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At least 1,441 records · Page 80
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DOE OSTI2021

Editorial: Forest Rhizosphere Interactions: Cascading Consequences for Ecosystem-Level Carbon and Nutrient Cycling

Mycorrhizal fungimine organicmatter and subsequently transfer plant-available nutrients to roots. While there is disagreement considering the role of mycorrhizal fungi in ecosystem carbon (C) and nutrient cycling relative to factors such as climate (Cotton, 2018; Bennett and Classen, 2020), soil nutrient availability (Brzostek et al., 2015; Frey, 2019), or host plant community composition (Read and Perez-Moreno, 2003), it is now clear that mycorrhizal fungal symbionts control a substantial proportion of C and nutrient flow belowground (Steidinger et al., 2019). Yet, determining the relative importance of arbuscular mycorrhizal (AM) and ectomycorrhizal (EM) fungi to these processes is still an open field of inquiry in ecosystemecology (Averill et al., 2019a) and earth system modeling (Sulman et al., 2019). At large scales, ecosystems dominated by EM fungi are thought to store more soil C per unit nitrogen (N) (Averill et al., 2014), have slower N cycles (Phillips et al., 2013), and respond more strongly to global change drivers such as N-deposition (Jo et al., 2019). However, it is unclear how generalizable these patterns are across sites, and plant and mycorrhizal taxa. If site or species-dependent relationships exist between mycorrhizal plants, fungi, and soil biogeochemical cycles, forecasting hot spots and hot moments of mycorrhizal fungal activities and their consistency across space and time would be evenmore challenging (Averill et al., 2019b; Kivlin and Hawkes, 2020).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Modulation of regional carbon uptake by AMOC and alkalinity changes in the subpolar North Atlantic under a warming climate

The slowdown of the Atlantic Meridional Overturning Circulation (AMOC) and associated consequences on ocean carbon uptake could have large implications for the Earth's climate system and its global carbon cycle. This study analyzes ten Earth System Models from the Coupled Model Intercomparison Project Phase 6 (CMIP6) and reveals that the regional carbon uptake in the subpolar North Atlantic under a high CO 2 emission scenario moderately correlates with the decline in AMOC at 40°N. AMOC transports warm and salty subtropical waters to the subpolar regions. Models with stronger AMOC slowdown generally exhibit weaker surface warming and larger decline of surface salinity and alkalinity. We consider two plausible mechanisms linking the AMOC slowdown to the decline of regional CO 2 uptake: the reduction in surface alkalinity and diminished subduction. The decline of surface salinity and alkalinity reduces the ocean's capacity to buffer acids leading to a reduced CO 2 uptake. This important contribution is unique to the North Atlantic. Diminished convective mixing and subduction of surface water can further decrease the downward transport of anthropogenic carbon, as also shown in previous research. The centennial trends of p CO 2 are decomposed into four components driven by temperature, salinity, alkalinity and dissolved inorganic carbon, revealing that alkalinity and dissolved inorganic carbon are both significant contributors. The alkalinity-driven p CO 2 essentially follows surface salinity, establishing the linkage between AMOC slowdown and alkalinity decline. Our results indicate that alkalinity changes are important for the interplay between AMOC and the regional carbon sequestration ability across the late 20 th and the entirety of the 21 st century in the subpolar North Atlantic.

AMOC↗
DOE OSTI2022

Increasing evapotranspiration decouples the positive correlation between vegetation cover and warming in the Tibetan plateau

Plant growth generally responds positively to an increase in ambient temperature. Hence, most Earth system models project a continuous increase in vegetation cover in the future due to elevated temperatures. Over the last 40 years, a considerable warming trend has affected the alpine ecosystem across the Tibetan Plateau. However, we found vegetation growth in the moderately vegetated areas of the plateau were negatively related to the warming temperatures, thus resulting in a significant degradation of the vegetative cover (LAI: slope = -0.0026 per year, p < 0.05). The underlying mechanisms that caused the decoupling of the relationship between vegetation growth and warming in the region were elaborated with the analysis of water and energy variables in the ecosystem. Results indicate that high temperatures stimulated evapotranspiration and increased the water consumption of the ecosystem (with an influence coefficient of 0.34) in these degrading areas, significantly reducing water availability (with an influence coefficient of -0.68) and limiting vegetation growth. Moreover, the negative warming effect on vegetation was only observed in the moderately vegetated areas, as evapotranspiration there predominantly occupied a larger proportion of available water (compared to the wet and highly vegetated areas) and resulted in a greater increase in total water consumption in a warmer condition (compared to dry areas with lower levels of vegetation cover). These findings highlight the risk of vegetation degradation in semi-arid areas, with the degree of vulnerability depending on the level of vegetation cover. Furthermore, results demonstrate the central role of evapotranspiration in regulating water stress intensity on vegetation under elevated temperatures.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

One thousand soils for molecular understanding of belowground carbon cycling

While significant progress has been made in understanding global carbon (C) cycling, the mechanisms regulating belowground C fluxes and storage are still uncertain. New molecular technologies have the power to elucidate these processes, yet we have no widespread standardized implementation of molecular techniques. To address this gap, we introduce the Molecular Observation Network (MONet), a decadal vision from the Environmental Molecular Sciences Laboratory (EMSL), to develop a national network for understanding the molecular composition, physical structure, and hydraulic and biological properties of soil and water. These data are essential for advancing the next generation of multiscale Earth systems models. In this paper, we discuss the 1000 Soils Pilot for MONet, including a description of standardized sampling materials and protocols and a use case to highlight the utility of molecular-level and microstructural measurements for assessing the impacts of wildfire on soil. While the 1000 Soils Pilot generated a plethora of data, we focus on assessments of soil organic matter (SOM) chemistry via Fourier-transform ion cyclotron resonance-mass spectrometry and microstructural properties via X-ray computed tomography to highlight the effects of recent fire history in forested ecosystems on belowground C cycling. We observed decreases in soil respiration, microbial biomass, and potential enzyme activity in soils with high frequency burns. Additionally, the nominal oxidation state of carbon in SOM increased with burn frequency in surface soils. This results in a quantifiable shift in the molecular signature of SOM and shows that wildfire may result in oxidation of SOM and structural changes to soil pore networks that persist into deeper soils.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Changing Characteristics of Tropical Extreme Precipitation–Cloud Regimes in Warmer Climates

In this study, we investigated the changing characteristics of climatic scale (monthly) tropical extreme precipitation in warming climates using the Energy Exascale Earth System Model (E3SM). The results are from Atmospheric Model Intercomparison Project (AMIP)-type simulations driven by (a) a control experiment with the present-day sea surface temperature (SST) and CO 2 concentration, (b) P4K, the same as in (a) but with a uniform increase of 4K in the SST globally, and (c) the same as in (a), but with an imposed SST and CO 2 concentration from the outputs of the coupled E3SM forced by a 4xCO 2 concentration. We found that as the surface warmed under P4K and 4xCO 2 , both convective and stratiform rain increased. Importantly, there was an increasing fractional contribution of stratiform rain as a function of the precipitation intensity, with the most extreme but rare events occurring preferentially over land more than the ocean, and more so under 4xCO 2 than P4K. Extreme precipitation was facilitated by increased precipitation efficiency, reflecting accelerated rates of recycling of precipitation cloud water (both liquid and ice phases) in regions with colder anvil cloud tops. Changes in the vertical profiles of clouds, condensation heating, and vertical motions indicate increasing precipitation–cloud–circulation organization from the control and P4K to 4xCO 2 . The results suggest that large-scale ocean warming, that is, P4K, was the primary cause contributing to an organization structure resembling the well-known mesoscale convective system (MCS), with increased extreme precipitation on shorter (hourly to daily) time scales. Additional 4xCO 2 atmospheric radiative heating and dynamically consistent anomalous SST further amplified the MCS organization under P4K. Analyses of the surface moist static energy distribution show that increases in the surface moisture (temperature) under P4K and 4xCO 2 was the key driver leading to enhanced convective instability over tropical ocean (land). However, a fast and large increase in the land surface temperature and lack of available local moisture resulted in a strong reduction in the land surface relative humidity, reflecting severe drying and enhanced convective inhibition (CIN). It is argued that very extreme and rare “record-breaking” precipitation events found over land under P4K, and more so under 4xCO 2 , are likely due to the delayed onset of deep convection, that is, the longer the suppression of deep convection by CIN, the more severe the extreme precipitation when it eventually occurs, due to the release of a large amount of stored surplus convective available potential energy in the lower troposphere during prolonged CIN.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Exploring ENSO-Induced Anomalies over North America in Historical and Future Climate Simulations That Use HadGEM2-ESM Output to Drive WRF

Projected changes to the El Niño Southern Oscillation (ENSO) climate mode have been explored using global Earth system models (ESMs). Regional expressions of such changes have yet to be fully advanced and may require the use of regional downscaling. Here, we employ regional climate modeling (RCM) using the Weather Research and Forecasting (WRF) model at convection-permitting resolution and nested in output from the HadGEM2 ESM. We quantify ENSO teleconnections to temperature and precipitation anomalies in historical and future climate scenarios over eastern North America. Two paired simulations are run, a strong El Niño (positive ENSO phase) and a weak La Niña (negative ENSO phase), for the historical and future years. The HadGEM2 direct output and HadGEM2-WRF simulation output are compared to the anomalies derived from the NOAA ENSO Climate Normals dataset. The near-surface temperature and precipitation differences by ENSO phase, as represented by the HadGEM2-WRF historical simulations, show a poor degree of association with the NOAA ENSO Climate Normals, in part because of the large biases in the HadGEM2 model. Downscaling with the WRF model does improve the agreement with the observations, and large discrepancies remain. The model chain HadGEM2-WRF reverses the sign of the ENSO phase response over eastern North America under simulations of the future climate with high greenhouse gas forcing, but due to the poor agreement with the NOAA ENSO Climate Normals it is difficult to assign confidence to this prediction.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Decline in Seasonal Snow during a Projected 20-Year Dry Spell

Snowpack loss in midlatitude mountains is ubiquitously projected by Earth system models, though the magnitudes, persistence, and time horizons of decline vary. Using daily downscaled hydroclimate and snow projections, we examine changes in snow seasonality across the U.S. Pacific Southwest region during a simulated severe 20-year dry spell in the 21st century (2051–2070) developed as part of the 4th California Climate Change Assessment to provide a “stress test” for water resources. Across California’s mountains, substantial declines (30–100% loss) in median peak annual snow water equivalent accompany changes in snow seasonality throughout the region compared to the historic period. We find that 80% of historic seasonal snowpacks transition to ephemeral conditions. Subsetting empirical-statistical wildfire projections for California by snow seasonality transition regions indicates a two-to-four-fold increase in the area burned, consistent with recent observations of high elevation wildfires following extended drought conditions. By analyzing six of the major California snow-fed river systems, we demonstrate snowpack reductions and seasonality transitions result in concomitant declines in annual runoff (47–58% of historical values). The negative impacts to statewide water supply reliability by the projected dry spell will likely be magnified by changes in snowpack seasonality and increased wildfire activity.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Quantifying snow darkening and atmospheric radiative effects of black carbon and dust on the South Asian monsoon and hydrological cycle: experiments using variable-resolution CESM

Black carbon (BC) and dust impart significant effects on the South Asian monsoon (SAM), which is responsible for ~80 % of the region's annual precipitation. This study implements a variable-resolution (VR) version of the Community Earth System Model (CESM) to quantify two radiative effects of absorbing BC and dust on the SAM. Specifically, this study focuses on the snow darkening effect (SDE), as well as how these aerosols interact with incoming and outgoing radiation to facilitate an atmospheric response (i.e., aerosol–radiation interactions, ARIs). By running sensitivity experiments, the individual effects of SDE and ARI are quantified, and a theoretical framework is applied to assess these aerosols'impacts on the SAM. It is found that ARIs of absorbing aerosols warm the atmospheric column in a belt coincident with the May–June averaged locationof the subtropical jet, bringing forth anomalous upper-tropospheric(lower-tropospheric) anticyclogenesis (cyclogenesis) and divergence(convergence). This anomalous arrangement in the mass fields brings forth enhanced rising vertical motion across South Asia and a stronger westerly low-level jet, the latter of which furnishes the Indian subcontinent with enhanced Arabian Gulf moisture. Precipitation increases of 2 mm d–1 or more (a 60 % increase in June) result across much of northern India from May through August, with larger anomalies (+5 to +10 mm d–1) in the western Indian mountains and southern Tibetan Plateau (TP) mountain ranges due to orographic and an abatic enhancement. Across the Tibetan Plateau foothills, SDE by BC aerosols drives large precipitation anomalies of > 6 mm d–1(a 21%–26 % increase in May and June), comparable to ARI of absorbing aerosols from April through August. Runoff changes accompany BC SDE-induced snow changes across Tibet, while runoff changes across India result predominantly from dust ARI. Finally, there are large differences in the simulated SDE between the VR and traditional 1° simulations, the latter of which simulates a much stronger SDE and more effectively modifies the regional circulation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Southern Ocean latitudinal gradients of cloud condensation nuclei

Abstract. The Southern Ocean region is one of the most pristine in the world and serves as an important proxy for the pre-industrial atmosphere. Improving our understanding of the natural processes in this region is likely to result in the largest reductions in the uncertainty of climate and earth system models. While remoteness from anthropogenic and continental sources is responsible for its clean atmosphere, this also results in the dearth of atmospheric observations in the region. Here we present a statistical summary of the latitudinal gradient of aerosol (condensation nuclei larger than 10 nm, CN10) and cloud condensation nuclei (CCN at various supersaturations) concentrations obtained from five voyages spanning the Southern Ocean between Australia and Antarctica from late spring to early autumn (October to March) of the 2017/18 austral seasons. Three main regions of influence were identified: the northern sector (40–45∘ S), where continental and anthropogenic sources coexisted with background marine aerosol populations; the mid-latitude sector (45–65∘ S), where the aerosol populations reflected a mixture of biogenic and sea-salt aerosol; and the southern sector (65–70∘ S), south of the atmospheric polar front, where sea-salt aerosol concentrations were greatly reduced and aerosol populations were primarily biologically derived sulfur species with a significant history in the Antarctic free troposphere. The northern sector showed the highest number concentrations with median (25th to 75th percentiles) CN10 and CCN0.5 concentrations of 681 (388–839) cm−3 and 322 (105–443) cm−3, respectively. Concentrations in the mid-latitudes were typically around 350 cm−3 and 160 cm−3 for CN10 and CCN0.5, respectively. In the southern sector, concentrations rose markedly, reaching 447 (298–446) cm−3 and 232 (186–271) cm−3 for CN10 and CCN0.5, respectively. The aerosol composition in this sector was marked by a distinct drop in sea salt and increase in both sulfate fraction and absolute concentrations, resulting in a substantially higher CCN0.5/CN10 activation ratio of 0.8 compared to around 0.4 for mid-latitudes. Long-term measurements at land-based research stations surrounding the Southern Ocean were found to be good representations at their respective latitudes; however this study highlighted the need for more long-term measurements in the region. CCN observations at Cape Grim (40∘39′ S) corresponded with CCN measurements from northern and mid-latitude sectors, while CN10 observations only corresponded with observations from the northern sector. Measurements from a simultaneous 2-year campaign at Macquarie Island (54∘30′ S) were found to represent all aerosol species well. The southernmost latitudes differed significantly from both of these stations, and previous work suggests that Antarctic stations on the East Antarctic coastline do not represent the East Antarctic sea-ice latitudes well. Further measurements are needed to capture the long-term, seasonal and longitudinal variability in aerosol processes across the Southern Ocean.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Subgrid-scale horizontal and vertical variation of cloud water in stratocumulus clouds: a case study based on LES and comparisons with in situ observations

Abstract. Stratocumulus clouds in the marine boundary layer cover a large fraction of ocean surface and play an important role in the radiative energy balance of the Earth system. Simulating these clouds in Earth system models (ESMs) has proven to be extremely challenging, in part because cloud microphysical processes such as the autoconversion of cloud water into precipitation occur at scales much smaller than typical ESM grid sizes. An accurate autoconversion parameterization needs to account for not only the local microphysical process (e.g., the dependence on cloud water content qc and cloud droplet number concentration Nc) but also the subgrid-scale variability of the cloud properties that determine the process rate. Accounting for subgrid-scale variability is often achieved by the introduction of a so-called enhancement factor E. Previous studies of E for autoconversion have focused more on its dependence on cloud regime and ESM grid size, but they have largely overlooked the vertical dependence of E within the cloud. In this study, we use a large-eddy simulation (LES) model, initialized and constrained with in situ and surface-based measurements from a recent airborne field campaign, to characterize the vertical dependence of the horizontal variation of qc in stratocumulus clouds and the implications for E. Similar to our recent observational study (Zhang et al., 2021), we found that the inverse relative variance of qc, an index of horizontal homogeneity, generally increases from cloud base upward through the lower two-thirds of the cloud and then decreases in the uppermost one-third of the cloud. As a result, E decreases from cloud base upward and then increases towards the cloud top. We apply a decomposition analysis to the LES cloud water field to understand the relative roles of the mean and variances of qc in determining the vertical dependence of E. Our analysis reveals that the vertical dependence of the horizontal qc variability and enhancement factor E is a combined result of condensational growth throughout the lower portion of the cloud and entrainment mixing at cloud top. The findings of this study indicate that a vertically dependent E should be used in ESM autoconversion parameterizations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Dust pollution in China affected by different spatial and temporal types of El Niño

Dust is an important aerosol affecting air quality in China in the winter and spring seasons. Dust in China is potentially influenced by the interannual climate variability associated with El Niño. Here, the impacts of El Niño with different temporal and spatial types on dust pollution in boreal winter and spring in China and the potential mechanisms are investigated using a state-of-the-art Earth system model (E3SMv1). We find that the eastern Pacific (EP) and central Pacific (CP) El Niño both increase wintertime dust concentrations by 5–50 µg m –3 over central-eastern China. Due to a stronger wind and lower relative humidity, which favor dust emissions near sources, and a strengthened northwesterly and reduced precipitation, which are conducive to dust transport, dust concentrations during the CP El Niño are 5–20 µg m –3 higher in northern China than during the EP El Niño, although the changes are mostly insignificant. El Niño with a short duration (SD) increases boreal winter dust concentrations by 20–100 µg m –3 over northern China relative to the climatological mean, while there is a decrease of 5–50 µg m –3 during the long-duration (LD) El Niño, which is also related to the El Niño-induced changes in atmospheric circulation, precipitation, and relative humidity. In the following spring season, all types of El Niño events enhance dust over northern China, but only the increase during the LD El Niño is statistically significant, suggesting that the weaker intensity but longer duration of the LD El Niño events can significantly affect spring dust in China. Our results contribute to the current knowledge of the influence of El Niño on dust pollution, which has profound implications for air pollution control and dust storm prediction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Primary and secondary ice production: interactions and their relative importance

A discrepancy of up to 5 orders of magnitude between ice crystal and ice nucleating particle (INP) number concentrations was found in the measurements, indicating the potentially important role of secondary ice production (SIP) in the clouds. However, the interactions between primary and SIP processes and their relative importance remain unexplored. In this study, we implemented five different ice nucleation schemes as well as physical representations of SIP processes (i.e., droplet shattering during rain freezing, ice-ice collisional break-up, and rime splintering) in the Community Earth System Model version 2 (CESM2). We ran CESM2 in the single column mode for model comparisons with the DOE Atmospheric Radiation Measurement (ARM) Mixed-Phase Arctic Cloud Experiment (M-PACE) observations. We found that the model experiments with aerosol-aware ice nucleation schemes and SIP processes yield the best simulation results for the M-PACE single-layer mixed-phase clouds. We further investigated the relative importance of ice nucleation and SIP to ice number and cloud phase as well as interactions between ice nucleation and SIP in the M-PACE single-layer mixed-phase clouds. Our results show that SIP contributes 80 % to the total ice formation and transforms ~30 % of pure liquid-phase clouds simulated in the model experiments without considering SIP into mixed-phase clouds. The SIP is not only a result of ice crystals produced from ice nucleation, but also competes with the ice nucleation by reducing the number concentrations of cloud droplets and cloud-borne dust INPs. Conversely, strong ice nucleation also suppresses SIP by glaciating mixed-phase clouds and thereby reducing the amount of precipitation particles (rain and graupel).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Relative importance of high-latitude local and long-range-transported dust for Arctic ice-nucleating particles and impacts on Arctic mixed-phase clouds

Dust particles, serving as ice-nucleating particles (INPs), may impact the Arctic surface energy budget and regional climate by modulating the mixed-phase cloud properties and lifetime. In addition to long-range transport from low-latitude deserts, dust particles in the Arctic can originate from local sources. However, the importance of high-latitude dust (HLD) as a source of Arctic INPs (compared to low-latitude dust, LLD) and its effects on Arctic mixed-phase clouds are overlooked. In this study, we evaluate the contribution to Arctic dust loading and INP population from HLD and six LLD source regions by implementing a source-tagging technique for dust aerosols in version 1 of the US Department of Energy's Energy Exascale Earth System Model (E3SMv1). Our results show that HLD is responsible for 30.7 % of the total dust burden in the Arctic, whereas LLD from Asia and North Africa contributes 44.2 % and 24.2 %, respectively. Due to its limited vertical transport as a result of stable boundary layers, HLD contributes more in the lower troposphere, especially in boreal summer and autumn when the HLD emissions are stronger. LLD from North Africa and East Asia dominates the dust loading in the upper troposphere with peak contributions in boreal spring and winter. The modeled INP concentrations show better agreement with both ground and aircraft INP measurements in the Arctic when including HLD INPs. The HLD INPs are found to induce a net cooling effect (-0.24 W m -2 above 60 °N) on the Arctic surface downwelling radiative flux by changing the cloud phase of the Arctic mixed-phase clouds. The magnitude of this cooling is larger than that induced by North African and East Asian dust (0.08 and -0.06 W m -2 , respectively), mainly due to different seasonalities of HLD and LLD. Uncertainties of this study are discussed, which highlights the importance of further constraining the HLD emissions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Fast climate responses to emission reductions in aerosol and ozone precursors in China during 2013-2017

China has been implementing a sequence of policies for clean air since the year 2013, and the aerosol pollution has been substantially improved, but ozone (O 3 )-related issues arose. Here, fast climate responses to emission reductions in aerosol and O 3 precursors over China during 2013–2017 are investigated using the Community Earth System Model version 2 (CESM2). The overall decreases in aerosols produced an anomalous warming of 0.09 ± 0.10°C in eastern China (22–40° N, 110–122.5° E), which is further intensified by the increase in O 3 in the lower troposphere, resulting in an enhanced warming of 0.16 ± 0.15° C in eastern China. Reductions in industrial emissions contributed the most to the aerosol-induced warming, while emission reductions from residential sector induced a cooling effect due to a substantial decrease in light-absorbing black carbon aerosols. This implies that switching the residential sector to cleaner energy is more effective to achieve climate and health benefits in China.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles

Abstract. We present a framework for estimating concentrations of episodically elevated high-temperature marine ice nucleating particles (INPs) in the sea surface microlayer and their subsequent emission into the atmospheric boundary layer. These episodic INPs have been observed in multiple ship-based and coastal field campaigns, but the processes controlling their ocean concentrations and transfer to the atmosphere are not yet fully understood. We use a combination of empirical constraints and simulation outputs from an Earth system model to explore different hypotheses for explaining the variability of INP concentrations, and the occurrence of episodic INPs, in the marine atmosphere. In our calculations, we examine the following two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (at 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. In this case study, we evaluate our framework at 253 K because reliable observational data at this temperature are available across three different ocean regions, but suitable data are sparse at higher temperatures. We find that heterotrophic bacteria and MBPAs acting as INPs provide only a partial explanation for the observed high INP concentrations. We note, however, that there are still substantial knowledge gaps, particularly concerning the identity of the oceanic INPs contributing most frequently to episodic high-temperature INPs, their specific ice nucleation activity, and the enrichment of their concentrations during the sea–air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs and drivers for their emissions are needed, ideally in combination with modeling studies focused on the potential cloud impacts of these high-temperature INPs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Evaluation of liquid cloud albedo susceptibility in E3SM using coupled eastern North Atlantic surface and satellite retrievals

The impact of aerosol number concentration on cloud albedo is a persistent source of spread in global climate predictions due to multi-scale, interactive atmospheric processes that remain difficult to quantify. We use 5 years of geostationary satellite and surface retrievals at the US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) eastern North Atlantic (ENA) site in the Azores to evaluate the representation of liquid cloud albedo susceptibility for overcast cloud scenes in the DOE Energy Exascale Earth System Model version 1 (E3SMv1) and provide possible reasons for model–observation discrepancies. The overall distribution of surface 0.2 % CCN concentration values is reasonably simulated, but simulated liquid water path (LWP) is lower than observed and layer mean droplet concentration (N d ) comparisons are highly variable depending on the N d retrieval technique. E3SMv1's cloud albedo is greater than observed for given LWP and N d values due to a lower cloud effective radius than observed. However, the simulated albedo response to N d is suppressed due to a correlation between the solar zenith angle (SZA) and N d created by the seasonal cycle that is not observed. Controlling for this effect by examining the cloud optical depth (COD) shows that E3SMv1's COD response to CCN concentration is greater than observed. For surface-based retrievals, this is only true after controlling for cloud adiabaticity because E3SMv1's adiabaticities are much lower than observed. Assuming a constant adiabaticity in surface retrievals as done in top-of-atmosphere (TOA) retrievals narrows the retrieved ln N d distribution, which increases the cloud albedo sensitivity to ln N d to match the TOA sensitivity. The greater sensitivity of COD to CCN is caused by a greater Twomey effect in which the sensitivity of N d to CCN is greater than observed for TOA-retrieved N d , and once model–observation cloud adiabaticity differences are removed, this is also true for surface-retrieved N d . The LWP response to N d in E3SMv1 is overall negative as observed. Despite reproducing the observed LWP–N d relationship, observed clouds become much more adiabatic as N d increases, while E3SMv1 clouds do not, associated with more heavily precipitating clouds that are partially but not completely caused by deeper clouds and weaker inversions in E3SMv1. These cloud property differences indicate that the negative LWP–N d relationship is likely not caused by the same mechanisms in E3SMv1 and observations. The negative simulated LWP response also fails to mute the excessively strong Twomey effect, highlighting potentially important confounding factor effects that likely render the LWP–N d relationship non-causal. N d retrieval scales and assumptions, particularly related to cloud adiabaticity, contribute to substantial spreads in the model–observation comparisons, though enough consistency exists to suggest that aerosol activation, drizzle, and entrainment processes are critical areas to focus E3SMv1 development for improving the fidelity of aerosol–cloud interactions in E3SM.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Evaluation of aerosol–cloud interactions in E3SM using a Lagrangian framework

A Lagrangian framework is used to evaluate aerosol–cloud interactions in the U.S. Department of Energy's Energy Exascale Earth System Model (E3SM) version 1 (E3SMv1) for measurements taken at Graciosa Island in the Azores where a U.S. Department of Energy Atmosphere Radiation Measurement (ARM) site is located. This framework uses direct measurements of cloud condensation nuclei (CCN) concentration (instead of relying on satellite retrievals of aerosol optical depth) and incorporates a suite of ground-based ARM measurements, satellite retrievals, and meteorological reanalysis products that when applied to over a 1500 trajectories provides key insights into the evolution of low-level clouds and aerosol radiative forcing that is not feasible from a traditional Eulerian analysis framework. Significantly lower concentrations (40 %) of surface CCN concentration are measured when precipitation rates in 48 h back trajectories average above 1.2 mm d -1 in the Integrated Multi-satellitE Retrievals for Global Precipitation Measurement (IMERG) product. The depletion of CCN concentration when precipitation rates are elevated is nearly twice as large in the ARM observations compared to E3SMv1 simulations. The model CCN concentration bias remains significant despite modifying the autoconversion and accretion rates in warm clouds. As the clouds in trajectories associated with larger surface-based CCN concentration advect away from Graciosa Island, they maintain higher values of droplet number concentrations (N d ) over multiple days in observations and E3SM simulations compared to trajectories that start with lower CCN concentrations. The response remains robust even after controlling for meteorological factors such as lower troposphere stability, the degree of cloud coupling with the surface, and island wake effects. E3SMv1 simulates a multi-day aerosol effect on clouds and a Twomey radiative effect that is within 30 % of the ARM and satellite observations. However, the mean cloud droplet concentration is more than 2–3 times larger than in the observations. While Twomey radiative effects are similar amongst autoconversion and accretion sensitivity experiments, the liquid water path and cloud fraction adjustments are positive when using a regression model as opposed to negative when using the present-day minus pre-industrial aerosol emissions approach. This result suggests that tuning the autoconversion and accretion alone is unlikely to produce the desired aerosol susceptibilities in E3SMv1.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Global source apportionment of aerosols into major emission regions and sectors over 1850–2017

Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past few decades around the world. In this study, the Explicit Aerosol Source Tagging (EAST) system is merged into the Energy Exascale Earth System Model version 1 (E3SMv1) to quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions across the globe during 1850–1980, 1980–2010, and 2010–2017. In North America and Europe, changes in anthropogenic PM 2.5 were mainly caused by changes in emissions from local energy and industrial sectors. The local industrial sector caused the largest increase in PM 2.5 in East Asia during 1980–2010 and decrease during 2010–2017. In South Asia, the increase in energy-related emissions dominated the rise in PM 2.5 levels during 1980–2017. During 1850–1980, the increases in emissions from North America contributed to the increase in the European PM 2.5 burden by 1.7 mg m -2 and the sources from the Europe were also responsible for the PM 2.5 burden increase in East Asia and South Asia by about 1.0 mg m -2 . During 1980–2010, East Asia contributed to an increase of 0.4–0.6 mg m -2 in the PM 2.5 burden in North America and Europe, while South Asia contributed about 0.3 mg m -2 . During 2010–2017, the contributions from East Asia to the PM 2.5 burdens in the North America, Europe, and South Asia declined by 0.3–0.6 mg m -2 due to the clean air actions in China, while the contributions from South Asia still increased due to the continuous increase in emissions in South Asia. The historical changes in aerosols had an impact on effective radiative forcing through aerosol–radiation interactions (ERF ari ). During 1980–2010, a decline in North American aerosols resulted in a positive ERF ari change (warming effect) in Europe and a decline in aerosols in Europe caused a warming effect in Russia and northern China. The changes in ERF ari from the increase and decrease in aerosols in China during 1980–2010 and 2010–2017, respectively, are comparable in magnitude. The continuous aerosol increases in South Asia from 1980 to 2017 resulted in negative ERF ari (cooling) changes in South Asia, Southeast Asia, and southern China.

54 ENVIRONMENTAL SCIENCES↗