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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Electroweak Nuclear Properties from Single Molecular Ions in a Penning Trap

Here, we present a novel technique to probe electroweak nuclear properties by measuring parity violation (PV) in single molecular ions in a Penning trap. The trap’s strong magnetic field Zeeman shifts opposite-parity rotational and hyperfine molecular states into near degeneracy. The weak interaction-induced mixing between these degenerate states can be larger than in atoms by more than 12 orders of magnitude, thereby vastly amplifying PV effects. The single molecule sensitivity would be suitable for applications to nuclei across the nuclear chart, including rare and unstable nuclei.

electronic structure of atoms & molecules↗
DOE OSTI2022

Experimental demonstration of necessary conditions for X-ray induced synthesis of cesium superoxide

Absorption of sufficiently energetic X-ray photons by a molecular system results in a cascade of ultrafast electronic relaxation processes which leads to a distortion and dissociation of its molecular structure. Here, in this work, we demonstrate that only decomposition of powdered cesium oxalate monohydrate induced by monochromatic X-ray irradiation under high pressure leads to the formation of cesium superoxide. Whereas, for an unhydrated form of cesium oxalate subjected to the same extreme conditions, only degradation of the electron density distribution is observed. Moreover, the corresponding model of X-ray induced electronic relaxation cascades with an emphasis on water molecules’ critical role is proposed. Our experimental results suggest that the presence of water molecules in initially solid-state systems (i.e. additional electronic relaxation channels) together with applied high pressure (reduced interatomic/intermolecular distance) could potentially be a universal criteria for chemical and structural synthesis of novel compounds via X-ray induced photochemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Molecular weight growth by the phenyl + cyclopentadienyl reaction: Well-skipping, ring-opening, and dissociation

Radical-radical reactions contribute to molecular weight growth of polycyclic aromatic hydrocarbons (PAHs), but their role is not well understood. The phenyl (Ph, C 6 H 5 ) + cyclopentadienyl (C 5 H 5 ) reaction has not been studied but can serve as a surrogate reaction for many reactions of larger aryl-σ radicals with resonance-stabilized π-radicals. The adducts of these reactions easily lose an H atom to produce a new π-radical. Here, through a combination of dilute flash pyrolysis experiments, theory, and simulation, we find that for the title reaction, substantial Ph—C 5 H 4 + H is formed, dominantly by a well-skipping pathway, at conditions around 30 Torr and 1400 K. This radical is thermally stable at moderate temperatures but decomposes at higher temperatures following ring opening of the 5-member ring. Products corresponding to the loss of H, C 2 H 2 , and C 3 H 3 are observed experimentally. Calculation of the C 11 H 9 potential energy surface affirms that these are expected decomposition products and reveals multiple possible pathways.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Design of Ru-Ni diatomic sites for efficient alkaline hydrogen oxidation

Anion exchange membrane fuel cells are limited by the slow kinetics of alkaline hydrogen oxidation reaction (HOR). Here, we establish HOR catalytic activities of single-atom and diatomic sites as a function of *H and *OH binding energies to screen the optimal active sites for the HOR. As a result, the Ru-Ni diatomic one is identified as the best active center. Guided by the theoretical finding, we subsequently synthesize a catalyst with Ru-Ni diatomic sites supported on N-doped porous carbon, which exhibits excellent catalytic activity, CO tolerance, and stability for alkaline HOR and is also superior to single-site counterparts. In situ scanning electrochemical microscopy study validates the HOR activity resulting from the Ru-Ni diatomic sites. Furthermore, in situ x-ray absorption spectroscopy and computational studies unveil a synergistic interaction between Ru and Ni to promote the molecular H 2 dissociation and strengthen OH adsorption at the diatomic sites, and thus enhance the kinetics of HOR.

25 ENERGY STORAGE↗
DOE OSTI2026

Connecting collisional and photofragmentation resonances in the ungerade symmetry states of H 2

A recently developed energy-dependent frame transformation theory that incorporates both ionisation and dissociation channels of the H 2 molecule, is extended to treat the ungerade states that occur both in dissociative recombination and as the final state in ground state photoabsorption. The theoretical treatment includes the rotational degrees of freedom and is benchmarked against a two-dimensional model that can be solved with high accuracy and also compared with photoabsorption experiments. Analysis of the resulting spectra demonstrates how the same resonances appear in very different observables, often with quite different line shapes.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Impact of nitrogen molecular breakup on divertor conditions in JET L-mode plasmas using SOLPS-ITER

SOLPS-ITER simulations of nitrogen-seeded, low-confinement mode plasmas in the Joint European Torus (JET) predict that the electron temperature in the low-field side (LFS) divertor leg is reduced locally by up to an order of magnitude when nitrogen is assumed to recycle as molecules (N 2 ) instead of atoms using a fixed nitrogen injection rate. The LFS divertor temperature reduction under the assumption of molecular recycling occurs due to a three-step mechanism: (1) the plasma penetration of nitrogen atoms is increased due to the strong triple bond of the N 2 molecule and the kinetic energy release in the dissociation event, both mechanisms contributing equally, (2) the abundance of (particularly multiply-charged) nitrogen ions in the divertor is increased and (3) the electron temperature is reduced due to the increase in radiation (by up to a factor of 4) from nitrogen ions. Setting the volume-integrated nitrogen radiated power to a constant value (0.6 MW) instead of the nitrogen injection rate, SOLPS-ITER predicts under the molecular nitrogen recycling assumption that the peak line-integrated N II, N III and N IV intensities in the LFS divertor are approximately within 15%, 35% and 5%, respectively, of the reference atomic nitrogen recycling case. The predicted peak N II, N III and N IV intensities under either assumption are within 30%, 65% and 5%, respectively, of measurements using the vertically viewing mirror-link divertor spectrometer (Meigs et al., 2010) in nitrogen-seeded JET L-mode plasmas (Lomanowski et al., 2019). ERO2.0 simulations using a constant nitrogen seeding rate on static background plasma solutions from EDGE2D-EIRENE (previously presented in Mäenpää et al., (2022), revised here to include fast reflections) predict that N II to N IV line emission is increased by 20% to 30% when nitrogen is assumed to recycle as molecules, demonstrating the importance of considering the effect of molecular dissociation reactions on the divertor plasma in a self-consistent manner.

Divertor↗
DOE OSTI2025

Transmission spectroscopy of CF 4 molecules in intense x-ray fields

The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF 4 . This approach unlocks the direct intrapulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broadband x-ray spectrum. The dynamics with and without initially producing fluorine 𝐾-shell holes are studied by tuning the central photon energy. The absorption spectra are measured at different FEL intensities to observe nonlinear effects. Transient isolated fluorine atoms and ions are spectroscopically recorded within the ultrashort pulse duration of a few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF 4 molecules and charged atomic fragments is observed near the fluorine 𝐾 edge. The dissociation dynamics and the multiphoton absorption-induced dynamics encoded in the spectra are theoretically interpreted. Overall, this study demonstrates the potential of high-intensity x-ray transmission spectroscopy to study ultrafast molecular dynamics with sensitivity to specific intermediate species and their electronic structure.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Diffusion quantum Monte Carlo approach to the polaritonic ground state

Making and using polaritonic states (i.e., hybrid electron-photon states) for chemical applications has recently become one of the most prominent and active fields that connects the communities of chemistry and quantum optics. Modeling of such polaritonic phenomena using ab initio approaches calls for new methodologies, leading to the reinvention of many commonly used electronic structure methods, such as Hartree-Fock, density functional, and coupled cluster theories. Here in this work, we explore the formally exact diffusion quantum Monte Carlo approach to obtain numerical solutions to the polaritonic ground state during the dissociation of the H 2 molecular system. Here, we examine various electron-nuclear-photon properties throughout the dissociation, such as changes to the minimum of the cavity Born-Oppenheimer surface, the localization of the electronic wave function, and the average mode occupation. Finally, we directly compare our results to that obtained with state-of-the-art, yet approximate, polaritonic coupled cluster approaches.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Investigations of atomic and molecular processes of NBI-heated discharges in the MAST Upgrade Super-X divertor with implications for reactors

This experimental study presents an in-depth investigation of the performance of the MAST-U Super-X divertor during NBI-heated operation (up to 2.5 MW) focussing on volumetric ion sources and sinks as well as power losses during detachment. The particle balance and power loss analysis revealed the crucial role of Molecular Activated Recombination and Dissociation (MAR and MAD) ion sinks in divertor particle and power balance, which remain pronounced in the change from ohmic to higher power (NBI heated) L-mode conditions. The importance of MAR and MAD remains with double the absorbed NBI heating. MAD results in significant power dissipation (up to ${\sim} 20\%$ of $P_\textrm{SOL}$), mostly in the cold ($T_e \lt 5$ eV) detached region. Theoretical and experimental evidence is found for the potential contribution of $D^-$ to MAR and MAD, which warrants further study. These results suggest that MAR and MAD can be relevant in higher power conditions than the ohmic conditions studied previously. Post-processing reactor-scale simulations suggests that MAR and MAD can play a significant role in divertor physics and synthetic diagnostic signals of reactor-scale devices, which are currently underestimated in exhaust simulations. This raises implications for the accuracy of reactor-scale divertor simulations of particularly tightly baffled (alternative) divertor configurations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Dynamics of resonant low-energy electron attachment to ethanol-producing hydroxide anions

Here, the dynamics of dissociative electron attachment to ethanol is experimentally investigated at the Feshbach resonance formed with incident electron energies near 9.5 eV. Highly differential laboratory-frame momentum distributions of OH – fragments are measured for a series of energies spanning the resonance width, using the velocity-map-imaging technique. The OH – kinetic-energy distribution indicates that the C-O breaking dissociation process could either be a three-body dissociation or a two-body dissociation with significant rovibrational excited fragments. The small, but significant, anisotropy in the OH – angular distribution provides signatures of the molecular symmetry of the associated resonant state under the axial recoil approximation, which assumes the dissociation is much faster than any rotation of the dissociation axis. Within these assumptions, the 9.5-eV Feshbach resonance can be assigned to the electronic transition from the ($10a'$) orbital with its ground-state C s symmetry to the empty ($4a''$) level, involving the simultaneous electron attachment. This dynamics could be a model for C-O dissociation in larger alcohols and ethers.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

On the Dynamics of the Carbon–Bromine Bond Dissociation in the 1-Bromo-2-Methylnaphthalene Radical Anion

This paper studies the mechanism of electrochemically induced carbon–bromine dissociation in 1-Br-2-methylnaphalene in the reduction regime. In particular, the bond dissociation of the relevant radical anion is disassembled at a molecular level, exploiting quantum mechanical calculations including steady-state, equilibrium and dissociation dynamics via dynamic reaction coordinate (DRC) calculations. DRC is a molecular-dynamic-based calculation relying on an ab initio potential surface. This is to achieve a detailed picture of the dissociation process in an elementary molecular detail. From a thermodynamic point of view, all the reaction paths examined are energetically feasible. The obtained results suggest that the carbon halogen bond dissociates following the first electron uptake follow a stepwise mechanism. Indeed, the formation of the bromide anion and an organic radical occurs. The latter reacts to form a binaphthalene intrinsically chiral dimer. This paper is respectfully dedicated to Professors Anny Jutand and Christian Amatore for their outstanding contribution in the field of electrochemical catalysis and electrosynthesis.

1-bromo-2-methylnaphthalene↗
DOE OSTI2026

Imaging Three-Dimensional Molecular Structure and Dynamics with Multiparticle Covariance and Cumulant Coulomb Explosion Analysis

Coulomb explosion imaging (CEI) provides a direct means of imaging molecular geometry by correlating fragment ion momenta following the fragmentation of a molecular polycation. Here, we demonstrate the use of three-body covariance and four-body cumulant analysis to extract three-dimensional (3D) structural information from the X-ray-induced Coulomb explosion of tert-butyl iodide (C4H9I). Site-selective ionization at the iodine 4d edge with intense femtosecond soft X-ray pulses from an X-ray free-electron laser (XFEL) enables rapid charge buildup and molecular breakup. By correlating ionic fragments in the molecular frame, we isolate complete dissociation channels and reveal subtle structural changes, such as umbrella-type motion of the branched alkyl chain, during the ionization process. Comparison with point-charge simulations of the Coulomb explosion shows close agreement, validating the approach. Furthermore, these results establish covariance/cumulant mapping as a powerful strategy for imaging complex three-dimensional molecular structures and point the way toward time-resolved CEI using both XFEL and tabletop sources for capturing ultrafast structural dynamics.

Imaging↗
DOE OSTI2022

Super‐Hydrophilic Microporous Ni(OH) x /Ni 3 S 2 Heterostructure Electrocatalyst for Large‐Current‐Density Hydrogen Evolution

Abstract Exploiting active and stable non‐precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER) at large current density plays a key role in realizing large‐scale industrial hydrogen generation. Herein, a self‐supported microporous Ni(OH) x /Ni 3 S 2 heterostructure electrocatalyst on nickel foam (Ni(OH) x /Ni 3 S 2 /NF) that possesses super‐hydrophilic property through an electrochemical process is rationally designed and fabricated. Benefiting from the super‐hydrophilic property, microporous feature, and self‐supported structure, the electrocatalyst exhibits an exceptional HER performance at large current density in 1.0 M KOH, only requiring low overpotential of 126, 193, and 238 mV to reach a current density of 100, 500, and 1000 mA cm −2 , respectively, and displaying a long‐term durability up to 1000 h, which is among the state‐of‐the‐art non‐precious metal electrocatalysts. Combining hard X‐rays absorption spectroscopy and first‐principles calculation, it also reveals that the strong electronic coupling at the interface of the heterostructure facilitates the dissociation of H 2 O molecular, accelerating the HER kinetics in alkaline electrolyte. This work sheds a light on developing advanced non‐precious metal electrocatalysts for industrial hydrogen production by means of constructing a super‐hydrophilic microporous heterostructure.

Chemistry↗
DOE OSTI2025

Resolving SPARC–HSA binding kinetics with an ultrasensitive photonic sensor based on bound states in the continuum

Secreted protein acidic and rich in cysteine (SPARC) is critical in cell-matrix interactions and tissue remodeling. It influences tumor progression through its affinity for human serum albumin (HSA) - the most abundant plasma protein, which also plays a crucial role in drug delivery. Strong molecular binding leads to a dissociation constant KD in the nanomolar range. Thus, determining KD requires detecting sub-nanomolar concentrations with ultrasensitive methods. This may be crucial for elucidating the nature of SPARC-HSA binding, as their interaction remains a subject of debate. Capturing these interactions accurately requires a platform capable of resolving rapid binding kinetics at extremely low analyte concentrations. In this work, we report on a microfluidics-integrated photonic nanostructure that supports bound states in the continuum (BICs) and is optimized for studying the fast kinetics of high-affinity protein-protein interactions. The unprecedented capability of detecting sub-nanomolar concentrations allows quantifying KD between SPARC and HSA beyond the state of the art. We leverage an all-dielectric photonic crystal slab (PhCS) sustaining two BIC branches arising from gapped Dirac cone dispersion. HSA is covalently immobilized on the PhCS bonded to a PDMS microfluidic chamber. SPARC dissociation is carried out using PBS buffer (pH 7.4), ensuring complete protein release through precise control of the flow rate and continuous spectral monitoring of the BICs. The measured KD=8.2±0.8 nM confirms the strong affinity of SPARC for HSA. This study highlights the potential of BIC-based sensing as a versatile tool for investigating protein interactions. These results also have implications for the optimization of drug delivery systems and cancer treatment strategies.

Albumin↗
DOE OSTI2024

Gas Stopper Developments for Improved Purity and Intensity of Low-Energy, Rare Isotope Ion Beams (Final Technical Report)

This final technical report summarizes the work of the Michigan State University (MSU) team supported by grant # DE-SC0021423 awarded by the Office of Nuclear Physics, Department of Energy. Objectives: The successful fulfillment of the FRIB science mission hinges on ensuring the availability of fast, stopped, and reaccelerated beams consisting of rare isotopes. This project's research and development focus was dedicated to supporting the advancement and creation of a cutting-edge linear gas stopper. The primary aim is to efficiently convert the high-intensity fast beams of rare isotopes provided by FRIB into high-quality, low-energy beams. These beams are essential for conducting stopped beam experiments or for subsequent reacceleration. The overarching goal is to advance technology, aiming to increase the beam rate capability of the linear gas stopper for medium-to-heavy-mass rare isotopes by more than tenfold compared to the currently most effective gas stopper in operation, and to improve the purity of the delivered beams. Project Description: The existing technology employed in gas stopping devices designed for low-energy, rare-isotope beams presents limitations in both the purity of extracted beams and the intensities of injected beams. These limitations are incompatible with the requirements of the recently commissioned rare isotope beam facility, FRIB. Our research and development efforts, aligned with the previously outlined objectives, focused on addressing the most critical aspects for enhancing beam-rate capability and purity. Specifically, advanced particle-in-cell simulations were developed and integrated into a simulation pipeline to explore the efficacy of multi-layer RF carpets on increasing ion transport efficiency with high incoming beam rates that generate space charge fields which can limit it. We also explored the possibility of using a collision-induced-dissociation (CID) gas cell to break up molecular contaminant ions that are generated during the stopping process. A prototype CID gas cell was constructed and tested with beams from an offline ion source, validating the concept with the successful demonstration of breaking of molecular ions. The outcome of this research enabled the formulation a conceptual design for a next-generation linear gas stopping device specifically tailored for FRIB. This device is envisioned to deliver rare-isotope-ion beams at a rate of 10 8 particles per second or higher, accompanied by advancements in purity. Methods employed: This project leverages advancements in technologies initially designed for the Advanced Cryogenic Gas Stopper (ACGS), the current state-of-the-art linear gas stopper, through the use of new simulations and beam purification via collision-induced-dissociation. The methods include: 1. Development of a prototype low-energy, low-pressure CID gas stopper. This prototype features a thin, approximately 20 nm, Si 3 N 4 entrance window designed for dissociating stable and rare-isotope molecular ions. The goal is to enhance beam purification and overall efficiency. 2. Creation of Particle-in-cell (PIC) simulations to assess the advantages of multi-layer RF carpets and multi-point extraction for ion transport efficiency. These simulations rely on the 3DCylPIC package, specifically designed for studying devices of this nature. The goal is to quantify and mitigate ion transport losses due to space charge generated in the stopping process of large numbers of ions. 3. Perform ion transport simulations across an RF carpet using an 8-phase travelling wave and evaluate its performance. Compared to the 4-phase RF carpets used in ACGS, the 8-phase carpets will double the wavelength of the generated traveling wave allowing for larger maximum RF amplitudes that could result in improved ion transport efficiency for high-intensity incoming beams when large space charge fields are present. Impact: Tackling the primary challenges associated with transforming high-energy projectile fragment beams into low-energy beams—specifically, addressing efficiency and purity—holds significant promise for advancing FRIB science. This advancement will particularly impact precision mass measurements, laser spectroscopy of short-lived nuclei, and studies in astrophysics and nuclear reactions using reaccelerated beams. These domains play a crucial role in addressing key questions outlined in the 2023 NSAC long-range plan, spanning nuclear structure, nuclear astrophysics, and fundamental symmetries. Additionally, they contribute to addressing 10 out of the 17 benchmarks identified by the NRC RISAC. The development of a next-generation gas stopping device capable of delivering low-energy, rare-isotope beams at a rate of 10 8 particles per second, or more, with high purity holds the potential to unlock experiments that would otherwise be unfeasible. Furthermore, it is expected to reduce the time required for experiments at FRIB, thereby maximizing scientific output. The research and development activities performed as part of this project bolstered essential competencies at FRIB in beam physics and ion source technologies, provided valuable training opportunities for junior scientists.

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

Understanding atom probe’s analytical performance for iron oxides using correlation histograms and ab initio calculations

Abstract Field evaporation from ionic or covalently bonded materials often leads to the emission of molecular ions. The metastability of these molecular ions, particularly under the influence of the intense electrostatic field (10 10 Vm −1 ), makes them prone to dissociation with or without an exchange of energy amongst them. These processes can affect the analytical performance of atom probe tomography (APT). For instance, neutral molecules formed through dissociation may not be detected at all or with a time of flight no longer related to their mass, causing their loss from the analysis. Here, we evaluated the changes in the measured composition of FeO, Fe 2 O 3 and Fe 3 O 4 across a wide range of analysis conditions. Possible dissociation reactions are predicted by density-functional theory calculations considering the spin states of the molecules. The energetically favoured reactions are traced on to the multi-hit ion correlation histograms, to confirm their existence within experiments, using an automated Python-based routine. The detected reactions are carefully analyzed to reflect upon the influence of these neutrals from dissociation reactions on the performance of APT for analysing iron oxides.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Low cost and massively parallel force spectroscopy with fluid loading on a chip

Current approaches for single molecule force spectroscopy are typically constrained by low throughput and high instrumentation cost. Herein, a low-cost, high throughput technique is demonstrated using microfluidics for multiplexed mechanical manipulation of up to ~4000 individual molecules via molecular fluid loading on-a-chip (FLO-Chip). The FLO-Chip consists of serially connected microchannels with varying width, allowing for simultaneous testing at multiple loading rates. Molecular force measurements are demonstrated by dissociating Biotin-Streptavidin and Digoxigenin-AntiDigoxigenin interactions along with unzipping of double stranded DNA of varying sequence under different dynamic loading rates and solution conditions. Rupture force results under varying loading rates and solution conditions are in good agreement with prior studies, verifying a versatile approach for single molecule biophysics and molecular mechanobiology. FLO-Chip enables straightforward, rapid, low-cost, and portable mechanical testing of single molecules that can be implemented on a wide range of microscopes to broaden access and may enable new applications of molecular force spectroscopy.

42 ENGINEERING↗
DOE OSTI2025

Calculation of ion–ion mutual neutralization rate constants using Landau–Zener theory coupled with trajectory simulations for Ar + –Cl − , Br − , I −

In this computational study, we self-consistently calculate the rate constants of mutual neutralization reactions by incorporating the electron transfer probability, using Landau–Zener state transition theory with inputs derived from ab initio quantum chemistry calculations, into classical trajectory simulations. Electronic structure calculations are done using correlation consistent basis sets with multi-reference configuration interaction to map all the molecular electronic states below the ion-dissociation limit as a function of the distance between the reacting species. Our electronic structure calculations have been significantly improved from our previous work through improved selection of molecular electronic configurations maintaining a fine grid of 1a 0 over a wide range of bond lengths and accurate treatment of spin–orbit couplings. Non-adiabatic coupling matrix elements are calculated with the three-point central difference method near each avoided crossing to estimate the exact crossing point R x and coupling parameter H if , which are inputs to the multi-channel Landau–Zener theory to calculate the electron transition probability. Our approach is applied to estimate the mutual neutralization rate constants for the following ion pairs: Ar + –Cl − , Ar + –Br − , Ar + –I − at ∼133 Pa. Furthermore, our predictions are compared against the experimental data reported. It is seen that the improvement in the electronic structure calculation results in excellent agreement between the simulation results and the available experimental data to within a factor of ∼2 or ∼±50%.

Complete-active space self-consistent field↗