the electronic interaction between the Bi dopant atom and the GaN nanostructure. Such one-dimensional nanowires permit the synthesis of dislocation-free highly mismatched alloys due to strain relaxation, allowing efficient light absorption and charge carrier extraction that is relevant for solar energy harvesting and artificial photosynthesis.

Materials Science↗
DOE OSTI2025

HfNb_BCC_SolidSolution_128atoms_VASP6

We performed density functional theory (DFT) calculations for body-centered-cubic (BCC) structures with 128 lattices sites of solid solution binary alloys hafnium-niobium (Hf-Nb). The electronic structures of alloys have been calculated using Vienna Ab initio Simulation Package (VASP). Within this package the DFT approach is used to reduce many-body Schrodinger equation to set of single particle Kohn-Sham (KS) equations. The generalized electronic exchange-correlation functional is described by generalized gradient approximation with the Perdew-Burke-Ernzerhof parametrization. The electron-ion interactions is described by pseudopotentials developed within the plane-wave basis projector augmented-wave (PAW) approach. These pseudopotentials are available at the VASP portal (http://cms.mpi.univie.ac.at/vasp/). Our calculations have been run with the pseudopotentials treating s and p semi-core states as valence in case for the elements Hf and Nb. The electronic densities and potentials are expanded over plane-waves with energy cutoff of 350 eV. 2x2x2 k-mesh and normal precision were used. The alloys were modeled by supercell containing 128 randomly distributed atoms. At initial step the atoms occupy perfect BCC lattice cites. This initial structure was optimized until energy changes less than 1e-6 eV, while forces acting on atoms don't exceed 1e-2 eV/angstrom. The electron-ion interaction is described by PAW pseudopotentials. The calculations have been collected by sampling chemical compositions across the entire compositional range. The chemical compositions have been sampled by progressively changing the number of atoms per constituent by 4. For each chemical composition of binaries and ternaries, the first-principle calculations have been run for 100 randomized arrangements of the constituents on the BCC lattice sites. We collected data for a total of 3,029 randomized atomic structures over 31 chemical compositions. Further methodological and structural information is contained in the dataset README.txt file.

36 MATERIALS SCIENCE↗
NASA NTRS1995

High latitude ion composition

A data base comprised of all available ionosphere satellite ion composition measurements - the Goddard Comprehensive Ionosphere Data Base (GCID) - has been set upon optical disks for convenient merging and accessing of data from different satellites. This data has recentely been expanded to include all accessible satellite electron density and plasma temperature measurements. This paper demonstrates with a couple examples, the potential of GCID as an alternative to empirical models for undertanding ionsophere physics and chemistry. Through binning techniques GCID provdes a tool that complements and improves on the International Reference Ionosphere model (IRI) in delineating the topology of high latitude ion composition. GCID provides at a glance a measure of the local statistical variabilty of the ion compostions that is not in empirical models such as IRI. Furthermusing the data to determine the spatial and geophysical parameter range over which the minor ion species are approximately in chemical equilibrium, the number of data points available for empirical ion composition models can be increased by using the statiscally more reliable neutral and electron empirical models to derive ions composition. Currently available empirical models are not capable of adequately defining the comples high latitude distribution - a measure of the variablity is needed.

Grebowsky, J. M.↗
DOE OSTI2019

Making many-body interactions nearly pairwise additive: The polarized many-body expansion approach

The Many-Body Expansion (MBE) is a useful tool to simulate condensed phase chemical systems, often avoiding the steep computational cost of usual electronic structure methods. However, it often requires higher than 2-body terms to achieve quantitative accuracy. In this work, we propose the Polarized MBE (PolBE) method where each MBE energy contribution is treated as an embedding problem. In each energy term, a smaller fragment is embedded into a larger, polarized environment and only a small region is treated at the high-level of theory using embedded mean-field theory. The role of polarized environment was found to be crucial in providing quantitative accuracy at the 2-body level. PolBE accurately predicts noncovalent interaction energies for a number of systems, including CO 2 , water, and hydrated ion clusters, with a variety of interaction mechanisms, from weak dispersion to strong electrostatics considered in this work. We further demonstrate that the PolBE interaction energy is predominantly pairwise unlike the usual vacuum MBE that requires higher-order terms to achieve similar accuracy. We numerically show that PolBE often performs better than other widely used embedded MBE methods such as the electrostatically embedded MBE. Finally,owing to the lack of expensive diagonalization of Fock matrices and its embarrassingly parallel nature, PolBE is a promising way to access condensed phase systems with hybrid density functionals that are difficult to treat with currently available methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗