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NASA NTRS2022

Importance of Different Parameterization Changes for the Updated Dust Cycle Modeling in the Community Atmosphere Model (Version 6.1)

The Community Atmosphere Model (CAM6.1), the atmospheric component of the Community Earth System Model (CESM; version 2.1), simulates the life cycle (emission, transport, and deposition) of mineral dust and its interactions with physio-chemical components to quantify the impacts of dust on climate and the Earth system. The accuracy of such quantifications relies on how well dust-related processes are represented in the model. Here we update the parameterizations for the dust module, including those on the dust emission scheme, the aerosol dry deposition scheme, the size distribution of transported dust, and the treatment of dust particle shape. Multiple simulations were undertaken to evaluate the model performance against diverse observations, and to understand how each update alters the modeled dust cycle and the simulated dust direct radiative effect. The model–observation comparisons suggest that substantially improved model representations of the dust cycle are achieved primarily through the new more physically-based dust emission scheme. In comparison, the other modifications induced small changes to the modeled dust cycle and model–observation comparisons, except the size distribution of dust in the coarse mode, which can be even more influential than that of replacing the dust emission scheme. We highlight which changes introduced here are important for which regions, shedding light on further dust model developments required for more accurately estimating interactions between dust and climate.

mineral dust parameterizations↗

DOE OSTI2015

Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κ v , was calculated. The κ v, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κ v, ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κ v ≈ 0.15) and a Colorado boreal forest (κ v ≈ 0.16). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κ v, p . The obtained κ v, p values overestimate the experimental FDHA-KIM-derived κ v, ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be partly explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (>300 nm) and supermicron aerosol particles possess core-shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10 −12 cm 2 s −1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

VERNE: Revealing the Mysteries and Histories of Venus

Introduction: The three Venus missions that were recently selected for upcoming flight (VERITAS, DAVINCI+, and EnVision) will be incredibly valuable to our understanding of Venus’ history, geology, and atmosphere. However, even once completed, key gaps in our knowledge of Venus, and more generally the formation and active processes on rocky, Earth-like planets, will still persist. Remaining questions include 1) how global intrinsic magnetic fields might be maintained on rocky worlds, and how they could then go extinct, and 2) what role atmospheric sulfur chemistry plays in climates of Earth-like planets, which is an increasingly timely subject as Earth’s own atmospheric sulfur content is climbing due to human activity. These questions require in-situ observations from Venus’ cloud deck, at the altitudes at which the UV absorber exists. The Venus Environment Research and Novel Exploration (VERNE) mission will address these questions with an aerial platform that will drift around the equatorial region of the planet for 9 days. VERNE will collect data to determine the identity of the mysterious UV absorber, while also taking magnetic field measurements over the tesserae, the regions on Venus that are most likely to retain remanent crustal magnetization, in order to understand the potential role of a past intrinsically-generated global magnetic field on Venus. Mission Objectives: The two major science objectives that drive the VERNE mission are: 1) Determine the identity of the Venusian unknown ultraviolet absorber(s). First observed approximately a century ago [1], the composition of Venus’ ultraviolet (UV) absorber is one of the oldest mysteries in Venus atmospheric chemistry [2,3]. While several candidate UV absorbers (mostly sulfur species) have been proposed, no consensus has been reached on its composition and its specific interactions with the atmosphere. Determining the identity of the UV absorber will aid climate models by showing how and where incident solar energy is absorbed by the atmosphere and make progress towards understanding the chemical and energetic processes taking place above Venus’ upper cloud deck [4]. 2) Determine if Venus retains evidence of a past, internally-generated magnetic field. While Venus does not currently have an intrinsically-generated magnetic field, evidence for the existence of a past field on Venus and a timeline of its decay will fill in a more holistic picture of the evolution of Venus’ geological record and atmosphere. As the oldest geologic units on the surface, Venus’ tesserae may still have remanent crustal magnetization signatures within the rocky composition [5]. In any case, the signatures detected will provide insight into Venus’ past geological and core dynamo activity. Mission Summary: VERNE includes a 3-part flight system made up of 1) an entry system with a HEEET (Heatshield for Extreme Entry Environment Technology) aeroshell, 2) an orbiter for data relay, and 3) an in-situ balloon and gondola. After entry into Venus’ atmosphere, the balloon will be deployed within the upper cloud deck, at an altitude of 62 km, over a tesserae region. The in-situ data collection will last for the duration of 2 full circumnavigations of the planet, which will take ~9 days. Instrumentation Suite: The four instruments that comprise VERNE’s instrument payload will enable the identification of the unknown UV absorber and the detection of remanent crustal magnetization if it exists in the tesserae. The proposed instrument suite cycle during mission operations is shown in Fig. 1. The four instruments are described below: 1) Adams (ion neutral mass spectrometer) has a range of 18-257 AMU and will detect and distinguish the mixing ratios of O₂, H₂O, H₂SO₄, S, S₂, S₃, S₄, S₅, S₆, S₇, S₈, SO, SO₂, OSSO, SO₃, Cl₂, FeCl₃ and other trace sulfur and organic species. The spatial (longitudinal) and temporal (day/night) variations will be observed throughout 2 circumnavigations with a sample cadence of 12 minutes. 2) Shelley (nephelometer) will determine the size distribution of the aerosols (0.4 to 36 um) in the atmosphere. With a size resolution of <0.7 um, it can determine which mode of H2SO4 is present and characterize the large (>30 um) organic particles previously detected by the Venera and Galileo missions [6,7]. 3) Herbert (UV imager) will measure UV radiance at 283 nm (the wavelength of SO2 absorption) and 365 nm (the unknown part of the absorber). UV images will be taken concurrently with the INMS and nephelometer to correlate UV absorption with abundances of the UV absorber species. 4) Vonnegut (magnetometer) has a range of >600 nT and a precision and accuracy of 1 nT. If magnetized by a past field, the crust may have retained a magnetization of up to 3 A/m2 [5]. With a noise floor of 10 nT, the magnetometer will be able to detect RCM from an altitude of 62 km, even if the thickness of the magnetized crust is just 1 km (Fig. 2). Mission Concept Design: VERNE will be launched with a mass of 3300 kg in an intermediate-high performance class vehicle with a 4-m fairing. The 475-day mission includes 466 days for the cruise, coasting, and orbit initialization phases before entry, descent, and balloon deployment. During the 9-day science phase, the aerial platform will make 2 circumnavigations of the planet at an altitude of 62 km. The INMS and the nephelometer will acquire data for 2 hours during the daytime and nighttime during each circumnavigation, while the UV imager will be on for the duration of the daytime, and the magnetometer will be operational throughout the entirety of the science phase. Data will be stored and processed with the JPL-designed Sphinx command and data handling system. Data will be sent from the balloon to the orbiter using an S-band relay link, stored on the orbiter, and then forwarded to Earth where it will be received by the DSN. Conclusion: VERNE will fill key gaps in our understanding of the history and ongoing processes related to the geology and atmosphere of Venus and rocky worlds in general. Even with adequate flight system contingencies and expected costs below the $900M New Frontiers cost cap, VERNE is not without its risks and challenges. Further trade spaces to explore include 1) using solely battery power vs. including solar panels to increase the mission duration and 2) investigating the use of lightweight materials and 3D-printed structures to reduce the gondola mass, among others. Acknowledgments: We would like to thank the JPL Planetary Science Summer School, especially our mentors Troy Hudson, Karl Mitchell, and Leslie Lowes, as well as our Team-X study lead Al Nash and the members of Team-X. We’d additionally like to thank our review panel for asking insightful questions and providing valuable feedback. References: [1] Ross, F. E. (1928) Astrophysical J., 68, 57-92. [2] Rossow, W. B. et al. (1980) J. Geophysical Research, 85, 8107-8128. [3] Pinto, J. P. et al. (2021) Nature Communications, 12, 175. [4] Titov, D. V. et al. (2007) Cosmic Research, 21, 401. [5] O’Rourke, J. et al. (2019) Geophysical Research Lett., 46, 5768–5777. [6] Limaye, S. S. et al. (2018) Astrobiology, 18(9), 1181-1198. [7] Grinspoon, D. H. et al. (2013) Planetary and Space Sci., 41(7), 515-542. [8] Parker, R. L. (2003) J. Geophysical Research, 108, 5006. *The cost information contained in this document is of a budgetary and planning nature and is intended for informational purposes only. It does not constitute a commitment on the part of JPL and/or Caltech.

H Alpert↗

NASA NTRS2012

Exploring the Longwave Radiative Effects of Dust Aerosols

Dust aerosols not only affect air quality and visibility where they pose a significant health and safety risk, but they can also play a role in modulating the energy balance of the Earth-atmosphere system by directly interacting with local radiative fields. Consequently, dust aerosols can impact regional climate patterns such as changes in precipitation and the evolution of the hydrological cycle. Assessing the direct effect of dust aerosols at the solar wavelengths is fairly straightforward due in part to the relatively large signal-to-noise ratio in broadband irradiance measurements. The longwave (LW) impacts, on the other hand, are rather difficult to ascertain since the measured dust signal level (10 Wm-2) is on the same order as the instrumental uncertainties. Moreover, compared to the shortwave (SW), limited experimental data on the LW optical properties of dust makes it a difficult challenge for constraining the LW impacts. Owing to the strong absorption features found in many terrestrial minerals (e.g., silicates and clays), the LW effects, although much smaller in magnitude compared to the SW, can still have a sizeable impact on the energetics of the Earth-atmosphere system, which can potentially trigger changes in the heat and moisture surface budgets, and dynamics of the atmosphere. The current endeavor is an integral part of an on-going research study to perform detailed assessments of dust direct aerosol radiative effects (DARE) using comprehensive global datasets from NASA Goddards mobile ground-based facility (cf. http://smartlabs.gsfc.nasa.gov/) during previous field experiments near key dust source regions. Here we examine and compare the results from two of these studies: the 2006 NASA African Monsoon Multidisciplinary Activities and the 2008 Asian Monsoon Years. The former study focused on transported Saharan dust at Sal Island (16.73N, 22.93W), Cape Verde along the west coast of Africa while the latter focused on Asian dust at Zhangye China (39.082N, 100.276E), a semi-arid region between the Taklimakan and Gobi deserts. NASA Goddards Giovanni system is used to help map out the spatial distribution of retrieved aerosol optical depths across the latter desert regions. 1-D radiative transfer model constrained by local measurements, including spectral photometry/interferometry and lidar for characterizing the spatiotemporal variability in dust properties and atmospheric conditions, is employed to evaluate the local instantaneous LW DARE of dust both at the surface and at the top of the atmosphere along with heating rate profiles for cloud-free atmospheres. The efficiency in LW DARE and its significance relative to the diurnally averaged SW effects are explored and compared in both studies. Found to be non-negligible, LW DARE is an important component in the study of regional climate variation with important implications for more detailed global assessments.

Hansell, Richard A., Jr.↗

DOE OSTI2016

Final DOE-ASR Report for the Project “Advancing our Understanding and the Remote Sensing of Ice Clouds”

This project has evolved during its execution, and what follows are the key project findings. This project has arguably provided the first global view of how cirrus cloud (defined as having cloud base temperature T < 235 K) nucleation physics (evaluated through satellite retrievals of ice particle number concentration Ni, effective diameter De and ice water content IWC) evolves with the seasons for a given temperature, latitude zone and surface type (e.g. ocean vs. land), based on a new satellite remote sensing method developed for this project. The retrieval method is unique in that it is very sensitive to the small ice crystals that govern the number concentration Ni, allowing Ni to be retrieved. The method currently samples single-layer cirrus clouds having visible optical depth ranging from about 0.3 to 3.0, using co-located observations from the Infrared Imaging Radiometer (IIR) and from the CALIOP (Cloud and Aerosol Lidar with Orthogonal Polarization) lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) polar orbiting satellite, employing IIR channels at 10.6 μm and 12.05 μm. Retrievals of Ni are primarily used to estimate the cirrus cloud formation mechanism; that is, either homo- or heterogeneous ice nucleation (henceforth hom and het). This is possible since, in general, hom produces more than an order of magnitude more ice crystals than does het. Thus the retrievals provide insight on how these mechanisms change with the seasons for a given latitude zone or region, based on the years 2008 and 2013. Using a conservative criterion for hom cirrus, on average, the sampled cirrus clouds formed through hom occur about 43% of the time in the Arctic and 50% of the time in the Antarctic, and during winter at mid-latitudes in the Northern Hemisphere, hom cirrus occur 37% of the time. Elsewhere (and during other seasons in the Northern Hemisphere mid-latitudes), this hom cirrus fraction is lower, and it is lowest in the tropics. Thus, the microphysical properties of cirrus clouds in the Polar Regions are much different than they are in the tropics; something unknown prior to this study. Moreover, the frequency of cirrus cloud occurrence in the Polar Regions varies strongly with season, peaking during winter in the Arctic and during spring in the Antarctic. Considering these seasonal changes in microphysics and inferred cloud coverage, this leads us to speculate that the buildup of Arctic cirrus during winter may significantly contribute to tropospheric heating in that region, possibly affecting winter jet-stream dynamics and mid-latitude weather patterns through the thermal-wind balance relationship. This cirrus cloud research provides essential guidance for realistically representing cirrus clouds in climate models; guidance previously unavailable. For example, mid-latitude hom cirrus were widespread during winter over or nearby mountainous terrain, evidently due to mountain-induced waves that produce strong updrafts at cirrus cloud levels. The treatment of turbulent mountain stress and gravity waves will likely need to be improved in climate models in order to adequately represent cirrus clouds outside the tropics. Another goal of this project was to develop a ground-based 94-GHz radar retrieval for winter snowstorms, based on (1) an improved analytical framework describing the interaction of radiation from radar with snowfall and (2) the development of a steady-state snow growth model that predicts the height-evolution of the ice particle size distribution through ice particle growth by vapor diffusion, aggregation and riming (i.e. the growth of snow through collisions with supercooled cloud droplets). Although activities (1) and (2) were completed, there was insufficient time to test and finalize the radar retrieval scheme. However, activity (2) provided a new method for relating ice particle mass “m” and projected area “A” to the ice particle maximum dimension “D”. The ice cloud microphysical processes (which determine ice cloud radiative properties) in climate models are parameterized in terms of these m-D and A-D relationships. By improving these relationships, the ice cloud radiative properties in Community Atmosphere Model version 5, or CAM5 (an atmosphere global climate model, or GCM) were improved. Student funding from the University of Nevada, Reno, was combined with funds from this project to conduct some basic research on the mechanism of the North American monsoon, or NAM. Federal research on the NAM has dwindled since 2006, but atmospheric soundings taken during research vessel cruises in the Gulf of California (GC) during the North American Monsoon Experiment (NAME) were used to reveal a likely mechanism that explains the relationship between an intrusion of tropical warm water into the GC during late spring-early summer and the onset of relatively heavy NAM rainfall in northwest Mexico and the southwestern United States. These soundings, combined with reanalysis data, satellite sea surface temperatures and satellite measurements of outgoing longwave radiation were used to develop and provide evidence for a planetary-scale NAM mechanism. As far as we know, no other physical explanation has been offered for the spring-summer evolution of the NAM system.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

Understanding and Utilizing PBL Height Data from Multiple Observing Systems in the GEOS System

The accuracy of PBL height simulation is a key issue in many applications including forecasting near surface meteorology and air quality, however, it is a very challenging problem due to the lack of not only comprehensive, global Planetary Boundary Layer (PBL) observations but also a strategy and infrastructure to utilize PBL height data from a variety of sensors. Following the designation of PBL as an incubation class observable in the 2017 Decadal Survey, the PBL Incubation Study Team Report [14] made clear that “a future global PBL observing system requires modeling and data assimilation as essential components.” There is an urgent need for global modeling development in order to utilize Program of Record (POR) observations, assess their impacts, and identify gaps to be filled by future PBL missions. Our overall objective is to develop PBL data assimilation capabilities in the NASA Global Earth Observing System (GEOS), focusing on PBL height from multiple observing systems, to support the assessment and use of future PBL observations. The NASA GEOS system is composed of the GEOS global atmospheric general circulation model (AGCM) and the atmospheric data assimilation system (ADAS). The PBL parameterizations include the “Lock” K-profile scheme driven by surface and cloud-top buoyancy fluxes ([4]), and the “Louis” local scheme for stable conditions based on the Richardson number ([5]). Above the mixed layer defined by the Lock surface plume, shallow cumulus convection is represented by the mass flux scheme of [9]. Additional parameterizations are summarized in [1]. The ADAS employs the hybrid 4D Ensemble- Variational (EnVar) configuration ([15]), with the ensemble providing flow-dependent background error covariance information. The resultant analysis increments are fed back to the forecast model through the 4D incremental analysis update (IAU) approach ([11]). In this study, PBL height data are being or have been generated from radiosondes, GNSS RO, satellite (CATS, CALIPSO and ICESat-2) and ground-based (MPLNET) lidars, and wind profiler. Investigations have been conducted to specify quality marks for PBL height retrievals for the data assimilation purpose. These PBL height data have different strengths and weaknesses ([2], [3], [6], [7], [8], [10]), and the satellite PBL height data provide better global coverage and complement in-situ PBL height data. Radiosondes offer high accuracy and in situ measurement of temperature and humidity profiles, but with poor spatio-temporal sampling. The in-situ observing systems like MPLNET and wind profiler provide long history of PBL height records at each station. The GNSS RO based PBL height is retrieved based on the sharp gradients in refractivity profile that represent the fine vertical structure of temperature and moisture changes above the PBL. However, not all RO refractivity profiles reach the surface depending on location and regime, and RO refractivity retrievals can be negatively biased below 2km. The PBL height data from satellite lidars provide high resolution along track PBL height retrievals, but over land they are affected by previous day convective PBL aerosol and strongly associated with mixing layer and retrievals cannot be made below thick, attenuating clouds. A successful assimilation of PBL height data requires a thorough understanding of the observing method and the retrieval algorithm for each observing system in order to use the PBL height data from multiple observing systems properly. Due to the sensitivity of PBL height data to the observing method and choice of algorithm, it is important to use a model definition appropriate for each observation type to compute differences between PBL height data and model PBL height (OmFs). The GEOS model currently includes two PBL height definitions suitable for direct comparison with observed PBL height, and additional definitions are being added in this study. Evaluation of different model PBL height definitions is underway. Meanwhile, efforts have been made in the GEOS data assimilation system to develop PBL height data assimilation capability. PBL height data can be assimilated using two different approaches. The traditional approach is to construct an observation operator and its tangent linear and adjoint, which link control variables to PBL height data from each observing system. This observation operator can be very complicated, e.g., the lidar-based PBL height observation operator includes the backscatter lidar forward observation operator, the algorithm to derive PBL height from attenuated total backscatter, interpolation, and calculations handling the mismatch between observed and model scales. The other approach is to augment PBL height to the control variable vector, and it is adopted in this study. The latter approach was also used in previous studies, e.g., the assimilation of PBL height data from radiosonde and aircraft in the Real Time Mesoscale Analysis (RTMA) system for a dispersion modelling study ([13]); the PBL height assimilation study using lidar PBL height data at Greensburg, Kansas for a field campaign ([12]). The PBL height assimilation from multiple observing systems in this study allows us to take advantage of the diverse PBL height data that provide much better global coverage collectively under different meteorological conditions and with different temporal and spatial scales. As all the PBL heights are tightly coupled with the PBL thermodynamic variables, the strong correlations, which are provided by the 4D ensemble forecast, enable PBL height data from various sources to interact and combine coherently and provide additional information for PBL temperature and moisture fields. The results of comparisons among PBL height data from different sources and the evaluation of the model PBL height definitions with the PBL height data will be presented, and the PBL height data synergy strategies and preliminary results will also be discussed at the conference.

Y. Zhu↗

DOE OSTI2025

Forest Breeze–Cold Pool Interactions Drive Convective Organization over Heterogeneous Vegetation

Heterogeneous landscapes can influence the development of convection through the generation of thermally driven mesoscale circulations. To assess the impacts of these circulations and their interaction with sea breezes, we simulated convection in an idealized coastal environment using the Regional Atmospheric Modeling System (RAMS). We compared simulations with striped patterns of surface vegetation to those of uniform vegetation to identify the importance of vegetation heterogeneity in impacting convective development. Under dry soil conditions representative of those during the Tracking Aerosol Convection Interactions Experiment (TRACER) and Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE) campaigns in June 2022, we found that these vegetation-induced circulations, referred to in the literature as “forest breezes,” are more important than the sea breeze in determining the location of convection initiation. Convection and precipitation are also found to be favored over forests and suppressed over pasture and suburban landscapes as a result of greater surface sensible heat flux over the forest. Our findings also indicate that forest breezes are important for initiating convection along the boundaries of the forest, but that cold pools may play a key role in propagating the forest breezes toward the center of the forest stripe. In our simulations, the collisions of these breezes in the center of the forest stripe lead to uplift and strong convection there; however, a different width of the forest stripe would alter when the forest breezes collide or whether they collide at all. The presence of these cold pools may therefore impact the “ideal stripe width,” the width of each vegetation stripe which maximizes domain-wide precipitation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Investigation of the Sensitivity of Tropical Cyclogenesis to Aerosol Intervention

Abstract As risks from tropical cyclones (TCs) are fueled by climate change escalation, there is an urgent need for transformational solutions to complement traditional approaches. Seeding TCs using aerosols can be a promising method to reduce cyclone intensity, supported by theoretical understanding of the microphysical effects of aerosols on TC clouds. The ideal time to intervene effectively in TCs is likely during their initial stage, before TC wind speeds reach their peak. However, studies exploring potential aerosol effects on TC formation remain scarce. This study investigates how a TC embryo responds to the addition of aerosols of varying sizes using the Weather Research & Forecasting (WRF) model coupled with a spectral‐bin microphysics model. We found that aerosols of different sizes and concentrations distinctively affect the pre‐TC vortex's microstructure and dynamics. Fine and ultrafine aerosols enhance the latent heat of condensation, freezing, deposition, and riming, initially intensifying the vortex. However, this results in enhancement of the cold pool, thereby reducing inflow and surface fluxes, subsequently weakening the vortex. Coarse aerosols produce the opposite effect to that of fine and ultrafine aerosols. Coarse aerosols lead to a slower initial acceleration owing to enhanced warm rain. However, the resulting weaker cold pool is insufficient to effectively reduce the strength of the vortex at the later stage. This study provides critical insights into how aerosols of varying sizes and concentrations modulate the energy cascade and impact the evolution of a TC embryo, laying the groundwork for further research on TC risk management through aerosol intervention.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Major improvements on the longwave radiative interactions between surface and clouds in the Polar Regions in atmospheric global circulation model (GCM). Final Project Report

1. Summary of Work and Accomplishments in Year 1 (01/15/2015-01/14/2016). We developed new ice cloud parameterizations based on state-of-the-art MODIS Collection 6 (MC6) ice particle model. Features of the model include the consideration of surface roughness of ice crystals and spectral consistency in cloud property retrievals. Using more than 14,000 particle size distributions (PSDs) from in-situ measurements and the latest ice particle single-scattering property library, our parameterizations provide band-averaged bulk-scattering properties. According to statistics of fittings, the parameterization schemes represent the band-averaged bulk-scattering properties very well. Compared to the ice particle model developed by Fu (1998), flux simulations with the MC6 particle model result in larger upward flux at the top of the atmosphere (TOA) and smaller at the surface for typical cirrus clouds. In the assessment of the effect of longwave light scattering, our results also support the conclusions of previous studies. The error in flux calculations reaches about 10 W/m 2 when a cirrus cloud is thin and its particle size is small. 2. Summary of Work and Accomplishments in Year 2 (01/15/2016-01/14/2017) Clouds are a major modulator of the global radiation budgets. However, representations of clouds in general circulation models (GCMs) neglect many important processes, particularly those related to ice clouds. One major uncertainty source is the radiative transfer scheme in GCMs. To reduce the computational burden in most GCMs, absorption is the only radiative transfer process considered in longwave spectral bands. Recently, a state-of-the-art MC6 ice model has been available, which provides spectral consistency in ice cloud retrievals. With an advanced light scattering library for ice particles, we performed sensitivity studies of the potential impacts on the climate including light scattering for MC6 model and other 11 ice cloud models. Specifically, we modified RRTMG_LW (the GCM version of Longwave Rapid Radiative Transfer Model), a radiative transfer module widely used in GCMs and numerical prediction models, to identify flux simulation differences with and without considering light scattering processes. The simulations with light scattering come from a rigorous radiative solver, DISORT (Discrete Ordinates Radiative Transfer Program for a Multi-Layered Plane-Parallel Medium), are used as benchmarks. The results show that the weighted annual mean biases of RRTMG_LW for the upward flux at the top of the atmosphere, the downward flux at the surface, and the net flux into the atmosphere are about 0.8 ± 0.3, -0.1 ± 0.05, and -0.7 ± 0.3 W m-2, respectively. According to the different the ice crystal shapes, the weighted annual mean bias for heating rate is about -0.006 ± 0.02 to 0.04 K/day. 3. Summary of Work and Accomplishments in Year 3 (01/15/2017-01/14/2018) Since absorption dominates optical properties of clouds in the longwave (LW) spectrum, most of general circulation models (GCMs) only take absorption properties of clouds into account in the radiative transfer modules in order to reduce computational costs. To quantify the biases of excluding LW scattering when clouds exist, we simulated fluxes and heating rates by using satellite data from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), CloudSat, Clouds and the Earth’s Radiant Energy System (CERES) and Moderate Resolution Imaging Spectrometer (MODIS) merged products (CCCM) in 2010. In annual global average, neglecting LW scattering causes overestimation by 2.6 W/m 2 for the top-of-atmosphere (TOA) upward fluxes and underestimation by 1.2 W/m 2 for surface downward fluxes. In particular, regional extreme biases are approximately 12 W/m 2 for TOA upward fluxes and are approximately -3.6 W/m 2 for surface downward fluxes, or are approximately 5% of the global averaged outgoing longwave radiation (OLR) and 1% of the global averaged surface downward fluxes, respectively. In terms of heating rates, on average, LW scattering heats the whole atmosphere column by 0.0045 K/day, heats the cloud layers by 0.0420 K/day, heats the surface by 0.028 K/day, and cools the tropopause by 0.018 K/day.

58 GEOSCIENCES↗

DOE OSTI2013

Bounding the Role of Black Carbon in the Climate System: A Scientific Assessment

Black carbon aerosol plays a unique and important role in Earth’s climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. Predominant sources are combustion related; namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr-1 in the year 2000 with an uncertainty range of 2000 to 29000. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption, influence on liquid, mixed-phase, and ice clouds, and deposition on snow and ice. These effects are calculated with models, but when possible, they are evaluated with both microphysical measurements and field observations. Global atmospheric absorption attributable to black carbon is too low in many models, and should be increased by about about 60%. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of black carbon is +0.43 W m-2 with 90% uncertainty bounds of (+0.17, +0.68) W m-2. Total direct forcing by all black carbon sources in the present day is estimated as +0.49 (+0.20, +0.76) W m-2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings and their rapid responses and feedbacks. The best estimate of industrial-era (1750 to 2005) climate forcing of black carbon through all forcing mechanisms is +0.77 W m-2 with 90% uncertainty bounds of +-0.06 to +1.53 W m-2. Thus, there is a 96% probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. With a value of +0.77 W m-2, black carbon is likely the second most important individual climate-forcing agent in the industrial era, following carbon dioxide. Sources that emit black carbon also emit other short- lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of co- emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil-fuel and biofuel) have a net climate forcing of +0.004 (-0.62 to +0.57) W m-2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all black- carbon-rich sources becomes slightly negative (-0.08 W m-2 with 90% uncertainty bounds of -1.23 to +0.81 W m-2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

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DOE OSTI2016

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Abstract. An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m−3 when LVOC fate corrected) compared to daytime (average 0.9 µg m−3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic compounds, and net production at lower ages followed by net consumption of terpenoid oxidation products as photochemical age increased. New particle formation was observed in the reactor after oxidation, especially during times when precursor gas concentrations and SOA formation were largest. Approximately 4.4 times more SOA was formed in the reactor from OH oxidation than could be explained by the VOCs measured in ambient air. To our knowledge this is the first time that this has been shown when comparing VOC concentrations with SOA formation measured at the same time, rather than comparing measurements made at different times. Several recently developed instruments have quantified ambient semivolatile and intermediate-volatility organic compounds (S/IVOCs) that were not detected by a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). An SOA yield of 18–58 % from those compounds can explain the observed SOA formation. S/IVOCs were the only pool of gas-phase carbon that was large enough to explain the observed SOA formation. This work suggests that these typically unmeasured gases play a substantial role in ambient SOA formation. Our results allow ruling out condensation sticking coefficients much lower than 1. These measurements help clarify the magnitude of potential SOA formation from OH oxidation in forested environments and demonstrate methods for interpretation of ambient OFR measurements.

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