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Optical radiation associated with gamma-ray bursts

Calculations are made of the approximate characteristics of the reprocessed optical radiation resulting from the absorption of a gamma-ray burst by a nearby star. The overall reprocessing time scale, including contributions from gamma-ray transfer and diffusion of the optical radiation, is estimated. It is noted that diffusive cooling occurs by either a 'self-similar' or a 'transparency' wave of postabsorption stellar surface temperatures greater or less than 10,000 K, respectively. Depending on the combination of stellar and gamma-ray burst properties, the reprocessing time scale can vary from the duration of the gamma-ray burst (approximately 1 s) to the maximum calculated cooling time (approximately 1000 s). Calculations for close binary systems are made of the number of optical photons per square centimeter expected at earth as a function of the observed gamma-ray burst fluences and likely distances. It is predicted that, if all gamma-ray bursters are in close binaries, the number of detections per year by an all sky monitor of 200 photons per sq cm sensitivity will be about 100.

London, R. A.↗

Magnetic photon splitting and gamma ray burst spectra

The splitting of photons into two photons becomes both possible and significant in magnetic fields in excess of 10(exp 12) Gauss. Below the threshold energy, 2m sub e c(exp 2) for single photon pair production, splitting can be an astronomically observable phenomenon evident in gamma ray burst spectra. In such circumstances, it was found that magnetic photon splitting reprocesses the gamma ray burst continuum by degrading the photon energy, with a net effect that is quite similar to pair cascade reprocessing of the spectrum. Results are presented for the spectral modifications due to splitting, taking into account the different probabilities for splitting for different polarization modes. Unpolarized and polarized pair cascade photon spectra form the input spectra for the model, which calculates the resulting splitting reprocessed spectra numerically by solving the photon kinetic equations for each polarization mode. This inclusion of photon polarizations is found to not alter previous predictions that splitting produce a significant flattening of the hard X ray continuum and a bump at MeV energies below a pair production turnover. The spectrum near the bump is always strongly polarized.

Baring, Matthew G.↗

Accretion Disks in Supersoft X-ray Sources

We examine the role of the accretion disk in the steady-burning white dwarf model for supersoft sources. The accretion luminosity of the disk is quite small compared to the nuclear burning luminosity of the central source. Thus, in contrast to standard accretion disks, the main role of the disk is to reprocess the radiation from the white dwarf. We calculate models of accretion disks around luminous white dwarfs and compare the resulting disk fluxes to optical and UV observations of the LMC supersoft sources CAL 83, CAL 87, and RX J0513.9-6951. We find that if the white dwarf luminosity is near the upper end of the steady-burning region, and the flaring of the disk is included, then reprocessing by the disk can account for the UV fluxes and a substantial fraction of the optical fluxes of these systems. Reprocessing by the companion star can provide additional optical flux, and here too the disk plays an important role: since the disk is fairly thick, it shadows a significant fraction of the companion's surface.

Popham, Robert↗

Complementary Reliability-Based Decodings of Binary Linear Block Codes

This correspondence presents a hybrid reliability-based decoding algorithm which combines the reprocessing method based on the most reliable basis and a generalized Chase-type algebraic decoder based on the least reliable positions. It is shown that reprocessing with a simple additional algebraic decoding effort achieves significant coding gain. For long codes, the order of reprocessing required to achieve asymptotic optimum error performance is reduced by approximately 1/3. This significantly reduces the computational complexity, especially for long codes. Also, a more efficient criterion for stopping the decoding process is derived based on the knowledge of the algebraic decoding solution.

Fossorier, Marc P. C.↗

SeaWiFS Postlaunch Calibration and Validation Analyses

The effort to resolve data quality issues and improve on the initial data evaluation methodologies of the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) Project was an extensive one. These evaluations have resulted, to date, in three major reprocessings of the entire data set where each reprocessing addressed the data quality issues that could be identified up to the time of each reprocessing. The number of chapters (21) needed to document this extensive work in the SeaWiFS Postlaunch Technical Report Series requires three volumes. The chapters in Volumes 9, 10, and 11 are in a logical order sequencing through sensor calibration, atmospheric correction, masks and flags, product evaluations, and bio-optical algorithms. The first chapter of Volume 9 is an overview of the calibration and validation program, including a table of activities from the inception of the SeaWiFS Project. Chapter 2 describes the fine adjustments of sensor detector knee radiances, i.e., radiance levels where three of the four detectors in each SeaWiFS band saturate. Chapters 3 and 4 describe the analyses of the lunar and solar calibration time series, respectively, which are used to track the temporal changes in radiometric sensitivity in each band. Chapter 5 outlines the procedure used to adjust band 7 relative to band 8 to derive reasonable aerosol radiances in band 7 as compared to those in band 8 in the vicinity of Lanai, Hawaii, the vicarious calibration site. Chapter 6 presents the procedure used to estimate the vicarious calibration gain adjustment factors for bands 1-6 using the waterleaving radiances from the Marine Optical Buoy (MOBY) offshore of Lanai. Chapter 7 provides the adjustments to the coccolithophore flag algorithm which were required for improved performance over the prelaunch version. Chapter 8 is an overview of the numerous modifications to the atmospheric correction algorithm that have been implemented. Chapter 9 describes the methodology used to remove artifacts of sun glint contamination for portions of the imagery outside the sun glint mask. Finally, Chapter 10 explains a modification to the ozone interpolation method to account for actual time differences between the SeaWiFS and Total Ozone Mapping Spectrometer (TOMS) orbits.

Hooker, Stanford B.↗

TRMM Version 7 Level 3 Gridded Monthly Accumulations of GPROF Precipitation Retrievals

In July 2011, improved versions of the retrieval algorithms were approved for TRMM. All data starting with June 2011 are produced only with the version 7 code. At the same time, version 7 reprocessing of all TRMM mission data was started. By the end of August 2011, the 14+ years of the reprocessed mission data became available online to users. This reprocessing provided the opportunity to redo and enhance upon an analysis of V7 impacts on L3 data accumulations that was presented at the 2010 EGU General Assembly. This paper will discuss the impact of algorithm changes made in th GPROF retrieval on the Level 2 swath products. Perhaps the most important change in that retrieval was to replacement of a model based a priori database with one created from Precipitation Radar (PR) and TMI brightness temperature (Tb) data. The radar pays a major role in the V7 GPROF (GPROF2010) in determining existence of rain. The level 2 retrieval algorithm also introduced a field providing the probability of rain. This combined use of the PR has some impact on the retrievals and created areas, particularly over ocean, where many areas of low-probability precipitation are retrieved whereas in version 6, these areas contained zero rain rates. This paper will discuss how these impacts get translated to the space/time averaged monthly products that use the GPROF retrievals. The level 3 products discussed are the gridded text product 3G68 and the standard 3A12 and 3B31 products. The paper provides an overview of the changes and explanation of how the level 3 products dealt with the change in the retrieval approach. Using the .25 deg x .25 degree grid, the paper will show that agreement between the swath product and the level 3 remains very high. It will also present comparisons of V6 and V7 GPROF retrievals as seen both at the swath level and the level 3 time/space gridded accumulations. It will show that the various L3 products based on GPROF level 2 retrievals are in close agreement. The paper concludes by outlining some of the challenges of the TRMM version 7 level 3 products.

Stocker, E. F.↗

A 40 Year Time Series of SBUV Observations: the Version 8.6 Processing

Under a NASA program to produce long term data records from instruments on multiple satellites (MEaSUREs), data from a series of eight SBUV and SBUV 12 instruments have been reprocessed to create a 40 year long ozone time series. Data from the Nimbus 4 BUV, Nimbus 7 SBUV, and SBUV/2 instruments on NOAA 9, 11, 14, 16, 17, and 18 were used covering the period 1970 to 1972 and 1979 to the present. In past analyses an ozone time series was created from these instruments by adjusting ozone itself, instrument by instrument, for consistency during overlap periods. In the version 8.6 processing adjustments were made to the radiance calibration of each instrument to maintain a consistent calibration over the entire time series. Data for all eight instruments were then reprocessed using the adjusted radiances. Reprocessing is necessary to produce an accurate latitude dependence. Other improvements incorporated in version 8.6 included the use of the ozone cross sections of Brion, Daumont, and Malicet, and the use of a cloud height climatology derived from Aura OMI measurements. The new cross sections have a more accurate temperature dependence than the cross sections previously used. The OMI-based cloud heights account for the penetration of UV into the upper layers of clouds. The consistency of the version 8.6 time series was evaluated by intra-instrument comparisons during overlap periods, comparisons with ground-based instruments, and comparisons with measurements made by instruments on other satellites such as SAGE II and UARS MLS. These comparisons show that for the instruments on NOAA 16, 17 and 18, the instrument calibrations were remarkably stable and consistent from instrument to instrument. The data record from the Nimbus 7 SBUV was also very stable, and SAGE and ground-based comparisons show that the' calibration was consistent with measurements made years laterby the NOAA 16 instrument. The calibrations of the SBUV/2 instruments on NOAA 9, 11, and 14 were more of a problem. The rapidly drifting orbits of these satellites resulted in relative time and altitude dependent differences that are significant. Despite these problems, total column ozone appears to be consistent to better than 1% over the entire time series, while the ozone vertical distribution is consistent to approximately 5%.

McPeters, Richard↗

GPM V05 Gridded Text Products

This presentation will summarize the changes in the products for the GPM V05 reprocessing cycle. It will concentrate on discussing the gridded text product from the core satellite retrievals. However, all aspects of the GPROF GMI changes in this product are equally appropriate to the other two gridded text products. The GPM mission reprocessed its products in May of 2017 as part of a continuing improvement of precipitation retrievals. This lead to important improvement in the retrievals and therefore also necessitated reprocessing the gridded test products. The V05 GPROF changes not only improved the retrievals but substantially alerted the format and this compelled changes to the gridded text products. Especially important in this regard is the GPROF2017 (used in V05) change from reporting the fraction of the total precipitation rate that occurring as convection or in liquid phase. Instead, GPROF2017, and therefore V05 gridded text products, report the rate of convective precipitation in mm/hr. The GPROF2017 algorithm now reports the frozen precipitation rate in mm/hr rather than the fraction of total precipitation that is liquid. Because of the aim of the gridded text product is to remain simple the radar and combined results will also change in V05 to reflect this change in the GMI retrieval. The presentation provides an analysis of these changes as well as presenting a comparison with the swath products from which the hourly text grids were derived.

PPS↗

Assessing Sensitivity of MERRA-2 to AMSU-A in the Upper Stratosphere

Microwavetemperaturesounders provide key observationsin data assimilation, both in the 9current and historical global observing systems, as they provide the largest amount of horizontal and vertical temperature information due to their insensitivity to clouds. In the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2),microwave sounder radiances from the Advanced Microwave Sounding Unit-A (AMSU-A)are assimilated beginning with NOAA-15and continuing through the current period. The time series of observation minus background statistics forAMSU-A channels sensitive to upper stratosphere and lower mesosphere show variabilities due to changes in AMSU-A constellation in the early AMSU-A period.Noted discrepancies are seen at the onset and exit of AMSU-A observations on the NOAA-15, NOAA-16, NOAA-17, and NASA EOS Aqua satellites.This effort characterizesthesensitivity, both in terms of the observations and the MERRA-2 analysis. Furthermore, it exploresthe use of reprocessed and inter-calibrated datasets to evaluatewhether these homogenized observations can reduce the disparity due to change in instrumental biases against the model background. The results indicate that the AMSU-A radiances used in MERRA-2 are the fundamental cause of this inter-platform sensitivitywhich can be mitigated by using reprocessed data.The results explore the importance of the reprocessing of the AMSU-A radiances as well as their inter-calibration.

MERRA-2↗

Validation Assessment for the Soil Moisture Active Passive (SMAP) Level 4 Carbon (L4_C) Data Product Version 5

The post-launch Cal/Val phase of the SMAP mission is guided by two primary objectives for each science product team: 1) to calibrate, verify, and improve the performance of the science algorithms, and 2) validate accuracies of the science data products as specified in the SMAP Level-1 mission science requirements. Algorithm science and product maintenance activities during the SMAP extended mission phase have also involved periodic algorithm calibration and product refinements to maintain or enhance product consistency and performance as well as science utility. This report provides an assessment of the latest (Version 5) SMAP Level 4 Carbon (L4_C) product. The L4_C Version 5 (v5) global record now spans more than six years (March 2015 – present) of SMAP operations and has benefited from five major reprocessing updates to the operational product. These reprocessing events and L4_C product release updates have incorporated various algorithm refinements and calibration adjustments to account for similar refinements to the upstream GEOS land model assimilation system, SMAP brightness temperatures, and MODIS vegetation inputs used for L4_C processing. The SMAP L4_C algorithms utilize a terrestrial carbon flux model informed by daily surface and root zone soil moisture information contributed from the SMAP Level 4 Soil Moisture (L4_SM) product along with optical remote sensing-based (e.g. MODIS-based) land cover and canopy fractional photosynthetic active radiation (fPAR), and other ancillary biophysical data. The carbon flux model estimates global daily net ecosystem CO2 exchange (NEE) and the component carbon fluxes, namely, vegetation gross primary production (GPP) and soil heterotrophic respiration (Rh). Other L4_C product elements include surface (~0-5 cm depth) soil organic carbon (SOC) stocks and associated environmental constraints to these processes, including soil moisture-related controls on GPP and ecosystem respiration (Kimball et al. 2014, Jones et al. 2017). The L4_C product addresses SMAP carbon cycle science objectives by: 1) providing a direct link between terrestrial carbon fluxes and underlying freeze/thaw and soil moisture-related constraints to these processes, 2) documenting primary connections between terrestrial water, energy and carbon cycles, and 3) improving understanding of terrestrial carbon sink activity. The SMAP L4_C algorithms and operational product are mature and at a CEOS Validation Stage 4 level (Jackson et al. 2012) based on extensive validation of the multi-year record against a diverse array of independent benchmarks, well characterized global performance, and systematic refinements gained from five major reprocessing events. There are no Level-1 mission science requirements for the L4_C product; however, self-imposed requirements have been established focusing on NEE as the primary product field for validation, and on demonstrating L4_C accuracy and success in meeting product science requirements (Jackson et al. 2012). The other L4_C product fields also have strong utility for carbon science applications (e.g., Liu et al. 2019, Endsley et al. 2020); however, analysis of these other fields is considered secondary relative to primary validation activities focusing on NEE. The L4_C targeted accuracy requirements are to meet or exceed a mean unbiased root-mean-square error (ubRMSE, or standard deviation of the error) for NEE of 1.6 g C m-2 d-1 and 30 g C m-2 yr-1, emphasizing northern (≥45°N) boreal and arctic ecosystems; this accuracy is similar to that of tower eddy covariance measurement-based observations (Baldocchi 2008). Methods used for the latest v5 L4_C product performance and validation assessment have been established from the SMAP Cal/Val plan and previous studies (Jackson et al. 2012, Jones et al. 2017) and include: 1) consistency evaluations of the product fields against earlier product releases (version 4 or earlier); 2) comparisons of daily carbon flux estimates with independent tower eddy 4covariance measurement-based daily carbon (CO2) flux observations from core tower validation sites (CVS); and 3) consistency checks against other global carbon products, including soil carbon inventory records, global GPP records derived from tower observation upscaling methods, and satellite-based observations of canopy solar induced chlorophyll fluorescence (SIF) as a surrogate for GPP. Metrics used to evaluate relative agreement between L4_C product fields and observational benchmarks include correlation (r-value), RMSE differences, bias and model sensitivity diagnostics. Following these validation criteria, the present report provides a validation assessment of the latest L4_C product release (v5). Detailed descriptions of the L4_C algorithm and additional global product accuracy and performance results are given elsewhere (Jones et al. 2017, Endsley et al. 2020). The v5 L4_C product replaces earlier product versions and continues to show: (i) accuracy and performance levels meeting or exceeding SMAP L4_C science requirements; (ii) improvement over the previous product version (version 4); and (iii) suitability for a diversity of science applications. Example L4_C applications from the recent literature include clarifying environmental trends and controls on the northern terrestrial carbon sink (Liu et al. 2019), diagnosing drought-related impacts on ecosystem productivity (Li et al. 2020), and regional monitoring of cropland conditions for projecting annual yields (Wurster et al. 2020). 2EXPECTED L4_C ALGORITHM AND PRODUCTPERFORMANCE The L4_C algorithm performance, including variance and uncertainty estimates of model outputs, was determined during the mission pre-launch phase through spatially explicit model sensitivity studies using available model inputs similar to those currently being used for operational production and evaluating the resulting model simulations over the observed range of northern (≥45 °N) and global conditions (Kimball et al. 2012, Entekhabi et al. 2014). The L4_C algorithm options were also evaluated during the mission prelaunch phase, including deriving canopy fPAR from lower order NDVI (Normalized Difference Vegetation Index) inputs in lieu of using MODIS (MOD15) fPAR; and including an explicit model representation of boreal fire disturbance recovery impacts. These results indicated that the L4_C accuracy requirements (i.e., NEE ubRMSE ≤ 30 g C m-2 yr-1or ≤ 1.6 g C m-2 d-1) could be met from the baseline algorithms over more than 82% and 89% of global and northern vegetated land areas, respectively (Yi et al. 2013, Kimball et al. 2014). The global L4_C algorithm error budget for NEE derived during the mission prelaunch phase indicated that the estimated NEE ubRMSE uncertainty is proportional to GPP and is therefore larger in higher biomass productivity areas, including forests and croplands (Kimball et al. 2014). Likewise, NEE ubRMSE uncertainty is expected to be lower in less-productive areas, including grasslands and shrublands. Expected model NEE ubRMSE levels were also generally within targeted accuracy levels for characteristically less-productive boreal and Arctic biomes, even though relative model error as a proportion of total productivity (NEE RMSE / GPP) may be large in these areas. The estimated NEE uncertainty was lower than expected in some warmer tropical high biomass productivity areas (e.g. Amazon rainforest) because of reduced low temperature and moisture constraints to the L4_C respiration calculations so that the bulk of model uncertainty is contributed by GPP in these areas. Model NEE uncertainty in the African Congo was estimated to

SMAP↗

Updates in Developing a Prototype Science Pipeline and Full-Volume, Global Hyperspectral Synthetic Data Sets for NASA’s Earth System Observatory’s Upcoming Surface, Biology and Geology Mission

The Surface Biology and Geology (SBG) mission recently passed mission confirmation review and has entered phase A – design and development. SBG will acquire high resolution solar-reflected spectroscopy and thermal infrared observations at a data rate of ~2.5 TB/day and generate products at ~40 TB/day. Given that the per-day volume is greater than NASA’s total extant airborne hyperspectral data collection, collecting, processing, disseminating, and exploiting the SBG data present new challenges. To meet these challenges, we have developed a prototype science pipeline and a full-volume global hyperspectral synthetic data set to help prepare for SBG’s flight (see poster GC42D-0730). Our science pipeline is based on the science processing technology developed for NASA’s Kepler and TESS planet-hunting missions. The pipeline infrastructure, Ziggy, provides a scalable architecture for robust, repeatable, and replicable science and application products that can be run on a range of systems from a laptop to the cloud or a supercomputer. Ziggy is compliant with NASA Procedural Requirement (NPR) 7150.2C, is at a technical readiness level (TRL) of 7 and has been released to github.com/nasa/ziggy. We integrated Ziggy with EO-1/Hyperion workflows to build a prototype pipeline and ingested the 17-year mission archive that provides globally sampled visible through shortwave infrared spectra that are representative of SBG data types and volumes. We fully implemented the first stage and processed the entire 55 TB Hyperion data set from the raw data (Level 0) to top-of-the-atmosphere radiance (Level 1R). We are currently evaluating the ISOFIT atmospheric correction module to convert the L1R data to surface reflectance (Level 2) before reprocessing the full data set to L2. Crosschecks are being performed with RadCalNet as well as with coincident observations by AVIRIS. We are also investigating modern methods for georectifying the Hyperion scenes. Finally, we describe an analysis of the cost to conduct forward processing and reprocessing campaigns for SBG on HECC with dedicated compute and storage resources using the resurrected Hyperion pipeline as a proxy for full-volume SBG data. The analysis demonstrates that SBG L0 data can be processed to L2 on HECC with full reprocessing campaigns every two years for ~$2.6M over a 7-year lifespan. Moreover, 69% of the system capacity would be available for other activities, possibly enabling future open-source science activities, including algorithm development, L3+ processing, .etc.

ESD↗

Considerations For Waste-to-Base Future Research Paths

Developing innovative technologies to reprocess low value waste into high value base products will enable a new “Waste-to-Base” (WtB) capability leading to innovative approaches to space mission design. Systems engineers and mission architects will work together under a new paradigm in logistics planning. Equipment, components, packaging, storage, and structures will be understood not only by functional requirements, but also in terms of useful lifetimes and materials of construction. The advent of a new technical discipline - reprocess engineering - will grow from the intersection between chemical, mechanical, and systems engineering, mission design, and logistics planning. A crowdsourcing approach was employed to gather low Technology Readiness Level (TRL) concepts into workable solutions for issues in trash management, CO 2 processing, foam reprocessing, and fecal processing. The results of the crowdsourcing activities are summarized along with a discussion for future technology development work.

Logistics reduction↗

Considerations For Waste-to-Base Future Research Paths

Developing innovative technologies to reprocess low value waste into high value base products will enable a new “Waste-to-Base” (WtB) capability leading to innovative approaches to space mission design. Systems engineers and mission architects will work together under a new paradigm in logistics planning. Equipment, components, packaging, storage, and structures will be understood not only by functional requirements, but also in terms of useful lifetimes and materials of construction. The advent of a new technical discipline - reprocess engineering - will grow from the intersection between chemical, mechanical, and systems engineering, mission design, and logistics planning. A crowdsourcing approach was employed to gather low Technology Readiness Level (TRL) concepts into workable solutions for issues in trash management, CO2 processing, foam reprocessing, and fecal processing. The results of the crowdsourcing activities are summarized along with a discussion for future technology development work.

Logistics reduction↗

TESS Data Release Notes: Sector 59, DR84

TESS Sector 59 observations include physical orbits 125 and 126 of the spacecraft around the Earth. Data collection was paused for a total of 0.63 days to download data. Data were downloaded approximately every seven days, once near apogee of each orbit and once near perigee. Note that the Sector 59 data were briefly made available on 2023 January 18–19 before an issue was identified that required reprocessing. Data have since been reprocessed. The reprocessing has a minimal impact on the final light curves, but resulted in a different set of TCEs than initially released. Users should re-download the data if retrieved before January 19th. In total, there are 25.79 days of science data collected in Sector 59.

TESS↗

Sensitivity and Uncertainty Quantification of Transition Scenario Simulations

This report documents the first collective attempt at developing and applying capabilities to quantify uncertainties, assess parametric sensitivities, and optimize multiple parameters and metrics in fuel cycle simulations generated by the SA&I Campaign. To do this, external codes that were designed to perform sensitivity analysis and uncertainty quantification (SA&UQ) needed to be coupled to the SA&I Campaign’s nuclear fuel cycle simulators (NFCS). In FY20, two approaches were pursued: 1) coupling Cyclus to an ORNL-internal code called MOT (Metaheuristic Optimization Tool) and 2) coupling DYMOND to the opensource SA&UQ tool kit Dakota. The primary objective of having these NFCS/SA&UQ coupled capabilities is to better inform DOE-NE and other stakeholders on the results generated from the NFCS. For a given set of fuel cycle strategies, policies, and technology assumptions that make up a fuel cycle scenario, these NFCS have traditionally been used by the SA&I Campaign to provide quantitative answers in terms of year-by-year mass flows, infrastructure requirements, costs, etc. With these newly developed coupled capabilities, the SA&I Campaign can now efficiently simulate hundreds or thousands of these scenarios, sample large ranges of parameters and assumptions, and use the unique features of the SA&UQ tools to process the data. This enables providing answers with known and propagated uncertainties, determining the sensitivity of important metrics to different parameters and assumptions, quantifying how much fuel cycle and technology parameters impact each other, and producing optimized fuel cycle strategies for single and multiple variables. To demonstrate these new capabilities, the Cyclus/MOT was used to model several scenarios ranging from simple fleet retirements to transitions to advanced reactors. Specifically, for a transition scenario from LWRs to SFRs and advanced LWRs, uncertainty quantification, sensitivity analysis, and optimization studies were applied to cases involving single and multiple parameter (input) and single and multiple metric (output) variations. In addition, a similar transition scenario was modeled to demonstrate how to optimize the reprocessing capacity parameter to minimize two performance metrics while taking into account uncertainties from two other parameters. Lastly, a depletion module based on SCALE/ORIGEN was added in Cyclus to simulate the third scenario that was designed to quantify the impact of the modeling assumption that all LWR used nuclear fuel have the same burnup. The newly developed DYMOND/Dakota capability was also applied to a transition scenario from the existing fleet to small modular reactors and fast reactors. This particular scenario involves not only explicit isotopic depletion via ORIGEN-2, but also includes multirecycling and utilizing the criticality search feature to determine the fresh fuel composition of recycled fuel, a feature unique to the DYMOND NFCS. A large database of simulations were run with 4 main parameters that were sampled: start date of reprocessing, reprocessing capacity, energy demand growth rate, and advanced reactor share of the fleet. The 4 main metrics were uranium consumption, enrichment requirements, waste generation, and levelized cost of electricity using data from the Cost Basis Report. The demonstrated SA&UQ results include those that inform on how to choose parameters to avoid “failed” scenarios, Sobol’ indices that inform on the importance of various parameters individually and synergistically, and Analysis of Variance (ANOVA) studies that decompose parameter ranges into groups and informs on whether variations are statistically significant.

Feng, B.↗

Gamma Radiolysis of Biphasic Acetohydroxamic Acid (AHA) Solvent Systems

Acetohydroxamic acid (AHA) has been proposed as a substitute for uranium(IV) and hydrazine as a plutonium complexant and neptunium reductant for simplified, single-cycle used nuclear fuel reprocessing flowsheets. However, the chemical behavior of AHA in an intense multi-component radiation field is poorly understood, especially under representative biphasic reprocessing solvent system conditions. In response to this critical knowledge gap, this study has investigated the gamma radiolytic integrity of AHA in aqueous nitric solutions in contact with an organic phase, comprising current and future reprocessing ligands (TBP, DEHBA, and DEHiBA) dissolved in n-dodecane diluent. Our data show negligible effect of the organic phase on the radiolytic behavior of AHA compared to complementary single-phase experiments.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Recent Advances in Radiation-Induced Actinide Redox Chemistry

The actinide series boasts many unique physical and chemical features worthy of both fundamental and applied study. However, the chemical influence of their inherent radiation field is often overlooked, especially as we begin to explore the late actinides in more detail than ever possible before. From the perspective of used nuclear fuel reprocessing, the absorption of ionizing radiation induces the formation of a variety of transient and steady-state excited states, radicals, ions, and molecular degradation products, many of which are highly redox active and can lead to significant changes in a reprocessing solvent system’s physical and chemical properties. For example, radiolysis of the actinides can drive steady-state redox distributions and the formation of non-traditional oxidation states which can complicate their separation and recovery from fission products. This scenario is further exacerbated when complexation is taken into account. Consequently, a molecular-level understanding of radiation effects on the actinides over multiple time, distance, and material domains is essential for supporting innovation in used nuclear fuel reprocessing technologies. Attaining this knowledge necessitates a firm grasp of actinide radiation chemistry to develop predictive, mechanistic, multiscale models to support engineering efforts. Presented here are several recent studies that highlight recent advances in actinide radiation chemistry, in particular, the effect of actinide complexation on ligand reactivity towards radiation-induced transients.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Chemical Recycling of Polybutadiene Rubber with Tailored Depolymerization Enabled by Microencapsulated Metathesis Catalysts

The effective management of plastic waste streams to prevent plastic land and water pollution is a growing problem that is also one of the most important challenges in polymer science today. Polymer materials that are stable over their lifetime and can also be cheaply recycled or repurposed as desired could more easily be diverted from waste streams. However, this is difficult for most commodity plastics. It is especially difficult to conceive this with intractable, cross-linked polymers such as rubbers. In this work, we explore the utility of microencapsulated Grubbs’ catalysts for the in-situ depolymerization and reprocessing of polybutadiene (PB) rubber. Second-generation Hoveyda-Grubbs catalyst (HG2) contained within glassy thermoplastic microspheres can be dispersed in PB rubber below the microsphere’s glass transition temperature (T g ) without adverse depolymerization, evidenced by rubber with and without these microspheres obtaining similar shear storage moduli of ≈16 and ≈28 kPa, respectively. The thermoplastic’s T g can be used to tune the depolymerization temperature, via release of HG2 into the rubber matrix. For example, using poly(lactic acid) (PLA) vs polysulfone results in an 85 and 162 °C depolymerization temperature, respectively. Liquefaction of rubber to a mixture of small molecules and oligomers is demonstrated using a 0.01 mol % catalyst loading using PLA as the encapsulant. Furthermore, at that same catalyst loading, depolymerization occurs to a greater extent in comparison to two ex-situ approaches, including a conventional solvent-assisted method, where it occurs at roughly twice the extent at each given catalyst loading. In addition, depolymerization of the microsphere-loaded rubbers was demonstrated for samples stored under nitrogen for 23 days. Lastly, we show that the depolymerized products can be reprocessed back into solid rubber with a shear storage modulus of ≈32 kPa. Thus, we envision that this approach could be used to recycle and reuse cross-linked rubbers at the end of their product lifetime.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗