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DOE OSTI2025

An Improved Convection Parameterization with Detailed Aerosol–Cloud Microphysics for a Global Model

Abstract A new microphysical treatment that includes aerosol–cloud interactions and secondary ice production (SIP) mechanisms is implemented in the convection scheme of the Community Atmosphere Model, version 6 (CAM6). The approach is to embed a 1D Lagrangian parcel model in the bulk convective plume of the existing deep convection parameterization. Aerosol activation, growth processes including collision/coalescence, and three processes of SIP mechanisms, two of which are normally overlooked in atmospheric models, are represented in this embedded parcel model. These microphysical processes are treated with a hybrid bin/bulk scheme and a high spatial and temporal resolution for the integration of the embedded parcel in 1D, allowing vertical velocity to determine the microphysical evolution following the in-cloud motion during ascent. Simulations of an observed case (Midlatitude Continental Convective Clouds Experiment) of a mesoscale convective system in Oklahoma, United States, with a single-column model (SCAM) version of CAM, are compared with aircraft in situ and ground-based observations of microphysical properties from the convection and precipitation. Results from the validation show the new microphysical scheme has a good representation of the ice initiation in the bulk convective plume, including the known and empirically quantified pathways of primary and secondary initiation, with benefits for the accuracy of properties of its supercooled cloud liquid. The sensitivity simulations and use of tagging tracers for the validated simulation confirm that the newly included SIP mechanisms are of paramount importance for convective microphysics and can be successfully treated in the global model.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2020

Historical (1850‐2014) Aerosol Evolution and Role on Climate Forcing Using the GISS Modele2.1 Contribution to CMIP6

The Earth’s climate is rapidly changing. Over the past centuries, aerosols, via their ability to absorb or scatter solar radiation and alter clouds, played an important role in counterbalancing some of the greenhouse gas (GHG) caused global warming. The multi-century anthropogenic aerosol cooling effect prevented present-day climate from reaching even higher surface air temperatures and subsequent more dramatic climate impacts. Trends in aerosol concentrations and optical depth show that in many polluted regions such as Europe and the United States of America, aerosol precursor emissions decreased back to levels of the 1950s. More recent polluting countries such as China may have reached a turning point in recent years as well, while India still follows an upward trend. Here we study aerosol trends in the CMIP6 simulations of the GISS ModelE2.1 climate model using a fully coupled atmosphere composition onfiguration, including interactive gas-phase chemistry, and either an aerosol microphysical (MATRIX) or a mass-based (OMA) aerosol module. Results show that whether global aerosol radiative forcing is already declining depends on the aerosol scheme used. Using the aerosol microphysical scheme, where the aerosol system reacts more strongly to the trend in sulfur dioxide (SO2) emissions, global peak direct aerosol forcing was reached in the 1980’s, whereas the mass-based scheme simulates peak direct aerosol forcing around 2010.

Aerosol forcing↗

NASA NTRSDate not supplied

Using PACE Aerosol Optical and Microphysical Properties to Capture Aerosol Composition

Improvements in air quality and Earth’s climate predictions can only be achieved through improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (e.g., clean marine, dust, polluted continental). We investigate the relative skill of various combinations of aerosol optical properties used as tools to define air mass aerosol types and how much these optical properties can capture dominant aerosol speciation.

Meloe Shenandoah Kacenelenbogen↗

DOE OSTI2021

Novel estimation of aerosol processes with particle size distribution measurements: a case study with the TOMAS algorithm v1.0.0

Atmospheric aerosol microphysical processes are a significant source of uncertainty in predicting climate change. Specifically, aerosol nucleation, emissions, and growth rates, which are simulated in chemical transport models to predict the particle size distribution, are not understood well. However, long-term size distribution measurements made at several ground-based sites across Europe implicitly contain information about the processes that created those size distributions. This work aims to extract that information by developing and applying an inverse technique to constrain aerosol emissions as well as nucleation and growth rates based on hourly size distribution measurements. We developed an inverse method based upon process control theory into an online estimation technique to scale aerosol nucleation, emissions, and growth so that the model–measurement bias in three measured aerosol properties exponentially decays. The properties, which are calculated from the measured and predicted size distributions, used to constrain aerosol nucleation, emission, and growth rates are the number of particles with a diameter between 3 and 6 nm, the number with a diameter greater than 10 nm, and the total dry volume of aerosol ( N 3–6 , N 10 , V dry ), respectively. In this paper, we focus on developing and applying the estimation methodology in a zero-dimensional “box” model as a proof of concept before applying it to a three-dimensional simulation in subsequent work. The methodology is first tested on a dataset of synthetic and perfect measurements that span diverse environments in which the true particle emissions, growth, and nucleation rates are known. The inverse technique accurately estimates the aerosol microphysical process rates with an average and maximum error of 2 % and 13 %, respectively. Next, we investigate the effect that measurement noise has on the estimated rates. The method is robust to typical instrument noise in the aerosol properties as there is a negligible increase in the bias of the estimated process rates. Finally, the methodology is applied to long-term datasets of in situ size distribution measurements in western Europe from May 2006 through June 2007. At Melpitz, Germany, and Hyytiälä, Finland, the average diurnal profiles of estimated 3 nm particle formation rates are reasonable, having peaks near noon local time with average peak values of 1 and 0.15 cm –3 s –1 , respectively. The normalized absolute error in estimated N 3–6 , N 10 , and V dry at three European measurement sites is less than 15 %, showing that the estimation framework developed here has potential to decrease model–measurement bias while constraining uncertain aerosol microphysical processes.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2016

Role of Atmospheric Chemistry in the Climate Impacts of Stratospheric Volcanic Injections

The climate impact of a volcanic eruption is known to be dependent on the size, location and timing of the eruption. However, the chemistry and composition of the volcanic plume also control its impact on climate. It is not just sulfur dioxide gas, but also the coincident emissions of water, halogens and ash that influence the radiative and climate forcing of an eruption. Improvements in the capability of models to capture aerosol microphysics, and the inclusion of chemistry and aerosol microphysics modules in Earth system models, allow us to evaluate the interaction of composition and chemistry within volcanic plumes in a new way. These modeling efforts also illustrate the role of water vapor in controlling the chemical evolution, and hence climate impacts, of the plume. A growing realization of the importance of the chemical composition of volcanic plumes is leading to a more sophisticated and realistic representation of volcanic forcing in climate simulations, which in turn aids in reconciling simulations and proxy reconstructions of the climate impacts of past volcanic eruptions. More sophisticated simulations are expected to help, eventually, with predictions of the impact on the Earth system of any future large volcanic eruptions.

Disrupting↗

NASA NTRSDate not supplied

Simulating Sulfate Aerosol Size in the Hunga Tonga Plume: Comparisons with Observations

Using the NASA GEOS Chemistry Climate Model (CCM) coupled to a detailed sectional aerosol microphysical model, we have simulated the January 2022 Hunga Tonga-Hunga Ha’apai (HTHH) plume. We have developed a version of the Global Modeling Initiative (GMI) chemistry mechanism to include the requisite sulfur chemistry and coupled it to the Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics within the GEOS CCM. Our simulations focus on the lifecycle of stratospheric sulfur injected by the eruption–from the oxidation of the injected sulfur dioxide to the nucleation, growth, coagulation, hydration, and eventual settling of the volcanic sulfate aerosol particles. In order to constrain the simulated microphysics, we focus on comparing our model to observations with aerosol size information, namely in-situ particle counter observations and multi-wavelength satellite observations from OMPS-LP and SAGE-III. This eruption provides an interesting test case for our model; both the modeled gas-phase chemistry as well as the modeled aerosol microphysics are perturbed by the massive injection of water that accompanied the primary sulfur emissions from the eruption.

aerosols↗

NASA NTRS2014

Aerosol, Cloud and Trace Gas Observations Derived from Airborne Hyperspectral Radiance and Direct Beam Measurements in Recent Field Campaigns

The AERONET (AErosol RObotic NETwork) ground-based suite of sunphotometers provides measurements of spectral aerosol optical depth (AOD), precipitable water and spectral sky radiance, which can be inverted to retrieve aerosol microphysical properties that are critical to assessments of aerosol-climate interactions. Because of data quality criteria and sampling constraints, there are significant limitations to the temporal and spatial coverage of AERONET data and their representativeness for global aerosol conditions. The 4STAR (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research) instrument, jointly developed by NASA Ames and PNNL with NASA Goddard collaboration, combines airborne sun tracking and AERONET-like sky scanning with spectroscopic detection. Being an airborne instrument, 4STAR has the potential to fill gaps in the AERONET data set. Dunagan et al. [2013] present results establishing the performance of the instrument, along with calibration, engineering flight test, and preliminary scientific field data. The 4STAR instrument operated successfully in the SEAC4RS [Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys] experiment in Aug./Sep. 2013 aboard the NASA DC-8 and in the DoE [Department of Energy]-sponsored TCAP [Two Column Aerosol Project, July 2012 & Feb. 2013] experiment aboard the DoE G-1 aircraft (Shinozuka et al., 2013), and acquired a wealth of data in support of mission objectives on all SEAC4RS and TCAP research flights. 4STAR provided direct beam measurements of hyperspectral AOD, columnar trace gas retrievals (H2O, O3, NO2; Segal-Rosenheimer et al., 2014), and the first ever airborne hyperspectral sky radiance scans, which can be inverted to yield the same products as AERONET ground-based observations. In addition, 4STAR measured zenith radiances underneath cloud decks for retrievals of cloud optical depth and effective diameter. In this presentation, we provide an overview of the new 4STAR capabilities for airborne field campaigns, with an emphasis on comparisons between 4STAR and AERONET sky radiances, and retrievals of aerosol microphysical properties based on sky radiance measurements, column trace gas amounts from spectral direct beam measurements and cloud property retrievals from zenith mode observations for a few select case studies in the SEAC4RS and TCAP experiments. We summarize the aerosol, trace gas, cloud and airmass characterization studies made possible by the combined 4STAR direct beam, and sky/zenith radiance observations.

Aerosol-Climate↗

NASA NTRS2018

Can Semi-Volatile Organic Aerosols Lead to Fewer Cloud Particles?

The impact of condensing organic aerosols on activated cloud number concentration is examined in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework coupled with the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. By including the condensation of organic aerosols, the new model produces less activated particles compared to the original model, which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly tested via a suite of Monte-Carlo simulations. Results show that by considering semi-volatile organics in MATRIX-VBS, there is lower activated particle number concentration, except in cases with low cloud updrafts, in clean environment at above freezing temperatures, and in polluted environments at high temperature (310K) and extremely low humidity conditions.

Gao, Chloe Y.↗

NASA NTRS2014

Aerosol Properties Derived from Airborne Sky Radiance and Direct Beam Measurements in Recent NASA and DoE Field Campaigns

The AERONET (AErosol RObotic NETwork) ground-based suite of sunphotometers provides measurements of spectral aerosol optical depth (AOD), precipitable water and spectral sky radiance, which can be inverted to retrieve aerosol microphysical properties that are critical to assessments of aerosol-climate interactions. Because of data quality criteria and sampling constraints, there are significant limitations to the temporal and spatial coverage of AERONET data and their representativeness for global aerosol conditions.The 4STAR (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research) instrument, jointly developed by NASA Ames and PNNL (Pacific Northwest National Laboratory) with NASA Goddard collaboration, combines airborne sun tracking and AERONET-like sky scanning with spectroscopic detection. Being an airborne instrument, 4STAR has the potential to fill gaps in the AERONET data set. The 4STAR instrument operated successfully in the SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys) experiment in Aug./Sep. 2013 aboard the NASA DC-8 and in the DoE (Department of Energy)-sponsored TCAP (Two Column Aerosol Project, July 2012 & Feb. 2013) experiment aboard the DoE G-1 aircraft. 4STAR provided direct beam measurements of hyperspectral AOD, columnar trace gas retrievals (H2O, O3, NO2), and the first ever airborne hyperspectral sky radiance scans, which can be inverted to yield the same products as AERONET ground-based observations. In this presentation, we provide an overview of the new 4STAR capabilities, with an emphasis on 26 high-quality sky radiance measurements carried out by 4STAR in SEAC4RS. We compare collocated 4STAR and AERONET sky radiances, as well as their retrievals of aerosol microphysical properties for a subset of the available case studies. We summarize the particle property and air-mass characterization studies made possible by the combined 4STAR direct beam and sky radiance observations.

DoE↗

DOE OSTI2024

Validating a microphysical prognostic stratospheric aerosol implementation in E3SMv2 using observations after the Mount Pinatubo eruption

Abstract. This paper describes the addition of a stratospheric prognostic aerosol (SPA) capability – developed with the goal of accurately simulating sulfate aerosol formation and evolution in the stratosphere – in the Department of Energy (DOE) Energy Exascale Earth System Model, version 2 (E3SMv2). The implementation includes changes to the four-mode Modal Aerosol Module microphysics in the stratosphere to allow for larger particle growth and more accurate stratospheric aerosol lifetime following the Pinatubo eruption. E3SMv2-SPA reasonably reproduces stratospheric aerosol lifetime, burden, aerosol optical depth, and top-of-atmosphere flux when compared to remote sensing observations. E3SMv2-SPA also has close agreement with the interactive chemistry–climate model CESM2-WACCM (Community Earth System Model version 2–Whole Atmosphere Community Climate Model) – which has a more complete chemical treatment – and the observationally constrained, prescribed volcanic aerosol treatment in E3SMv2. Global stratospheric aerosol size distributions identify the nucleation and growth of sulfate aerosol from volcanically injected SO2 from both major and minor volcanic eruptions from 1991 to 1993. The modeled aerosol effective radius is consistently lower than satellite and in situ measurements (max differences of ∼ 30 %). Comparisons with in situ size distribution samples indicate that this simulated underestimation in both E3SMv2-SPA and CESM2-WACCM is due to overly small accumulation and coarse-mode aerosols 6–18 months post-eruption, with E3SMv2-SPA simulating ∼ 50 % of the coarse-mode geometric mean diameters of observations 11 months post-eruption. Effective radii from the models and observations are used to calculate offline scattering and absorption efficiencies to explore the implications of smaller simulated aerosol size for the Pinatubo climate impacts. Scattering efficiencies at wavelengths of peak solar irradiance (∼ 0.5 µm) are 10 %–80 % higher for daily samples in models relative to observations through 1993, suggesting higher diffuse radiation at the surface and a larger cooling effect in the models due to the smaller simulated aerosol; absorption efficiencies at the peak wavelengths of outgoing terrestrial radiation (∼ 10 µm) are 15 %–40 % lower for daily samples in models relative to observations, suggesting an underestimation in stratospheric heating in the models due to the smaller simulated aerosol. These potential biases are based on aerosol size alone and do not take into account differences in the aerosol number. The overall agreement of E3SMv2-SPA with observations and its similar performance to the well-validated CESM2-WACCM makes E3SMv2-SPA a viable alternative to simulating climate impacts from stratospheric sulfate aerosols.

Brown, Hunter York (ORCID:0000000218147874)↗

NASA NTRS2012

Aerosol Direct, Indirect, Semidirect, and Surface Albedo Effects from Sector Contributions Based on the IPCC AR5 Emissions for Preindustrial and Present-day Conditions

The anthropogenic increase in aerosol concentrations since preindustrial times and its net cooling effect on the atmosphere is thought to mask some of the greenhouse gas-induced warming. Although the overall effect of aerosols on solar radiation and clouds is most certainly negative, some individual forcing agents and feedbacks have positive forcing effects. Recent studies have tried to identify some of those positive forcing agents and their individual emission sectors, with the hope that mitigation policies could be developed to target those emitters. Understanding the net effect of multisource emitting sectors and the involved cloud feedbacks is very challenging, and this paper will clarify forcing and feedback effects by separating direct, indirect, semidirect and surface albedo effects due to aerosols. To this end, we apply the Goddard Institute for Space Studies climate model including detailed aerosol microphysics to examine aerosol impacts on climate by isolating single emission sector contributions as given by the Coupled Model Intercomparison Project Phase 5 (CMIP5) emission data sets developed for Intergovernmental Panel on Climate Change (IPCC) AR5. For the modeled past 150 years, using the climate model and emissions from preindustrial times to present-day, the total global annual mean aerosol radiative forcing is -0.6 W/m(exp 2), with the largest contribution from the direct effect (-0.5 W/m(exp 2)). Aerosol-induced changes on cloud cover often depends on cloud type and geographical region. The indirect (includes only the cloud albedo effect with -0.17 W/m(exp 2)) and semidirect effects (-0.10 W/m(exp 2)) can be isolated on a regional scale, and they often have opposing forcing effects, leading to overall small forcing effects on a global scale. Although the surface albedo effects from aerosols are small (0.016 W/m(exp 2)), triggered feedbacks on top of the atmosphere (TOA) radiative forcing can be 10 times larger. Our results point out that each emission sector has varying impacts by geographical region. For example, the single sector most responsible for a net positive radiative forcing is the transportation sector in the United States, agricultural burning and transportation in Europe, and the domestic emission sector in Asia. These sectors are attractive mitigation targets.

Bauer, Susanne E.↗

DOE OSTI2021

The Shortwave Spectral Radiometer for Atmospheric Science: Capabilities and Applications from the ARM User Facility

Industry advances have greatly reduced the cost and size of ground-based shortwave (SW) sensors for the ultraviolet, visible, and near-infrared spectral ranges that make up the solar spectrum, while simultaneously increasing their ruggedness, reliability, and calibration accuracy needed for outdoor operation. These sensors and collocated meteorological equipment are an important part of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility, which has supported parallel integrated measurements of atmospheric and surface properties for more than two decades at fixed and mobile sites around the world. The versatile capability of these ground-based measurements includes 1) rich spectral information required for retrieving cloud and aerosol microphysical properties, such as cloud phase, cloud particle size, and aerosol size distributions, and 2) high temporal resolution needed for capturing fast evolution of cloud microphysical properties in response to rapid changes in meteorological conditions. Here we describe examples of how ARM's spectral radiation measurements are being used to improve understanding of the complex processes governing microphysical, optical, and radiative properties of clouds and aerosol.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2019

SPEX Airborne Spectropolarimeter Calibration and Performance

To improve our understanding of the complex role of aerosols in the climate system and on air quality, measurements are needed of optical and microphysical aerosol. From many studies, it has become evident that a satellite-based multiangle, multiwavelength polarimeter will be essential to provide such measurements. Here, high accuracy (∼0.003) on the degree of linear polarization (DoLP) measurements is important to retrieve aerosol properties with an accuracy needed to advance our understanding of the aerosol effect on climate. SPEX airborne, a multiangle hyperspectral polarimeter, has been developed for observing and characterizing aerosols from NASA’s high-altitude research aircraft ER-2. It delivers measurements of radiance and DoLP at visual wavelengths with a spectral resolution of 3 and 7–30 nm, respectively, for radiance and polarization, at nine fixed equidistant viewing angles from −56° to +56° oriented along the ground track, and a swath of 7° oriented across-track. SPEX airborne uses spectral polarization modulation to determine the state of linear polarization of scattered sunlight. This technique has been developed in the Netherlands and has been demonstrated with ground-based instruments. SPEX airborne serves as a demonstrator for a family of space-based SPEX instruments that have the ability to measure and characterize atmospheric aerosol by multiangle hyperspectral polarimetric imaging remotely from a satellite platform. SPEX airborne was calibrated radiometrically and polarimetrically using Jet Propulsion Laboratory (JPL) facilities including the Polarization Stage Generator-2 (PSG-2), which is designed for polarimetric calibration and validation of the Airborne Multiangle SpectroPolarimetric Imager (AirMSPI). Using the PSG-2, the accuracy of the SPEX airborne DoLP measurements in the laboratory setup is found to be 0.002–0.004. Radiometric calibration is realized with an estimated accuracy of 4%. In 2017, SPEX airborne took part in the “Aerosol Characterization from Polarimeters and Lidar” campaign on the ER-2 that included four polarimeters and two lidars. Polarization measurements of SPEX airborne and the coflying Research Scanning Polarimeter (RSP), recorded during the campaign, were compared and display root-mean-square (RMS) differences ranging from 0.004 (at 555 nm) up to 0.02 (at 410 nm). For radiance measurements, excellent agreement between SPEX airborne and RSP is obtained with an RMS difference of ∼4%. The lab- and flight-performance values for polarization are similar to those recently published for AirMSPI, where also an intercomparison with RSP was made using data from field campaigns in 2013. The intercomparison of radiometric and polarimetric data both display negligible bias. The in-flight comparison results provide verification of SPEX airborne’s capability to deliver high-quality data.

Aerosols↗

NASA NTRSDate not supplied

TPSAS-NF1676L-34796-DND

The recently completed 2015-2017 EVS-2 mission NAAMES (The North Atlantic Aerosols and Marine Ecosystems Study) provides a unique set of airborne remote sensing and ship-based in situ measurements in a remote and under-sampled region of the Earth?s ocean. The NASA SABOR (Ship-Aircraft Bio-Optical Research) campaign was conducted during the summer of 2014, also in the Atlantic Ocean, out of the Chesapeake Bay and in the eastern coastal region of the United States. For both campaigns, the NASA GISS Research Scanning Polarimeter, a multi-angle, multi-spectral polarimeter measured the upwelling polarized radiances from aircraft. And for both campaigns, ship-based in situ measurements of the ocean were collected jointly with the aircraft measurements. We present results from the new RSP-MAPP (1) that is based on optimal estimation and that can retrieve simultaneous aerosol microphysical properties (including effective radius, single-scattering albedo, and real refractive index) and ocean color products using accurate radiative transfer, Mie calculations, and the DP (Detritus Plankton) series of accurate, numerically efficient ocean bio-optical models. The RSP-MAPP algorithm was applied to data collected during SABOR and NAAMES to retrieve aerosol microphysics and ocean products for all Aerosols-Above-Ocean (AAO) scenes. The RSP-MAPP products are compared against i) collocated aerosol extinction and backscatter profiles collected by the NASA LaRC airborne High Spectral Resolution Lidar (HSRL-1), including lidar depth profiles of the ocean diffuse attenuation coefficient and the hemispherical backscatter coefficient, and ii) collocated ship-based in situ measurements of the ocean.

Snorre Stamnes↗

NASA NTRS1989

Self-limiting physical and chemical effects in volcanic eruption clouds

One-dimensional aerosol microphysical and photochemical models are used to study the chemistry of stratospheric volcanic clouds. The results indicate that the aerosol microphysical processes of condensation and coagulation produce larger particles as the SO2 injection rate is increased. Larger particles have a smaller optical depth per unit mass and settle out of the stratosphere at a faster rate than smaller ones, restricting the total number of particles in the stratosphere. The microphysical processes moderate the impact of volcanic clouds on the earth's radiation budget and climate, suggesting that volcanic effects may be self limiting. It is noted that the injection of HCl into the stratosphere, which could lead to large ozone changes, is limited by a cold trap effect in which HCl and water vapor condense on ash particles in the rising volcanic plume and fall out as ice.

Pinto, Joseph P.↗

DOE OSTI2022

Theory of In-Cloud Activation of Aerosols and Microphysical Quasi-Equilibrium in a Deep Updraft

The microphysical quasi-equilibrium in an ascending adiabatic parcel is elucidated by an analytical theory in 0D with drastic simplifications. The theory predicts how in-cloud activation is most likely to be triggered by the onset of precipitation during sufficient ascent, with the ascent only needing to approach almost twice the cloud-base updraft speed aloft. The precipitation and cloud condensate mass fields are coupled in a closed system in a simplified version of the model. The initial state of no precipitation is unstable with respect to a perturbation. In the 2D phase space of both mass fields, there is a neutral line. Unstable growth of precipitation mass drives the system to cross the line into a regime of stability. An attractor is then approached consisting of precipitation mass balanced by accretion of cloud mass and fallout. The cloud-particle number concentration also approaches a stable equilibrium governed by the balance between in-cloud activation aloft from the inexorably increasing supersaturation during vertical acceleration and accretion of cloud droplets by precipitation. Dimensionless numbers characterizing the microphysical equilibria and their stability are derived mathematically, including a condensation–precipitation efficiency and an in-cloud activation efficiency. The theory explains common observations of the orders of magnitude of liquid water content in convective and stratiform clouds. Finally, sensitivity tests of the numerically integrated theoretical equations are documented with respect to variations in cloud condensation nucleus (CCN) aerosols and updraft speed. In conclusion, it is shown that this theory of in-cloud activation, with an increasing supersaturation during ascent, applies to both ice-only and liquid-only cloud.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2003

Remote Sensing of Aerosol Optical and Microphysical Properties using Polarization and Lidar Techniques

Tropospheric aerosols cause a substantial forcing of the terrestrial climate, but the magnitude of this forcing remains largely unknown. This explains the significant interest of the climate community to the prospect of measuring key aerosol properties from space using advanced remote sensing techniques. It has been known for a long time that polarization of the scattered light is much more sensitive to the aerosol microphysics than the scattered intensity. It is, therefore, not surprising that the most recent addition to the New Polar Orbiting Operational Environmental Satellite System (NPOESS) payload is the so-called Aerosol Polarimetry Sensor (APS). The main objective of this instrument is to measure the aerosol and cloud properties with accuracy and coverage sufficient for a reliable estimate of the direct and indirect aerosol forcings of climate. Accordingly, the first part of this lecture course will focus on describing the basic concept of the APS, the physical principles of polarization data analyses, and the results already obtained with an aircraft version of the APS. Polar stratospheric clouds (PSCs) represent another poorly understood aerosol component of the terrestrial atmosphere which affects the climate by supporting chemical reactions destroying the ozone layer. The high altitude of the PSCs and their predominant occurrence in high latitude and polar regions make it very difficult to study PSCs using conventional in situ techniques. Most of the information that we have about this type of clouds has been gathered using ground-based polarization lidars. The second part of the course will focus on explaining the physical principles of the polarization lidar technique and describing retrievals of PSC particle microphysical characteristics by converting I multispectral lidar measurements of the backscattered intensity and depolarization.

Mishchenko, Michael↗

DOE OSTI2025

Immersion Freezing in Particle-Based Aerosol-Cloud Microphysics: A Probabilistic Perspective on Singular and Time-Dependent Models

Cloud droplets containing immersed ice-nucleating particles (INPs) may freeze at temperatures above the homogeneous freezing threshold temperature in a process referred to as immersion freezing. In modeling studies, immersion freezing is often described using either so-called “singular” or “time-dependent” parameterizations. Here, we compare both approaches and discuss them in the context of probabilistic particle-based (super-droplet) cloud microphysics modeling. First, using a box model, we contrast how both parameterizations respond to idealized ambient cooling rate profiles and quantify the impact of the polydispersity of the immersed surface spectrum on the frozen fraction evolution. Presented simulations highlight that the singular approach, constituting a time-integrated form of a more general time-dependent approach, is only accurate under a limited range of ambient cooling rates. The time-dependent approach is free from this limitation. Second, using a prescribed-flow two-dimensional cloud model, we illustrate the macroscopic differences in the evolution in time of ice particle concentrations in simulations with flow regimes relevant to ambient cloud conditions. The flow-coupled aerosol-budget-resolving simulations highlight the benefits and challenges of modeling cloud condensation nuclei activation and immersion freezing on insoluble ice nuclei with super-particle methods. The challenges stem, on the one hand, from heterogeneous ice nucleation being contingent on the presence of relatively sparse immersed INPs, and on the other hand, from the need to represent a vast population of particles with relatively few so-called super particles (each representing a multiplicity of real particles). We discuss the critical role of the sampling strategy for particle attributes, including the INP size, the freezing temperature (for singular scheme) and the multiplicity.

54 ENVIRONMENTAL SCIENCES↗