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Kreidenweis, Sonia M.

Publications and source records attributed to Kreidenweis, Sonia M..

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Constraining Present‐Day Anthropogenic Total Iron Emissions Using Model and Observations

Abstract Iron emissions from human activities, such as oil combustion and smelting, affect the Earth's climate and marine ecosystems. These emissions are difficult to quantify accurately due to a lack of observations, particularly in remote ocean regions. In this study, we used long‐term, near‐source observations in areas with a dominance of anthropogenic iron emissions in various parts of the world to better estimate the total amount of anthropogenic iron emissions. We also used a statistical source apportionment method to identify the anthropogenic components and their sub‐sources from bulk aerosol observations in the United States. We find that the estimates of anthropogenic iron emissions are within a factor of 3 in most regions compared to previous inventory estimates. Under‐ or overestimation varied by region and depended on the number of sites, interannual variability, and the statistical filter choice. Smelting‐related iron emissions are overestimated by a factor of 1.5 in East Asia compared to previous estimates. More long‐term iron observations and the consideration of the influence of dust and wildfires could help reduce the uncertainty in anthropogenic iron emissions estimates.

Meteorology & Atmospheric Sciences↗
DOE OSTI2024

Characterizing Ice Nucleating Particles Over the Southern Ocean Using Simultaneous Aircraft and Ship Observations

Abstract Supercooled liquid clouds are ubiquitous over the Southern Ocean (SO), even to temperatures below −20°C, and comprise a large fraction of the marine boundary layer (MBL) clouds. Earth system models and reanalysis products have struggled to reproduce the observed cloud phase distribution and occurrence of cloud ice in the region. Recent simulations found the microphysical representation of ice nucleation and growth has a large impact on these properties, however, measurements of SO ice nucleating particles (INPs) to validate simulations are sparse. This study presents measurements of INPs from simultaneous aircraft and ship campaigns conducted over the SO in austral summer 2018, which include the first in situ observations in and above cloud in the region. Our results confirm recent observations that INP concentrations are uniformly lower than measurements made in the late 1960s. While INP concentrations below and above cloud are similar, higher ice nucleation efficiency above cloud supports model simulations that the dominant INP composition varies with height. Model parameterizations based solely on aerosol properties capture the mean relationship between INP concentration and temperature but not the observed variability, which is likely related to the only modest correlations observed between INPs and environmental or aerosol metrics. Including wind speed in addition to activation temperature in a marine INP parameterization reduces bias but does not explain the large range of observed INP concentrations. Direct and indirect inference of marine INP size suggests MBL INPs, at least during Austral summer, are dominated by particles with diameters smaller than 500 nm.

Meteorology & Atmospheric Sciences↗
DOE OSTI2023

Simulating Southern Ocean Aerosol and Ice Nucleating Particles in the Community Earth System Model Version 2

Southern Ocean (SO) low-level mixed phase clouds have been a long-standing challenge for Earth system models to accurately represent. While improvements to the Community Earth System Model version 2 (CESM2) resulted in increased supercooled liquid in SO clouds and improved model radiative biases, simulated SO clouds in CESM2 now contain too little ice. Previous observational studies have indicated that marine particles are major contributor to SO low-level cloud heterogeneous ice nucleation, a process that initiates a number of cloud processes that govern cloud radiative properties. In this study, we utilize detailed aerosol and ice nucleating particle (INP) measurements from two recent measurement campaigns to assess simulated aerosol abundance, number size distributions, and composition and INP parameterizations for use in CESM2. Our results indicate that CESM2 has a positive bias in simulated surface-level total aerosol surface area at latitudes north of 58°S. Measured INP populations were dominated by marine INPs and we present evidence of refractory INPs present over the SO assumed here to be mineral dust INPs. Results highlight a critical need to assess simulated mineral dust number and size distributions in CESM2 in order to adequately represent SO INP populations and their response to long-term changes in atmospheric transport patterns and land use change. Furthermore, we also discuss important cautions and limitations in applying a commonly used mineral dust INP parameterization to remote regions like the pristine SO.

58 GEOSCIENCES↗
DOE OSTI2022

Estimation of Sea Spray Aerosol Surface Area Over the Southern Ocean Using Scattering Measurements

This study focuses on methods to estimate dry marine aerosol surface area (SA) from bulk optical measurements. Aerosol SA is used in many models' ice nucleating particle (INP) parameterizations, as well as influencing particle light scattering, hygroscopic growth, and reactivity, but direct observations are scarce in the Southern Ocean (SO). Two campaigns jointly conducted in austral summer 2018 provided co-located measurements of aerosol SA from particle size distributions and lidar to evaluate SA estimation methods in this region. Mie theory calculations based on measured size distributions were used to test a proposed approximation for dry aerosol SA, which relies on estimating effective scattering efficiency (Q) as a function of Ångström exponent (å). For distributions with dry å < 1, Q = 2 was found to be a good approximation within ±50%, but for distributions with dry å > 1, an assumption of Q = 3 as in some prior studies underestimates dry aerosol SA by a factor of 2 or more. We propose a new relationship between dry å and Q, which can be used for –0.2 < å < 2, and suggest å = 0.8 as the cutoff between primary and secondary marine aerosol-dominated distributions. Application of a published methodology to retrieve dry marine aerosol SA from lidar extinction profiles overestimated aerosol SA by a factor of 3–5 during these campaigns. Using Microtops aerosol optical thickness measurements, we derive alternative lidar conversion parameters from our observations, applicable to marine aerosol over the SO.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Experimental Determination of the Relationship Between Organic Aerosol Viscosity and Ice Nucleation at Upper Free Tropospheric Conditions

Abstract This work presents measurements of the ice nucleating ability of secondary organic material recorded between −40 and −70°C and relative humidity with respect to ice (RH ice ) between 150% and 220%. For a subset of systems, temperature and humidity dependence of particle viscosity as well as dry glass transition temperature were characterized using the dual tandem differential mobility analyzer method. Eleven unique monoterpene, sesquiterpene and aromatic precursors were used to generate secondary organic material (SOM) using either an oxidation flow reactor (OFR) or an environmental chamber (EC). For the SOM for which viscosity was measured, the particle glass transition temperatures varied between 6 and 23°C ( n = 8). Measurements were performed to verify that increased relative humidity did not plasticize the particles below −10°C at residence times similar to those in the ice nucleation instrument. No heterogeneous ice nucleation was observed at the ∼0.5% onset threshold for any of the materials generated. The ice nucleation occurs by the freezing of SOM solution droplets consistent with homogeneous freezing indicating that they form an aqueous solution, or the SOM particles required water saturation to freeze, indicating that they were hydrophobic. Experiments exploring the influence of functional groups and mass loading did not reveal any obvious influence of particle chemistry or generation conditions on the results. Close structural matches between known organic ice nucleating particles as precursor or formed products did not yield materials that promoted freezing. These experiments suggest that heterogeneous ice formation of glassy secondary organic materials is likely uncommon under upper free tropospheric conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Ice Nucleating Particle Connections to Regional Argentinian Land Surface Emissions and Weather During the Cloud, Aerosol, and Complex Terrain Interactions Experiment

Abstract Here, we present a multi‐season study of ice‐nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north‐central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95°C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Heat labile INPs, which we define as “biological” herein, dominated the population active at −5 to −20°C, while non‐heat‐labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from −20 to −28°C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around −12°C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non‐heat‐labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single particle mass spectrometry showed that soil particles aerosolized from a regionally common agricultural topsoil contained known mineral INP sources (K‐feldspar and illite) as well as a significant organic component. The INP activity observed in this study correlates well with agricultural soil INP activities from this and other regions of the world, suggesting that the observed INP spectra might be typical of many arable landscapes. These results demonstrate the strong influence of regional continental landscapes, emitting INPs of types that are not yet well represented in global models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Utilizing a Storm-Generating Hotspot to Study Convective Cloud Transitions: The CACTI Experiment

The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign was designed to improve understanding of orographic cloud life cycles in relation to surrounding atmospheric thermodynamic, flow, and aerosol conditions. The deployment to the Sierras de Córdoba range in north-central Argentina was chosen because of very frequent cumulus congestus, deep convection initiation, and mesoscale convective organization uniquely observable from a fixed site. The C-band Scanning Atmospheric Radiation Measurement (ARM) Precipitation Radar was deployed for the first time with over 50 ARM Mobile Facility atmospheric state, surface, aerosol, radiation, cloud, and precipitation instruments between October 2018 and April 2019. An intensive observing period (IOP) coincident with the RELAMPAGO field campaign was held between 1 November and 15 December during which 22 flights were performed by the ARM Gulfstream-1 aircraft. A multitude of atmospheric processes and cloud conditions were observed over the 7-month campaign, including numerous orographic cumulus and stratocumulus events; new particle formation and growth producing high aerosol concentrations; drizzle formation in fog and shallow liquid clouds; very low aerosol conditions following wet deposition in heavy rainfall; initiation of ice in congestus clouds across a range of temperatures; extreme deep convection reaching 21-km altitudes; and organization of intense, hail-containing supercells and mesoscale convective systems. These comprehensive datasets include many of the first ever collected in this region and provide new opportunities to study orographic cloud evolution and interactions with meteorological conditions, aerosols, surface conditions, and radiation in mountainous terrain.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Observations of Clouds, Aerosols, Precipitation, and Surface Radiation over the Southern Ocean: An Overview of CAPRICORN, MARCUS, MICRE, and SOCRATES

Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF–NCAR G-V aircraft flying north–south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. Furthermore, the combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

A Multi-Instrument Cloud Condensation Nuclei Spectrum Product (Final Technical Report)

A wealth of observational data exists on the characteristics of atmospheric particulate matter, over multiple years, at the DOE ARM Southern Great Plains (SGP) Central Facility site. This site is located in a region of the country that frequently experiences weather extremes, and that is removed from many local sources of pollution but is affected by transported smoke, dust, and urban emissions. The relationships between particulate matter, cloud formation and evolution, and precipitation are therefore of strong interest, and are being explored via modeling on a variety of scales. These models require as input detailed information on the characteristics of particles capable of serving as the nuclei for cloud formation. Sufficient data exist to be able to put together a picture of the nature of the total aerosol and the cloud condensation nuclei (CCN) subset, and their variability, through merged data products. This study was aimed at exploiting the multiple measurement types at SGP to develop the first such multi-year estimates. Further, the resulting data were analyzed to understand temporal patterns ranging from hourly to seasonal, thereby gaining insights into the particle sources affecting the atmosphere in this region. DOE-funded datasets that were analyzed in this study include total particle number concentrations, submicron aerosol scattering coefficients, dry aerosol size distributions, and more recently, time-resolved submicron aerosol chemical composition. Data are also available for the number concentrations of particles that are activated in a cloud condensation nucleus instrument at a series of setpoint supersaturations, providing direct observations of the number concentrations of “CCN”. This variable is the quantity that is generally desired for inclusion in numerical models that seek to represent and predict the impacts of varying aerosol characteristics on the formation and microphysical properties of clouds. One limitation of the use of direct CCN observations is that they are not available for supersaturations larger than about 1%, which is insufficient for deep convection and may be insufficient even for shallow convection, depending on the nature of the available CCN and the dynamics of the cloud. We developed a data-based approach to representing the full aerosol size spectrum with size-dependent hygroscopicity, and used this to extrapolate CCN spectra beyond the limited measurements. Five years of SGP aerosol data (2009 -2013) were analyzed. As a side product of our work, we identified and communicated several previously-unflagged data quality issues. The resulting merged aerosol distributions, along with fits for seasonal averages, were published and submitted to the ARM archive as a special value-added product (VAP; submitted as a PI product). CCN spectra were computed for the same data period and will similarly be published and submitted to the archive for use by the community. We also note that our methodologies and findings have been discussed at several Joint ARM User Facility/Atmospheric System Research (ASR) Principal Investigators Meetings and that recent ARM/ASR aerosol data reporting strategies have included similar ideas for data merging, indicating that this work has had a lasting impact on ARM aerosol data acquisition and reporting. The proposed work advances the science of the interactions of aerosols, clouds and precipitation, with direct application to improve representation of such interactions for clouds in regional and global climate models. The archived data will continue to serve research studies in the future.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds

Significance The Earth’s climate is affected by the radiative properties of clouds. In clouds containing both supercooled water droplets and ice particles (mixed-phase clouds), cloud lifetime and albedo are affected by the presence of ice nucleating particles (INP). After decades of research, the importance of black carbon (BC) as an INP remains unresolved. In this work, we determined the contribution of BC to INP concentrations ([INP]) from real-world wildfires and prescribed burns. We found that BC does not contribute significantly to [INP] in near-field biomass burning plumes. These results were applied as parameterizations to global climate model output. Combined with previous work on diesel-engine exhaust, we find that BC does not contribute significantly to global [INP] relevant to mixed-phase clouds.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2016

Aerosol Meteorology of Maritime Continent for the 2012 7SEAS Southwest Monsoon Intensive Study - Part 2: Philippine Receptor Observations of Fine-Scale Aerosol Behavior

The largest 7 Southeast Asian Studies (7SEAS) operations period within the Maritime Continent (MC) occurred in the August-September 2012 biomass burning season. Data included were observations aboard the MY Vasco, dispatched to the Palawan Archipelago and Sulu Sea of the Philippines for September 2012. At these locations, the Vasco observed MC smoke and pollution entering the southwest monsoon (SWM) monsoonal trough. Here we describe the research cruise findings and the finer-scale aerosol meteorology of this convectively active region. This 2012 cruise complemented a 2-week cruise in 2011 and was generally consistent with previous findings in terms of how smoke emission and transport related to monsoonal flows, tropical cyclones (TC), and the covariance between smoke transport events and the atmosphere's thermodynamic structure. Biomass burning plumes were usually mixed with significant amounts of anthropogenic pollution. Also key to aerosol behavior were squall lines and cold pools propagating across the South China Sea (SCS) and scavenging aerosol particles in their path. However, the 2012 cruise showed much higher modulation in aerosol frequency than its 2011 counterpart. Whereas in 2011 large synoptic-scale aerosol events transported high concentrations of smoke into the Philippines over days, in 2012 measured aerosol events exhibited a much shorter-term variation, sometimes only 312h. Strong monsoonal flow reversals were also experienced in 2012. Nucleation events in cleaner and polluted conditions, as well as in urban plumes, were observed. Perhaps most interestingly, several cases of squall lines preceding major aerosol events were observed, as opposed to 2011 observations where these lines largely scavenged aerosol particles from the marine boundary layer. Combined, these observations indicate pockets of high and low particle counts that are not uncommon in the region. These perturbations are difficult to observe by satellite and very difficult to model. Indeed, the Navy Aerosol Analysis and Prediction System (NAAPS) simulations captured longer period aerosol events quite well but largely failed to capture the timing of high-frequency phenomena. Ultimately, the research findings of these cruises demonstrate the real world challenges of satellite-based missions, significant aerosol life cycle questions such as those the future Aerosol/Clouds/Ecosystems (ACE) will investigate, and the importance of small-scale phenomena such as sea breezes, squall lines, and nucleation events embedded within SWM patterns in dominating aerosol life cycle and potential relationships to clouds.

Reid, Jeffrey S.↗
NASA NTRS2016

Improving Our Fundamental Understanding of the Role of Aerosol Cloud Interactions in the Climate System

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol−cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol−cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol−cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

general circulation models↗
NASA NTRS2012

Critical Reflectance Derived from MODIS: Application for the Retrieval of Aerosol Absorption over Desert Regions

Aerosols are tiny suspended particles in the atmosphere that scatter and absorb sunlight. Smoke particles are aerosols, as are sea salt, particulate pollution and airborne dust. When you look down at the earth from space sometimes you can see vast palls of whitish smoke or brownish dust being transported by winds. The reason that you can see these aerosols is because they are reflecting incoming sunlight back to the view in space. The reason for the difference in color between the different types of aerosol is that the particles arc also absorbing sunlight at different wavelengths. Dust appears brownish or reddish because it absorbs light in the blue wavelengths and scatters more reddish light to space, Knowing how much light is scattered versus how much is absorbed, and knowin~ that as a function of wavelength is essential to being able to quantify the role aerosols play in the energy balance of the earth and in climate change. It is not easy measuring the absorption properties of aerosols when they are suspended in the atmosphere. People have been doing this one substance at a time in the laboratory, but substances mix when they are in the atmosphere and the net absorption effect of all the particles in a column of air is a goal of remote sensing that has not yet been completely successful. In this paper we use a technique based on observing the point at which aerosols change from brightening the surface beneath to darkening it. If aerosols brighten a surface. they must scatter more light to space. If they darken the surface. they must be absorbing more. That cross over point is called the critical reflectance and in this paper we show that critical reflectance is a monotonic function of the intrinsic absorption properties of the particles. This parameter we call the single scattering albedo. We apply the technique to MODIS imagery over the Sahara and Sahel regions to retrieve the single scattering albedo in seven wavelengths, compare these retrievals to ground-based retrievals from AERONET instruments and compute error bars on each retrieval. The results show that we can retrieve single scattering albedo for pure dust to within +/-0.02 and mixtures of dust and smoke to within +/-0.03. No other space based instrument has achieved a retrieval of single scattering albedo that spans the spectrum from 0.47 microns to 2.13 microns and produces regional maps of aerosol absorption showing gradients and changes. Applied in a more operational fashion, such information will narrow uncertainties in estimating aerosol forcing on climate.

Wells, Kelley C.↗