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NASA NTRS2017

Ice Nucleation in the Tropical Tropopause Layer: Implications for Cirrus Occurrence, Cirrus Microphysical Properties, and Dehydration of Air Entering the Stratosphere

Recent laboratory experiments have advanced our understanding of the physical properties and ice nucleating abilities of aerosol particles atlow temperatures. In particular, aerosols containing organics will transition to a glassy state at low temperatures, and these glassy aerosols are moderately effective as ice nuclei. These results have implications for ice nucleation in the cold Tropical Tropopause Layer (TTL; 13-19 km). We have developed a detailed cloud microphysical model that includes heterogeneous nucleation on a variety of aerosol types and homogeneous freezing of aqueous aerosols. This model has been incorporated into one-dimensional simulations of cirrus and water vapor driven by meteorological analysis temperature and wind fields. The model includes scavenging of ice nuclei by sedimenting ice crystals. The model is evaluated by comparing the simulated cloud properties and water vapor concentrations with aircraft and satellite measurements. In this presentation, I will discuss the relative importance of homogeneous and heterogeneous ice nucleation, the impact of ice nuclei scavenging as air slowly ascends through the TTL, and the implications for the final dehydration of air parcels crossing the tropical cold-point tropopause and entering the tropical stratosphere.

tropopause↗

DOE OSTI2020

Chemical Imaging of Fine Mode Atmospheric Particles Collected from a Research Aircraft over Agricultural Fields

Vegetation and crops in agricultural areas are a significant source of both biogenic secondary organic aerosols and of directly emitted primary biological atmospheric particles (PBAPs) composed of plant fragments/debris, fungal spores, pollen, and bacteria among others. Seasonal crop harvesting significantly intensifies regional PBAP emissions and aerosolizes soil organic matter and dust particulates. In this paper, the atmospheric contributions and impact of PBAPs have been insufficiently investigated due to limited real-time observations and ambiguity in their detection by existing measurement techniques. We collected ambient particles on-board an instrumented Beechcraft BE76 Duchess research aircraft flying above actively harvested agriculture fields of corn and soybean crops. In this work, particle samples were analyzed using complementary chemical imaging techniques, including computer-controlled scanning electron microscopy coupled with elemental microanalysis to describe particle-type population and scanning transmission X-ray microscopy to provide quantitative metrics on particle internal heterogeneity. We show the particle-class contribution is consistent between corn and soybean harvesting across altitudes of 100–300 m AGL. The contribution of PBAPs in the size range of 0.15–1.25 μm is estimated to be 10–12% of ~39,000 analyzed particles. Determining viscosity with X-ray microanalysis has shown that the fine-mode organic particles collected are viscous/semisolid (10 2 –10 12 Pa s) while the majority of PBAP fragments are solid (>10 12 Pa s). The observation of submicrometer, solid carbonaceous fragments of biogenic origin has implications for the regional cloud condensation nuclei and ice nuclei budget. Therefore, seasonal harvesting of crops may play an important, yet unrecognized, role in regional cloud formation and climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Wind-driven emissions of coarse-mode particles in an urban environment

Abstract. Quantifying surface–atmosphere exchange rates of particles is important for understanding the role of suspended particulate matter in radiative transfer, clouds, precipitation, and climate change. Emissions of coarse-mode particles with a diameter greater than 0.5 µm provide giant cloud condensation nuclei and ice nuclei. These emissions are critical for understanding the evolution of cloud microphysical properties yet remain poorly understood. Here we introduce a new method that uses lidar retrievals of the elastic backscatter and Doppler velocity to obtain surface number emissions of particles with a diameter greater than 0.53 µm. The technique is applied to study particle number fluxes over a 2-month period from 1 June to 10 August 2022 during the TRACER campaign at an urban site near Houston, TX, USA. We found that all the observed fluxes were positive (upwards), indicating particle emission from the surface. The fluxes followed a diurnal pattern and peaked near noon local time. Flux intensity varied through the 2 months with multi-day periods of strong fluxes and multi-day periods of weak fluxes. Emission particle number fluxes peaked near ∼ 100 cm−2 s−1. The daily averaged emission fluxes correlated with friction velocity and were anticorrelated with surface relative humidity. The emission flux can be parameterized as F= 3000 u*4, where u* is the friction velocity in m s−1 and the emission flux F is in cm−2 s−1. The u* dependence is consistent with emission from wind-driven erosion. Estimated values for the mass flux are in the lower range of literature values from non-urban sites. These results demonstrate that urban environments may play an important role in supplying coarse-mode particles to the boundary layer. We anticipate that quantification of these emissions will help constrain aerosol–cloud interaction models that use prognostic aerosol schemes.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2014

Far-Reaching Impacts of African Dust- A Calipso Perspective

African dust can transport across the tropical Atlantic and reach the Amazon basin, exerting far-reaching impacts on climate in downwind regions. The transported dust influences the surface-atmosphere interactions and cloud and precipitation processes through perturbing the surface radiative budget and atmospheric radiative heating and acting as cloud condensation nuclei and ice nuclei. Dust also influences biogeochemical cycle and climate through providing nutrients vital to the productivity of ocean biomass and Amazon forests. Assessing these climate impacts relies on an accurate quantification of dust transport and deposition. Currently model simulations show extremely large diversity, which calls for a need of observational constraints. Kaufman et al. (2005) estimated from MODIS aerosol measurements that about 144 Tg of dust is deposited into the tropical Atlantic and 50 Tg of dust into the Amazon in 2001. This estimated dust import to Amazon is a factor of 3-4 higher than other observations and models. However, several studies have argued that the oversimplified characterization of dust vertical profile in the study would have introduced large uncertainty and very likely a high bias. In this study we quantify the trans-Atlantic dust transport and deposition by using 7 years (2007-2013) observations from CALIPSO lidar. CALIPSO acquires high-resolution aerosol extinction and depolarization profiles in both cloud-free and above-cloud conditions. The unique CALIPSO capability of profiling aerosols above clouds offers an unprecedented opportunity of examining uncertainties associated with the use of MODIS clear-sky data. Dust is separated from other types of aerosols using the depolarization measurements. We estimated that on the basis of 7-year average, 118142 Tg of dust is deposited into the tropical Atlantic and 3860 Tg of dust into the Amazon basin. Substantial interannual variations are observed during the period, with the maximum to minimum ratio of about 1.6 and 2.5 for the deposition to the tropical Atlantic and Amazon, respectively. The MODIS-based estimates appear to fall within the range of CALIPSO-based estimates; and the difference between MODIS and CALIPSO estimates can be largely attributed to the interannual variability, which is corroborated by long-term surface dust concentration observations in the tropical Atlantic. Considering that CALIPSO generally tends to underestimate the aerosol loading, our estimate is likely to represent a low bound for the dust transport and deposition estimate. The finding suggests that models have substantial biases and considerable effort is needed to improve model simulations of dust cycle.

dust↗

NASA NTRS2015

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

Aerosols↗

NASA NTRS2016

A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.

aerosols↗

NASA NTRSDate not supplied

TPSAS-NF1676L-33032-DND

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES; http://naames.larc.nasa.gov) is a five-year NASA Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. The objectives of this study are to determine the major transport pathways for North American pollution outflow to the North Atlantic, and to quantify the terrestrial and marine sources of aerosols during NAAMES using ground, ship, aircraft, and remote sensing observations in conjunction with a state-of-the-art global 3-D chemical transport model (GEOS-Chem). This poster presents an initial evaluation of GEOS-Chemfor the periods of NAAMES campaigns #1 (Nov. 2015) and #2 (May 2016).

Hongyu Liu↗

NASA NTRS1980

Ice nucleus concentrations measured during the 1975 Florida Area Cumulus Experiment /FACE/

Ice nuclei measurements were made aboard a cloud-base aircraft during the 1975 Florida Area Cumulus Experiment. Two techniques were used to obtain the ice nuclei concentrations; membranes were collected and analyzed using the NCAR membrane development chamber and continuous ice nuclei concentrations were obtained using the NCAR acoustical counter. Results showed that the membrane technique failed to effectively detect ice nuclei in this maritime tropical area. However, the concentrations recorded by the acoustical counter showed natural afternoon diurnal increases which may have ramifications on cloud development and seeding potential within the particular study area.

Wisniewski, J.↗

NASA NTRS1997

SUCCESS Evidence for Cirrus Cloud Ice Nucleation Mechanisms

During the SUCCESS mission, several measurements were made which should improve our understanding of ice nucleation processes in cirrus clouds. Temperature and water vapor concentration were made with a variety of instruments on the NASA DC-8. These observations should provide accurate upper tropospheric humidities. In particular, we will evaluate what humidities are required for ice nucleation. Preliminary results suggest that substantial supersaturations frequently exist in the upper troposphere. The leading-edge region of wave-clouds (where ice nucleation occurs) was sampled extensively at temperatures near -40 and -60C. These observations should give precise information about conditions required for ice nucleation. In addition, we will relate the observed aerosol composition and size distributions to the ice formation observed to evaluate the role of soot or mineral particles on ice nucleation. As an alternative technique for determining what particles act as ice nuclei, numerous samples of aerosols inside ice crystals were taken. In some cases, large numbers of aerosols were detected in each crystal, indicating that efficient scavenging occurred. Analysis of aerosols in ice crystals when only one particle per crystal was detected should help with the ice nucleation issue. Direct measurements of the ice nucleating activity of ambient aerosols drawn into airborne cloud chambers were also made. Finally, measurements of aerosols and ice crystals in contrails should indicate whether aircraft exhaust soot particles are effective ice nuclei.

Jensen, Eric↗

DOE OSTI2023

A numerical simulation of CCN impacts on weather modification efficiency

Aerosols affect development of clouds and precipitation by serving as cloud condensation nuclei (CCN) and ice nuclei (IN). Considering the dramatically changing ambient aerosol concentration, it is important to examine the potential “side effect” of aerosol pollution on precipitation enhancement by weather modification. In this study, the cloud seeding was performed on a precipitation event in Beijing in the summer of 2008, which is simulated by the NSSL two-moment cloud scheme of the Weather Research and Forecasting (WRF) model. Sensitivity tests were conducted by modifying the ambient aerosol concentration and the ice crystal seeding amount to investigate the cloud seeding efficacy in different CCN concentration scenarios. There was a slight difference in the precipitation distribution between the simulations with two ambient CCN concentrations: the northern precipitation center in polluted scenario was weaker and the southern center was stronger. Compared with normal CCN scenario, the cloud liquid water mass and ice crystal mass in the severe pollution scenario is larger, and the total contents of snow and graupel were not sensitive to the CCN concentration. With the same amount of man-made ice crystals seeding, the precipitation enhancement was quite different under different CCN conditions. The higher the CCN concentration usually leads to stronger precipitation suppression. As CCN concentration increase, the deposition growth of snow, auto-conversion and accretion of ice crystals to snow were weakened, as well as the conversion of melting snow and graupel into rainwater.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1978

Airborne measurements of cloud forming nuclei and aerosol particles at Kennedy Space Center, Florida

Results of airborne measurements of the sizes and concentrations of aerosol particles, ice nuclei, and cloud condensation nuclei that were taken at Kennedy Space Center, Florida, are presented along with a detailed description of the instrumentation and measuring capabilities of the University of Washington airborne measuring facility (Douglas B-23). Airborne measurements made at Ft. Collins, Colorado, and Little Rock, Arkansas, during the ferry of the B-23 are presented. The particle concentrations differed significantly between the clean air over Ft. Collins and the hazy air over Little Rock and Kennedy Space Center. The concentrations of cloud condensation nuclei over Kennedy Space Center were typical of polluted eastern seaboard air. Three different instruments were used to measure ice nuclei: one used filters to collect the particles, and the others used optical and acoustical methods to detect ice crystals grown in portable cloud chambers. A comparison of the ice nucleus counts, which are in good agreement, is presented.

Radke, L. F.↗

NASA NTRS2014

Interannual Variations in Aerosol Sources and Their Impact on Orographic Precipitation Over California's Central Sierra Nevada

Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater I field campaign (2009-2011), the impacts of aerosol sources on precipitation were investigated in the California Sierra Nevada. In 2009, the precipitation collected on the ground was influenced by both local biomass burning (up to 79% of the insoluble residues found in precipitation) and long-range transported dust and biological particles (up to 80% combined), while in 2010, by mostly local sources of biomass burning and pollution (30-79% combined), and in 2011 by mostly long-range transport from distant sources (up to 100% dust and biological). Although vast differences in the source of residues was observed from year-to-year, dust and biological residues were omnipresent (on average, 55% of the total residues combined) and were associated with storms consisting of deep convective cloud systems and larger quantities of precipitation initiated in the ice phase. Further, biological residues were dominant during storms with relatively warm cloud temperatures (up to -15 C), suggesting these particles were more efficient IN compared to mineral dust. On the other hand, lower percentages of residues from local biomass burning and pollution were observed (on average 31% and 9%, respectively), yet these residues potentially served as CCN at the base of shallow cloud systems when precipitation quantities were low. The direct connection of the source of aerosols within clouds and precipitation type and quantity can be used in models to better assess how local emissions versus long-range transported dust and biological aerosols play a role in impacting regional weather and climate, ultimately with the goal of more accurate predictive weather forecast models and water resource management.

Creamean, J. M.↗

NASA NTRS1982

Measurements of cloud nuclei in the effluents from launches of liquid- and solid-fueled rockets

Airborne measurements of two types of cloud nuclei, cloud condensation nuclei (CCN) and ice nuclei (IN), were conducted in the stabilized ground clouds which resulted from the launches of a liquid-fueled ATLAS/Centaur rocket and a solid-fueled TITAN III rocket. Results show that the concentrations of CCN in both types of clouds were greater than ambient values for the 2 hours duration of the measurements. The initial production of CCN active at 0.5% supersaturation in the ATLAS and TITAN clouds was found to be equivalent to a 20 and 700 sec emission, respectively, by the city of Denver, Colorado. After the initial production, the clouds continued to generate CCN at a rate of about 1/cu cm sec. However, concentrations of IN in the ATLAS cloud were greater than ambient values for only a short period after launch, and it appears that the nuclei resulted from entrained launch pad and ground debris. The concentrations of IN in the TITAN cloud were found to be at or below ambient levels until about 2 hours after launch when they increased substantially above ambient values.

Hindman, E. E.↗

NASA NTRSDate not supplied

TPSAS-NF1676L-20101-DND

Aerosols influence climate through their direct and indirect effects. The aerosol indirect effect is based on the way they interact with surrounding clouds. During cloud formation and development, aerosols act as cloud nucleation nuclei (CCN) or ice nuclei, which modifies cloud micro-, macro-physical and radiative properties, and hence helps to shape the Earth's radiation budget. Dominant sources of ocean-derived aerosols that may serve as CCN include sea spray and biogenic aerosol. In this study, we used 10-years global observations from the A-Train satellites to show seasonal variations of cloud droplet number concentrations (CDNC), ocean chlorophyll concentrations, aerosol angstrom parameter, and rainfall. Potential cloud-aerosol interactions are further discussed based on seasonal and spatial correlations between microphysics of clouds and aerosols. Emphasis for this study is placed on the southern ocean and tropical Pacific.

Shan Zeng↗

DOE OSTI2022

Ice nucleating particle concentrations measured by the CSU-CFDC during the AGINSGP field experiment

Real-time, immersion mode ambient ice nucleating particle (INP) concentrations were measured at ARM’s Southern Great Plains (SGP) site during the AGINSGP field experiment using a continuous flow diffusion chamber (CFDC) from Colorado State University (CSU). The CSU-CFDC is an ice-thermal gradient diffusion chamber that optically detects the freezing of single aerosol particles (Rogers 1988; Rogers et al. 2001; and Eidhammer et al. 2010). The instrument was located in the guest instrument facility (GIF) and measured INP concentrations from April 8th to April 29th. Air was drawn into the GIF through custom aluminum stack inlets (6” inner diameter) attached vertically to the outer GIF wall and the GIF outside platform. A blower pulled air through the stacks at a velocity of 1 m/s. Aerosol instruments subsampled via wall ports, through either 3/8” or 1/4" copper lines, depending on sample flow of the instrument. Rogers, D. C., Development of a continuous flow thermal gradient diffusion chamber for ice nucleation studies, Atmospheric Research, 22(2), 149-181, doi:10.1016/0169-8095(88)90005-1, 1988. Rogers, D. C., P. J. DeMott, S. M. Kreidenweis and Y. Chen, A continuous flow diffusion chamber for airborne measurements of ice nuclei, J. Atmos. Oceanic Technol., 18, 725-741, doi:10.1175/1520-0426(2001)018<0725:ACFDCF>2.0.CO;2, 2001. Eidhammer, T., DeMott, P. J., Prenni, A. J., Petters, M. D., Twohy, C. H., Rogers, D. C., Stith, J., Heymsfield, A., Wang, Z., Haimov, S., French, J., Pratt, K., Prather, K., Murphy, S., Seinfeld, J., Subramanian, R., and Kreidenweis, S. M., Ice initiation by aerosol particles: Measured and predicted ice nuclei concentrations versus measured ice crystal concentrations in an orographic wave cloud, J. Atmos. Sci., 67, 2417-2436, doi:10.1175/2010JAS3266.1, 2010

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2009

Diagnosing the Ice Crystal Enhancement Factor in the Tropics

Recent modeling studies have revealed that ice crystal number concentration is one of the dominant factors in the effect of clouds on radiation. Since the ice crystal enhancement factor and ice nuclei concentration determine the concentration, they are both important in quantifying the contribution of increased ice nuclei to global warming. In this study, long-term cloud-resolving model (CRM) simulations are compared with field observations to estimate the ice crystal enhancement factor in tropical and midlatitudinal clouds, respectively. It is found that the factor in tropical clouds is ~10 3-104 times larger than that of mid-latitudinal ones, which makes physical sense because entrainment and detrainment in the Tropics are much stronger than in middle latitudes. The effect of entrainment/detrainment on the enhancement factor, especially in tropical clouds, suggests that cloud microphysical parameterizations should be coupled with subgrid turbulence parameterizations within CRMs to obtain a more accurate depiction of cloud-radiative forcing.

Zeng, Xiping↗

NASA NTRS2012

On the Ice Nucleation Spectrum

This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation is physically-based and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, surface area and composition. This is achieved by introducing the concepts of ice nucleation coefficient (the number of ice germs present in a particle) and nucleation probability dispersion function (the distribution of ice nucleation coefficients within the aerosol population). The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation the new formulation consistently describes singular and stochastic behavior within a single framework. Using a fundamentally stochastic approach, both cooling rate independence and constancy of the ice nucleation fraction over time, features typically associated with singular behavior, were reproduced. Analysis of the temporal dependency of the ice nucleation spectrum suggested that experimental methods that measure the ice nucleation fraction over few seconds would tend to underestimate the ice nuclei concentration. It is shown that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework where theoretical predictions, laboratory measurements and field campaign data can be reconciled, and that is suitable for application in atmospheric modeling studies.

Barahona, D.↗

NASA NTRS1983

Space shuttle exhaust cloud properties

A data base describing the properties of the exhaust cloud produced by the launch of the Space Transportation System and the acidic fallout observed after each of the first four launches was assembled from a series of ground and aircraft based measurements made during the launches of STS 2, 3, and 4. Additional data were obtained from ground-based measurements during firings of the 6.4 percent model of the Solid Rocket Booster at the Marshall Center. Analysis indicates that the acidic fallout is produced by atomization of the deluge water spray by the rocket exhaust on the pad followed by rapid scavening of hydrogen chloride gas aluminum oxide particles from the Solid Rocket Boosters. The atomized spray is carried aloft by updrafts created by the hot exhaust and deposited down wind. Aircraft measurements in the STS-3 ground cloud showed an insignificant number of ice nuclei. Although no measurements were made in the column cloud, the possibility of inadvertent weather modification caused by the interaction of ice nuclei with natural clouds appears remote.

Anderson, B. J.↗