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DOE OSTI2021

Effect of Confinement on the Density and Diffusivity of Organic Molecules in Single-Digit Nanopores Relative to Bulk Fluid Behavior

Prediction of fluid properties in microporous and mesoporous confinement is non-trivial due to distinct influences from pore surface functionality and shape and fluid molecular characteristics. The vast majority of literature focuses nearly exclusively on a small number of components that are generally low molecular weight gases and vapors. Missing are studies that utilize a relatively large number of compounds that are liquid at ambient conditions to probe the impact of molecular shape and size on confined fluid properties. Such materials are of great interest in the extraction of oil and gas from shale reservoirs or for the design of selective adsorbents for chemical separation. In this work, we reveal non-intuitive relationships that emerge when comparing bulk fluid properties to those when confined in amorphous silica single-digit nanopores (approx. 5 nm SBA-15), specifically the confined density and self-diffusivity. A counterintuitive result was obtained where larger molecules had relatively faster self-diffusivities; however, this behavior was revealed to be caused by these larger compounds exhibiting a relatively low density when confined. As the prediction of confined fluid properties impacts a diversity of disciplines, the results highlight the need for additional investigations where consistent and large-scale experimental procedures are employed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Unusual Seismic Signals in the Sevier Desert, Utah Possibly Related to the Black Rock Volcanic Field

Abstract On September 12, 2018 and April 14, 2019 shallow (<2.5 km from the surface, <1 km relative to sea level) earthquakes ( M w 4.0 and 4.1, respectively) struck a relatively aseismic area in south‐central Utah, within the Black Rock Desert volcanic field. Seismic waveforms are dominated by long‐period energy, no clear direct S‐wave arrivals, and signal durations of ∼100 s. Using co‐seismic interferograms, we detect clear and distinguishable surface deformation confirming the shallowness of the two mainshocks, while full moment tensor solutions rule out an isotropic source, such as an explosion or collapse. For the April 2019 sequence, we build an earthquake catalog using a dense temporary geophone array. The enhanced earthquake catalog shows a rapidly decaying aftershock sequence, with 85% of aftershocks occurring during the first three hours. Combining these observations, we argue that these earthquake sequences are related to the Black Rock Desert volcanic field.

Mesimeri, Maria↗

DOE OSTI2024

Quantifying the Effect of Pore‐Size Dependent Wettability on Relative Permeability Using Capillary Bundle Model

Abstract Relative permeability is a key parameter for characterizing the multiphase flow dynamics in porous media at macroscopic scale while it can be significantly impacted by wettability. Recently, it has been reported in microfluidic experiments that wettability is dependent on the pore size (Van Rooijen et al., 2022). To investigate the effect of pore‐size‐dependent wettability on relative permeability, we propose a theoretical framework informed by digital core samples to quantify the deviation of relative permeability curves due to wettability change. We find that the significance of impact is highly dependent on two factors: (i) the function between contact angle and pore size (ii) overall pore size distribution. Under linear function, this impact can be significant for tight porous media with a maximum deviation of 1,000%.

Yu, Siqin↗

DOE OSTI2024

Learning Constitutive Relations From Soil Moisture Data via Physically Constrained Neural Networks

Abstract The constitutive relations of the Richardson‐Richards equation encode the macroscopic properties of soil water retention and conductivity. These soil hydraulic functions are commonly represented by models with a handful of parameters. The limited degrees of freedom of such soil hydraulic models constrain our ability to extract soil hydraulic properties from soil moisture data via inverse modeling. We present a new free‐form approach to learning the constitutive relations using physically constrained neural networks. We implemented the inverse modeling framework in a differentiable modeling framework, JAX, to ensure scalability and extensibility. For efficient gradient computations, we implemented implicit differentiation through a nonlinear solver for the Richardson‐Richards equation. We tested the framework against synthetic noisy data and demonstrated its robustness against varying magnitudes of noise and degrees of freedom of the neural networks. We applied the framework to soil moisture data from an upward infiltration experiment and demonstrated that the neural network‐based approach was better fitted to the experimental data than a parametric model and that the framework can learn the constitutive relations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Fine root and soil carbon stocks are positively related in grasslands but not in forests

Increasing fine root carbon (FRC) inputs into soils has been proposed as a solution to increasing soil organic carbon (SOC). However, FRC inputs can also enhance SOC loss through priming. Here, we tested the broad-scale relationships between SOC and FRC at 43 sites across the US National Ecological Observatory Network. We found that SOC and FRC stocks were positively related with an across-ecosystem slope of 7 ± 3 kg SOC m −2 per kg FRC m −2 , but this relationship was driven by grasslands. Grasslands had double the across-ecosystem slope while forest FRC and SOC were unrelated. Furthermore, deep grassland soils primarily showed net SOC accrual relative to FRC input. Conversely, forests had high variability in whether FRC inputs were related to net SOC priming or accrual. We conclude that while FRC increases could lead to increased SOC in grasslands, especially at depth, the FRC-SOC relationship remains difficult to characterize in forests.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Active Learning-driven Quantitative Synthesis-Structure-Property Relations for Improving Performance and Revealing Active Sites of Nitrogen-Doped Carbon for the Hydrogen Evolution Reaction

While quantitative structure-properties relations (QSPRs) have been developed successfully in multiple fields, catalyst synthesis affects structure and in turn performance, making simple QSPRs inadequate. Furthermore, catalysts often have multiple active sites preventing one from obtaining insights into structure-property relations. Here, we develop a data-driven quantitative synthesis-structure-property relation (QS2PRs) methodology to elucidate correlations between catalyst synthesis conditions, structural properties as well as observed performance and to provide fundamental insights into active sites and a systematic way to optimize practical catalysts. Here, we demonstrate the approach to the synthesis of nitrogen-doped catalysts (NDC) made via pyrolysis for the performance of the electrochemical hydrogen evolution reaction (HER), quantified by the onset potential and the current density. We determine crystallinity, nitrogen species type and fraction, surface area, and pore structure of the NDC’s using XRD, XPS, and BET characterization. We demonstrated that an active learning-based optimization combined with various elementary machine learning tools (regression, principal component analysis, partial least squares) can efficiently identify optimum pyrolysis conditions to tune structural characteristics and performance with concomitant savings in materials and experimental time. Unlike previous reports on the importance of pyridinic or graphitic nitrogen, we discover that the electrochemical performance is not driven by a single catalyst property; rather, it arises from a multivariate influence of nitrogen dopants, pore structure and disorder in the NDC materials. Identification of active sites can help mechanistic understanding and further catalyst improvement.

42 ENGINEERING↗

DOE OSTI2022

Mass–metallicity and star formation rate in galaxies: A complex relation tuned to stellar age

In this work we study the stellar mass–metallicity relation (MZR) of an extended sample of star-forming galaxies in the local Universe and its possible dependence on the star formation rate (SFR). We selected a sample of approximately 195 000 Sloan Digital Sky Survey (SDSS) star-forming galaxies up to z = 0.22 with the aim of analysing the behaviour of the MZR with respect to SFR whilst taking into account the age of their stellar populations. For the first time, with this sample, we obtained aperture corrected oxygen and nitrogen-to-oxygen abundances (O/H and N/O, respectively) and SFR using the empirical prescriptions from the Calar Alto Legacy Integral Field Area (CALIFA) survey. To perform this study we also make use of the stellar mass of the galaxies and the parameter Dn(4000) as a proxy for the age of the stellar population. We derive a robust MZR locus, which is found to be fully consistent with the ‘anchoring’ points of a selected set of well-studied nearby galaxies for which the chemical abundance has been derived using the direct method. We observe a complex relation between MZR and SFR across the whole range of galaxy mass and metallicity, where the slope changes seen in the O/H–SFR plane present a pattern that seems to be tuned to the stellar age of the galaxies, and therefore stellar age has to be taken into account in the stellar mass–metallicity–SFR relation. In order to provide an answer to the question of whether or not the MZR depends on the SFR, it is essential to take into account the age of the stellar populations of galaxies. A strong dependence of the MZR on SFR is observed mainly for star-forming galaxies with strong SFR values and low D n (4000). The youngest galaxies of our SDSS sample show the highest SFR measured for their stellar mass.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Spatially resolved mass–metallicity relation at $z$ ~ 0.26 from the MUSE-Wide Survey

Galaxies in the local universe have a spatially resolved star-forming main sequence (rSFMS) and mass–metallicity relation (rMZR). We know that the global mass–metallicity relation (MZR) results from the integral of the rMZR, and it evolves with redshift. However, the evolution of the rMZR with redshift is still unclear because the spatial resolution and signal-to-noise ratio are low. Currently, too few observations beyond the local universe are available, and only simulations can reproduce the evolution of the rMZR with redshift. We selected ten emission-line galaxies with an average redshift of $z$ ~ 0.26 from the MUSE-Wide DR1. We obtained the spatially resolved star formation rate (SFR) and metallicity from integral field spectroscopy (IFS), as well as the stellar mass surface density from 3D-HST photometry. We derived the rSFMS and rMZR at $z$ ~ 0.26 and compared them with those of local galaxies. We find that the rSFMS of galaxies at $z$ ~ 0.26 has a slope of ~0.771. The rMZR exists at z ~ 0.26, showing a similar shape to that of the local universe, but a lower average metallicity that is about ~0.11 dex lower than the local metallicity. In addition, we also study the spatially resolved fundamental metallicity relation (rFMR) of these galaxies. However, there is no obvious evidence that an rFMR exists at $z$ ~ 0.26, and it is not an extension of rMZR at a high SFR. Similar to their global versions, the rSFMS and rMZR of galaxies also evolve with redshift. At fixed stellar mass, galaxies at higher redshift show a higher SFR and lower metallicity. In conclusion, these suggest that the evolution of the global galaxy properties with redshift may result from integrating the evolution of the spatially resolved galaxy properties.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Relative permeability as a stationary process: Energy fluctuations in immiscible displacement

Relative permeability is commonly used to model immiscible fluid flow through porous materials. In this work, we derive the relative permeability relationship from conservation of energy, assuming that the system to be non-ergodic at large length scales and relying on averaging in both space and time to homogenize the behavior. Explicit criteria are obtained to define stationary conditions: (1) there can be no net change for extensive measures of the system state over the time averaging interval; (2) the net energy inputs into the system are zero, meaning that the net rate of work done on the system must balance with the heat removed; and (3) there is no net work performed due to the contribution of internal energy fluctuations. Results are then evaluated based on direct numerical simulation. Dynamic connectivity is observed during steady-state flow, which is quantitatively assessed based the Euler characteristic. We show that even during steady-state flow at low capillary number ([Formula: see text]), typical flow processes will explore multiple connectivity states. The residence time for each connectivity state is captured based on the time-and-space average. The distribution for energy fluctuations is shown to be multi-modal and non-Gaussian when terms are considered independently. However, we demonstrate that their sum is zero. Given an appropriate choice of the thermodynamic driving force, we show that the conventional relative permeability relationship is sufficient to model the energy dissipation in systems with complex pore-scale dynamics that routinely alter the structure of fluid connected pathways.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Relative sensitivity of plastic scintillator: A comparative analysis with 60 Co gamma rays, deuterium–deuterium, and deuterium–tritium neutrons

A plastic scintillator has found extensive application in the realm of high-energy physics and national security science. Many applications in those fields often involve the simultaneous production of photons, neutrons, and charged particles, which makes the relative sensitivity information for these different radiation types important. In this study, we have adopted a multi-head detector comprised of a plastic scintillator and high gain phototubes, which provides a large dynamic range and linearity. A comparative study on the relative sensitivities of plastic scintillators was facilitated by adopting three distinct radiation calibration sources (i.e., 60 Co γ rays, DD neutrons, and DT neutrons). Neutrons from a DD source generate a comparable level of scintillation to gamma rays emitted by 60 Co (i.e., 60 Co-γ/DD-n = 0.92 ± 16%). DT neutrons induce ~3.5 times the scintillation observed with DD neutrons (i.e., DT-n/DD-n = 3.5 ± 28%). In addition, the Geant4 simulation granted us valuable insights into the relative sensitivity of the scintillator. This comparative study will provide a useful database for users in diverse applications.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Solid organic-coated ammonium sulfate particles at high relative humidity in the summertime Arctic atmosphere

The ability of atmospheric aerosols to impact climate through water uptake and cloud formation is fundamentally determined by the size, composition, and phase (liquid, semisolid, or solid) of individual particles. Particle phase is dependent on atmospheric conditions (relative humidity and temperature) and chemical composition and, importantly, solid particles can inhibit the uptake of water and other trace gases, even under humid conditions. Particles composed primarily of ammonium sulfate are presumed to be liquid at the relative humidities (67 to 98%) and temperatures (–2 to 4 °C) of the summertime Arctic. Under these atmospheric conditions, we report the observation of solid organic-coated ammonium sulfate particles representing 30% of particles, by number, in a key size range (<0.2 µm) for cloud activation within marine air masses from the Arctic Ocean at Utqiagvik, AK. The composition and size of the observed particles are consistent with recent Arctic modeling and observational results showing new particle formation and growth from dimethylsulfide oxidation to form sulfuric acid, reaction with ammonia, and condensation of marine biogenic sulfate and highly oxygenated organic molecules. Aqueous sulfate particles typically undergo efflorescence and solidify at relative humidities of less than 34%. Therefore, the observed solid phase is hypothesized to occur from contact efflorescence during collision of a newly formed Aitken mode sulfate particle with an organic-coated ammonium sulfate particle. With declining sea ice in the warming Arctic, this particle source is expected to increase with increasing open water and marine biogenic emissions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Identification of dislocation-related and point-defects in III-As layers for silicon photonics applications

Abstract The aim of this paper is to identify, analyze and compare the defects present in III-As, as a function of dislocation density, and as a function of the presence/absence of quantum dots (QDs). Such materials are of fundamental importance for the development of lasers and photodiodes for silicon photonics. The study is based on an extensive deep-level transient spectroscopy investigation, carried out on GaAs pin diodes grown on Si and on GaAs (that differ in the dislocation density), with and without embedded QDs. The original results described in this paper demonstrate that: (a) we were able to identify four different defects within the device grown on Si (three electron and one hole traps) and one defect (hole trap) in the device on GaAs, common to both samples; (b) all the majority carrier traps identified are located near midgap, i.e. are efficient non-radiative recombination centers; (c) such defects are absent (or non-detectable) in the sample grown on GaAs substrate, having a very low dislocation density; (d) the presence of QDs does not result in additional defects within the semiconductor material; (e) the analysis of the capture kinetics revealed that two of the identified traps are related to point defects, whereas the other two traps can be associated with point defects located near a dislocation; (f) a comparison with previous reports indicate that the detected traps are related to native III-As defects, or to oxygen-related complexes.

Physics↗

DOE OSTI2023

Microbiome-enabled genomic selection improves prediction accuracy for nitrogen-related traits in maize

Root-associated microbiomes in the rhizosphere (rhizobiomes) are increasingly known to play an important role in nutrient acquisition, stress tolerance, and disease resistance of plants. However, it remains largely unclear to what extent these rhizobiomes contribute to trait variation for different genotypes and if their inclusion in the genomic selection protocol can enhance prediction accuracy. To address these questions, we developed a microbiome-enabled genomic selection method that incorporated host SNPs and amplicon sequence variants from plant rhizobiomes in a maize diversity panel under high and low nitrogen (N) field conditions. Our cross-validation results showed that the microbiome-enabled genomic selection model significantly outperformed the conventional genomic selection model for nearly all time-series traits related to plant growth and N responses, with an average relative improvement of 3.7%. The improvement was more pronounced under low N conditions (8.4–40.2% of relative improvement), consistent with the view that some beneficial microbes can enhance N nutrient uptake, particularly in low N fields. However, our study could not definitively rule out the possibility that the observed improvement is partially due to the amplicon sequence variants being influenced by microenvironments. Using a high-dimensional mediation analysis method, our study has also identified microbial mediators that establish a link between plant genotype and phenotype. Some of the detected mediator microbes were previously reported to promote plant growth. The enhanced prediction accuracy of the microbiome-enabled genomic selection models, demonstrated in a single environment, serves as a proof-of-concept for the potential application of microbiome-enabled plant breeding for sustainable agriculture.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2020

CODEX weak lensing mass catalogue and implications on the mass–richness relation

The COnstrain Dark Energy with X-ray clusters (CODEX) sample contains the largest flux limited sample of X-ray clusters at 0.35 < z < 0.65. It was selected from ROSAT data in the 10 000 square degrees of overlap with BOSS, mapping a total number of 2770 high-z galaxy clusters. We present here the full results of the CFHT CODEX programme on cluster mass measurement, including a reanalysis of CFHTLS Wide data, with 25 individual lensing-constrained cluster masses. We employ lensfit shape measurement and perform a conservative colour–space selection and weighting of background galaxies. Using the combination of shape noise and an analytic covariance for intrinsic variations of cluster profiles at fixed mass due to large-scale structure, miscentring, and variations in concentration and ellipticity, we determine the likelihood of the observed shear signal as a function of true mass for each cluster. We combine 25 individual cluster mass likelihoods in a Bayesian hierarchical scheme with the inclusion of optical and X-ray selection functions to derive constraints on the slope α, normalization β, and scatter σln λ|μ of our richness–mass scaling relation model in log-space: ${\langle {\rm In}\,\, \lambda\!\!\mid\!\!\mu\rangle = \alpha\mu + \beta,} $ with μ = ln (M 200c /M piv ), and M piv = 10 14.81 M ⊙ . We find a slope $\alpha = 0.49^{+0.20}_{-0.15}$, normalization $\exp (\beta) = 84.0^{+9.2}_{-14.8}$, and $\sigma _{\ln \lambda | \mu } = 0.17^{+0.13}_{-0.09}$ using CFHT richness estimates. In comparison to other weak lensing richness–mass relations, we find the normalization of the richness statistically agreeing with the normalization of other scaling relations from a broad redshift range (0.0 < z < 0.65) and with different cluster selection (X-ray, Sunyaev–Zeldovich, and optical).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Standardizing reverberation-measured Mg II time-lag quasars, by using the radius–luminosity relation, and constraining cosmological model parameters

ABSTRACT We use 78 reverberation-measured Mg II time-lag quasars (QSOs) in the redshift range 0.0033 ≤ z ≤ 1.89 to constrain cosmological parameters in six different cosmological models. The basis of our method is the use of the radius–luminosity or R−L relation to standardize these 78 Mg II QSOs. In each cosmological model, we simultaneously determine R−L relation and cosmological model parameters, thus avoiding the circularity problem. We find that the R−L relation parameter values are independent of the cosmological model used in the analysis, thus, establishing that current Mg II QSOs are standardizable candles. Cosmological constraints obtained using these QSOs are significantly weaker than, but consistent with, those obtained from a joint analysis of baryon acoustic oscillation (BAO) observations and Hubble parameter [H(z)] measurements. So, we also analyse these QSOs in conjunction with the BAO + H(z) data and find cosmological constraints consistent with the standard spatially flat ΛCDM model as well as with mild dark energy dynamics and a little spatial curvature. A larger sample of higher quality reverberation-measured QSOs should have a smaller intrinsic dispersion and so should provide tighter constraints on cosmological parameters.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

How well do local relations predict gas-phase metallicity gradients? Results from SDSS-IV MaNGA

ABSTRACT Gas-phase metallicity gradients in galaxies provide important clues to those galaxies’ formation histories. Using SDSS-IV MaNGA data, we previously demonstrated that gas metallicity gradients vary systematically and significantly across the galaxy mass–size plane: at stellar masses beyond approximately $10^{10}\, \mathrm{M_\odot }$, more extended galaxies display steeper gradients (in units of dex/Re) at a given stellar mass. Here, we set out to develop a physical interpretation of these findings by examining the ability of local ∼kpc-scale relations to predict the gradient behaviour along the mass–size plane. We find that local stellar mass surface density, when combined with total stellar mass, is sufficient to reproduce the overall mass–size trend in a qualitative sense. We further find that we can improve the predictions by correcting for residual trends relating to the recent star formation histories of star-forming regions. However, we find as well that the most extended galaxies display steeper average gradients than predicted, even after correcting for residual metallicity trends with other local parameters. From these results, we argue that gas-phase metallicity gradients can largely be understood in terms of known local relations, but we also discuss some possible physical causes of discrepant gradients.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Galaxy–halo size relation from Sloan Digital Sky Survey Data Release 7 and the ELUCID simulation

ABSTRACT Based on galaxies in the Sloan Digital Sky Survey Data Release 7 and dark matter haloes in the dark matter only, cosmological, and constrained ELUCID simulation, we investigate the relation between the observed radii of central galaxies with stellar mass $\gtrsim\!{10}^{8} \, h^{-2}\, {\rm M}_\odot$ and the virial radii of their host dark matter haloes with virial mass $\gtrsim\!{10}^{10.5} \, h^{-1}\, {\rm M}_\odot$, and the dependence of galaxy–halo size relation on the halo spin and concentration. Galaxies in observation are matched to dark matter (sub)haloes in the ELUCID simulation using a novel neighbourhood subhalo abundance matching method. For galaxy two-dimensional (2D) half-light radii R50, we find that early- and late-type galaxies have the same power-law index 0.55 with $R_{50} \propto R_{\rm vir}^{0.55}$, although early-type galaxies have smaller 2D half-light radii than late-type galaxies at fixed halo virial radii. When converting the 2D half-light radii R50 to 3D half-mass radii r1/2, both early- and late-type galaxies display similar galaxy–halo size relations with $\log r_{1/2} = 0.55 \log (R_{\rm vir}/210 \, h^{-1}\, {\rm kpc}) + 0.39$. We find that the galaxy–halo size ratio r1/2/Rvir decreases with increasing halo mass. At fixed halo mass, there is no significant dependence of galaxy–halo size ratio on the halo spin or concentration.

Astronomy & Astrophysics↗

DOE OSTI2023

Interpreting Sunyaev–Zel’dovich observations with MillenniumTNG: mass and environment scaling relations

ABSTRACT Sunyaev–Zel’dovich (SZ) measurements can dramatically improve our understanding of the intergalactic medium and the role of feedback processes in galaxy formation, allowing us to calibrate important astrophysical systematics in cosmological constraints from weak lensing galaxy clustering surveys. However, the signal is only measured in a two-dimensional projection, and its correct interpretation relies on understanding the connection between observable quantities and the underlying intrinsic properties of the gas, in addition to the relation between the gas and the underlying matter distribution. One way to address these challenges is through the use of hydrodynamical simulations such as the high-resolution, large-volume MillenniumTNG suite. We find that measurements of the optical depth, τ, and the Compton-y parameter, Y, receive large line-of-sight contributions that can be removed effectively by applying a compensated aperture photometry filter. In contrast with other τ probes (e.g. X-rays and fast radio bursts), the kinematic SZ-inferred τ receives most of its signal from a confined cylindrical region around the halo due to the velocity decorrelation along the line of sight. Additionally, we perform fits to the Y–M and τ–M scaling relations and report best-fitting parameters adopting the smoothly broken power law formalism. We note that subgrid physics modelling can broaden the error bar on these by 30 per cent for intermediate-mass haloes (${\sim }10^{13} \, {\rm M}_{\odot }$). The scatter of the scaling relations can be captured by an intrinsic dependence on concentration and an extrinsic dependence on tidal shear. Finally, we comment on the effect of using galaxies rather than haloes in observations, which can bias the inferred profiles by ∼20 per cent for L* galaxies.

Hadzhiyska, Boryana (ORCID:0000000223123121)↗