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DOE OSTI2025

Transverse-momentum-dependent pion structures from lattice QCD: Collins-Soper kernel, soft factor, TMDWF, and TMDPDF

We present the first lattice quantum chromodynamics (QCD) calculation of the pion valence-quark transverse-momentum-dependent parton distribution function (TMDPDF) within the framework of large-momentum effective theory (LaMET). Using correlators fixed in the Coulomb gauge (CG), we computed the quasi-TMD beam function for a pion with a mass of 300 MeV, a fine lattice spacing of 𝑎 =0.06 fm, and multiple large momenta up to 3 GeV. The intrinsic soft functions in the CG approach are extracted from form factors with large momentum transfer, and as a byproduct, we also obtain the corresponding Collins-Soper (CS) kernel. Our determinations of both the soft function and the CS kernel agree with perturbation theory at small transverse separations (𝑏 ⊥ ) between the quarks. At larger 𝑏 ⊥ , the CS kernel remains consistent with recent results obtained using both CG and gauge-invariant TMD correlators in the literature. By combining next-to-leading logarithmic factorization of the quasi-TMD beam function and the soft function, we obtain an 𝑥-dependent pion valence-quark TMDPDF for transverse separations 𝑏 ⊥ ≳1 fm. Interestingly, we find that the 𝑏 ⊥ dependence of the phenomenological parametrizations of TMDPDF for moderate values of 𝑥 are in reasonable agreement with our QCD determinations. In addition, we present results for the transverse-momentum-dependent wave function for a heavier pion with 670 MeV mass.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Ionization of HCCI Neutral and Cations by Strong Laser Fields Simulated With Time Dependent Configuration Interaction

Strong field ionization of neutral iodoacetylene (HCCI) can produce a coherent superposition of the X and A cations. This superposition results in charge migration between the CC π orbital and the iodine π-type lone pair which can be monitored by strong field ionization with short, intense probe pulses. Strong field ionization of the X and A states of HCCI cation was simulated with time-dependent configuration interaction using singly ionized configurations and singly excited, singly ionized configurations (TD-CISD-IP) and an absorbing boundary. Studies with static fields were used to obtain the 3-dimensional angular dependence of instantaneous ionization rates by strong fields and the orbitals involved in producing the cations and dications. The frequency of charge oscillation is determined by the energy separation of the X and A states; this separation can change depending on the direction and strength of the field. Furthermore, fields along the molecular axis can cause extensive mixing between the field-free X and A configurations. For coherent superpositions of the X and A states, the charge oscillations are characterized by two frequencies–the driving frequency of the laser field of the probe pulse and the intrinsic frequency due to the energy separation between the X and A states. For linear and circularly polarized pulses, the ionization rates show marked differences that depend on the polarization direction of the pulse, the carrier envelope phase and initial phase of the superposition. Varying the initial phase of the superposition at the beginning of the probe pulse is analogous to changing the delay between the pump and probe pulses. The charge oscillation in the coherent superposition of the X and A states results in maxima and minima in the ionization yield as a function of the superposition phase

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Dependable classical-quantum computing systems engineering

Increasing evidence suggests quantum computing (QC) complements traditional High-Performance Computing (HPC) by leveraging its unique capabilities, leading to the emergence of a new, hybrid paradigm, QHPC. However, this integration introduces new challenges, with dependability–defined by reproducibility, resiliency, and security and privacy–emerging as a central concern for building trustworthy systems that provide an advantage to the users. This paper proposes a framework for dependable QHPC system design, organized around these three pillars. We identify integration challenges, anticipate roadblocks, and highlight productive synergies across QC, HPC, cloud platforms, and network security. Drawing from both classical computing principles and quantum-specific insights, we present a roadmap for co-design that supports robust hybrid architectures. Our approach offers concrete metrics for assessing dependability, provides design guidance for engineers working at the QC-HPC interface, and surfaces new engineering questions around complexity, scale, and fault tolerance. Ultimately, designing for dependability is key to realizing practical, scalable QHPC systems and accelerating the broader quantum ecosystem capable of translating quantum promises into actual application delivery.

HPC↗

NASA NTRS2014

Time-Dependent Response Versus Scan Angle for MODIS Reflective Solar Bands

The Moderate Resolution Imaging Spectroradiometer (MODIS) instruments currently operate onboard the National Aeronautics and Space Administration (NASA's) Terra and Aqua spacecraft, launched on December 18, 1999 and May 4, 2002, respectively. MODIS has 36 spectral bands, among which 20 are reflective solar bands (RSBs) covering a spectral range from 0.412 to 2.13 μm. The RSBs are calibrated on orbit using a solar diffuser (SD) and an SD stability monitor and with additional measurements from lunar observations via a space view (SV) port. Selected pseudo-invariant desert sites are also used to track the RSB on-orbit gain change, particularly for short-wavelength bands. MODIS views the Earth surface, SV, and the onboard calibrators using a two-sided scan mirror. The response versus scan angle (RVS) of the scan mirror was characterized prior to launch, and its changes are tracked using observations made at different angles of incidence from onboard SD, lunar, and Earth view (EV) measurements. These observations show that the optical properties of the scan mirror have experienced large wavelength-dependent degradation in both the visible and near infrared spectral regions. Algorithms have been developed to track the on-orbit RVS change using the calibrators and the selected desert sites. These algorithms have been applied to both Terra and Aqua MODIS Level 1B (L1B) to improve the EV data accuracy since L1B Collection 4, refined in Collection 5, and further improved in the latest Collection 6 (C6). In C6, two approaches have been used to derive the time-dependent RVS for MODIS RSB. The first approach relies on data collected from sensor onboard calibrators and mirror side ratios from EV observations. The second approach uses onboard calibrators and EV response trending from selected desert sites. This approach is mainly used for the bands with much larger changes in their time-dependent RVS, such as the Terra MODIS bands 1-4, 8, and 9 and the Aqua MODIS bands 8- and 9. In this paper, the algorithms of these approaches are described, their performance is demonstrated, and their impact on L1B products is discussed. In general, the shorter wavelength bands have experienced a larger on-orbit RVS change, which, in general, are mirror side and detector dependent. The on-orbit RVS change due to the degradation of band 8 can be as large as 35 percent for Terra MODIS and 20 percent for Aqua MODIS. Vital to maintaining the accuracy of the MODIS L1B products is an accurate characterization of the on-orbit RVS change. The derived time-independent RVS, implemented in C6, makes an important improvement to the quality of the MODIS L1B products.

MODIS↗

NASA NTRS2014

Challenges in Modelling of Lightning-Induced Delamination; Effect of Temperature-Dependent Interfacial Properties

Lightning is a major cause of damage in laminated composite aerospace structures during flight. Due to the dielectric nature of Carbon fiber reinforced polymers (CFRPs), the high energy induced by lightning strike transforms into extreme, localized surface temperature accompanied with a high-pressure shockwave resulting in extensive damage. It is crucial to develop a numerical tool capable of predicting the damage induced from a lightning strike to supplement extremely expensive lightning experiments. Delamination is one of the most significant failure modes resulting from a lightning strike. It can be extended well beyond the visible damage zone, and requires sophisticated techniques and equipment to detect. A popular technique used to model delamination is the cohesive zone approach. Since the loading induced from a lightning strike event is assumed to consist of extreme localized heating, the cohesive zone formulation should additionally account for temperature effects. However, the sensitivity to this dependency remains unknown. Therefore, the major focus point of this work is to investigate the importance of this dependency via defining various temperature dependency profiles for the cohesive zone properties, and analyzing the corresponding delamination area. Thus, a detailed numerical model consisting of multidirectional composite plies with temperature-dependent cohesive elements in between is subjected to lightning (excessive amount of heat and pressure) and delamination/damage expansion is studied under specified conditions.

interlaminar damage↗

NASA NTRS2018

Initial Investigation of the Angular Dependence of the NOAA-20 VIIRS Solar Diffuser BRDF Change Factor

The NOAA-20 (formerly the Joint Polar Satellite System-1) satellite was launched on November 18, 2017. One of the five scientific instruments aboard the NOAA-20 satellite (N20) is the Visible Infrared Imaging Radiometer Suite (VIIRS). The VIIRS scans the earth surface in 22 spectral bands, of which 14 are denoted as the reflective solar bands (RSBs) with design band central wavelengths from 412 to 2250 nm. The VIIRS regularly performs on-orbit radiometric calibration of its RSBs, primarily through observations of an onboard sunlit solar diffuser (SD). The on-orbit change of the SD bidirectional reflectance distribution function (BRDF) value, denoted as the H-factor, is determined by an onboard solar diffuser stability monitor (SDSM). We have shown that the H-factor for the SD on the VIIRS instrument on the Suomi National Polar-orbiting Partnership (SNPP) satellite is both incident and outgoing sunlight direction dependent. This angular dependence profoundly affects the on-orbit radiometric calibration process and results. Here, we give preliminary results for the angular dependence for the N20 VIIRS SD H-factor, and compare the dependence with that for the SNPP VIIRS.

radiometric calibration↗

NASA NTRS2021

Positional Dependence of SNPP VIIRS Solar Diffuser BRDF Change Factor: An Empirical Approach

The Earth-observing Visible Infrared Imaging Radiometer Suite (VIIRS) on the Suomi National Polar-orbiting Partnership satellite regularly performs on-orbit radiometric calibration of its reflective solar bands (RSBs), primarily through observations of an onboard sunlit solar diffuser (SD). The on-orbit change of the SD bidirectional reflectance distribution function (BRDF) value, quantified by a numerical factor called the H-factor, is determined by the onboard SD stability monitor. Our previous study showed that the H-factor is solar angle and view direction dependent. In this study, we determine the dependence of the H-factor on the detector SD view footprint location. We fit an empirical model to the NASA Collection 1 SNPP VIIRS Level 1B (L1B) spectral reflectance difference across the detectors in an RSB over uniform Earth scenes of the Libya 4 desert and deep convective clouds. We apply the model predicted SD positional dependent H-factor to calibrate the RSBs. Under this new calibration scheme, the original unreal striping is removed from the homogeneous Libya 4 desert and the deep convective cloud images, as well as the original unreal striping from the Dunhuang desert image. The SD positional dependent H-factor has been used to calculate the SNPP VIIRS RSB radiometric correction factor for the NASA Collection 2.0 SNPP VIIRS L1B products.

SNPP VIIRS↗

DOE OSTI2020

One-loop matching for spin-dependent quasi-TMDs

Transverse momentum dependent parton distribution functions (TMDPDFs) provide a unique probe of the three-dimensional spin structure of hadrons. We construct spin-dependent quasi-TMDPDFs that are amenable to lattice QCD calculations and that can be used to determine spin-dependent TMDPDFs. We calculate the short-distance coefficients connecting spin-dependent TMDPDFs and quasi-TMDPDFs at one-loop order. We find that the helicity and transversity distributions have the same coefficient as the unpolarized TMDPDF. We also argue that the same is true for pretzelosity and that this spin universality of the matching will hold to all orders in αs. Thus, it is possible to calculate ratios of these distributions as a function of longitudinal momentum and transverse position utilizing simpler Wilson line paths than have previously been considered.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Constraining the Chiral Magnetic Effect with charge-dependent azimuthal correlations in Pb-Pb collisions at $ \sqrt{s_{\mathrm{NN}}} $ = 2.76 and 5.02 TeV

Systematic studies of charge-dependent two- and three-particle correlations in Pb-Pb collisions at $ \sqrt{s_{\mathrm{NN}}} $ = 2.76 and 5.02 TeV used to probe the Chiral Magnetic Effect (CME) are presented. These measurements are performed for charged particles in the pseudorapidity ( η ) and transverse momentum ( p T ) ranges | η | < 0 . 8 and 0 . 2 < p T < 5 GeV/ c . A significant charge-dependent signal that becomes more pronounced for peripheral collisions is reported for the CME-sensitive correlators γ 1, 1 =$\langle4cos( φ α + φ β - 2Ψ 2 )$\rangle$ and γ 1, - 3 = $\langle$cos( φ α - 3 φ β + 2Ψ 2 )$\rangle$. The results are used to estimate the contribution of background effects, associated with local charge conservation coupled to anisotropic flow modulations, to measurements of the CME. A blast-wave parametrisation that incorporates local charge conservation tuned to reproduce the centrality dependent background effects is not able to fully describe the measured γ 1 , 1 . Finally, the charge and centrality dependence of mixed-harmonics three-particle correlations, of the form γ 1, 2 = $\langle$cos( φ α + 2 φ β - 3Ψ 3 )$\rangle$, which are insensitive to the CME signal, verify again that background contributions dominate the measurement of γ 1 , 1 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Submicron immunoglobulin particles exhibit FcγRII-dependent toxicity linked to autophagy in TNFα-stimulated endothelial cells

In intravenous immunoglobulins (IVIG), and some other immunoglobulin products, protein particles have been implicated in adverse events. Role and mechanisms of immunoglobulin particles in vascular adverse effects of blood components and manufactured biologics have not been elucidated. We have developed a model of spherical silica microparticles (SiMPs) of distinct sizes 200–2000 nm coated with different IVIG- or albumin (HSA)-coronas and investigated their effects on cultured human umbilical vein endothelial cells (HUVEC). IVIG products (1–20 mg/mL), bare SiMPs or SiMPs with IVIG-corona, did not display significant toxicity to unstimulated HUVEC. In contrast, in TNFα-stimulated HUVEC, IVIG-SiMPs induced decrease of HUVEC viability compared to HSA-SiMPs, while no toxicity of soluble IVIG was observed. 200 nm IVIG-SiMPs after 24 h treatment further increased ICAM1 (intercellular adhesion molecule 1) and tissue factor surface expression, apoptosis, mammalian target of rapamacin (mTOR)-dependent activation of autophagy, and release of extracellular vesicles, positive for mitophagy markers. Toxic effects of IVIG-SiMPs were most prominent for 200 nm SiMPs and decreased with larger SiMP size. Using blocking antibodies, toxicity of IVIG-SiMPs was found dependent on FcγRII receptor expression on HUVEC, which increased after TNFα-stimulation. Similar results were observed with different IVIG products and research grade IgG preparations. In conclusion, submicron particles with immunoglobulin corona induced size-dependent toxicity in TNFα-stimulated HUVEC via FcγRII receptors, associated with apoptosis and mTOR-dependent activation of autophagy. Testing of IVIG toxicity in endothelial cells prestimulated with proinflammatory cytokines is relevant to clinical conditions. Our results warrant further studies on endothelial toxicity of sub-visible immunoglobulin particles.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Grain size dependencies of intergranular solute segregation in nanocrystalline materials

Grain boundary segregation is of increasing importance for stabilizing nanocrystalline alloys, and while segregation is typically modeled as a scale-independent phenomenon, at the finest nanocrystalline grain sizes there are several sources of grain size dependence. Here we provide quantitative detail on two grain size dependencies not previously elaborated, both of which arise from the spectrality of intergranular segregation sites. The first of these arises because a change in grain size affects which portions of the segregation spectrum are occupied by the solutes, with no change in the shape or nature of the spectrum itself. The second of these arises from the presence of higher-order grain junctions, which have unique segregation behaviors and an increasing relative presence at finer grain sizes. This paper uses molecular statics to quantify these size dependencies in detail for the case of an Al(Mg) binary alloy. Together, these two effects combined have a significant effect on the effective McLean segregation energy of more than 6 kJ/mol (from approximately -18.5 kJ/mol at 5 nm to -12.5 kJ/mol at more than 40 nm), with the majority of grain size dependence arising from the spectrality of segregation sites.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Zng1 is a GTP-dependent zinc transferase needed for activation of methionine aminopeptidase

The evolution of zinc (Zn) as a protein cofactor altered the functional landscape of biology, but dependency on Zn also created an Achilles' heel, necessitating adaptive mechanisms to ensure Zn availability to proteins. A debated strategy is whether metallochaperones exist to prioritize essential Zn-dependent proteins. Here, we present evidence for a conserved family of putative metal transferases in human and fungi, which interact with Zn-dependent methionine aminopeptidase type I (MetAP1/Map1p/Fma1). Deletion of the putative metal transferase in Saccharomyces cerevisiae (ZNG1; formerly YNR029c) leads to defective Map1p function and a Zn-deficiency growth defect. In vitro, Zng1p can transfer Zn 2+ or Co 2+ to apo-Map1p, but unlike characterized copper chaperones, transfer is dependent on GTP hydrolysis. Proteomics reveal mis-regulation of the Zap1p transcription factor regulon due to loss of ZNG1 and Map1p activity, suggesting that Zng1p is required to avoid a compounding effect of Map1p dysfunction on survival during Zn limitation.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

Temperature-dependent changes in gas chromatographic separation metrics for trihexyl(tetradecyl)phosphonium-based ionic liquid stationary phases and comparison to conventional polysiloxane stationary phases

Here, to assess whether the trihexyl(tetradecyl)phosphonium chloride ([P 66614 + ][Cl - ]) ionic liquid (IL), employed as a gas chromatographic stationary phase, exhibits temperature-dependent phase transitions or structural heterogeneity, retention thermodynamics for probe molecules of varied chemical structure were investigated by gas chromatography (GC) over the temperature range of 25 to 64 °C using van’t Hoff analysis. All van’t Hoff plots for n-alkanes (C8–C12) and other probe analytes were linear, indicating the absence of detectable phase-transition behavior. The [P 66614 + ][Cl - ] IL was further compared with the [P 66614 + ] bis[(trifluoromethyl)sulfonyl]imide ([P 66614 + ][NTf 2 - ]) IL and commercial polysiloxane stationary phases in terms of temperature-dependent resolution behavior and chromatographic selectivity over the temperature range of 28–52 °C. The resolution factors of analytes in mixtures obtained using gas chromatography–mass spectrometry (GC–MS) and the summation of resolution values decreased smoothly with temperature on both IL stationary phases and on the dimethylphenylcyano-substituted polymeric stationary phase (OV-1701), whereas the poly(50% diphenyl/50% dimethyl siloxane) stationary phase (SPB-50) exhibited irregularities in its temperature-dependent summation of resolution profile, showing a distinct maximum in the temperature range of 34–40 °C. Selectivity values for the IL stationary phases were largely determined by the anion, with the [P 66614 + ][Cl - ] IL providing enhanced separation between polar and aromatic analytes, while the [P 66614 + ][NTf 2 - ] IL favored dispersive and π-π interactions that resulted in a reversal of elution order for some aliphatic–aromatic and alkyne-containing analyte pairs. Capillary columns prepared using different surface activation methods and coated with identical [P 66614 + ][Cl - ] IL stationary phase showed indistinguishable temperature-dependent trends in summation of resolution value and selectivity. An evaluation of analyte-specific selectivity provides insight into the characteristic separation behavior of the stationary phases and enables identification of analyte classes that are more efficiently separated on the [P 66614 + ]-based IL stationary phases compared to conventional stationary phase materials.

Chromatographic selectivity↗

DOE OSTI2021

Spin-dependent Seebeck and Nernst effects in an ideal skyrmion gas

In this work, we theoretically and numerically study spin-dependent Seebeck and Nernst effects in 2D ferromagnetic materials with the topological spin texture (skyrmion and vortex) ideal gas. From the numerical solution of the matrix Boltzmann equation for a nonequilibrium distribution function and the Lippmann–Schwinger equation for a T-matrix we find the strong nonlinear behaviors in the thermoelectric coefficients depending on skyrmion/vortex diameters and electron concentrations. In particular, the dramatic dependences in the Seebeck and Nernst coefficients take place at larger magnetic texture sizes where the abrupt sign flip in the vortex Seebeck and Nernst coefficients occurs in the narrow region of electron concentrations. In this case the normalized Nernst coefficient changes from +5 to -7. The spin-dependent thermoelectric coefficients are proportional to T at low temperatures for all skyrmion/vortex sizes.

36 MATERIALS SCIENCE↗

DOE OSTI2024

In-situ determination of strain during transient burst testing and the temperature dependence of Zircaloy-4 claddings

Understanding fuel system behavior during postulated loss-of-coolant accidents is pertinent for continued safe and efficient operation of light water reactors, particularly as higher burnups are being pursued and safety margins re-evaluated. Conventional mechanical models for the incumbent Zr alloys typically rely on the assumption that steady-state creep is the dominant fuel cladding response during transient accident conditions. To investigate this assumption, simulated accident burst testing was performed on Zircaloy-4 claddings with balloon behavior measured in-situ. Here, two distinct loading conditions were utilized during burst testing: (1) constant-gas-inventory where pressure was allowed to increase with temperature and (2) constant pressure. In-situ strains and strain rates were measured via 2-dimensional digital image correlation techniques and synchronized with temperature to determine deformation dependencies. The temperature dependence of strain rate was characterized by a two segment Arrhenius relationship, with a distinct transition between the high and low temperature/strain regimes. The average activation energy of the lower temperature/strain regime was 328 ± 25 kJ/mol, in agreement with the ~320 kJ/mol used for conventional LOCA models. However, the higher temperature/strain segment, which encompassed most of ballooning, showed increased activation energies as well as a dependence on whether the burst region was in view. For tests that burst away from the camera view, the average high temperature/strain segment activation energy was 635 ± 150 kJ/mol. For samples where the rupture opening formed in view, the average activation energy was 1015 ± 179 kJ/mol. This observed shift in temperature dependence indicates a transition in deformation mechanism at the end of life, possibly to time independent failure mechanisms, which has not yet been visualized in the literature for Zr alloys. Parameters at the transition points were analyzed to determine thresholds for this change in behavior, which occurred at an average hoop strain of 6.9 ± 2.1 %.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Line tension induced character angle dependence of dislocation mobility in FCC alloys

Here, we explore the character angle dependence of dislocation-solute interactions in a face-centered cubic random Fe0.70Ni0.11Cr0.19 alloy through molecular dynamics (MD) simulations of dislocation mobility. Using the MD mobility data, we determine the phonon and thermally activated solute drag parameters which govern mobility for each dislocation character angle. The resulting parameter set indicates that, surprisingly, the solute energy barrier does not depend on character angle. Instead, only the zero-temperature flow stress—which is dictated by the activation area for thermal activation—is dependent on character angle. By analyzing the line roughness from MD simulations and the geometry of a bowing dislocation line undergoing thermal activation, we conclude that the character angle dependence of the activation area in this alloy is governed by the dislocation line tension, rather than the dislocation-solute interaction itself. Our findings motivate further investigation into the line geometry of dislocations in solid solutions.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Shape- and Orientation-Dependent Scattering of Isolated Gold Nanostructures Using Polarized Dark-Field Microscopy

In this work, we demonstrate a simple and robust method for measuring the shape- and orientation-dependent optical scattering of various plasmonic nanostructures adsorbed onto a solid surface using polarized dark-field microscopy. By analyzing the dark-field scattering images of gold nanostructures using grazing incidence polarized light with a bench-top microscope, we are able to correlate optical scattering from the individual nanostructures with their shape and orientation. Depending on the size, shape, and orientation of the plasmonic nanostructures, they exhibit characteristic angle- and polarization-dependent scattering signals. Extracting the red, green, and blue channels of the scattering signals from a color-imaging detector as a function of azimuthal angle provides a polar plot of color intensity values that is characteristic of the underlying nanostructure. Examples are presented for various nanostructures, including spherical nanoparticles, nanotriangles, and nanorods. Experimental results are complemented by numerical calculations of the scattering spectra of representative model nanostructures. We demonstrate that the polarization- and orientation-dependent scattering behavior is a consequence of various localized surface plasmon modes existing in the nanostructures and can be used to verify the shape of individual objects as well as quickly identify the orientation of numerous objects on a densely populated substrate. We anticipate that this method will provide a rapid and efficient complement to the typical structural analysis of nanoparticles that is achieved by electron microscopy as well as providing a simple method for generating detailed information of the optical scattering of various types of individual plasmonic nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Resolving the Coverage Dependence of Surface Reaction Kinetics with Machine Learning and Automated Quantum Chemistry Workflows

Microkinetic models for catalytic systems require estimation of many thermodynamic and kinetic parameters that can be calculated for isolated species and transition states using ab initio methods. However, the presence of nearby coadsorbates on the surface can dramatically alter these thermodynamic and kinetic parameters causing them to be dependent on species coverage fractions. As there are combinatorially many coadsorbed configurations on the surface, computing the coverage dependence of these parameters is far less straightforward. We present a framework for generating and applying machine learning models to predict coverage-dependent parameters for microkinetic models. Our toolkit enables automatic calculation and evaluation of coadsorbed configurations allowing us to sample 2,000 coadsorbed adsorbates and transition states (TSs) for a diverse set of 9 reactions on Cu(111), a challenging surface, with four possible coadsorbates. This dataset was then used to train subgraph isomorphic decision trees (SIDTs) to predict the stability and association energy of configurations. We were able to achieve mean absolute errors (MAEs) of 0.106 eV on adsorbates, 0.172 eV on TSs, and due to natural error cancellation in SIDTs for relative properties, 0.130 eV on reaction energies and 0.180 eV on activation barriers. In conclusion, we describe how to use these models to predict coverage-dependent corrections for adsorbates and TSs and demonstrate on H*, HO*, and O* comparing the generated SIDT model with an iteratively refined version.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗