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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 1,261 records · Page 70
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Equation-of-motion internally contracted multireference unitary coupled-cluster theory

The accurate computation of excited states remains a challenge in electronic structure theory, especially for systems with a ground state that requires a multireference treatment. In this work, we introduce a novel equation-of-motion (EOM) extension of the internally contracted multireference unitary coupled-cluster framework (ic-MRUCC), termed EOM-ic-MRUCC. EOM-ic-MRUCC follows the transform-then-diagonalize approach, in analogy to its non-unitary counterpart. By employing a projective approach to optimize the ground state, the method retains additive separability and proper scaling with system size. We show that excitation energies are size-intensive if the EOM operator satisfies the “killer” and the projective conditions. Furthermore, we propose to represent changes in the reference state upon electron excitation via projected many-body operators that span the active orbitals and show that the EOM equations formulated in this way are invariant with respect to active orbital rotations. We test the EOM-ic-MRUCC method truncated to single and double excitations by computing the potential energy curves for several excited states of a BeH2 model system, the HF molecule, and water undergoing symmetric dissociation. Across these systems, our method delivers accurate excitation energies and potential energy curves within 5 mE h (∼0.14 eV) from full configuration interaction. Here, we find that truncating the Baker–Campbell–Hausdorff series to fourfold commutators contributes negligible errors (on the order of 10 −5 E h or less), offering a practical route to highly accurate excited-state calculations with reduced computational overhead.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

External perturbation-driven Sabatier breakthrough

The Sabatier reaction (CO 2 + 4H 2 → CH 4 + 2H 2 O) is gaining renewed interest due to its potential to reduce energy carrier storage costs, serve as a feedstock for various organic chemicals, and supply in-situ propellant and life-support resources for long-duration Mars missions. This study demonstrates that combining a modest 2 mA electric field with H 2 feed modulation markedly elevates the CO 2 hydrogenation activity of 2 wt% Ru/CeO 2 catalyst. CO 2 conversion reaches 88 % and 93 % with a CH 4 yield of 83 % and 89 % at 350 °C and 450 °C, respectively. A simple lumped kinetic model reveals that the combined external perturbations not only shift the reaction mechanism but also redistribute key surface-adsorbed intermediates such as hydrogen adatoms and hydrogen-activated CO 2 among the Ru clusters, Ru/CeO 2 interface, and ceria surface. The electric field accelerates the conversion of adsorbed CO 2 to the hydrogenated CO 2 species on Ru and boosts CH 4 formation rate constant, while simultaneously suppresses the formation of undesired, non-reactive surface intermediates. Degree-of-rate-control analysis pinpoints proton migration across the metal-support interface as the decisive lever under these coupled perturbations. In conclusion, these findings establish that rational pairing of metal-support design with well-tuned electric fields and feed oscillations can unlock unprecedented Sabatier rates, guiding the development of next-generation reactors for efficient CO 2 to CH 4 conversion.

10 - SYNTHETIC FUELS↗
DOE OSTI2021

Clustering in massive neutrino cosmologies via Eulerian Perturbation Theory

We introduce an Eulerian Perturbation Theory to study the clustering of tracers for cosmologies in the presence of massive neutrinos. Our approach is based on mapping recently-obtained Lagrangian Perturbation Theory results to the Eulerian framework. We add Effective Field Theory counterterms, IR-resummations and a biasing scheme to compute the one-loop redshift-space power spectrum. To assess our predictions, we compare the power spectrum multipoles against synthetic halo catalogues from the QUIJOTE simulations, finding excellent agreement on scales k ≲ 0.25 h Mpc-1. One can obtain the same fitting accuracy using higher wave-numbers, but then the theory fails to give a correct estimation of the linear bias parameter. We further discuss the implications for the tree-level bispectrum. Finally, calculating loop corrections is computationally costly, hence we derive an accurate approximation wherein we retain only the main features of the kernels, as produced by changes to the growth rate. As a result, we show how FFTLog methods can be used to further accelerate the loop computations with these reduced kernels.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Ab Initio Computation of the Longitudinal Response Function in 40 Ca

In this work, we present a consistent ab initio computation of the longitudinal response function RL in 40 Ca using the coupled-cluster and Lorentz integral transform methods starting from chiral nucleon-nucleon and three-nucleon interactions. We validate our approach by comparing our results for R L in 4 He and the Coulomb sum rule in 40 Ca against experimental data and other calculations. For R L in 40 Ca we obtain a very good agreement with experiment in the quasielastic peak up to intermediate momentum transfers, and we find that final state interactions are essential for an accurate description of the data. This work presents a milestone towards ab initio computations of neutrino-nucleus cross sections relevant for experimental long-baseline neutrino programs.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Two Large-Scale Meteorological Patterns are Associated with Short-Duration Dry Spells in the Northeastern United States

Large-scale meteorological pattern (LSMP)–based analysis is used in a novel way to understand meteorological conditions before and during short-duration dry spells over the northeastern United States. These LSMPs are useful to assess models and select better-performing models for future projections. Dry-spell events are identified from histograms of consecutive dry days below a daily precipitation threshold. Events lasting 12 days or longer, which correspond to ~10% of dry-spell events, are examined. The 500-hPa stream-function anomaly fields for the first 12 days of each event are time averaged, and k -means clustering is applied to isolate the dry-spell-related LSMPs. The first cluster has a strong low pressure anomaly over the Atlantic Ocean, southeast of the region, and is more common in winter and spring. The second cluster has strong high pressure over east-central North America and is most common during autumn. Over the region, both clusters have negative specific humidity anomalies, negative integrated vapor transport from the north, and subsidence associated with a midlatitude jet stream dipole structure that reinforces upper-level convergence. Subsidence is supported by cold-air advection in the first cluster and the location on the east side of the lower-level high pressure in the second cluster. Extratropical cyclone storm tracks are generally shifted southward of the region during the dry spells. Individual events lie on a continuum between two distinct clusters. These clusters have similar local, but different remote, properties. Although dry spells occur with greater frequency during drought months, most dry spells occur during nondrought months. Significance Statement: This study examines the large-scale weather patterns and meteorological conditions associated with dry-spell events lasting at least 2 weeks while affecting the northeastern United States. A statistical approach groups events together on the basis of similar atmospheric features. We find two distinct sets of patterns that we call large-scale meteorological patterns. These patterns reduce moisture, foster localized sinking, and shift the storm track southward along the Atlantic seaboard, all of which reduce precipitation. Besides greater understanding, knowing the meteorological patterns during short-term dryness in the region provides an important tool to assess how well atmospheric models reproduce these specific patterns. More dry spells occur in non-drought months than in drought months, which means that dry spells can occur without preexisting drought conditions.

58 GEOSCIENCES↗
DOE OSTI2020

Visual Orbits of Spectroscopic Binaries with the CHARA Array. III. HD 8374 and HD 24546

We present the visual orbits of two long-period spectroscopic binary stars, HD 8374 and HD 24546, using interferometric observations acquired with the CHARA Array and the Palomar Testbed Interferometer. We also obtained new radial velocities from echelle spectra using the APO 3.5 m and Fairborn 2.0 m telescopes. By combining the visual and spectroscopic observations, we solve for the full, three-dimensional orbits and determine the stellar masses and distances to within 3% uncertainty. We then estimate the effective temperature and radius of each component star through Doppler tomography and spectral energy distribution analyses, in order to compare the observed stellar parameters to the predictions of stellar evolution models. For HD 8374, we find masses of M {sub 1} = 1.636 ± 0.050M {sub ⊙} and M {sub 2} = 1.587 ± 0.049M {sub ⊙}, radii of R {sub 1} = 1.84 ± 0.05R {sub ⊙} and R {sub 2} = 1.66 ± 0.12R {sub ⊙}, temperatures of T{sub eff1}=7280±110 K and T{sub eff2}=7280±120 K, and an estimated age of 1.0 Gyr. For HD 24546, we find masses of M {sub 1} = 1.434 ± 0.014M {sub ⊙} and M {sub 2} = 1.409 ± 0.014M {sub ⊙}, radii of R {sub 1} = 1.67 ± 0.06R {sub ⊙} and R {sub 2} = 1.60 ± 0.10R {sub ⊙}, temperatures of T{sub eff1}=6790±120 K and T{sub eff2}=6770±90 K, and an estimated age of 1.4 Gyr. HD 24546 is therefore too old to be a member of the Hyades cluster, despite its physical proximity to the group.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Building Alternative Indices of Socioeconomic Status for Population Modeling in Data-Sparse Contexts (Short Paper)

Population modeling requires clear definitions of socioeconomic status (SES) to ensure overall estimate accuracy and locate potentially underserved subpopulations. This presents a challenge as SES can be measured in myriad ways and for divergent purposes, and the data required to calculate these metrics may be lacking, particularly in low and middle income countries (LMICs). To support more refined SES measurement, we explore improvements upon the Demographic and Health Survey’s (DHS) Wealth Index (DHS-WI) using alternative characterizations of SES based on multiple correspondence analysis (MCA) and hierarchical clustering. We produce the MCA-derived metrics first on a full suite of household economic, demographic, and dwelling variables, then on a reduced set of occupant-only SES characteristics. We explore the utility of these metrics relative to DHS-WI based on their ability to 1) differentiate DHS household types and 2) identify mixtures of SES levels within DHS samples and mapped at high spatial resolution. We find that our full suite MCA yields more clearly defined SES segments and that our reduced MCA delineates occupant SES most clearly, suggesting potential pathways to improve upon the DHS-WI in future population modeling efforts for LMICs.

Cunningham, Angela↗
DOE OSTI2025

The approximate second order coupled-cluster method based on a size-consistent Brillouin–Wigner partitioning

We present a variant of the approximate second order coupled-cluster method (CC2) with a two-parameter size-consistent Brillouin–Wigner (BW-s) partitioning instead of a Møller–Plesset (MP) partitioning for the unperturbed Hamiltonian, which we refer to as BWs-CC2. The computational complexity of this model scales identically to CC2 with molecular size. Conventional CC2 and its regularized BWs-CC2 variants, as well as conventional MP2 and two of its regularized BW-s2 variants, were assessed on a 535 element database spanning thermochemistry, non-covalent interactions, barrier heights, and isomerization energies. To ensure a well-defined model chemistry, the assessment was performed using internally stable spin-polarized Hartree–Fock (HF) orbitals in the finite aug-cc-pVQZ basis without counterpoise corrections. As a result of using stable orbitals, contrary to conventional wisdom, we find that CC2 substantially outperforms MP2 on molecules with significantly spin contaminated reference orbitals without a significant increase in error on systems with a spin-pure reference, showing the value of its single substitutions. While no single choice of regularization parameters can be optimal for all datasets, we find that BWs-CC2 generally outperforms both CC2 and BW-s2 with a single judicious parameter choice. Additional tests on dipole moments and bond lengths of diatomics provide further support for the utility of this choice. Furthermore, the main outliers and poorest performing cases are associated with large amounts of spin-contamination in the HF reference, which is indicative of systems with either strong correlation or extensive artificial symmetry breaking. Overall, these findings argue that the perception of the quality of the CC2 ground state should be reevaluated and that it can be further improved upon by the soundly based BWs-CC2 variant with the recommended parameter choice.

Correlation energy↗
DOE OSTI2022

How a Formate Dehydrogenase Responds to Oxygen: Unexpected O 2 Insensitivity of an Enzyme Harboring Tungstopterin, Selenocysteine, and [4Fe–4S] Clusters

The reversible two-electron interconversion of formate and CO 2 is catalyzed by both nonmetallo- and metallo-formate dehydrogenases (FDHs). The latter group comprises molybdenum- or tungsten-containing enzymes with the metal coordinated by two equivalents of a pyranopterin cofactor, a cysteinyl or selenocysteinyl (Sec) ligand supplied by the polypeptide, and a catalytically essential terminal sulfido ligand. In addition, these biocatalysts incorporate one or more [4Fe–4S] clusters for facilitating long-distance electron transfer. However, an interesting dichotomy arises when attempting to understand how the metallo-FDHs react with O 2 . Whereas existing scholarship portrays these enzymes as being unable to perform in air due to extreme O 2 lability of their metal centers, studies dating as far back as the 1930s emphasize that some of these systems exhibit formate oxidase (FOX) activity, coupling formate oxidation to O 2 reduction. Therefore, to reconcile these conflicting views, we explored context-dependent functional linkages between metallo-FDHs and their cognate electron acceptors within the same organism vis-à-vis catalysis under atmospheric O 2 . Here, we report the discovery and characterization of an O 2 -insensitive FDH2 from the sulfate-reducing bacterium Desulfovibrio vulgaris Hildenborough (DvH) that ligates tungsten, Sec, and four [4Fe–4S] clusters. By advancing a robust expression platform for its recombinant production, we eliminate both the requirement of nitrate or azide during purification and reductive activation with thiols and/or formate prior to catalysis. Because the distinctive spectral signatures of formate-reduced DvH-FDH2 remain invariant under anaerobic and aerobic conditions, we benchmarked the enzyme activity in air, identifying CO 2 as the catalytic product. Full reaction progress curve analysis discloses a high catalytic efficiency when probed with a high-potential artificial electron acceptor. Furthermore, we show that DvH-FDH2 enables near-stoichiometric hydrogen peroxide production without superoxide release to achieve O 2 insensitivity. Notably, simultaneous electron transfer to cytochrome c and O 2 reveals that metal-based electron bifurcation is operational in this system. Taken together, our work proves the co-occurrence of redox bifurcated FDH and FOX activities within a metalloenzyme scaffold. These findings set the stage for uncovering previously unknown O 2 -insensitive flavin-based electron bifurcation mechanisms, as well as for developing authentic formate/air biofuel cells, engineering O 2 -stable FDHs and biohybrid metallocatalysts, and discerning formate bioenergetics of gut microbiota.

13C NMR↗
DOE OSTI2025

Porous and Amorphous Mn x Mo 3 S 13 Chalcogel Electrode for High-Capacity Conversion-Based Lithium-Ion Batteries

While Li-ion batteries (LIBs) are a leading energy storage technology, their energy densities are limited by the low capacity of conventional intercalation cathodes, driving interest in high energy-density Li–S batteries that make use of conversion chemistry. Achieving high capacity, reversibility, and cycle stability, and controlling volume changes in conversion batteries during the charge–discharge process, however, remains challenging. Here, in this study, we present a porous, amorphous, sulfide-based Mn x Mo 3 S 13 chalcogel, which concurrently offers high capacity and cycle stability. The solution-processable room temperature synthesized Mn x Mo 3 S 13 (x = 0.25) chalcogel exhibits a local structure that resembles the Mo 3 S 13 cluster with Mn 2+ distributed across the Mo 3 S 13 matrix, as determined by synchrotron X-ray pair distribution function (PDF) and extended X-ray absorption fine structure (EXAFS). Ab initio molecular dynamics (AIMD) simulations reveal that Mn 2+ incorporation shortens the polysulfide chain in the gel matrix compared to the Mo 3 S 13 chalcogel, while forming a coordination environment with disulfide groups, analogous to the experimental findings. A Li/Mn 0.25 Mo 3 S 13 half-cell delivers 897 mAh g –1 capacity during the first discharge and retains 571 mAh g –1 capacity after 100 cycles at a C/3 rate. Distribution of relaxation time (DRT) unveils a stable solid–electrolyte interphase (SEI) formation upon cycling that enables charge–discharge reversibility. Here, the enhanced capacity retention and cycle stability compared to those of the Li/Mo 3 S 13 cell are attributed to the reduced dissolution of active mass into the electrolyte, facilitated by the formation of shorter polysulfide chains within the Mn 0.25 Mo 3 S 13 structure and the strong affinity of Lewis-acidic Mn 2+ for polysulfide anions generated during the charge–discharge process of the Li/Mn 0.25 Mo 3 S 13 cell. Thus, this work illustrates a design principle of material for high-capacity and cycle-stable Li-metal sulfide batteries.

25 ENERGY STORAGE↗
DOE OSTI2025

Achieving Higher Activity of Acidic Oxygen Evolution Reaction Using an Atomically Thin Layer of IrO x over Co 3 O 4

The development of electrocatalysts with reduced iridium (Ir) loading for the oxygen evolution reaction (OER) is essential to produce low-cost green hydrogen from water electrolysis under acidic conditions. Herein, an atomically thin layer of iridium oxide (IrO x ) has been uniformly dispersed onto cobalt oxide (Co 3 O 4 ) nanocrystals to improve the efficient use of Ir for acidic OER. In situ characterization and theoretical calculations reveal that compared to the conventional IrOx cluster, the atomically thin layer of IrO x shows stronger interaction with the Co 3 O 4 and consequently higher OER activity due to the Ir-O-Co bond formation at the interface. Equally important, the facile synthetic method and the promising activity in the proton exchange membrane water electrolyzer, reaching 1 A cm -2 at 1.7 V with remarkable durability, enable potential scale-up applications. In conclusion, these findings provide a mechanistic understanding for designing active, stable and lower-cost electrocatalysts with well-defined structures for acidic OER.

58 GEOSCIENCES↗
DOE OSTI2026

Predicting Atomistic Transitions with Transformers

Accurate knowledge of the atomistic transition pathways in materials and material surfaces is crucial for many material science problems. However, conventional simulation techniques used to find these transitions are extremely computationally intensive. Even with large-scale, accelerated material simulations, the computational cost constrains the applicable domain in practice. Machine learning models, with the potential to learn the complex emergent behaviors governing atomistic transitions as a fast surrogate model, have great promise to predict transitions with a vastly reduced computational cost. Here, we demonstrate how transformers can be trained to predict atomistic transitions in nano-clusters. We show how we evaluate physical validity of the predictions and how a multitude of additional, different microstates can be generated by slightly varying the data provided to the model.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Cosmic variance and the inhomogeneous UV luminosity function of galaxies during reionization

When the first galaxies formed and starlight escaped into the intergalactic medium to reionize it, galaxy formation and reionization were both highly inhomogeneous in time and space, and fully coupled by mutual feedback. To show how this imprinted the UV luminosity function (UVLF) of reionization-era galaxies, we use our large-scale, radiation-hydrodynamics simulation CoDa II to derive the time- and space-varying halo mass function and UVLF, from z ≃ 6–15. That UVLF correlates strongly with local reionization redshift: earlier-reionizing regions have UVLFs that are higher, more extended to brighter magnitudes, and flatter at the faint end than later-reionizing regions observed at the same z. In general, as a region reionizes, the faint-end slope of its local UVLF flattens, and, by z = 6 (when reionization ended), the global UVLF, too, exhibits a flattened faint-end slope, ‘rolling-over’ at M UV ≳ -17. CoDa II’s UVLF is broadly consistent with cluster-lensed galaxy observations of the Hubble Frontier Fields at z = 6–8, including the faint end, except for the faintest data point at z = 6, based on one galaxy at M UV = -12.5. According to CoDa II, the probability of observing the latter is $\sim 5~{{\ \rm per\ cent}}$. However, the effective volume searched at this magnitude is very small, and is thus subject to significant cosmic variance. Here, we find that previous methods adopted to calculate the uncertainty due to cosmic variance underestimated it on such small scales by a factor of 2–4, primarily by underestimating the variance in halo abundance when the sample volume is small.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2026

Lyman-$α$ forest holography: 3D predictions from 1D measurements

Cosmological analyses of Lyman-$α$ forest clustering rely on either one-dimensional correlations along individual sightlines or three-dimensional correlations between different sightlines. Because these observables probe the matter distribution on very different scales, they have traditionally been analyzed independently. In this work, we bridge this gap using ForestFlow, an emulator trained on a suite of cosmological hydrodynamical simulations that provides a unified description of Lyman-$α$ forest clustering from linear to nonlinear scales. This framework enables us to determine the range of three-dimensional clustering models compatible with the DESI one-dimensional flux power spectrum ($P_{\rm 1D}$). The resulting predictions successfully reproduce the large-scale clustering measured by the DESI BAO analysis and provide physically motivated priors on nonlinear clustering that are used in a companion paper presenting the full-shape analysis of the DESI DR2 Lyman-$α$ forest. We validate our methodology using the large-volume, high-resolution hydrodynamical simulation ACCEL-2, demonstrating excellent agreement across the full range of scales considered. Finally, we combine constraints from the $P_{\rm 1D}$ and BAO analyses on the parameter combinations $b_δσ_8$ and $b_ηf σ_8$, finding that the two probes provide comparable constraining power while exhibiting complementary parameter degeneracies. Our results establish a direct connection between one- and three-dimensional Lyman-$α$ forest measurements through ForestFlow, an approach we term Lyman-$α$ holography by analogy with the reconstruction of higher-dimensional structure from lower-dimensional information.

Chaves-Montero, J. [Barcelona, IFAE] (ORCID:000000↗
DOE OSTI2020

Ensembles of Metastable States Govern Heterogeneous Catalysis on Dynamic Interfaces

Heterogeneous catalysis is at the heart of chemical industry. Being able to tune and design efficient catalysts for processes of interest is of an utmost importance, and for this, the molecular-level understanding of heterogeneous catalysts is the first step, and indeed a prime focus of the modern catalysis research. For a long time, a single most thermodynamically stable structure of the catalytic interface attained in reaction conditions had been envisioned as the reactive phase. However, some catalytic interfaces continue to undergo structural dynamics in the steady state, triggered by high temperatures, pressures, and binding and changing reagents. Among particularly dynamic interfaces are such widely-used catalysts as crystalline and amorphous surfaced supporting (sub-)nano metallic clusters. Recently, it became clear that this dynamic fluxionality causes the supported clusters to populate many distinct structural and stoichiometric states in catalytic conditions. Hence, the catalytic interface should be viewed as an evolving statistical ensemble of many (not one) structures. As such, every member in the ensemble contributes to the properties of the catalyst differently, and in proportion to its probability to be populated. This new notion flips the established paradigm and calls for new theory, modeling approaches, operando measurements, and updated design strategies. The statistical ensemble nature of surface-supported sub-nano cluster catalysts can be exemplified by oxide-supported and adsorbate-covered Pt, Pd, Cu, CuPd clusters, catalytic toward oxidative and non-oxidative dehydrogenation. They have access to a variety of 3D and quasi-2D shapes. The compositions of their thermal ensembles are dependent on the cluster size, leading to size-specific catalytic activities and the famous “every atom counts” phenomenon. The support and adsorbates affect catalyst structures, and state of the reacting species causes the ensemble to change in every reaction intermediate. The most stable member of the ensemble dominates the thermodynamic properties of the corresponding intermediate, whereas the kinetics can be determined by more active but less populated metastable catalyst states, and that suggests that many earlier studies might have overlooked the actual active sites. Both effects depend on the relative time-scales of catalyst restructuring and reaction dynamics. The catalyst may routinely operate off-equilibrium. Ensemble phenomena lead to surprising exceptions from established rules of catalysis, such as scaling relations, and Arrhenius behavior. Catalyst deactivation is also an ensemble property, and its extent of mitigation can be predicted through the new paradigm. These findings were enabled by advances in theory, such as global optimization and subsequent utilization of multiple local minima, and pathways sampling, as well as operando catalyst characterization. The fact that the per-site and per-species resolution is needed for the description and predicting of catalyst properties gives theory the central role in catalysis research, as most experiments provide ensemble-average information and cannot detect the crucial minority species that may be responsible for the catalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

The Localized Active Space Method with Unitary Selective Coupled Cluster

Here, we introduce a hybrid quantum-classical algorithm, the localized active space unitary selective coupled cluster singles and doubles (LAS-USCCSD) method. Derived from the localized active space unitary coupled cluster (LAS-UCCSD) method, LAS-USCCSD first performs a classical LASSCF calculation, then selectively identifies the most important parameters (cluster amplitudes used to build the multireference UCC ansatz) for restoring interfragment interaction energy using this reduced set of parameters with the variational quantum eigensolver method. We benchmark LAS-USCCSD against LAS-UCCSD by calculating the total energies of (H 2 ) 2 , (H 2 ) 4 , and trans-butadiene, and the magnetic coupling constant for a bimetallic compound [Cr 2 (OH) 3 (NH 3 ) 6 ] 3+ . For these systems, we find that LAS-USCCSD reduces the number of required parameters and thus the circuit depth by at least 1 order of magnitude, an aspect which is important for the practical implementation of multireference hybrid quantum-classical algorithms like LAS-UCCSD on near-term quantum computers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Identification and characterization of a small-molecule metallophore involved in lanthanide metabolism

Many bacteria secrete metallophores, low-molecular-weight organic compounds that bind ions with high selectivity and affinity, in order to access essential metals from the environment. Previous work has elucidated the structures and biosynthetic machinery of metallophores specific for iron, zinc, nickel, molybdenum, and copper. No physiologically relevant lanthanide-binding metallophore has been discovered despite the knowledge that lanthanide metals (Ln) have been revealed to be essential cofactors for certain alcohol dehydrogenases across a diverse range of phyla. Here, we report the biosynthetic machinery, the structure, and the physiological relevance of a lanthanophore, methylolanthanin. The structure of methylolanthanin exhibits a unique 4-hydroxybenzoate moiety which has not previously been described in other metallophores. We find that production of methylolanthanin is required for normal levels of Ln accumulation in the methylotrophic bacterium Methylobacterium extorquens AM1, while overexpression of the molecule greatly increases bioaccumulation and adsorption. Our results provide a clearer understanding of how Ln-utilizing bacteria sense, scavenge, and store Ln; essential processes in the environment where Ln are poorly bioavailable. More broadly, the identification of this lanthanophore opens doors for study of how biosynthetic gene clusters are repurposed for additional functions and the complex relationship between metal homeostasis and fitness.

Science & Technology - Other Topics↗
DOE OSTI2022

The effect of quasar redshift errors on Lyman-α forest correlation functions

ABSTRACT Using synthetic Lyman-α forests from the Dark Energy Spectroscopic Instrument (DESI) survey, we present a study of the impact of errors in the estimation of quasar redshift on the Lyman-α correlation functions. Estimates of quasar redshift have large uncertainties of a few hundred km s−1 due to the broadness of the emission lines and the intrinsic shifts from other emission lines. We inject Gaussian random redshift errors into the mock quasar catalogues, and measure the auto-correlation and the Lyman-α-quasar cross-correlation functions. We find a smearing of the BAO feature in the radial direction, but changes in the peak position are negligible. However, we see a significant unphysical correlation for small separations transverse to the line of sight which increases with the amplitude of the redshift errors. We interpret this contamination as a result of the broadening of emission lines in the measured mean continuum, caused by quasar redshift errors, combined with the unrealistically strong clustering of the simulated quasars on small scales.

79 ASTRONOMY AND ASTROPHYSICS↗