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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Anthropogenic extremely low volatility organics (ELVOCs) Govern the Growth of Molecular Clusters over the Southern Great Plains during the Springtime

New particle formation (NPF) and growth govern cloud condensation nuclei (CCN) concentrations in many regions. The mechanisms governing the nucleation of molecular clusters vary substantially in different regions of the atmosphere. Additionally, the growth of these clusters from ~2 to 20 nm sizes is often governed by the availability of extremely low volatility organic vapours (ELVOCs). While the pathways to ELVOC formation from the oxidation of biogenic monoterpenes with ozone is better understood, the chemical and mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are not well understood. We integrate measurements and three-dimensional regional model simulations with the Weather Research and Forecasting Model coupled to chemistry (WRF-Chem) to understand the processes governing new particle formation and growth and secondary organic aerosol (SOA) formation during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) field campaign at the Southern Great Plains (SGP) observatory in Oklahoma, and contrast it with a site within the Bankhead National Forest (BNF), Alabama in Southeast USA, where 5-year long measurements will begin in 2024. Simulations show that nucleation rates are at least an order of magnitude higher at SGP compared to BNF during the springtime days (April 28 and May 14, 2016), largely due to lower H2SO4 concentrations at BNF, which are needed for nucleation. In addition, the larger CS at BNF (compared to SGP) increase the loss of molecular clusters by coagulation to pre-existing particles. Among the 8 different nucleation mechanisms in WRF-Chem, we find that the amine+H2SO4 nucleation mechanism dominates at the SGP site, while the pure organic ion induced nucleation mechanism dominates over BNF. Through various WRF-Chem sensitivity simulations, we find that anthropogenic ELVOCs are critical for explaining the growth of newly formed particles and the resulting number size distribution observed near the surface at the SGP site during the daytime. In addition, we show that treating organic particles as semisolid, with strong diffusion-limited uptake of organic vapours, brings model predictions into closer agreement with the observed evolution of particle size distribution. Simulations also predict that anthropogenic SOA, formed by the oxidation of aromatic volatile organic compounds (VOCs), is the dominant organic aerosol component at SGP, while biogenic SOA dominates particle composition at the BNF site in Southeast USA on these days.

Shrivastava, ManishKumar B.↗
DOE OSTI2022

Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO 2 regimes

Abstract. The atmospheric oxidation of dimethyl sulfide (DMS) represents a major natural source of atmospheric sulfate aerosols. However, there remain large uncertainties in our understanding of the underlying chemistry that governs the product distribution and sulfate yield from DMS oxidation. Here, chamber experiments were conducted to simulate gas-phase OH-initiated oxidation of DMS under a range of reaction conditions. Most importantly, the bimolecular lifetime (τbi) of the peroxy radical CH3SCH2OO was varied over several orders of magnitude, enabling the examination of the role of peroxy radical isomerization reactions on product formation. An array of analytical instruments was used to measure nearly all sulfur-containing species in the reaction mixture, and results were compared with a near-explicit chemical mechanism. When relative humidity was low, “sulfur closure” was achieved under both high-NO (τbi<0.1 s) and low-NO (τbi>10 s) conditions, though product distributions were substantially different in the two cases. Under high-NO conditions, approximately half the product sulfur was in the particle phase, as methane sulfonic acid (MSA) and sulfate, with most of the remainder as SO2 (which in the atmosphere would eventually oxidize to sulfate or be lost to deposition). Under low-NO conditions, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), formed from CH3SCH2OO isomerization, dominates the sulfur budget over the course of the experiment, suppressing or delaying the formation of SO2 and particulate matter. The isomerization rate constant of CH3SCH2OO at 295 K is found to be 0.13±0.03 s−1, in broad agreement with other recent laboratory measurements. The rate constants for the OH oxidation of key first-generation oxidation products (HPMTF and methyl thioformate, MTF) were also determined (kOH+HPMTF=2.1×10-11 cm3 molec.−1 s−1, kOH+MTF=1.35×10-11 cm3 molec.−1 s−1). Product measurements agree reasonably well with mechanistic predictions in terms of total sulfur distribution and concentrations of most individual species, though the mechanism overpredicts sulfate and underpredicts MSA under high-NO conditions. Lastly, results from high-relative-humidity conditions suggest efficient heterogenous loss of at least some gas-phase products.

Ye, Qing (ORCID:0000000337978988)↗
DOE OSTI2025

Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles

Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O 2 atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each P O$_2$ , with activation energies of 228 ± 7 kJ/mol for 20 kPa O 2 and 188 ± 8 kJ/mol for 0.2 kPa O 2 . At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O2. In 0.2 kPa O 2 , oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low P O$_2$ , leading to SiO 2 buildup in porous nodules. Here, this phenomenon was not observed at any temperature in 20 kPa O 2 environments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Gas-Phase Temperature Mapping of Evaporating Microdroplets

Evaporation is a ubiquitous and complex phenomenon of importance to many natural and industrial systems. Evaporation occurs when molecules near the free interface overcome intermolecular attractions with the bulk liquid. As molecules escape the liquid phase, heat is removed, causing evaporative cooling. The influence of evaporative cooling on inducing a temperature difference with the surrounding atmosphere as well as within the liquid is poorly understood. Here, we develop a technique to overcome past difficulties encountered during the study of heterogeneous droplet evaporation by coupling a piezo-driven droplet generation mechanism to a controlled micro-thermocouple to probe microdroplet evaporation. The technique allowed us to probe the gas-phase temperature distribution using a micro-thermocouple (50 μm) in the vicinity of the liquid–vapor interface with high spatial (±10 μm) and temporal (±100 ms) resolution. We experimentally map the temperature gradient formed surrounding sessile water droplets having varying curvature dictated by the apparent advancing contact angle (100° ≲ θ ≲ 165°). The experiments were carried out at temperatures below and above ambient for a range of fixed droplet radii (130 μm ≲ R ≲ 330 μm). Our results provide a primary validation of the centuries-old theoretical framework underpinning heterogeneous droplet evaporation mediated by the working fluid, substrate, and gas thermophysical properties, droplet apparent contact angle, and droplet size. We show that microscale droplets residing on low-thermal-conductivity substrates such as glass absorb up to 8× more heat from the surrounding gas compared to droplets residing on high-thermal-conductivity substrates such as copper. Finally, our work not only develops an experimental understanding of the heat transfer mechanisms governing droplet evaporation but also presents a powerful platform for the study and characterization of liquid–vapor transport at curved interfaces wetting and nonwetting advanced functional surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Tropical Cirrus in Global Storm-Resolving Models. Part II: Cirrus Life Cycle and Top-of-Atmosphere Radiative Fluxes

Cirrus clouds of various thicknesses and radiative characteristics extend over much of the tropics, especially around deep convection. They are difficult to observe due to their high altitude and sometimes small optical depths. They are also difficult to simulate in conventional global climate models, which have coarse grid spacings and simplified parameterizations of deep convection and cirrus formation. We investigate the representation of tropical cirrus in global storm-resolving models (GSRMs), which have higher spatial resolution and explicit convection and could more accurately represent cirrus cloud processes. This study uses GSRMs from the DYnamics of the Atmospheric general circulation Modeled On Non-hydrostatic Domains (DYAMOND) project. The aggregate life cycle of tropical cirrus is analyzed using joint albedo and outgoing longwave radiation (OLR) histograms to assess the fidelity of models in capturing the observed cirrus cloud populations over representative tropical ocean and land regions. The proportions of optically-thick deep convection, anvils, and cirrus vary across models and are portrayed in the vertical distribution of cloud cover and top-of-atmosphere radiative fluxes. Model differences in cirrus populations, likely driven by subgrid processes such as ice microphysics, dominate over regional differences between convectively-active tropical land and ocean locations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

The Potential Benefits of Handling Mixture Statistics via a Bi-Gaussian EnKF: Tests With All-Sky Satellite Infrared Radiances

The meteorological characteristics of cloudy atmospheric columns can be very different from their clear counterparts. Thus, when a forecast ensemble is uncertain about the presence/absence of clouds at a specific atmospheric column (i.e., some members are clear while others are cloudy), that column's ensemble statistics will contain a mixture of clear and cloudy statistics. Such mixtures are inconsistent with the ensemble data assimilation algorithms currently used in numerical weather prediction. Hence, ensemble data assimilation algorithms that can handle such mixtures can potentially outperform currently used algorithms. In this study, we demonstrate the potential benefits of addressing such mixtures through a bi-Gaussian extension of the ensemble Kalman filter (BGEnKF). The BGEnKF is compared against the commonly used ensemble Kalman filter (EnKF) using perfect model observing system simulated experiments (OSSEs) with a realistic weather model (the Weather Research and Forecast model). Synthetic all-sky infrared radiance observations are assimilated in this study. In these OSSEs, the BGEnKF outperforms the EnKF in terms of the horizontal wind components, temperature, specific humidity, and simulated upper tropospheric water vapor channel infrared brightness temperatures. This study is one of the first to demonstrate the potential of a Gaussian mixture model EnKF with a realistic weather model. Our results thus motivate future research toward improving numerical Earth system predictions though explicitly handling mixture statistics.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Increased Asian Sulfate Aerosol Emissions Remarkably Enhance Sahel Summer Precipitation

Observational evidence shows that Sahel summer precipitation has experienced a considerable increase since the 1980s, coinciding with significant diverging trends of increased sulfate emissions in Asia and decreased emissions in Europe (dipole pattern of aerosols between Asia and Europe). The decrease in European sulfate aerosols has substantial effects on the Sahel summer precipitation increase, but the corresponding effect of increased Asian sulfate is unknown. Multi-model simulations in the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) show, compared to decreased European aerosols, that increased Asian aerosols similarly enhance the Sahel summer precipitation but with different large-scale atmospheric circulation changes. Further analysis of the Sixth Coupled Model Intercomparison Project (CMIP6) simulations under historical attribution and various emission scenarios reinforces the results about the climate impacts of anthropogenic aerosols and suggests that in future scenarios with strong international cooperation and rapid climate mitigations (SSP2-45), the Sahel drought will be intensified likely due to the decline in Asian aerosol emissions. Our results suggest that Asian anthropogenic aerosols are likely a non-negligible driver of the recent recovery in Sahel precipitation amounts

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Arctic Ocean annual high in ${{\boldsymbol{p}}}_{{{\bf{CO}}}_{{\bf{2}}}}$ could shift from winter to summer

Long-term stress on marine organisms from ocean acidification will differ between seasons. As atmospheric carbon dioxide (CO 2 ) increases, so do seasonal variations of ocean CO 2 partial pressure (p co 2 ), causing summer and winter long-term trends to diverge. Trends may be further influenced by an unexplored factor—changes in the seasonal timing of p co 2 . In Arctic Ocean surface waters, the observed timing is typified by a winter high and summer low because biological effects dominate thermal effects. Here we show that 27 Earth system models simulate similar timing under historical forcing but generally project that the summer low, relative to the annual mean, eventually becomes a high across much of the Arctic Ocean under mid-to-high-level CO 2 emissions scenarios. Often the greater increase in summer p co 2 , although gradual, abruptly inverses the chronological order of the annual high and low, a phenomenon not previously seen in climate-related variables. The main cause is the large summer sea surface warming from earlier retreat of seasonal sea ice. Warming and changes in other drivers enhance this century’s increase in extreme summer p co 2 by 29 ± 9 per cent compared with no change in driver seasonalities. Thus the timing change worsens summer ocean acidification, which in turn may lower the tolerance of endemic marine organisms to increasing summer temperatures.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Experiment to Investigate the On-set of Transient Fission Gas Release Under Simulated LOCA Conditions

Continuing efforts to better understand the phenomenon of transient fission gas release in irradiated commercial light water reactor fuel undergoing a simulated loss of coolant accident (LOCA) will be discussed in this work. During heating associated with LOCA conditions there is an additional release of fission gas beyond what is typically released during steady state operation. The exact timing of this release could impact the cladding balloon and rupture as the LOCA progresses in an actual accident. Recent experiments performed on the upgraded Severe Accident Test Station at Oak Ridge National Laboratory have expanded the current assessment of transient fission gas release. This system evaluates fission gas release by sweeping fission gas out of the LOCA test furnace and into cryogenically cooled cold traps where radioactive noble gas fission products are measured by gamma spectrometry. Additionally, the sweep gas can be monitored by a gas mass spectrometer to provide additional data on noble gas release and changes in the sweep gas atmosphere during heating. Several different conditions have been evaluated that explored the response of irradiated fuel to different thermal ramp conditions and different overpressure conditions. This further confirmed the impact of an overpressure in suppressing transient fission gas release. Further experiments are planned to evaluate the on-set temperature of transient fission gas release under a known overpressure. This test will progressively step through different temperature conditions while maintaining hydrostatic pressure on the fuel that is representative of high burnup fuel conditions. The available results from this type of testing will be discussed. Post-test microscopy will be compared to other transient fission gas release and standard LOCA tests to further understand the microstructural source of transient fission gas release.

Harp, Jason [ORNL] (ORCID:0000000253458440)↗
DOE OSTI2023

Development of Binder Jet Compatible Silicon Carbide Mixtures for Increased Sintered Density

Binder jet additive manufacturing can process a variety of ceramic powder feedstocks to manufacture near net shape green parts that are subsequently sintered to achieve densification. In particular, silicon carbide (SiC) is a promising ceramic material for heat exchangers in energy storage applications and binder jet is a well-suited process for manufacturing these heat exchangers due to the often geometrically complex designs. However, the need for good powder flowability in binder jet printing often limits the feedstock powder to be larger particles rather than that of ultra fine submicron powders used in conventional ceramic processing, which are more readily densified during sintering. The present work explores the use of various powder mixtures and sintering settings to identify strategies for achieving high density sintered parts in binder jet compatible systems without the use of infiltration. Liquid-phase sintering additives and bimodal powder mixtures are explored alongside different sintering temperatures, rates, atmospheres, and hold times. Two mixtures were found to be good candidates for further exploration: 1) 90 wt% 0.6 µm SiC + 6.25 wt% Al 2 O 3 + 3.75 wt% Y 2 O 3 mixture achieved the highest sintered relative density of 91.2%; and 2) a bimodal mixture comprised of 45 wt% 10 µm SiC + 45 wt% 0.6 µm SiC + 6.25 wt% Al 2 O 3 + 3.75 wt% Y 2 O 3 had the best powder flowability of the powders measured and a 75.1% sintered relative density.

25 ENERGY STORAGE↗
DOE OSTI2022

Enhanced convection for higher module and system efficiency (Final Technical Report)

The goal of this work is to develop new solar photovoltaic (PV) modules and solar system-scale designs that promote an increase of the convective heat transfer coefficient of at least 40%, reducing the operating temperature of the solar PV panels, and leading to a boost on the annual energy yield by at least 5%. By achieving this goal, we further foresee decreasing solar panel degradation by +0.3%/year, reducing the LCOE by 2.9-4.5¢/kWh. Currently, this question and/or approach is not considered though it is a relevant factor in performance/efficiency. The technology proposed will be at a mature stage by the end of the project and could be aligned to be proven on a full-field test. PV users, installers and manufacturers will be interested in the technology due to the aforementioned benefits. The work was conducted through a suite of wind tunnel experiments, numerical simulations and field experiments. These were then evaluated through a correlation encompassing the entire data set and implementing findings into NREL SAM. The work resulted in eight peer reviewed publications with three others in preparation. The key results of the project are 1.) Showing the capability of increasing the solar farm power production by increasing the heat transfer coefficient; 2.) Providing strategies for achieving this through large scale arrangement manipulation (heights, spacings, angles), flow deflectors and vortex generators; 3.) Demonstrating scalability of results by comparing numerical simulations, wind tunnel experiments and field experiments; 4.) Providing a correlation to be able to capture the various arrangements while exploiting the heat transfer coefficient; and 5.) Proving the feasibility of such strategies and their capacity through a comprehensive techno-economic analysis. For the heat transfer coefficients, gains of 40% were attained and increases in power in the excess of 5% were observed. For heat mitigation strategies, consideration at the PV array scale were inter-panel spacing, panel height and panel angles while at the module level, wind breaks such as solid walls and selected gaps were evaluated as well as vortex generators on the panel. All proposed strategies saw an increase in heat transfer coefficient. For scalability, results were compared against field experiments and a correlation for the heat transfer quantity was attained leading to a parametric understanding of the variations and impact in the heat transfer coefficient independent of tools implemented (wind tunnel/numerical simulations). The strategies were also further assessed by a technoeconomic analysis finding improvements based on LCOE with respect to location (several states with varies atmospheric conditions/geographic locations) yielded different results. Improvements on this end were also observed especially towards the colder climates and when considering bi-facial modules. The quantitative demonstrations of such conclusions are provided in the main portion of this document with complementary results and their narration. Milestones and go/no-go points were successfully met in the project.

14 SOLAR ENERGY↗
DOE OSTI2024

Evaluation of dynamical downscaling in a fully coupled regional earth system model

A set of decadal simulations has been completed and evaluated for gains using the Regional Arctic System Model (RASM) to dynamically downscale data from a global Earth system model and two atmospheric reanalyses. RASM is a fully coupled atmosphere–land–ocean–sea ice regional Earth system model. Nudging to the forcing data is applied to approximately the top half of the atmospheric domain. RASM simulations were also completed with a modification to the atmospheric physics for evaluating changes to the modeling system. The results show that for the top half of the atmosphere, the RASM simulations follow closely to that of the forcing data, regardless of the forcing data. The results for the lower half of the atmosphere, as well as the surface, show a clustering of atmospheric state and surface fluxes based on the modeling system. At all levels of the atmosphere the imprint of the weather from the forcing data is present as indicated in the pattern of the annual means. Biases, in comparison to reanalyses, are evident in the Earth system model forced simulations for the top half of the atmosphere but are not present in the lower atmosphere. This suggests that bias correction is not needed for fully coupled dynamical downscaling simulations. While the RASM simulations tended to go to the same mean state for the lower atmosphere, there are a differences in the variability and changes of weather patterns across the ensemble of simulations. These differences in the weather result in variances in the sea ice and oceanic states.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Thermodynamic and kinematic drivers of atmospheric boundary layer stability in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC)

Observations collected during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) provide a detailed description of the impact of thermodynamic and kinematic forcings on atmospheric boundary layer (ABL) stability in the central Arctic. This study reveals that the Arctic ABL is stable and near-neutral with similar frequencies, and strong stability is the most persistent of all stability regimes. MOSAiC radiosonde observations, in conjunction with observations from additional measurement platforms, including a 10 m meteorological tower, ceilometer, microwave radiometer, and radiation station, provide insight into the relationships between atmospheric stability and various atmospheric thermodynamic and kinematic forcings of ABL turbulence and how these relationships differ by season. We found that stronger stability largely occurs in low-wind (i.e., wind speeds are slow), low-radiation (i.e., surface radiative fluxes are minimal) environments; a very shallow mixed ABL forms in low-wind, high-radiation environments; weak stability occurs in high-wind, moderate-radiation environments; and a near-neutral ABL forms in high-wind, high-radiation environments. Surface pressure (a proxy for synoptic staging) partially explains the observed wind speeds for different stability regimes. Cloud frequency and atmospheric moisture contribute to the observed surface radiation budget. Unique to summer, stronger stability may also form when moist air is advected from over the warmer open ocean to over the colder sea ice surface, which decouples the colder near-surface atmosphere from the advected layer, and is identifiable through observations of fog and atmospheric moisture.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types

Abstract. Secondary organic aerosol (SOA) constitutes a large fraction of atmospheric aerosol. To assess its impacts on climate and air pollution, knowledge of the number of phases in internal mixtures of different SOA types is required. Atmospheric models often assume that different SOA types form a single phase when mixed. Here, we present visual observations of the number of phases formed after mixing different anthropogenic and biogenic SOA types. Mixing SOA types generated in environmental chambers with oxygen-to-carbon (O/C) ratios between 0.34 and 1.05, we found 6 out of 15 mixtures of two SOA types to result in two phase particles. We demonstrate that the number of phases depends on the difference in the average O/C ratio between the two SOA types (Δ(O/C)). Using a threshold Δ(O/C) of 0.47, we can predict the phase behavior of over 90 % of our mixtures, with one- and two-phase particles predicted for Δ(O/C)<0.47 and Δ(O/C)≥0.47, respectively. This threshold ΔO/C value provides a simple parameter to predict whether mixtures of fresh and aged SOA form one- or two-phase particles in the atmosphere. In addition, we show that phase-separated SOA particles form when mixtures of volatile organic compounds emitted from real trees are oxidized.

Mahrt, Fabian (ORCID:0000000270596765)↗
DOE OSTI2021

Atmospheric Electric Field-Mill Sensor Field Campaign Report

The foundation stone of atmospheric electricity is the existence of a Global Electric Circuit (GEC) influencing all of the planet. In fact, global thunderstorm activity acts as a voltage source that imposes a potential difference between the ionosphere (positively charged) and the Earth’s surface (negatively charged) of about ~300 kV. Such potential difference is discharged through the poorly conducting atmosphere in fair-weather regions, with atmospheric electric fields of ~100 V/m. First evidence of the GEC was gathered by scientists involved on the Carnegie vessel expeditions (early 20th Century), in which they describe a similar daily variation of the atmospheric electric field in different parts of the Pacific Ocean. Such variation become known as the Carnegie Curve (CC).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Are 100 Ensemble Members Enough to Capture the Remote Atmospheric Response to +2°C Arctic Sea Ice Loss?

This study presents results from the Polar Amplification Multimodel Intercomparison Project (PAMIP) single-year time-slice experiments that aim to isolate the atmospheric response to Arctic sea ice loss at global warming levels of +2°C. Using two general circulation models (GCMs), the ensemble size is increased up to 300 ensemble members, beyond the recommended 100 members. After partitioning the response in groups of 100 ensemble members, the reproducibility of the results is evaluated, with a focus on the response of the midlatitude jet streams in the North Atlantic and North Pacific. Both atmosphere-only and coupled ocean–atmosphere PAMIP experiments are analyzed. Substantial differences in the midlatitude response are found among the different experiment subsets, suggesting that 100-member ensembles are still significantly influenced by internal variability, which can mislead conclusions. Despite an overall stronger response, the coupled ocean–atmosphere runs exhibit greater spread due to additional ENSO-related internal variability when the ocean is interactive. The lack of consistency in the response is true for anomalies that are statistically significant according to Student’s t and false discovery rate tests. This is problematic for the multimodel assessment of the response, as some of the spread may be attributed to different model sensitivities whereas it is due to internal variability. Here, we propose a method to overcome this consistency issue that allows for more robust conclusions when only 100 ensemble members are used.

58 GEOSCIENCES↗
DOE OSTI2022

Uncertainty in land carbon budget simulated by terrestrial biosphere models: the role of atmospheric forcing

Global estimates of the land carbon sink are often based on simulations by terrestrial biosphere models (TBMs). The use of a large number of models that differ in their underlying hypotheses, structure and parameters is one way to assess the uncertainty in the historical land carbon sink. Here we show that the atmospheric forcing datasets used to drive these TBMs represent a significant source of uncertainty that is currently not systematically accounted for in land carbon cycle evaluations. We present results from three TBMs each forced with three different historical atmospheric forcing reconstructions over the period 1850–2015. We perform an analysis of variance to quantify the relative uncertainty in carbon fluxes arising from the models themselves, atmospheric forcing, and model-forcing interactions. We find that atmospheric forcing in this set of simulations plays a dominant role on uncertainties in global gross primary productivity (GPP) (75% of variability) and autotrophic respiration (90%), and a significant but reduced role on net primary productivity and heterotrophic respiration (30%). Atmospheric forcing is the dominant driver (52%) of variability for the net ecosystem exchange flux, defined as the difference between GPP and respiration (both autotrophic and heterotrophic respiration). In contrast, for wildfire-driven carbon emissions model uncertainties dominate and, as a result, model uncertainties dominate for net ecosystem productivity. At regional scales, the contribution of atmospheric forcing to uncertainty shows a very heterogeneous pattern and is smaller on average than at the global scale. We find that this difference in the relative importance of forcing uncertainty between global and regional scales is related to large differences in regional model flux estimates, which partially offset each other when integrated globally, while the flux differences driven by forcing are mainly consistent across the world and therefore add up to a larger fractional contribution to global uncertainty.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Optimal Estimation Retrievals and Their Uncertainties: What Every Atmospheric Scientist Should Know

Remote sensing instruments are heavily used to provide observations for both the operational and research communities. These sensors do not provide direct observations of the desired atmospheric variables, but instead, retrieval algorithms are necessary to convert the indirect observations into the variable of interest. It is critical to be aware of the underlying assumptions made by many retrieval algorithms, including that the retrieval problem is often ill posed and that there are various sources of uncertainty that need to be treated properly. In short, the retrieval challenge is to invert a set of noisy observations to obtain estimates of atmospheric quantities. The problem is often complicated by imperfect forward models, by imperfect prior knowledge, and by the existence of nonunique solutions. Optimal estimation (OE) is a widely used physical retrieval method that combines measurements, prior information, and the corresponding uncertainties based on Bayes’s theorem to find an optimal solution for the atmospheric state. Furthermore, OE also allows the relative contributions of the different sources of error to the uncertainty in the final retrieved atmospheric state to be understood. Here, we provide a novel Python library to illustrate the use of OE for inverse problems in the atmospheric sciences. We introduce two example problems: how to retrieve drop size distribution parameters from radar observations and how to retrieve the temperature profile from ground-based microwave sensors. Using these examples, we discuss common pitfalls, how the various error sources impact the retrieval, and how the quality of the retrieval results can be quantified.

54 ENVIRONMENTAL SCIENCES↗