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At least 1,657 records · Page 92

A model-independent data assimilation (MIDA) module and its applications in ecology

Models are an important tool to predict Earth system dynamics. An accurate prediction of future states of ecosystems depends on not only model structures but also parameterizations. Model parameters can be constrained by data assimilation. However, applications of data assimilation to ecology are restricted by highly technical requirements such as model-dependent coding. To alleviate this technical burden, we developed a model-independent data assimilation (MIDA) module. MIDA works in three steps including data preparation, execution of data assimilation, and visualization. The first step prepares prior ranges of parameter values, a defined number of iterations, and directory paths to access files of observations and models. The execution step calibrates parameter values to best fit the observations and estimates the parameter posterior distributions. The final step automatically visualizes the calibration performance and posterior distributions. MIDA is model independent, and modelers can use MIDA for an accurate and efficient data assimilation in a simple and interactive way without modification of their original models. We applied MIDA to four types of ecological models: the data assimilation linked ecosystem carbon (DALEC) model, a surrogate-based energy exascale earth system model: the land component (ELM), nine phenological models and a stand-alone biome ecological strategy simulator (BiomeE). The applications indicate that MIDA can effectively solve data assimilation problems for different ecological models. Additionally, the easy implementation and model-independent feature of MIDA breaks the technical barrier of applications of data–model fusion in ecology. MIDA facilitates the assimilation of various observations into models for uncertainty reduction in ecological modeling and forecasting.

Earth system dynamics↗

Optical Activity of Chiral Excitons

Recent activity in the area of chiroptical phenomena has been focused on the connection between structural asymmetry, electron spin configuration and light/matter interactions in chiral semiconductors. In these systems, spin‐splitting phenomena emerge due to inversion symmetry breaking and the presence of extended electronic states, yet the connection to chiroptical phenomena is lacking. Here, in this study, we develop an analytical effective mass model of chiral excitons, parameterized by density functional theory. The model accounts for parity mixing of the band edge Bloch functions resulting from polar distortions, resulting in allowed magnetic dipole transitions. Through the study of a prototypical chiral 2D hybrid perovskite semiconductor, we show that circular dichroism of the chiral exciton and its interband continuum emerges from spin‐splitting via cross‐coupling of Rashba‐like and chiral/helical spin‐texture components. To demonstrate the generality of our approach, and as a counterpoint, we apply our model to describe chiroptical properties of three‐dimensionally confined excitons in perovskite nanocrystals that occur without chiral lattice distortions.

14 SOLAR ENERGY↗

Interatomic Potential Model Development: Finite-Temperature Dynamics Machine Learning

Developing an accurate interatomic potential model is a prerequisite for achieving reliable results from classical molecular dynamics (CMD) simulations; however, most of the potentials are biased as specific simulation purposes or conditions are considered in the parameterization. Here, for developing an unbiased potential, a finite-temperature dynamics machine learning (FTD-ML) approach is proposed, and its processes and feasibility are demonstrated using the Buckingham potential model and aluminum (Al) as an example. Compared with conventional machine learning approaches, FTD-ML exhibits three distinguished features: 1) FTD-ML intrinsically incorporates more extensive configurational and conditional space for enhancing the transferability of developed potentials; 2) FTD-ML employs various properties calculated directly from CMD, for ML model training and prediction validation against experimental data instead of first-principles data; 3) FTD-ML is much more computationally cost effective than first-principles simulations, especially when the system size increases over 10 3 atoms as employed in this research for ensuring reliable training data. The Al Buckingham potential developed by the FTD-ML approach exhibits good performance for general simulation purposes. Thus, the FTD-ML approach is expected to contribute to a fast development of interatomic potential model suitable for various simulation purposes and conditions, without limitation of model type, while maintaining experimental-level accuracy.

42 ENGINEERING↗

Selection of solvents for integrated CO 2 absorption and electrochemical reduction systems

Abstract Solvent‐based electrochemical CO 2 reduction (CO 2 R) enables the production of chemicals or fuels using CO 2 from a preceding absorption process. Employing previously tested CO 2 capture solvents does not ensure their suitability for either CO 2 R or integrated CO 2 absorption‐reduction. We propose solvent selection criteria that include the CO 2 solubility, kinetic constant, ionic conductivity, concentration of the bicarbonate, carbamate, and solvent cation in the CO 2 ‐loaded solution, and sustainability indicators. They are implemented for solvent selection (a) from novel, aqueous mixtures of N ‐methylcyclohexylamine (MCA) with piperazine (PZ), 2‐amino‐2‐methyl‐1‐propanol (AMP), potassium hydroxide (KOH), and potassium chloride (KCl) and (b) from aqueous monoethanolamine (MEA), AMP, KOH, MCA, and PZ solutions. Versions of a modified Kent‐Eisenberg model for strong bases, carbamate, and non‐carbamate‐forming amine solutions are developed and parameterized through experimental equilibrium measurements. CO 2 R experimental results are presented for solutions of KOH and MCA + KOH, as these indicate desired trade‐offs for CO 2 absorption and reduction.

Amines↗

3D‐Printed Carbon Nanoneedle Electrodes for Dopamine Detection in Drosophila

In vivo electrochemistry in small brain regions or synapses requires nanoelectrodes with long straight tips for submicron scale measurements. Nanoelectrodes can be fabricated using a Nanoscribe two-photon printer, but annealed tips curl if they are long and thin. We propose a new pulling-force strategy to fabricate a straight carbon nanoneedle structure. A micron-width bridge is printed between two blocks. The annealed structure shrinks during pyrolysis, and the blocks create a pulling force to form a long, thin, and straight carbon bridge. Parameterization study and COMSOL modeling indicate changes in the block size, bridge size and length affect the pulling force and bridge shrinkage. Electrodes were printed on niobium wires, insulated with aluminum oxide, and the bridge cut with focused ion beam (FIB) to expose the nanoneedle tip. Annealed needle diameters ranged from 400 nm to 5.25 μm and length varied from 50.5 μm to 146 μm. The electrochemical properties are similar to glassy carbon, with good performance for dopamine detection with fast-scan cyclic voltammetry. Nanoelectrodes enable biological applications, such as dopamine detection in a specific Drosophila brain region. Long and thin nanoneedles are generally useful for other applications such as cellular sensing, drug delivery, or gas sensing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Fuel‐Driven π‐Conjugated Superstructures to Form Transient Conductive Hydrogels

Despite advances in creating dissipative materials with transient properties, such as hydrogels and active droplets, their application remains confined to temporal changes in structural properties. Developing out-of-equilibrium materials whose electronic functions are parameterized by a chemical reaction cycle is challenging. Yet, this class of materials is required to construct biomimetic materials. In contrast to traditional chemical reaction cycles that exploit molecularly dissolved building blocks at thermodynamic equilibrium, we show that fiber structures derived from reactive naphthalene diimide (NDI) building blocks can be used as resting states to form far-from-equilibrium conductive hydrogels after the addition of chemical fuels. Upon fueling the NDI-derived fibers, a dual-component activation and deactivation pathway is deduced by kinetic analysis and is absent when using a molecularly dissolved resting state. Investigating the solid-state morphologies of the structures formed throughout the fuel-driven reaction cycle using cryo-EM reveals that the resting thermodynamic fibers evolve to transient thicker fibrils and layered superstructures. We show that the transient redox-active hydrogels exhibit a nearly threefold increase in electrical conductivity upon fuel consumption before reverting to their original value over hours. In conclusion, these far-from-equilibrium materials are potential candidates in applications such as programmable biorobotics and chemical computing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Generalized Brønsted‐Evans‐Polanyi Relationships for Reactions on Metal Surfaces from Machine Learning

Abstract Brønsted‐Evans‐Polanyi (BEP) relationships, i. e., a linear scaling between reaction and activation energies, lie at the core of computational design of heterogeneous catalysts. However, BEPs are not general and often require reparameterization for each class of reactions. Here we construct generalized BEPs (gBEPs), which can predict activation energies for a diverse dataset of reactions of C, O, N and H containing molecules on metal surfaces. In a first step we develop a set of descriptors based on scaling relationships that can capture the change in chemical identity of reactants during the reaction. Subsequently, we use the reaction energy, these descriptors and a single descriptor for the surface structure to parameterize machine learning based regression approaches for the prediction of activation energies. The best approach we developed shows a Mean Absolute Error (MAE) of 0.11 eV for the training set (80 % of the data set) and 0.23 eV for the test set (20 % of the data set). The methodology presented here allows to calculate activation energies within fractions of seconds on a typical personal computer and due to its generality, accuracy and simplicity in application it might prove to be useful in transition metal catalyst design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum optimization algorithms: Energetic implications

Since the dawn of quantum computing (QC), theoretical developments like Shor's algorithm proved the conceptual superiority of QC over traditional computing. However, such quantum supremacy claims are difficult to achieve in practice because of the technical challenges of realizing noiseless qubits. In the near future, QC applications will need to rely on noisy quantum devices that offload part of their work to classical devices. One way to achieve this is by using parameterized quantum circuits in optimization or even in machine learning tasks. The energy requirements of quantum algorithms have not yet been studied extensively. Here in this article, we explore several optimization algorithms using both theoretical insights and numerical experiments to understand their impact on energy consumption. Specifically, we highlight why and how algorithms like quantum natural gradient descent, simultaneous perturbation stochastic approximations or circuit learning methods, are at least 2x to 4x more energy efficient than their classical counterparts; why feedback-based quantum optimization is energy-inefficient; and how techniques like Rosalin can improve the energy efficiency of other algorithms by a factor of ≥2 0 x. Finally, we use the NchooseK high-level programming model to run optimization problems on both gate-based quantum computers and quantum annealers. Empirical data indicate that these optimization problems run faster, have better success rates, and consume less energy on quantum annealers than on their gate-based counterparts.

97 MATHEMATICS AND COMPUTING↗

Assessing dynamic vegetation model parameter uncertainty across Alaskan arctic tundra plant communities

Abstract As the Arctic region moves into uncharted territory under a warming climate, it is important to refine the terrestrial biosphere models (TBMs) that help us understand and predict change. One fundamental uncertainty in TBMs relates to model parameters, configuration variables internal to the model whose value can be estimated from data. We incorporate a version of the Terrestrial Ecosystem Model (TEM) developed for arctic ecosystems into the Predictive Ecosystem Analyzer (PEcAn) framework. PEcAn treats model parameters as probability distributions, estimates parameters based on a synthesis of available field data, and then quantifies both model sensitivity and uncertainty to a given parameter or suite of parameters. We examined how variation in 21 parameters in the equation for gross primary production influenced model sensitivity and uncertainty in terms of two carbon fluxes (net primary productivity and heterotrophic respiration) and two carbon (C) pools (vegetation C and soil C). We set up different parameterizations of TEM across a range of tundra types (tussock tundra, heath tundra, wet sedge tundra, and shrub tundra) in northern Alaska, along a latitudinal transect extending from the coastal plain near Utqiaġvik to the southern foothills of the Brooks Range, to the Seward Peninsula. TEM was most sensitive to parameters related to the temperature regulation of photosynthesis. Model uncertainty was mostly due to parameters related to leaf area, temperature regulation of photosynthesis, and the stomatal responses to ambient light conditions. Our analysis also showed that sensitivity and uncertainty to a given parameter varied spatially. At some sites, model sensitivity and uncertainty tended to be connected to a wider range of parameters, underlining the importance of assessing tundra community processes across environmental gradients or geographic locations. Generally, across sites, the flux of net primary productivity (NPP) and pool of vegetation C had about equal uncertainty, while heterotrophic respiration had higher uncertainty than the pool of soil C. Our study illustrates the complexity inherent in evaluating parameter uncertainty across highly heterogeneous arctic tundra plant communities. It also provides a framework for iteratively testing how newly collected field data related to key parameters may result in more effective forecasting of Arctic change.

54 ENVIRONMENTAL SCIENCES↗

Bringing function to structure: Root–soil interactions shaping phosphatase activity throughout a soil profile in Puerto Rico

Abstract Large areas of highly productive tropical forests occur on weathered soils with low concentrations of available phosphorus (P). In such forests, root and microbial production of acid phosphatase enzymes capable of mineralizing organic phosphorus is considered vital to increasing available P for plant uptake. We measured both root and soil phosphatase throughout depth and alongside a variety of root and soil factors to better understand the potential of roots and soil biota to increase P availability and to constrain estimates of the biochemical mineralization within ecosystem models. We measured soil phosphatase down to 1 m, root phosphatase to 30 cm, and collected data on fine‐root mass density, specific root length, soil P, bulk density, and soil texture using soil cores in four tropical forests within the Luquillo Experimental Forest in Puerto Rico. We found that soil phosphatase decreased with soil depth, but not root phosphatase. Furthermore, when both soil and root phosphatase were expressed per soil volume, soil phosphatase was 100‐fold higher that root phosphatase. Both root and soil factors influenced soil and root phosphatase. Soil phosphatase increased with fine‐root mass density and organic P, which together explained over 50% of the variation in soil phosphatase. Over 80% of the variation in root phosphatase per unit root mass was attributed to specific root length (positive correlation) and available (resin) P (negative correlation). Synthesis : Fine‐root traits and soil P data are necessary to understand and represent soil and root phosphatase activity throughout the soil column and across sites with different soil conditions and tree species. These findings can be used to parameterize or benchmark estimates of biochemical mineralization in ecosystem models that contain fine‐root biomass and soil P distributions throughout depth.

59 BASIC BIOLOGICAL SCIENCES↗

Establishing connectivity patterns of eastern oysters ( Crassostrea virginica ) on regional oceanographic scales

Localized depletion of marine and estuarine populations often results from large-scale natural and anthropogenic disturbances (e.g., hurricanes, oil spills) as well as overharvest of fisheries resources. Understanding how such localized depletions may affect populations at larger regional scales requires knowledge of connectivity among local populations within the larger regional landscape or metapopulation. Efforts to restore populations following such decreases require similar knowledge. During the 2010 Deepwater Horizon oil spill, dramatic declines of oysters occurred throughout estuaries west and east of the Mississippi River. We examined trajectories of particles, which were parameterized to mimic oyster larvae, using the ADvanced CIRCulation (ADCIRC; https://adcirc.org ) model to evaluate potential connectivity within and among embayments from Western Louisiana to Alabama. Patterns of larval settlement, which we defined as the intersection of a larval particle with known or expected oyster habitat at any point 13–21 days post-release, reflected much greater local contributions, with 50%–90% of settled particles originating within the same subdivision of embayments. Exchange among subdivision was much less (0%–40%) and settlement originating from outside the embayment of release was trivial under most scenarios (0%–14%). Connectivity between adjacent basins was greatest for larvae released in the southern portions of the embayment, whereas connectivity among nonadjacent basins was not predicted under the scenarios modeled. Because most local populations are relatively isolated on ecological timescales, areas suffering from extensive local depletion are likely to require extensive time to recover due to the lack of larval subsidy from the overall regional population. Restoration would require building stepping-stone populations or reefs within and among basin to restore a high degree of connectivity.

59 BASIC BIOLOGICAL SCIENCES↗

Simulation-based characterization of the variability of earthquake risk to buildings in the near-field

Recent advancements in high performance computing platforms and computational workflow for regional-scale simulations are enabling unprecedented modeling of fault-to-structure earthquake processes. Regional simulations resolving ground motions at frequencies relevant to engineered systems are becoming computationally viable and provide a new capability to improve understanding of the geographical distribution and intensity of risk to buildings and critical infrastructure. As computational capabilities advance, it is essential to move beyond illustrative single rupture realizations for scenario earthquake events towards the development of a full suite of rupture realizations that appropriately characterize the range of risk to building systems. The work described in this article investigates the application of a suite of fault rupture realizations with the objective of assessing near-fault, site-specific seismic demand variability for building structures. A representative high-performance regional-scale computational model is utilized to execute ground motion and building response simulations based on 18 kinematic rupture realizations of an M7 strike-slip scenario earthquake. The fault rupture models for the scenario earthquake are created by systematically perturbing the hypocenter location and stochastically generating rupture parameters (slip, rise time, rake angle) to represent a breadth of ground motion intensities resulting from the spatial and temporal variabilities of an earthquake rupture process. The resulting seismic demand variability for three-story (short period) and forty-story (long period) steel moment-resisting frame buildings is characterized in terms of the median and distribution of peak inter-story drift ratio for a range of near-fault sites. The full suite of 18 fault rupture realizations and approximately 280,000 nonlinear dynamic building simulations indicate that the three-story building undergoes higher median seismic demand and significantly greater variability of demand at a given site than the forty-story building, which has important implications for the level of certainty in predicting building performance during an earthquake. The simulations performed provide deeper insight into the relationship between fault rupture parameterization and building response, which is essential information for developing a representative suite of rupture realizations for specific earthquake scenarios.

58 GEOSCIENCES↗

Connecting suborganismal data to bioenergetic processes: killifish embryos exposed to a dioxin-like compound

A core challenge for ecological risk assessment is to integrate molecular responses into a chain of causality to organismal or population level outcomes. Bioenergetic theory may be a useful approach for integrating suborganismal responses to predict organismal level responses that influence population dynamics. In this work, we describe a novel application of Dynamic Energy Budget (DEB), theory in the context of a toxicity framework (Adverse Outcome Pathways, AOP) to make quantitative predictions of chemical exposures to individuals, starting from suborganismal data. We use early life stage exposure of Fundulus heteroclitus to dioxin-like chemicals (DLCs) and connect AOP Key Events (KEs) to DEB processes through “damage” that is produced at a rate proportional to the internal toxicant concentration. We use transcriptomic data of fish embryos exposed to DLCs to translate molecular indicators of damage into changes in DEB parameters (damage increases somatic maintenance costs) and use DEB models to predict sublethal and lethal effects of young fish. By changing a small subset of model parameters, we predict the evolved tolerance to DLCs in some wild F. heteroclitus populations, a data set not used in model parameterization. The differences in model parameters points to reduced sensitivity and altered damage repair dynamics as contributing to this evolved resistance. Our methodology has potential extrapolation to untested chemicals of ecological concern.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

A Data Library of Liquid Clouds Modelled With a Large Eddy Simulation Framework

We describe a library of atmospheric large eddy simulations (LES) of liquid-phase boundary layer clouds constructed to enable aerosol–cloud–turbulence interaction studies, support parameterization evaluation and development, and provide training data for machine learning applications. The simulations use a modern LES framework designed for high numerical accuracy, coupled to a detailed spectral bin microphysical scheme. Case studies are configured to represent observed conditions in four key global cloud regions—the Northeastern Atlantic, Northeastern Pacific, Continental United States and Southern Ocean—following a semi-idealised approach. The library also includes aerosol concentration halving and doubling experiments to expose the sensitivities of the case studies to aerosol perturbations. Simulation results are compared to observations on a case-by-case basis, then the library's coverage is evaluated in terms of spreads in meteorological factors and atmospheric boundary layer attributes.

aerosol↗

The importance of explicitly representing the streambed in watershed models

Abstract The streambed is the critical interface between the aquatic and terrestrial systems and hosts important biogeochemical hot spots within river corridors. Although the streambed characteristics are significantly different from those of its surrounding soil, the streambed itself has not been explicitly represented in watershed models. Here, we explicitly incorporated a streambed layer into an integrated hydrologic model through model parameterization and discretization. We examined the hydrological effects of streambed characteristics, including hydraulic conductivity ( K ), layer thickness, and resolution, on the exchange fluxes across the streambed as well as the streamflow at the watershed outlet. The numerical experiments were performed in the American River Watershed, a headwater, mountainous watershed within the Yakima River Basin in central Washington. Despite having a negligible effect on the watershed streamflow, an explicit representation of the streambed with distinctive properties dramatically changed the magnitude and variability of the exchange flux. In general, a larger streambed K along with a thicker streambed layer induced larger exchange fluxes. The exchange flux was most sensitive to the streambed resolution. A finer streambed resolution increased exchange fluxes per unit area while reducing the overall exchange volumes across the entire streambed. The amount of baseflow decreased by 6% as the streambed resolution increased from 250 to 50 m. This finding is important because these hydrological changes may, in turn, affect the exchange of nutrients and contaminants between surface water and groundwater and the associated biogeochemical processes. Our work demonstrated the importance of representing streambeds in fully distributed, process‐based watershed models to better capture the exchange flow dynamics in river corridors.

54 ENVIRONMENTAL SCIENCES↗

Modelling the Effects of Wetland Restoration on Coastal Hydrology: A Case Study of Elkhorn Slough Watershed, California

ABSTRACT Coastal wetlands, some of the most productive ecosystems on Earth, provide critical ecosystem services, including support of biodiversity, carbon sequestration and flood protection. In recent decades, these ecosystems have experienced extensive coastal wetland loss. Coastal wetland restoration provides a beacon of hope, offering a chance to reclaim these important habitats. However, even with billions of dollars invested worldwide in restoring coastal wetlands, we still lack comprehensive knowledge about the effectiveness of these restoration efforts in recovering wetland ecosystem functions and how future climate change may affect these efforts. The ability to evaluate how these ecosystems will function in the future is vital for examining current investments and developing future protection and management plans. We selected Elkhorn Slough, a tidal estuary, in California, to investigate the impact of wetland restoration and sea level rise (SLR) on coastal hydrology using the process‐based coastal hydrologic model, Advanced Terrestrial Simulator (ATS), informed by site‐specific data. We designed a novel modelling workflow for incorporating wetland restoration features into land cover and soil properties for the model parameterization. The validation results demonstrate a strong agreement between modelled and observed data. We studied the characteristics of coastal watershed hydrology, then focused on the surface water dynamics at two wetland sites within Elkhorn Slough, a reference site and a restored site. Our simulation results indicate that the restored site successfully maintains surface elevation, resulting in reduced surface inundation. We also examined the impact of wetland restoration under expected SLR over the next few decades. The low‐lying Yampah Marsh, the reference site, is likely to be inundated due to future SLR when highest tides arrive, while a higher percentage of Hester Marsh, the restored site, would retain marsh vegetation in coming decades, regardless of tidal conditions. Our study provides important information for examining the outcome of restoration practices that include surface elevation in tidal wetlands under climate changes.

advanced terrestrial simulator↗

Estimating dermal contact soil exposure for amphibians

Abstract Chemical exposure estimation through the dermal route is an underemphasized area of ecological risk assessment for terrestrial animals. Currently, there are efforts to create exposure models to estimate doses from this pathway for use in ecological risk assessment. One significant limitation has been insufficient published data to characterize exposure and to support the selection and parameterization of appropriate models, particularly for amphibians in terrestrial habitats. Recent publications measuring pesticide doses to terrestrial‐phase amphibians have begun to rectify this situation. We collated and summarized available measurements of terrestrial amphibian dermal exposure to pesticides from 11 studies in which researchers measured tissue concentrations associated with known pesticide experimental application rates. This data set included tissue concentrations in 11 amphibian species and 14 different pesticides. We then compared the results of two screening exposure models that differed based on surface area scaling approaches as a function of body weight (one based on birds as surrogates for amphibians and another amphibian‐specific) to the measured tissue residue concentrations. We define a false‐negative rate for each screening model as the proportion of amphibians for which the predicted concentration is less than the observed concentration (i.e., underestimate), contrary to the intent of screening models, which are intended to have a bias for higher exposure concentrations. The screening model that uses birds as surrogates did not have any instances where estimated expected avian doses were less than measured amphibian body burdens. When using the amphibian‐specific exposure model that corrected for differences between avian and amphibian surface area, measured concentrations were greater than model estimates for 11.3% of the 1158 comparisons. The database of measured pesticide concentrations in terrestrial amphibians is provided for use in calculating bioconcentration factors and for future amphibian dermal exposure model development. Integr Environ Assess Manag 2023;19:9–16. © 2022 SETAC. This article has been contributed to by U.S. Government employees and their work is in the public domain in the USA.

Environmental Sciences & Ecology↗

Number of sites-based solver for determining coverages from steady-state mean-field micro-kinetic models

Kinetic models parameterized by ab-initio calculations have led to significant improvements in understanding chemical reactions in heterogeneous catalysis. These studies have been facilitated by implementations which determine steady-state coverages and rates of mean-field micro-kinetic models. As implemented in the open-source kinetic modeling program, CatMAP, the conventional solution strategy is to use a root-finding algorithm to determine the coverage of all intermediates through the steady-state expressions, constraining all coverages to be non-negative and to properly sum to unity. Though intuitive, this root-finding strategy causes issues with convergence to solution due to these imposed constraints. In this work, we avoid explicitly imposing these constraints, solving the mean-field steady-state micro-kinetic model in the space of number of sites instead of solving it in the space of coverages. Here, we transform the constrained root-finding problem to an unconstrained least-squares minimization problem, leading to significantly improved convergence in solving micro-kinetic models and thus enabling the efficient study of more complex catalytic reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗