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DOE OSTI2017

Mapping the Extinction Curve in 3D: Structure on Kiloparsec Scales

Near-infrared spectroscopy from APOGEE and wide-field optical photometry from Pan-STARRS1 have recently made precise measurements of the shape of the extinction curve possible for tens of thousands of stars, parameterized by R ( V ). These measurements revealed structures in R ( V ) with large angular scales, which are challenging to explain in existing dust paradigms. In this work, we combine three-dimensional maps of dust column density with R ( V ) measurements to constrain the three-dimensional distribution of R ( V ) in the Milky Way. We find that the variations in R ( V ) are correlated on kiloparsec scales. In particular, most of the dust within one kiloparsec in the outer Galaxy, including many local molecular clouds (Orion, Taurus, Perseus, California, and Cepheus), has a significantly lower R ( V ) than more distant dust in the Milky Way. These results provide new input to models of dust evolution and processing, and complicate the application of locally derived extinction curves to more distant regions of the Milky Way and to other galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Field intercomparison of ice nucleation measurements: the Fifth International Workshop on Ice Nucleation Phase 3 (FIN-03)

Abstract. The third phase of the Fifth International Ice Nucleation Workshop (FIN-03) was conducted at the Storm Peak Laboratory in Steamboat Springs, Colorado, in September 2015 to facilitate the intercomparison of instruments measuring ice-nucleating particles (INPs) in the field. Instruments included two online and four offline measurement systems for INPs, which are a subset of those utilized in the laboratory study that comprised the second phase of FIN (FIN-02). The composition of the total aerosols was characterized using the Particle Analysis by Laser Mass Spectrometry (PALMS) and Wideband Integrated Bioaerosol Sensor (WIBS) instruments, and aerosol size distributions were measured by a laser aerosol spectrometer (LAS). The dominant total particle compositions present during FIN-03 were composed of sulfates, organic compounds, and nitrates, as well as particles derived from biomass burning. Mineral-dust-containing particles were ubiquitous throughout and represented 67 % of supermicron particles. Total WIBS fluorescing particle concentrations for particles with diameters of > 0.5 µm were 0.04 ± 0.02 cm−3 (0.1 cm−3 highest; 0.02 cm−3 lowest), typical of the warm season in this region and representing ≈ 9 % of all particles in this size range as a campaign average. The primary focus of FIN-03 was the measurement of INP concentrations via immersion freezing at temperatures > −33 °C. Additionally, some measurements were made in the deposition nucleation regime at these same temperatures, representing one of the first efforts to include both mechanisms within a field campaign. INP concentrations via immersion freezing agreed within factors ranging from nearly 1 to 5 times on average between matched (time and temperature) measurements, and disagreements only rarely exceeded 1 order of magnitude for sampling times coordinated to within 3 h. Comparisons were restricted to temperatures lower than −15 °C due to the limits of detection related to sample volumes and very low INP concentrations. Outliers of up to 2 orders of magnitude occurred between −25 and −18 °C; a better agreement was seen at higher and lower temperatures. Although the 5–10 factor agreement of INP measurements found in FIN-03 aligned with the results of the FIN-02 laboratory comparison phase, giving confidence in progress of this measurement field, this level of agreement still equates to temperature uncertainties of 3.5 to 5 °C that may not be sufficient for numerical cloud modeling applications that utilize INP information. INP activity in the immersion-freezing mode was generally found to be an order of magnitude or more, making it more efficient than in the deposition regime at 95 %–99 % water relative humidity, although this limited data set should be augmented in future efforts. To contextualize the study results, an assessment was made of the composition of INPs during the late-summer to early-fall period of this study inferred through comparison to existing ice nucleation parameterizations and through measurement of the influence of thermal and organic carbon digestion treatments on immersion-freezing ice nucleation activity. Consistent with other studies in continental regions, biological INPs dominated at temperatures of > −20 °C and sometimes colder, while arable dust-like or other organic-influenced INPs were inferred to dominate below −20 °C.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Model Intercomparison of the Impacts of Varying Cloud Droplet–Nucleating Aerosols on the Life Cycle and Microphysics of Isolated Deep Convection

The microphysical impacts of aerosol particles on scattered isolated deep convective cells near Houston, Texas, on 19 June 2013, are examined using multiple cloud-resolving model (CRM) simulations initialized with vertical profiles of low and high concentrations of cloud droplet–nucleating aerosols. These simulations formed part of the Model Intercomparison Project (MIP) conducted by the Deep Convective Working Group of the Aerosol, Cloud, Precipitation and Climate (ACPC) initiative. Each CRM generated a field of convective cells representing those observed during the case study with varying degrees of accuracy. The Tracking and Object-Based Analysis of Clouds (tobac) cell-tracking algorithm was applied to each MIP CRM simulation to track relatively long-lived convective cells (20–60 min). Most of the CRMs produced similar aerosol loading impacts on the warm phase of tracked cell properties with reduced autoconversion and accretion growth of rain, increased cloud water, reduced rainfall, and reduced near-surface evaporation of rain. The sign of aerosol impacts on the warm-phase properties of the convective cells was also quite consistent over cell lifetimes with the greatest magnitude of influence in the first half of the life cycle in most CRMs. In contrast, the ice-phase response to aerosol loading was highly variable among CRMs and included increases or decreases in ice amounts at inconsistent stages of the cell life cycle and midlevel versus upper-level changes in ice. This intermodel variability in ice is indicative both of the complex indirect interactions between aerosols and ice-phase processes in deep convection and their associated parameterizations.

Aerosol-cloud interaction↗

DOE OSTI2015

The effect of large-scale model time step and multiscale coupling frequency on cloud climatology, vertical structure, and rainfall extremes in a superparameterized GCM

The effect of global climate model (GCM) time step—which also controls how frequently global and embedded cloud resolving scales are coupled—is examined in the Superparameterized Community Atmosphere Model ver 3.0. Systematic bias reductions of time-mean shortwave cloud forcing (~10 W/m 2 ) and longwave cloud forcing (~5 W/m 2 ) occur as scale coupling frequency increases, but with systematically increasing rainfall variance and extremes throughout the tropics. An overarching change in the vertical structure of deep tropical convection, favoring more bottom-heavy deep convection as a global model time step is reduced may help orchestrate these responses. The weak temperature gradient approximation is more faithfully satisfied when a high scale coupling frequency (a short global model time step) is used. These findings are distinct from the global model time step sensitivities of conventionally parameterized GCMs and have implications for understanding emergent behaviors of multiscale deep convective organization in superparameterized GCMs. Lastly, the results may also be useful for helping to tune them.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

Exploring the impacts of physics and resolution on aqua-planet simulations from a nonhydrostatic global variable-resolution modeling framework

Advances in computing resources are gradually moving regional and global numerical forecasting simulations towards sub-10 km resolution, but global high resolution climate simulations remain a challenge. The non-hydrostatic Model for Prediction Across Scales (MPAS) provides a global framework to achieve very high resolution using regional mesh refinement. Previous studies using the hydrostatic version of MPAS (H-MPAS) with the physics parameterizations of Community Atmosphere Model version 4 (CAM4) found notable resolution dependent behaviors. This study revisits the resolution sensitivity using the non-hydrostatic version of MPAS (NH-MPAS) with both CAM4 and CAM5 physics. A series of aqua-planet simulations at global quasi-uniform resolutions ranging from 240 km to 30 km and global variable resolution simulations with a regional mesh refinement of 30 km resolution over the tropics are analyzed, with a primary focus on the distinct characteristics of NH-MPAS in simulating precipitation, clouds, and large-scale circulation features compared to H-MPAS-CAM4. The resolution sensitivity of total precipitation and column integrated moisture in NH-MPAS is smaller than that in H-MPAS-CAM4. This contributes importantly to the reduced resolution sensitivity of large-scale circulation features such as the inter-tropical convergence zone and Hadley circulation in NH-MPAS compared to H-MPAS. In addition, NH-MPAS shows almost no resolution sensitivity in the simulated westerly jet, in contrast to the obvious poleward shift in H-MPAS with increasing resolution, which is partly explained by differences in the hyperdiffusion coefficients used in the two models that influence wave activity. With the reduced resolution sensitivity, simulations in the refined region of the NH-MPAS global variable resolution configuration exhibit zonally symmetric features that are more comparable to the quasi-uniform high-resolution simulations than those from H-MPAS that displays zonal asymmetry in simulations inside the refined region. Overall, NH-MPAS with CAM5 physics shows less resolution sensitivity compared to CAM4. These results provide a reference for future studies to further explore the use of NH-MPAS for high-resolution climate simulations in idealized and realistic configurations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

A Review of Ice Particle Shapes in Cirrus formed In Situ and in Anvils

Results from 22 airborne field campaigns, including more than 10 million high–resolution particle images collected in cirrus formed in situ and in convective anvils, are interpreted in terms of particle shapes and their potential impact on radiative transfer. Emphasis is placed on characterizing ice particle shapes in tropical maritime and midlatitude continental anvil cirrus, as well as in cirrus formed in situ in the upper troposphere, and subvisible cirrus in the upper tropical troposphere layer. There is a distinctive difference in cirrus ice particle shapes formed in situ compared to those in anvils that are generated in close proximity to convection. More than half the mass in cirrus formed in situ are rosette shapes (polycrystals and bullet rosettes). Cirrus formed from fresh convective anvils is mostly devoid of rosette–shaped particles. However, small frozen drops may experience regrowth downwind of an aged anvil in a regime with RH ice > ~120% and then grow into rosette shapes. Identifiable particle shapes in tropical maritime anvils that have not been impacted by continental influences typically contain mostly single plate–like and columnar crystals and aggregates. Midlatitude continental anvils contain single–rimed particles, more and larger aggregates with riming, and chains of small ice particles when in a highly electrified environment. Here, the particles in subvisible cirrus are < ~100 μm and quasi–spherical with some plates and rare trigonal shapes. Percentages of particle shapes and power laws relating mean particle area and mass to dimension are provided to improve parameterization of remote retrievals and numerical simulations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Quantifying Uncertainty in Ice Particle Velocity–Dimension Relationships Using MC3E Observations

Abstract Ice particle terminal fall velocity ( V t ) is fundamental for determining microphysical processes, yet remains extremely challenging to measure. Current theoretical best estimates of V t are functions of Reynolds number. The Reynolds number is related to the Best number, which is a function of ice particle mass, area ratio ( A r ), and maximum dimension ( D max ). These estimates are not conducive for use in most models since model parameterizations often take the form , where ( α , β ) depend on habit and D max . A previously developed framework is used to determine surfaces of equally plausible ( α , β ) coefficients whereby ice particle size/shape distributions are combined with V t best estimates to determine mass- ( V M ) or reflectivity-weighted ( V Z ) velocities that closely match parameterized V M ,SD or V Z ,SD calculated using the ( α , β ) coefficients using two approaches. The first uses surfaces of equally plausible ( a , b ) coefficients describing mass ( M )–dimension relationships (i.e., ) to calculate mass- or reflectivity-weighted velocity from size/shape distributions that are then used to determine ( α , β ) coefficients. The second investigates how uncertainties in A r , D max , and size distribution N ( D ) affect V M or V Z . For seven of nine flight legs flown on 20 and 23 May 2011 during the Mesoscale Continental Convective Clouds Experiment (MC3E), uncertainty from natural parameter variability—namely, the variability in ice particle parameters in similar meteorological conditions—exceeds uncertainties arising from different A r assumptions or D max estimates. The combined uncertainty between A r , D max , and N ( D ) produced smaller variability in ( α , β ) compared to varying M ( D ), demonstrating M ( D ) must be accurately quantified for model fall velocities. Primary sources of uncertainty vary considerably depending on environmental conditions. Significance Statement Ice particle fall velocity is fundamental for numerous processes within clouds, and hence is a critical property that must be accurately represented in weather and climate models. Using aircraft observations of ice particle shapes and sizes obtained in clouds behind midlatitude thunderstorms, this work develops a new framework for estimating ice particle fall velocities and their uncertainty, including quantifying the importance of different uncertainty sources from cloud microphysics measurements. Natural parameter variability contributes the most uncertainty in ice particle fall velocity estimates, although other sources can also be important contributors to uncertainty in certain conditions. Additional work examining ice particle data is needed to further understand how dependent uncertainty in certain ice particle properties are to local environmental conditions.

Meteorology & Atmospheric Sciences↗

DOE OSTI2024

Assessing the Atmospheric Response to Subgrid Surface Heterogeneity in the Single-Column Community Earth System Model, Version 2 (CESM2)

Land-atmosphere interactions are central to the evolution of the atmospheric boundary layer and the subsequent formation of clouds and precipitation. Existing global climate models represent these connections with bulk approximations on coarse spatial scales, but observations suggest that small-scale variations in surface characteristics and co-located turbulent and momentum fluxes can significantly impact the atmosphere. Recent model development efforts have attempted to capture this phenomenon by coupling existing representations of subgrid-scale (SGS) heterogeneity between land and atmosphere models. Such approaches are in their infancy and it is not yet clear if they can produce a realistic atmospheric response to surface heterogeneity. Here, we implement a parameterization to capture the effects of SGS heterogeneity in the Community Earth System Model (CESM2), and compare single-column simulations against high-resolution Weather Research and Forecasting (WRF) large-eddy simulations (LESs), which we use as a proxy for observations. The CESM2 experiments increase the temperature and humidity variances in the lowest atmospheric levels, but the response is weaker than in WRF-LES. In part, this is attributed to an underestimate of surface heterogeneity in the land model due to a lack of SGS meteorology, a separation between deep and shallow convection schemes in the atmosphere, and a lack of explicitly represented mesoscale secondary circulations. These results highlight the complex processes involved in capturing the effects of SGS heterogeneity and suggest the need for parameterizations that communicate their influence not only at the surface but also vertically.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

UNIFORM ATMOSPHERIC RETRIEVAL ANALYSIS OF ULTRACOOL DWARFS. I. CHARACTERIZING BENCHMARKS, Gl 570D AND HD 3651B

Interpreting the spectra of brown dwarfs is key to determining the fundamental physical and chemical processes occurring in their atmospheres. Powerful Bayesian atmospheric retrieval tools have recently been applied to both exoplanet and brown dwarf spectra to tease out the thermal structures and molecular abundances to understand those processes. In this manuscript we develop a significantly upgraded retrieval method and apply it to the SpeX spectral library data of two benchmark late T dwarfs, Gl 570D and HD 3651B, to establish the validity of our upgraded forward model parameterization and Bayesian estimator. Our retrieved metallicities, gravities, and effective temperatures are consistent with the metallicity and presumed ages of the systems. We add the carbon-to-oxygen ratio as a new dimension to benchmark systems and find good agreement between carbon-to-oxygen ratios derived in the brown dwarfs and the host stars. Furthermore, we have for the first time unambiguously determined the presence of ammonia in the low-resolution spectra of these two late T dwarfs. We also show that the retrieved results are not significantly impacted by the possible presence of clouds, though some quantities are significantly impacted by uncertainties in photometry. This investigation represents a watershed study in establishing the utility of atmospheric retrieval approaches on brown dwarf spectra.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Incorporating the Effect of Large‐Scale Vertical Motion on Convection Through Convective Mass Flux Adjustment in E3SMv2

Abstract Recent observational studies suggest that the large‐scale dynamical forcing (vertical motion) plays important roles in deep convection development. In this study we propose a convective mass flux adjustment (MAdj) approach to represent the dynamical effects of large‐scale vertical motion on convection in the Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). With MAdj, convection is enhanced (suppressed) when there is large‐scale ascending (descending) motion at the planetary boundary layer top. The coupling of convection with large‐scale circulation significantly improves the simulation of climate variability in E3SMv2 across multiple scales from the diurnal cycle, convectively coupled equatorial waves, to the Madden‐Julian Oscillation (MJO). The standard E3SMv2 tends to simulate overly weak diurnal amplitude of precipitation and overly weak variance of convectively coupled equatorial Kelvin and westward inertio‐gravity (WIG) waves. It also fails to simulate the essential characteristics of the MJO: continuous eastward propagation. With MAdj, the amplitude of diurnal cycle of precipitation is systematically increased and its probability density distribution is much closer to observations. The MAdj can also simulate more realistic eastward propagation of the MJO and much stronger convectively coupled Kelvin and WIG waves. Moreover, the MAdj approach slightly improves the climatology simulations in precipitation, cloud, radiation, circulation, temperature, and moisture fields, with overall root‐mean‐square error (RMSE) of major climatological fields reduced by about 2%. The MAdj approach suppresses excessive grid‐scale precipitation, reducing precipitation wet biases over South China Sea, Philippine Sea, Himalayas, and South Pacific Convergence Zone in western Pacific in summer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Predictive Proxies of Present and Future Lightning in a Superparameterized Model

Abstract A superparameterized climate model is used to assess the global performance of several previously proposed proxies for lightning. In particular, predictors incorporating hydrometeor (ice, graupel) profiles and convective vertical velocities are compared to observations, then used to estimate changes in flash rates with global warming. The choice of microphysics parameterization is also investigated, with all predictors showing higher correlations with Lightning Imaging Sensor/Optical Transient Detector observations when using a 2‐moment scheme compared to a 1‐moment representation. All proxies generally agree in their response to warming over tropical land, with notable decreases in Africa, the Middle East, and northern South America, but disagree over oceans and the midlatitudes. The product of convective available potential energy and precipitation predicts increases over these latter areas, as do the 2‐moment ice‐based proxies, while those of the 1‐moment model tend to show decreases, highlighting the importance of cloud microphysics when using climate models to simulate lightning.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

High sensitivity of simulated fog properties to parameterized aerosol activation in case studies from ParisFog

Aerosols influence fog properties such as visibility and lifetime by affecting fog droplet number concentrations (N d ). Numerical weather prediction (NWP) models often represent aerosol–fog interactions using highly simplified approaches. Incorporating prognostic size-resolved aerosol microphysics from climate models could allow them to simulate N d and aerosol–fog interactions without incurring excessive computational expense. However, microphysics code designed for coarse spatial resolution may struggle with sub-kilometer-scale grid spacings. Here, we test the ability of the UK Met Office Unified Model to simulate aerosol and fog properties during case studies from the ParisFog field campaign in 2011. We examine the sensitivity of fog properties to variations in N d caused by modifications to simulated aerosol activation. Our model, with a 500 m horizontal resolution and interactive aerosol and cloud microphysics, significantly underpredicts N d , although it only slightly underestimates the cloud condensation nuclei concentration. With an updated version of the Abdul-Razzak and Ghan (2000) activation scheme, we produce N d that are more consistent with those predicted by a cloud parcel model under fog-like conditions. We activate droplets only by adiabatic cooling. We incorporate more realistic hygroscopicities for sulfate and organic aerosols and explore the sensitivity of simulated N d to unresolved updrafts. We find that both N d and simulated fog liquid water content are very sensitive to the updated activation scheme but remain less affected by the update to hygroscopicities. Our improvements offer insights into the physical processes regulating N d in stable conditions, potentially laying foundations for improved operational fog forecasts that incorporate interactive aerosol simulations or aerosol climatologies.

Ghosh, Pratapaditya [Carnegie Mellon University, P↗

DOE OSTI2022

Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package, version 1: assessing E3SM aerosol predictions using aircraft, ship, and surface measurements

Abstract. An Earth system model (ESM) aerosol–cloud diagnostics package is developed to facilitate the routine evaluation of aerosols, clouds, and aerosol–cloud interactions simulated by the Energy Exascale Earth System Model (E3SM) from the US Department of Energy (DOE). The first version focuses on comparing simulated aerosol properties with aircraft, ship, and surface measurements, which are mostly measured in situ. The diagnostics currently cover six field campaigns in four geographical regions: eastern North Atlantic (ENA), central US (CUS), northeastern Pacific (NEP), and Southern Ocean (SO). These regions produce frequent liquid- or mixed-phase clouds, with extensive measurements available from the Atmospheric Radiation Measurement (ARM) program and other agencies. Various types of diagnostics and metrics are performed for aerosol number, size distribution, chemical composition, cloud condensation nuclei (CCN) concentration, and various meteorological quantities to assess how well E3SM represents observed aerosol properties across spatial scales. Overall, E3SM qualitatively reproduces the observed aerosol number concentration, size distribution, and chemical composition reasonably well, but it overestimates Aitken-mode aerosols and underestimates accumulation-mode aerosols over the CUS and ENA regions, suggesting that processes related to particle growth or coagulation might be too weak in the model. The current version of E3SM struggles to reproduce the new particle formation events frequently observed over both the CUS and ENA regions, indicating missing processes in current parameterizations. The diagnostics package is coded and organized in a way that can be extended to other field campaign datasets and adapted to higher-resolution model simulations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Evaluating Climate Model Simulations of the Radiative Forcing and Radiative Response at Earth’s Surface

In this work, we analyze the radiative forcing and radiative response at Earth’s surface, where perturbations in the radiation budget regulate the atmospheric hydrological cycle. By applying a radiative kernel-regression technique to CMIP5 climate model simulations where CO 2 is instantaneously quadrupled, we evaluate the intermodel spread in surface instantaneous radiative forcing, radiative adjustments to this forcing, and radiative responses to surface warming. The cloud radiative adjustment to CO 2 forcing and the temperature-mediated cloud radiative response exhibit significant intermodel spread. In contrast to its counterpart at the top of the atmosphere, the temperature-mediated cloud radiative response at the surface is found to be positive in some models and negative in others. Also, the compensation between the temperature-mediated lapse rate and water vapor radiative responses found in top-of-atmosphere calculations is not present for surface radiative flux changes. Instantaneous radiative forcing at the surface is rarely reported for model simulations; as a result, intermodel differences have not previously been evaluated in global climate models. We demonstrate that the instantaneous radiative forcing is the largest contributor to intermodel spread in effective radiative forcing at the surface. We also find evidence of differences in radiative parameterizations in current models and argue that this is a significant, but largely overlooked, source of bias in climate change simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Improving Prediction of Surface Solar Irradiance Variability by Integrating Observed Cloud Characteristics and Machine Learning

A 5-year, 1-minute resolution observational dataset of clouds and solar radiation was produced that includes two metrics of the variability in surface solar irradiance due to cloud type and fractional sky cover. Multiple regression models were trained to fit observations of surface solar irradiance variability from those two cloud property predictors. We found that ensemble tree-based methods, Random Forest and Gradient Boosting Machine, have the least overfitting issues and showed the best performance with an R2 of 0.42. While the observational data trained in this study was only from one site, the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in Oklahoma, initial comparisons of the seasonality of the statistics suggest that these results are relatively weather regime independent; the generality of such a finding across sites will be tested in future work. The observational data and developed machine learning model are being used to create a numerical weather prediction model parameterization to enable day-ahead solar variability prediction in a computationally efficient way. This is a first step towards creating a new paradigm of predicting day-ahead variability with the potential to provide a new tool to improve grid operation, planning, and resilience.

Riihimaki, Laura↗

DOE OSTI2018

Radiative effect and climate impacts of brown carbon with the Community Atmosphere Model (CAM5)

Abstract. A recent development in the representation of aerosols in climate models is the realization that some components of organic aerosol (OA), emitted from biomass and biofuel burning, can have a significant contribution to shortwave radiation absorption in the atmosphere. The absorbing fraction of OA is referred to as brown carbon (BrC). This study introduces one of the first implementations of BrC into the Community Atmosphere Model version 5 (CAM5), using a parameterization for BrC absorptivity described in Saleh et al. (2014). Nine-year experiments are run (2003–2011) with prescribed emissions and sea surface temperatures to analyze the effect of BrC in the atmosphere. Model validation is conducted via model comparison to single-scatter albedo and aerosol optical depth from the Aerosol Robotic Network (AERONET). This comparison reveals a model underestimation of single scattering albedo (SSA) in biomass burning regions for both default and BrC model runs, while a comparison between AERONET and the model absorption Ångström exponent shows a marked improvement with BrC implementation. Global annual average radiative effects are calculated due to aerosol–radiation interaction (REari; 0.13±0.01 W m -2 ) and aerosol–cloud interaction (REaci; 0.01±0.04 W m -2 ). REari is similar to other studies' estimations of BrC direct radiative effect, while REaci indicates a global reduction in low clouds due to the BrC semi-direct effect. The mechanisms for these physical changes are investigated and found to correspond with changes in global circulation patterns. Comparisons of BrC implementation approaches find that this implementation predicts a lower BrC REari in the Arctic regions than previous studies with CAM5. Implementation of BrC bleaching effect shows a significant reduction in REari ( 0.06±0.008 W m -2 ). Also, variations in OA density can lead to differences in REari and REaci, indicating the importance of specifying this property when estimating the BrC radiative effects and when comparing similar studies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Radiative Effect and Climate Impacts of Brown Carbon with the Community Atmosphere Model (CAM5)

A recent development in the representation of aerosols in climate models is the realization that some components of organic aerosol (OA), emitted from biomass and biofuel burning, can have a significant contribution to shortwave radiation absorption in the atmosphere. The absorbing fraction of OA is referred to as brown carbon (BrC). This study introduces one of the first implementations of BrC into the Community Atmosphere Model version 5 (CAM5), using a parameterization for BrC absorptivity described in Saleh et al. (2014). Nine-year experiments are run (2003–2011) with prescribed emissions and sea surface temperatures to analyze the effect of BrC in the atmosphere. Model validation is conducted via model comparison to single-scatter albedo and aerosol optical depth from the Aerosol Robotic Network (AERONET). This comparison reveals a model underestimation of single scattering albedo (SSA) in biomass burning regions for both default and BrC model runs, while a comparison between AERONET and the model absorption Ångström exponent shows a marked improvement with BrC implementation. Global annual average radiative effects are calculated due to aerosol–radiation interaction (REari; 0.13 ± 0.01W m -2 ) and aerosol–cloud interaction (REaci; 0.01 ± 0.04W m -2 ). REari is similar to other studies’ estimations of BrC direct radiative effect, while REaci indicates a global reduction in low clouds due to the BrC semidirect effect. The mechanisms for these physical changes are investigated and found to correspond with changes in global circulation patterns. Comparisons of BrC implementation approaches find that this implementation predicts a lower BrC REari in the Arctic regions than previous studies with CAM5. Implementation of BrC bleaching effect shows a significant reduction in REari (0.06 ± 0.008 W m -2 ). Also, variations in OA density can lead to differences in REari and REaci, indicating the importance of specifying this property when estimating the BrC radiative effects and when comparing similar studies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Atmospheric processing of iron in mineral and combustion aerosols: development of an intermediate-complexity mechanism suitable for Earth system models

Abstract. Atmospheric processing of iron in dust and combustion aerosols is simulated using an intermediate-complexity soluble iron mechanism designed for Earth system models. The solubilization mechanism includes both a dependence on aerosol water pH and in-cloud oxalic acid. The simulations of size-resolved total, soluble and fractional iron solubility indicate that this mechanism captures many but not all of the features seen from cruise observations of labile iron. The primary objective was to determine the extent to which our solubility scheme could adequately match observations of fractional iron solubility. We define a semi-quantitative metric as the model mean at points with observations divided by the observational mean (MMO). The model is in reasonable agreement with observations of fractional iron solubility with an MMO of 0.86. Several sensitivity studies are performed to ascertain the degree of complexity needed to match observations; including the oxalic acid enhancement is necessary, while different parameterizations for calculating model oxalate concentrations are less important. The percent change in soluble iron deposition between the reference case (REF) and the simulation with acidic processing alone is 63.8 %, which is consistent with previous studies. Upon deposition to global oceans, global mean combustion iron solubility to total fractional iron solubility is 8.2 %; however, the contribution of fractional iron solubility from combustion sources to ocean basins below 15∘ S is approximately 50 %. We conclude that, in many remote ocean regions, sources of iron from combustion and dust aerosols are equally important. Our estimates of changes in deposition of soluble iron to the ocean since preindustrial climate conditions suggest roughly a doubling due to a combination of higher dust and combustion iron emissions along with more efficient atmospheric processing.

Scanza, Rachel A.↗