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DOE OSTI2020

An evaluation of global organic aerosol schemes using airborne observations

Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different model OA schemes within the standard GEOS-Chem chemical transport model and evaluate the simulations against a suite of 15 globally distributed airborne campaigns from 2008 to 2017, primarily in the spring and summer seasons. These include the ATom, KORUS-AQ, GoAmazon,FRAPPE, SEAC4RS, SENEX, DC3, CalNex, OP3, EUCAARI, ARCTAS and ARCPAC campaigns and provide broad coverage over a diverse set of atmospheric composition regimes – anthropogenic, biogenic, pyrogenic and remote. The schemes include significant differences in their treatment of the primary and secondary components of OA – a “simple scheme” that models primary OA (POA) as non-volatile and takes a fixed-yield approach to secondary OA (SOA) formation and a “complex scheme” that simulates POA as semi-volatile and uses a more sophisticated volatility basis set approach for non-isoprene SOA, with an explicit aqueous uptake mechanism to model isoprene SOA. Despite these substantial differences, both the simple and complex schemes perform comparably across the aggregate dataset in their ability to capture the observed variability (with an R2 of 0.41 and 0.44, respectively). The simple scheme displays greater skill in minimizing the overall model bias (with a normalized mean bias of 0.04 compared to 0.30 for the complex scheme). Across both schemes, the model skill in reproducing observed OA is superior to previous model evaluations and approaches the fidelity of the sulfate simulation within the GEOS-Chem model. However,there are significant differences in model performance across different chemical source regimes, classified here into seven categories.Higher-resolution nested regional simulations indicate that model resolution is an important factor in capturing variability in highly localized campaigns, while also demonstrating the importance of well-constrained emissions inventories and local meteorology, particularly over Asia. Our analysis suggests that a semi-volatile treatment of POA is superior to anon-volatile treatment. It is also likely that the complex scheme parameterization overestimates biogenic SOA at the global scale. While this study identifies factors within the SOA schemes that likely contribute to OA model bias (such as a strong dependency of the bias in the complex scheme on relative humidity and sulfate concentrations), comparisons with the skill of the sulfate aerosol scheme in GEOS-Chem indicate the importance of other drivers of bias, such as emissions, transport and deposition, that are exogenous to the OA chemical scheme.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Tethered Balloon System (TBS) Instrument Handbook

The Tethered Balloon System (TBS) is an unmanned aerial system composed of a helium-filled balloon, tether, winch, and sensors. Individual components of the system may change with each flight based on the desired measurements, atmospheric conditions, and flight strategy. The TBS operates within the U.S. Department of Energy (DOE)’s R-2204 Restricted Airspace, which encompasses a two-nautical-mile radius centered on Oliktok Point, Alaska that is segmented by altitude into R-2204 Low (0-1,499’ MSL or 0-457 m MSL) and R-2204 High (1,500-6,999’ MSL or 457-2133 m MSL). The TBS may operate outside of R-2204 if allowed to do so under a Certificate of Authorization from the Federal Aviation Administration.

42 ENGINEERING↗

DOE OSTI2023

Limited Role of Absolute Humidity in Intraurban Heat Variability

Abstract Monitoring and understanding the variability of heat within cities is important for urban planning and public health, and the number of studies measuring intraurban temperature variability is growing. Recognizing that the physiological effects of heat depend on humidity as well as temperature, measurement campaigns have included measurements of relative humidity alongside temperature. However, the role the spatial structure in humidity, independent from temperature, plays in intraurban heat variability is unknown. Here we use summer temperature and humidity from networks of stationary sensors in multiple cities in the United States to show spatial variations in the absolute humidity within these cities are weak. This variability in absolute humidity plays an insignificant role in the spatial variability of the heat index and humidity index (humidex), and the spatial variability of the heat metrics is dominated by temperature variability. Thus, results from previous studies that considered only intraurban variability in temperature will carry over to intraurban heat variability. Also, this suggests increases in humidity from green infrastructure interventions designed to reduce temperature will be minimal. In addition, a network of sensors that only measures temperature is sufficient to quantify the spatial variability of heat across these cities when combined with humidity measured at a single location, allowing for lower-cost heat monitoring networks. Significance Statement Monitoring the variability of heat within cities is important for urban planning and public health. While the physiological effects of heat depend on temperature and humidity, it is shown that there are only weak spatial variations in the absolute humidity within nine U.S. cities, and the spatial variability of heat metrics is dominated by temperature variability. This suggests increases in humidity will be minimal resulting from green infrastructure interventions designed to reduce temperature. It also means a network of sensors that only measure temperature is sufficient to quantify the spatial variability of heat across these cities when combined with humidity measured at a single location.

Meteorology & Atmospheric Sciences↗

DOE OSTI2025

Regional-Scale Modeling Parameterizations for Secondary Organic Aerosol Formation from Isoprene Epoxydiols: Experimentally Based Evaluation and Optimization

Isoprene is an abundant volatile organic compound emitted from broadleaf forests. Under low nitric oxide concentrations, isoprene is photochemically oxidized to form gas-phase isoprene epoxydiols (IEPOX). In the presence of acidified sulfate aerosols, IEPOX enhances the secondary organic aerosol (SOA) formation. Predictions of IEPOX-SOA in regional-scale models, e.g., the Community Multiscale Air Quality Model (CMAQ), are uncertain due to homogeneous aerosol assumptions, underpredictions of water uptake (hygroscopicity), and aerosol surface area. Here, we used experimental measurements of IEPOX-SOA tracers, 2-methyltetrols (2-MT) and 2-methyltetrol sulfates (2-MTS), formed at initial IEPOX-to-inorganic sulfate ratios ranging from 1–10.5, at ∼50% relative humidity to constrain key IEPOX-SOA parameters: phase separation, organic shell diffusivity (D org ), acidity, hygroscopic growth, mass accommodation, and kinetics. The base CMAQ parametrization overpredicted experimental IEPOX-SOA with an average normalized mean bias (NMB average ) of 1.63. CMAQ with phase separation underpredicted IEPOX-SOA (NMB average = −0.71). Using the phase-separated model, CMAQ model performance was optimized (NMB average = 0.077) with an increased D org = 2 × 10 –16 m 2 s –1 and increased rate constants (k 2-MT = 1 × 10 –3 M 2 s –1 , k 2-MTS = 8.83 × 10 –3 M 2 s –1 ). The optimized model explicitly accounted for hygroscopic growth by utilizing experimentally derived growth rates, improving aerosol surface area predictions. Our model highlights the importance of the aerosol mixing state (homogeneous versus phase-separated), aerosol size dynamics, and hygroscopic growth in modeling heterogeneous reactive uptake of IEPOX.

aerosols↗

DOE OSTI2020

General Analysis of Data Collected from DOE Lidar Buoy Deployments Off Virginia and New Jersey

Pacific Northwest National Laboratory (PNNL) operates two AXYS WindSentinel lidar buoys for the U.S. Department of Energy’s Wind Energy Technologies. The purpose of these buoys is to collect hub-height winds and supporting meteorological and oceanographic information to facilitate the development of offshore wind energy in the U.S. In general, each buoy is deployed for a year or more at a given location in order to capture at least a full annual cycle of weather conditions. The initial deployment for one buoy was off the coast of Virginia beginning in 2015, and the other buoy was first deployed off the coast of New Jersey beginning in 2016. Over the last two years, PNNL has had an opportunity to analyze the data collected during these first two deployments. This report describes a substantial analysis of data collected by the two lidar buoys operated off the coasts of Virginia and New Jersey. The centerpiece instrument for each buoy as deployed off Virginia and New Jersey is a lidar system, which is designed to measure the horizontal wind vector from approximately 40 m to 200 m above the sea surface with vertical resolution of 40 m. Since the initial deployments, the original lidars have been replaced with more powerful Leosphere 866 v2 systems. The analyses in this report will apply to the original Vindicator systems. In addition to the wind profiles from the lidars, the buoys collect near-surface measurements of wind speed and direction, air temperature, relative humidity, barometric pressure, and solar irradiance. Oceanographic variables measured include the two-dimensional wave spectrum, water temperature and conductivity, and ocean current vectors to a depth of 90 m. An assessment of overall data recovery and a basic analysis of the data collected was provided in a previous report This report substantially extends that analysis. The various sections describe the development and application of an inertial measurement unit (IMU) data recovery scheme for the New Jersey deployment; a climatological analysis of winds at hub height and at the surface together with thermodynamic variables measured at the surface for the full deployment periods; an analysis of oceanographic observations describe sea state; the development of a refinement for NOAA’s WaveWatch III model to allow its application to near-shore areas; a basic climatology of ocean currents observed from the buoys; an analysis of observed winds in the framework of Monin-Obukhov Similarity Theory; and the development and evaluation of techniques to extract turbulence intensity and turbulence kinetic energy from the lidars. The analyses contained in this report provide a great deal of new information about offshore conditions on the U.S. East Coast. In addition, the experience gained will inform both configurations and analysis of data from future deployments of these lidar buoy systems.

17 WIND ENERGY↗

DOE OSTI2020

Modeling Streamflow and Sediment Transport Under Current and Future Climates at the West Valley Site - 20231

Performance Assessment models often require inputs representing specific hydrologic processes such as streamflow and sediment flux. This paper details the development of a process-level hydrologic model and its use in a Probabilistic Performance Assessment (PPA) system-level model for the West Valley Site in western New York. For this PPA model, a watershed model was developed using SWAT (Soil and Water Assessment Tool) and used to evaluate water and sediment fluxes in nearby streams draining the Site. A particular challenge of probabilistic modeling over long periods of time is scaling parameters appropriately so that outcomes are not grossly over- or underestimated. This challenge is especially important when the spatial and temporal scales of process and system level models differ. In this instance, the SWAT watershed model and GoldSim PPA model have similar spatial scales of stream reaches and sub-catchments within a single watershed (approximately hundreds to tens of thousands of square meters, but the temporal scales differ considerably. The SWAT model calculates streamflow and sediment transport rates at the daily scale, while the PPA model requires long-term average values that are applied over hundreds to thousands of year-long periods. As such, distributions of daily climatic parameters such as average precipitation rate, temperature, wind speed, and relative humidity were developed to force a transient SWAT model that captures the dynamic behavior of the watershed in response to daily changes in the weather. Output from the model, which includes stream flow (m{sup 3}/y) and sediment transport rate (Mg/y) is then averaged over a 100-year period as an approximation for the long-term average values which can be applied in GoldSim. A single SWAT model was run 5000 times with varying climatic inputs and deterministic soil, land use, and elevation data, and the range of outputs were compiled into a distribution which can be implemented stochastically into the PPA Model. Additionally, this paper includes a high-level discussion of how changes in future climate affect weather input distributions, and a summary of how those changes in weather affect the outcomes from the SWAT model and the inputs into the PPA model. In this analysis, future climate distributions were developed based on climate research documenting the expected changes to precipitation and temperature in western New York. The 5,000 SWAT simulations were then repeated with these future climate distributions, and the resulting output was implemented into the PPA Model as hydrologic conditions under a future climate. In the current version of the PPA Model, hydrologic parameters change linearly from the 'current climate' conditions to the 'future climate' conditions over a period of 100 years, after which they remain constant. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

A Greening Future Elevates Flash Drought Risk in Northern Mid‐to‐High Latitudes

Flash droughts have become a growing concern, as they can emerge rapidly and increase the risk of crop failure. Although past studies have investigated the meteorological drivers and future changes of flash drought, why flash drought is more frequent over humid and vegetated regions remains underexplored. This study delves further into the mechanism by which vegetation regulates flash drought and its future change using observations from multiple data sets and large ensemble simulations from three Earth system models. On an interannual timescale, both observations and simulations show robust increases in flash drought frequency and a higher flash-to-sub-seasonal drought ratio during spring or antecedent conditions with dense vegetation, supporting the important role of vegetation in flash drought occurrence, especially in the northern mid-to-high latitudes. In the latter regions, the large ensemble simulations show robust increases in flash drought (e.g., 67% and 46% increases in Eastern U.S. and North Asia in 2050–2100 relative to 1950–2000 under the high emission scenario), where the growing season is lengthening. Although greening might suggest reduced drought stress, it drives precipitation-soil moisture-evapotranspiration decoupling by increasing evapotranspiration partitioning to transpiration. As transpiration can access deep soil water through the plant root system, its increased portion can weaken the constraints of concurrent precipitation on evapotranspiration, thus accelerating soil moisture depletion under high evaporative demand, driving a slow-to-rapid drought transition. How vegetation regulates flash drought by regulating surface moisture budget is supported by observations and simulations. Although warming supports early planting, agriculture may increasingly be threatened by surging flash drought risk.

Drought↗

DOE OSTI2023

Direct Measurement of Small Particle Growth and Aging at the Atmospheric Radiation Measurement Southern Great Plains Observatory Field Campaign Report

Two identical Captive Aerosol Growth and Evolution (CAGE) chambers were operated at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) observatory in the late summer and fall of 2021. The field study was scheduled to begin in spring, 2020, but was delayed because of the pandemic. CAGE chambers are designed to expose particles to an environment that mirrors that of the surroundings with or without a controlled perturbation designed to assess a sensitivity. The analysis here focuses on roughly the last two months of the overall study period during which measurements were almost continuous and when several perturbation experiments were conducted. Though the utility of a dual-chamber system is the ability to measure the influence of a single change on top of ambient conditions, both chambers were initially operated in the same way, with ambient air pulled through the gas exchange channel in both and ammonium sulfate particles injected into both. The similar time-dependent particle growth observed in the chambers for those periods provides confidence in differences observed during the subsequent perturbation experiments. The growth rate of particles in the reference chamber into which only ammonium sulfate particles were injected and for which only ambient air was pulled through were used to describe time-of-day averages. The average growth rate was highest in the evening and in the morning after sunrise and lowest in the late afternoon. The sensitivity of particle growth to secondary aerosol precursor gases was studied by adding them at a controlled rate to the ambient air flow pulled through one of the two chambers. Addition of 5 ppb of α-pinene resulted in an average particle growth rate of 4.4 nm hr -1 , compared with that of just 0.8 nm hr -1 in the reference chamber. The added α-pinene also triggered one new particle formation (NPF) event in the early evening just before sunset and another in the morning just after sunrise. Similarly, addition of 5 ppb of SO 2 to one chamber led to a pair of NPF events and to increased particle growth rate, though unlike the impact of added α-pinene, growth was enhanced only during the daytime when OH concentration is highest. The influence of aerosol liquid water on secondary aerosol formation and particle growth was investigated by injecting ammonium sulfate seed particles into one chamber and potassium sulfate particles into the other. Particles were injected into the two chambers four times over a 1.5-day period. The chamber relative humidity (RH) history during and following each injection was used to determine whether each particle type was crystalline or aqueous. For the case when both particle types remained crystalline throughout the period, they were tracked and for the case when they remained aqueous, the magnitude and time-dependence of the growth of both were almost exactly the same. For the other two cases the ammonium sulfate particles deliquesced upon injection and remained aqueous, while the potassium sulfate particles remained crystalline. For those two cases, the aqueous particles grew substantially faster than did the crystalline particles, providing evidence of the role of aerosol liquid water on secondary aerosol formation and particle growth.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

SPRUCE Photosynthesis and Respiration of Picea mariana and Larix laricina in SPRUCE Experimental Plots, 2016-2017

This dataset contains empirical physiological, morphological, and chemical data collected on two dominant conifer species, Picea mariana and Larix laricina, between May 2016 and August 2017 at the SPRUCE (Spruce and Peatland Responses Under Changing Environments) experimental site within the Marcell Experimental Forest in northern Minnesota, USA. Analyses assessed the response of conifers to whole-ecosystem warming and elevated atmospheric carbon dioxide (CO2) concentrations. Measurements include light-saturated net photosynthesis and dark respiration at ambient atmospheric carbon dioxide (CO2) concentration (2016), CO2 response curves of light-saturated net photosynthesis (2017), leaf morphology (leaf mass per unit leaf area) and nitrogen content (on both mass and area basis). Leaf photosynthesis and respiration were measured with portable photosynthesis systems (LI6400XT, LI6800, LI-COR Biosciences, USA). In 2016, photosynthesis and respiration were measured at a common temperature of 25 ˚C to assess thermal acclimation, and at growth temperatures (for each of the five treatment temperatures) to assess field performance. In 2017, CO2 response curves of net photosynthesis (so-called A-Ci curves) were conducted at different leaf temperatures (15, 25, 32.5, 40 and 45 ˚C) for assessment of biochemical parameters and their temperature sensitivity. In addition, dark respiration measurements at different leaf temperatures (10, 15, 20, 25, 30, 35, 40, and 45 ºC) were also taken. This dataset contains one data file in comma-separate values (*.csv) and Microsoft Excel (*.xlsx) format. Additional metadata are provided: a data dictionary and a file-level metadata file in comma-separate values (.csv) format and a user guide in PDF (*.pdf) format.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Aerosol hygroscopicity over the southeast Atlantic Ocean during the biomass burning season – Part 1: From the perspective of scattering enhancement

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f(RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f(80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f(80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f(80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κ OA ) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κ OA at lower altitudes. We propose a parameterization that quantifies f(RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH 4 ) 2 SO 4 –BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH 4 ) 2 SO 4 –BC internal mixture with respect to the f(RH) prediction. The sensitivity of f(RH) to κ OA indicates that applying a constant κ OA is only suitable when the OA fraction is low and κ OA shows limited variation. However, in situations deviating these two criteria, κ OA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κ OA variability is recommended.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Enriched Background Isotope Study (EBIS): Analysis of 14C-Enriched Carbon Cycle in Soils and Litter at Forested Oak Ridge and AmeriFlux Sites, 2001-2011

These data provide a record of the multi-year, multi-institutional Enriched Background Isotope Studies (EBIS) projects that ran from 2000 through 2011. Elevated levels of 14C enriched CO2 in the air and soil atmosphere as well as leaf, stem, and root tissues were observed on the Oak Ridge Reservations (ORR) during the summer of 1999, and were attributed to local incinerator activities on and/or near the ORR (Trumbore et al. 2002). The isolated enrichment of the background levels of 14C in local forest ecosystem represented a unique opportunity to study unresolved carbon cycling processes such as the contribution of leaf versus root litter contributions to soil carbon accumulation, the rate of vertical transport of carbon into deep soil storage pools, and the differential contribution of physicochemical versus faunal driven processes to soil carbon cycling and sequestration. Leaf litter from the local enriched forest was transplanted to selected sites on the ORR and to selected AmeriFlux study sites to study soil C cycling across a range of soils and climates. The EBIS research projects provide data on C flux from litter sources to mineral soil sinks for United States eastern hardwood forests necessary for testing process hypotheses and judging efficacy of soil C cycling models. Experimental results from this study are being used to parameterize and refine existing carbon dynamics models, the quantification of the long-term fate of ecosystem carbon inputs and as a means to judge the potential for ecosystem carbon sequestration via enhance litter inputs to soil. EBIS observations support conclusions that intra- and inter-annual soil carbon cycling in hardwood forest soils should be characterized as a least a two-compartment system where surface leaf-litter and belowground root turnover represent primary carbon sources for organic-layer and mineral-soil carbon cycles, respectively. EBIS experiments were conducted to complete enriched litterfall maniplations in upland forests on Ultisol and Inceptisol soils of the Oak Ridge Reservation, Oak Ridge, Tennessee. We also collected additional14C-enriched materials for new experimental applications, and applied those materials to multiple AmeriFlux sites over a range of climatic, edaphic and biological conditions. The research provided data for addressing DOE's goal of understanding mechanisms controlling C flux, and for the improvement of models to be applied to policy discussions regarding the safe levels of greenhouse gases for the earth's system. There are 5 data files provided in comma separated (*.csv) format for vegetation, field litter, soil and air [C] and C isotope data from the EBIS studies and associated environmental data.

54 ENVIRONMENTAL SCIENCES↗