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DOE OSTI2024

Enhancing predictive understanding and accuracy in geological carbon dioxide storage monitoring: Simulation and history matching of tracer transport dynamics

Co-injection of conservative tracers with carbon dioxide (CO 2 ) is a viable tool for monitoring subsurface processes during geological CO 2 storage (GCS). This research investigates the simulation and history-matching of a gas tracer (sulfur hexafluoride, SF 6 ) during CO 2 flooding, employing a core flooding result in Berea sandstone. Four extensively used saturation functions are assessed for their efficacy in history matching of CO 2 /SF 6 injection at the core scale. The history-matching process incorporates particle swarm optimization (PSO) to fine-tune constitutive relationships parameters. Next, employing transport models at the aquifer scale, we interrogate the impact on tracer transport and mixing of saturation function uncertainties, arising from the non-uniqueness of constitutive relationships parameters and saturation function types. To assess the effects of geological heterogeneity on behavior of tracer breakthrough curves (BTCs), we employ two normalized parameters assessing the degree of mixing and SF 6 breakthrough time. The aquifer-scale investigation encompasses both homogeneous and heterogeneous systems with and without capillary heterogeneity effects. Our findings underscore the critical importance of addressing saturation function uncertainties, emphasizing the significance of auxiliary experiments and innovative methodologies to enhance predictive accuracy. The findings highlight significant disparities in arrival times, BTC peaks, tails, and mixing levels, even under optimal conditions. Heterogeneity, with or without capillary heterogeneity, plays a crucial role in shaping BTC variations, resulting in accelerated SF 6 breakthrough times and reduced BTC peaks. Evaluation of monitoring points distant from the injector reveals a dampening effect on the SF6 BTC peak, particularly in heterogeneous systems with capillary heterogeneity, where the peak is halved. These insights underscore the challenges associated with tracer monitoring and the necessity for enhanced methodologies to improve predictive accuracy in subsurface processes during GCS.

58 GEOSCIENCES↗

DOE OSTI2025

Size-resolved Eddy-Covariance Particle Flux Measurement during the TRACER Campaign (Final Report)

The main goal of the TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign was to study aerosol–cloud interactions during deep convection over the Houston area. This project deployed a suite of instrumentation with the aim to (1) quantify turbulent vertical particle fluxes during at DOE-ARM sites, including TRACER, (2) assess hygroscopic growth factors and hygroscopicity parameters of the material driving modal aerosol growth during new particle formation and growth events, (3) derive turbulent aerosol mass fluxes using co-located Doppler LIDAR measurements, and (4) create quality-controlled PI data products to support future research utilizing data collected during the TRACER campaign. This report summarized the main findings from the deployments at two DOE-ARM sites. Briefly, we found that new particle formation may occur aloft, in a residual layer, near the top of the boundary layer. Small grown particles appear later due to downward mixing with daytime turbulence. The species that are responsible for aerosol modal growth had hygroscopicity parameters varying between 0.05 and 0.34. These values systematically depended on the wind sector, suggesting that the chemical composition of the precursors differed. This work demonstrated that lidar retrievals of the elastic backscatter and Doppler velocity can be used to obtain surface number emissions of particles with a diameter greater than 0.53 µm. During TRACER, emission particle number fluxes peaked near ∼ 100 cm−2 s−1. Multiple quality-controlled PI data products that will support future TRACER related science were generated and made publically available.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

TAMU TRACER: Targeted Mobile Measurements to Isolate the Impacts of Aerosols and Meteorology on Deep Convection

Difficulty in using observations to isolate the impacts of aerosols from meteorology on deep convection often stems from inability to resolve the spatiotemporal variations in the environment serving as the storm’s inflow region. During the DOE TRacking Aerosol Convection interactions ExpeRiment (TRACER) in June-September 2022, a Texas A&M University (TAMU) team conducted a mobile field campaign to characterize the meteorological and aerosol variability in airmasses that serve as inflow to convection across the ubiquitous mesoscale boundaries associated with the sea- and bay-breezes in the Houston, Texas, region. These boundaries propagate inland over the fixed DOE Atmospheric Radiation Measurement (ARM) sites. However, convection occurs on either or both the continental or maritime sides or along the boundary. The maritime and continental airmasses serving as convection inflow may be quite distinct, with different meteorological and aerosol characteristics that fixed-site measurements cannot simultaneously sample. Thus, a primary objective of TAMU TRACER was to provide mobile measurements similar to those at the fixed sites, but in the opposite airmass across these moving mesoscale boundaries. TAMU TRACER collected radiosonde, lidar, aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) measurements on 29 enhanced operations days covering a variety of maritime, continental, outflow, and pre-frontal airmasses. This paper summarizes the TAMU TRACER deployment and measurement strategy, instruments, available datasets, and provides sample cases highlighting differences between these mobile measurements and those made at the ARM sites. We also highlight the exceptional TAMU TRACER undergraduate student participation in high impact learning activities through forecasting and field deployment opportunities.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1984

Analysis techniques for tracer studies of oxidation

Analysis techniques to obtain quantitative diffusion data from tracer concentration profiles were developed. Mass balance ideas were applied to determine the mechanism of oxide growth and to separate the fraction of inward and outward growth of oxide scales. The process of inward oxygen diffusion with exchange was theoretically modelled and the effect of lattice diffusivity, grain boundary diffusivity and grain size on the tracer concentration profile was studied. The development of the tracer concentration profile in a growing oxide scale was simulated. The double oxidation technique was applied to a FeCrAl-Zr alloy using 0-18 as a tracer. SIMS was used to obtain the tracer concentration profile. The formation of lacey oxide on the alloy was discussed. Careful consideration was given to the quality of data required to obtain quantitative information.

Basu, S. N.↗

DOE OSTI2024

Using Convex Optimization to Efficiently Apportion Tracer and Pollutant Sources From Point Concentration Observations

Abstract Rivers transport elements, minerals, chemicals, and pollutants produced in their upstream basins. A sample from a river is a mixture of all of its upstream sources, making it challenging to pinpoint the contribution from each individual source. Here, we show how a nested sample design and convex optimization can be used to efficiently unmix downstream samples of a well‐mixed, conservative tracer in a steady state system into the contributions of their upstream sources. Our approach is significantly faster than previous methods. We represent the river's sub‐catchments, defined by sampling sites, using a directed acyclic graph. This graph is used to build a convex optimization problem which, thanks to its convexity, can be quickly solved to global optimality—in under a second on desktop hardware for data sets of ∼100 samples or fewer. Uncertainties in the upstream predictions can be generated using Monte Carlo resampling. We provide an open‐source implementation of this approach in Python. The inputs required are straightforward: a table containing sample locations and observed tracer concentrations, along with a D8 flow‐direction raster map. As a case study, we use this method to map the elemental geochemistry of sediment sources for rivers draining the Cairngorms mountains, UK. This method could be extended to non‐conservative and non‐steady state tracers. We also show, theoretically, how multiple tracers could be simultaneously inverted to recover upstream run‐off or erosion rates as well as source concentrations. Overall, this approach can provide valuable insights to researchers in various fields, including water quality, geochemical exploration, geochemistry, hydrology, and wastewater epidemiology.

Barnes, Richard↗

NASA NTRS1979

A secondary tracer approach to the derivation of galactic cosmic-ray source isotopic abundances

A formalism has been developed for deriving cosmic-ray source isotopic abundances from observed local abundances using a purely secondary nuclide as a tracer of spallation production during propagation. Although the formalism is based on the leaky-box model of cosmic-ray propagation, it is shown that source abundances derived by the tracer technique are reasonably independent of detailed propagation models. The tracer formalism also permits a quantitative evaluation of the effects of observational uncertainties on deduced source abundances. It is shown that statistical errors in the observed abundances and uncertainties in the spallation cross sections are at present the dominant sources of uncertainty. The latter error can be reduced with increased detector size or exposure time, while the former can be minimized by measurements of the relative production cross sections. As a specific example, the tracer technique is applied to the isotopes of sulfur and calcium, and the level of uncertainties which must be achieved to distinguish evolutionary differences between solar-system material and cosmic ray-source material are established.

Stone, E. C.↗

NASA NTRS1986

A deliberate tracer experiment in Santa Monica Basin

A tracer technique was developed for measurements of diffusion across oceanic density strata using SF6 and perfluorodecalin (PFD) tracers in the Santa Monica Basin. Fifty days after injection, the tracers were found to have mixed along the isopycnal surface to nearly every part of the basin. The diapycnal spreading of the tracer distributions yielded an apparent eddy diffusivity of 0.33 + or - 0.08 sq cm/s at the ambient density gradient of 4.0 + or - 0.5 x 10 to the -9th g/cm to the 4th.

Ledwell, J. R.↗

NASA NTRS1988

Tracer water transport and subgrid precipitation variation within atmospheric general circulation models

A capability is developed for monitoring tracer water movement in the three-dimensional Goddard Institute for Space Science Atmospheric General Circulation Model (GCM). A typical experiment with the tracer water model follows water evaporating from selected grid squares and determines where this water first returns to the Earth's surface as precipitation or condensate, thereby providing information on the lateral scales of hydrological transport in the GCM. Through a comparison of model results with observations in nature, inferences can be drawn concerning real world water transport. Tests of the tracer water model include a comparison of simulated and observed vertically-integrated vapor flux fields and simulations of atomic tritium transport from the stratosphere to the oceans. The inter-annual variability of the tracer water model results is also examined.

Koster, Randal D.↗

NASA NTRS1995

Tracer transport for realistic aircraft emission scenarios calculated using a three-dimensional model

A three-dimensional transport model, which uses winds from a stratospheric data assimilation system, is used to study the transport of supersonic aircraft exhaust in the lower stratosphere. A passive tracer is continuously injected into the transport model. The tracer source distribution is based on realistic scenarios for the daily emission rate of reactive nitrogen species for all forecasted flight routes. Winds are from northern hemisphere winter/spring months for 1979 and 1989; there are minimal differences between the tracer integrations for the 2 years. During the integration, peak tracer mixing ratios in the flight corridors are compared with the zonal mean and found to be greater by a factor of 2 or less. This implies that the zonal mean assumption used in two dimensional models is reasonable during winter and spring. There is a preference for pollutant buildup in the heavily traveled North Pacific and North Atlantic flight corridors. Pollutant concentration in the corridors depends on the position of the Aleutian anticyclone and the northern hemisphere polar vortex edge.

Weaver, Clark J.↗

NASA NTRS2001

Water Vapor Tracers as Diagnostics of the Regional Hydrologic Cycle

Numerous studies suggest that local feedback of evaporation on precipitation, or recycling, is a significant source of water for precipitation. Quantitative results on the exact amount of recycling have been difficult to obtain in view of the inherent limitations of diagnostic recycling calculations. The current study describes a calculation of the amount of local and remote sources of water for precipitation, based on the implementation of passive constituent tracers of water vapor (termed water vapor tracers, WVT) in a general circulation model. In this case, the major limitation on the accuracy of the recycling estimates is the veracity of the numerically simulated hydrological cycle, though we note that this approach can also be implemented within the context of a data assimilation system. In this approach, each WVT is associated with an evaporative source region, and tracks the water until it precipitates from the atmosphere. By assuming that the regional water is well mixed with water from other sources, the physical processes that act on the WVT are determined in proportion to those that act on the model's prognostic water vapor. In this way, the local and remote sources of water for precipitation can be computed within the model simulation, and can be validated against the model's prognostic water vapor. Furthermore, estimates of precipitation recycling can be compared with bulk diagnostic approaches. As a demonstration of the method, the regional hydrologic cycles for North America and India are evaluated for six summers (June, July and August) of model simulation. More than 50% of the precipitation in the Midwestern United States came from continental regional tracers, and the local source was the largest of the regional tracers (14%). The Gulf of Mexico and Atlantic 2 regions contributed 18% of the water for Midwestern precipitation, but further analysis suggests that the greater region of the Tropical Atlantic Ocean may also contribute significantly. In general, most North American land regions showed a positive correlation between evaporation and recycling ratio (except the Southeast United States) and negative correlations of recycling ratio with precipitation and moisture transport (except the Southwestern United States). The Midwestern local source is positively correlated with local evaporation, but it is not correlated with water vapor transport. This is contrary to bulk diagnostic estimates of precipitation recycling. In India, the local source of precipitation is a small percentage of the precipitation owing to the dominance of the atmospheric transport of oceanic water. The southern Indian Ocean provides a key source of water for both the Indian continent and the Sahelian region.

Bosilovich, Michael G.↗

NASA NTRS2001

Water Vapor Tracers as Diagnostics of the Regional Hydrologic Cycle

Numerous studies suggest that local feedback of surface evaporation on precipitation, or recycling, is a significant source of water for precipitation. Quantitative results on the exact amount of recycling have been difficult to obtain in view of the inherent limitations of diagnostic recycling calculations. The current study describes a calculation of the amount of local and remote geographic sources of surface evaporation for precipitation, based on the implementation of three-dimensional constituent tracers of regional water vapor sources (termed water vapor tracers, WVT) in a general circulation model. The major limitation on the accuracy of the recycling estimates is the veracity of the numerically simulated hydrological cycle, though we note that this approach can also be implemented within the context of a data assimilation system. In the WVT approach, each tracer is associated with an evaporative source region for a prognostic three-dimensional variable that represents a partial amount of the total atmospheric water vapor. The physical processes that act on a WVT are determined in proportion to those that act on the model's prognostic water vapor. In this way, the local and remote sources of water for precipitation can be predicted within the model simulation, and can be validated against the model's prognostic water vapor. As a demonstration of the method, the regional hydrologic cycles for North America and India are evaluated for six summers (June, July and August) of model simulation. More than 50% of the precipitation in the Midwestern United States came from continental regional sources, and the local source was the largest of the regional tracers (14%). The Gulf of Mexico and Atlantic regions contributed 18% of the water for Midwestern precipitation, but further analysis suggests that the greater region of the Tropical Atlantic Ocean may also contribute significantly. In most North American continental regions, the local source of precipitation is correlated with total precipitation. There is a general positive correlation between local evaporation and local precipitation, but it can be weaker because large evaporation can occur when precipitation is inhibited. In India, the local source of precipitation is a small percentage of the precipitation owing to the dominance of the atmospheric transport of oceanic water. The southern Indian Ocean provides a key source of water for both the Indian continent and the Sahelian region.

Bosilovich, Michael G.↗

NASA NTRS2002

A Wavelet Based Suboptimal Kalman Filter for Assimilation of Stratospheric Chemical Tracer Observations

A suboptimal Kalman filter system which evolves error covariances in terms of a truncated set of wavelet coefficients has been developed for the assimilation of chemical tracer observations of CH4. The truncation is carried out in such a way that the resolution of the error covariance, is reduced only in the zonal direction, where gradients are smaller. Assimilation experiments which last 24 days, and used different degrees of truncation were carried out. These reduced the covariance, by 90, 97 and 99 % and the computational cost of covariance propagation by 80, 93 and 96 % respectively. The difference in both error covariance and the tracer field between the truncated and full systems over this period were found to be not growing in the first case, and a growing relatively slowly in the later two cases. The largest errors in the tracer fields were found to occur in regions of largest zonal gradients in the tracer field.

Auger, Ludovic↗

NASA NTRS2003

Using Neural Networks to Describe Tracer Correlations

Neural networks are ideally suited to describe the spatial and temporal dependence of tracer-tracer correlations. The neural network performs well even in regions where the correlations are less compact and normally a family of correlation curves would be required. For example, the CH4-N2O correlation can be well described using a neural network trained with the latitude, pressure, time of year, and CH4 volume mixing ratio (v.m.r.). In this study a neural network using Quickprop learning and one hidden layer with eight nodes was able to reproduce the CH4-N2O correlation with a correlation co- efficient of 0.9995. Such an accurate representation of tracer-tracer correlations allows more use to be made of long-term datasets to constrain chemical models. Such as the dataset from the Halogen Occultation Experiment (HALOE) which has continuously observed CH4, (but not N2O) from 1991 till the present. The neural network Fortran code used is available for download.

Lary, D. J.↗

NASA NTRS2011

Comparison of Four Mixed Layer Mesoscale Parameterizations and the Equation for an Arbitrary Tracer

In this paper we discuss two issues, the inter-comparison of four mixed layer mesoscale parameterizations and the search for the eddy induced velocity for an arbitrary tracer. It must be stressed that our analysis is limited to mixed layer mesoscales since we do not treat sub-mesoscales and small turbulent mixing. As for the first item, since three of the four parameterizations are expressed in terms of a stream function and a residual flux of the RMT formalism (residual mean theory), while the fourth is expressed in terms of vertical and horizontal fluxes, we needed a formalism to connect the two formulations. The standard RMT representation developed for the deep ocean cannot be extended to the mixed layer since its stream function does not vanish at the ocean's surface. We develop a new RMT representation that satisfies the surface boundary condition. As for the general form of the eddy induced velocity for an arbitrary tracer, thus far, it has been assumed that there is only the one that originates from the curl of the stream function. This is because it was assumed that the tracer residual flux is purely diffusive. On the other hand, we show that in the case of an arbitrary tracer, the residual flux has also a skew component that gives rise to an additional bolus velocity. Therefore, instead of only one bolus velocity, there are now two, one coming from the curl of the stream function and other from the skew part of the residual flux. In the buoyancy case, only one bolus velocity contributes to the mean buoyancy equation since the residual flux is indeed only diffusive.

Canuto, V. M.↗

NASA NTRS2016

Hemispheric Differences in Tropical Lower Stratospheric Transport and Tracers Annual Cycle

Transport of long-lived tracers (such as O, CO, and N O) in the lower stratosphere largely determines the composition of the entire stratosphere. Stratospheric transport includes the mean residual circulation (with air rising in the tropics and sinking in the polar and middle latitudes), plus two-way isentropic (quasi-horizontal) mixing by eddies. However, the relative importance of two transport components remains uncertain. Previous studies quantified the relative role of these processes based on tropics-wide average characteristics under common assumption of well-mixed tropics. However, multiple instruments provide us with evidence that show significant differences in the seasonal cycle of ozone between the Northern (0-20N) and Southern (0-20S) tropical (NT and ST respectively) lower stratosphere. In this study we investigate these differences in tracer seasonality and quantify transport processes affecting tracers annual cycle amplitude using simulations from Goddard Earth Observing System Chemistry Climate Model (GEOSCCM) and Whole Atmosphere Community Climate Model (WACCM) and compare them to observations from the Microwave Limb Sounder (MLS) on the Aura satellite. We detect the observed contrast between the ST and NT in GEOSCCM and WACCM: annual cycle in ozone and other chemical tracers is larger in the NT than in the ST but opposite is true for the annual cycle in vertical advection. Ozone budgets in the models, analyzed based on the Transformed Eulerian Mean (TEM) framework, demonstrate a major role of quasi-horizontal mixing vertical advection in determining the NTST ozone distribution and behavior. Analysis of zonal variations in the NT and ST ozone annual cycles further suggests important role of North American and Asian Summer Monsoons (associated with strong isentropic mixing) on the lower stratospheric ozone in the NT. Furthermore, multi model comparison shows that most CCMs reproduce the observed characteristic of ozone annual cycle quite well. Thus, latitudinal variations within the tropics have to be considered in order to understand the balance between upwelling and quasi- horizontal mixing in the tropical lower stratosphere and the paradigm of well mixed tropics has to be reconsidered.

Chemistry-Climate Models↗

DOE OSTI2026

A Unified Tracer Analysis of DESI DR2 Baryon Acoustic Oscillations

We improve upon previous efforts to optimally combine overlapping galaxy samples in the DESI baryon acoustic oscillation analysis. By weighting each galaxy by its linear bias, overlapping galaxies are combined into a single, unified catalog, naturally avoiding double counting of cosmic volume and including all auto- and cross- information at the catalog level. Improvements over the previous effort include the addition of QSO out to $z=1.6$ to account for all overlapping DR2 tracers and redshift-dependent bias treatment to improve reconstruction. We report distance measurements using this unified tracer, and find them to be highly consistent with the baseline DR2 BAO analysis. We also test for tracer-dependent systematics within the DESI data, and find no evidence of tracer-dependent systematics within $0.8

Sanders, N. [Ohio U., Athens] (ORCID:0009000800202↗

DOE OSTI2025

Data and scripts associated with “Sequential Precipitation Input Tagging (SPIT) to Estimate Water Transit Times and Hydrologic Tracer Dynamics within Water-Tagging Enabled Hydrologic Models” (v3)

This data package is associated with the publication “Sequential Precipitation Input Tagging (SPIT) to Estimate Water Transit Times and Hydrologic Tracer Dynamics within Water-Tagging Enabled Hydrologic Models” submitted to Journal of Advances in Modeling Earth Systems (Butler et al. 2025). This study developed the Sequential Precipitation Input Tagging (SPIT) framework to tag input precipitation and estimate water transit times and hydrologic tracers. SPIT tags all precipitation events at regular intervals over an extended period (monthly tags over seven years) in a hydrologic model from 2016-2022. SPIT is applied at six National Ecological Observatory Network (NEON) sites across the continental United States to calculate transit time distributions (TTD) and derive from these mean transit times (MTT), fractions of young water (Fyw), and hydrologic tracer concentrations in stream water (δ18O) within a water-tagging enabled version of the Weather Research and Forecast (WT-WRF-Hydro) model with national water model (NWM) configurations. We go on to validate WT-WRF-Hydro estimates against Butler et al. (2023), who analyzed the same NEON sites using stable water isotope data to estimate water transit times. This new tracking method provides a detailed picture of water movement and helps improve predictions about water availability in the future. This data package was originally published in January 2025. It was updated May 2025 (v2; new and modified files) and October 2025 (v3; new and modified files). File and folder names were not revised to indicate changes. See the change history section in the readme for more details. This data package contains the data and scripts used to develop the SPIT framework WT-WRF-Hydro (Water Tagging Weather Research and Forecasting Hydrologic) model and is associated with the following GitHub repository: https://github.com/zbutler33/SPIT-Framework. This data package contains five parent folders: (1) “Manipulated_outputs”, (2) “Metadata”, (3) “Observed”, (4) “Outputs”, and (5) “Scripts”. Each of these parent folders contains additional subfolders and files. Please see the FLMD (“v*_Butler_2024_WT_WRF_Hydro_flmd.csv”) for a list of all the files contained in this data package and descriptions for each. See the data dictionary (“v*_Butler_2024_WT_WRF_Hydro_dd.csv”) for definitions and units of all of the tabular (files ending in “.csv” and ".tsv") column headers.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Numerical Water Tracers in the Atmospheric Component of the Energy Exascale Earth System Model: Implementation and Changes in Moisture Origin

Numerical water tracers are implemented in the Energy Exascale Earth System Model version 2. Simulations performed with the water‐tag‐enabled model for both pre‐industrial and future greenhouse gas concentrations reveal a marked increase in the role of mid‐latitude and southern subtropical regions as exporters of atmospheric moisture—to the extratropical upper troposphere and the tropical free troposphere. For the latter, the northward shift of the Intertropical Convergence Zone increases cross‐hemispheric transport of subtropical water vapor to the Northern Hemisphere. In the polar regions, most of the lower tropospheric moistening instead arises from increases in local evaporation. These findings illustrate the utility of the water tags, underscore critical changes in global hydrologic cycle, and provide insight into atmospheric dynamics under future climate scenarios. For applications when a global grid is desired, we additionally propose a novel statistical reconstruction, based on copula modeling, of the joint distribution of origin of water vapor, which reduces the number of tracers from order $\mathcal{O}\left({n}^{2}\right)$to order $\mathcal{O}(n)$, substantially ameliorating the considerable computational cost of water tracers. This statistical reconstruction is particularly beneficial to the interpretation of the relationship between latitude and longitude of origin of moisture over the tropical oceans and in the lower troposphere over land.

copula modeling↗