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NASA NTRS1992

Atmospheric measurements of peroxyacetyl nitrate and other organic nitrates at high latitudes - Possible sources and sinks

Measurements of PAN and other reactive nitrogen species during the NASA Arctic Boundary Layer Expedition (ABLE 3A) are described, their north-south and east-west gradients in the free troposphere are characterized, and the sources and sinks of PAN and NO(y) are assessed. Large concentrations of PAN and NO(y) are present in the Arctic/sub-Arctic troposphere of the Northern Hemisphere during the summer. Mixing ratios of PAN and a variety of other molecules are more abundant in the free troposphere compared to the boundary layer. Coincident PAN and O3 atmospheric structures suggest that phenomena that define PAN also define the corresponding O3 behavior. Model calculations, correlations between NO(y) and anthropogenic tracers, and the compositions of NO(y) itself suggest that the Arctic/sub-Arctic reactive nitrogen measured during ABLE 3A is predominantly of anthropogenic origin with a minor component from the stratosphere.

Singh, H. B.↗

NASA NTRS1999

Comparison of Model and Observed Regional Temperature Changes During the Past 40 Years

Results are presented for six simulations of the Goddard Institute for Space Studies (GISS) global atmosphere-ocean model for the years 1950 to 2099. There are two control simulations with constant 1950 atmospheric composition from different initial states, two GHG experiments with observed greenhouse gases up to 1990 and compounded .5% CO2 annual increases thereafter, and two GHG+SO4 experiments with the same varying greenhouse gases plus varying tropospheric sulfate aerosols. Surface air temperature trends in the two GHG experiments are compared between themselves and with the observed temperature record from 1960 and 1998. All comparisons show high positive spatial correlation in the northern hemisphere except in summer when the greenhouse signal is weakest. The GHG+SO4 experiments show weaker correlations. In the southern hemisphere, correlations are either weak or negative which in part are due to the model's unrealistic interannual variability of southern sea ice cover. The model results imply that temperature changes due to forcing by increased greenhouse gases have risen above the level of regional interannual temperature variability in the northern hemisphere over the past 40 years. This period is thus an important test of reliability of coupled climate models.

Russell, Gary L.↗

DOE OSTI2021

Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer

The ultra-high-sensitivity aerosol spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 min, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a differential mobility analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles cannot explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though mis-sizing due to non-sphericity cannot be ruled out. A small fraction (10 %–30 %) of the particles were undersized by 25 % to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, because particles heat to their vaporization point and shrink. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised the median particle diameter by 18 nm, from 163 to 181 nm, during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though aerodynamic particle sizer (APS) data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2013

Quantifying the Impact of BOReal Forest Fires on Tropospheric Oxidants Over the Atlantic Using Aircraft and Satellites (BORTAS) Experiment: Design, Execution, and Science Overview

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of airmasses that contain the emission products from seasonal boreal wildfires and how these airmasses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada. The planned July 2010 deployment of the ARA was postponed by 12 months because of activities related to the dispersal of material emitted by the Eyjafjallaj¨okull volcano. However, most other planned model and measurement activities, including ground-based measurements at the Dalhousie University Ground Station (DGS), enhanced ozonesonde launches, and measurements at the Pico Atmospheric Observatory in the Azores, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 included the same measurements, but included the ARA, special satellite observations and a more comprehensive measurement suite at the DGS. Integrating these data helped us to describe pyrogenic plumes from wildfires on a wide spectrum of temporal and spatial scales. We interpret these data using a range of chemistry models, from a near-explicit gas-phase chemical mechanism to regional and global models of atmospheric transport and lumped chemistry. We also present an overview of some of the new science that has originated from this project.

BORTAS↗

NASA NTRS2004

Surface-Satellite Measurements for Atmospheric Radiative Transfer (SMART)and Chemical, Optical and Microphysical Measurements of In-Situ Troposphere (COMMIT) Research Activities

The GSFC SMART consists of a suite of remote sensing instruments, including many commercially available radiometers, spectrometer, interferometer, and three in-house developed inskuments: micro-pulse lidar (MPL), scanning microwave radiometer (SMiR), and sun-sky-surface photometer (S(sup 3)). SMART cover the spectral range from UV to microwave, and passive to active remote sensing. This is to enrich the EOS-like research activities (i.e., EOS validation, innovative investigations, and long-term local environmental observations). During past years, SMART has been deployed in many NASA supported field campaigns to collocate with satellite nadir overpass for intercomparisons, and for initializing model simulations. Built on the successful experience of SMART, we are currently developing a new ground-based in-situ sampling package, COMMIT, including measurements of trace gases (CO, SO2, NOx, and O3,) concentrations, fine/coarse particle sizers and chemical composition, single- and three-wavelength nephelometers, and surface meteorological probes. COMMIT is built for seeking a relationship between surface in-situ measurements and boundary layer characteristics. This is to enrich EOS-like research on removing boundary layer signal from the entire column from space observation - to deduce the stable (less variability) free-troposphere observations. The COMMIT will try its best to link the chemical, microphysical, and optical properties of the boundary layer with radiation. The next major activities for SMART-COMMIT are scheduled for 2004-2006 in BASE-ASIA and EAST-AIRE. The expected close collaboration of BASE-ASIA with various research projects in Asia (i.e., ABC in South Asia, led by Ramanathan et al.; EAST-AIRE in East Asia, led by Li et al.; and APEX in Northeast Asia, led by Nakajima et al.) will definitely provide a better understanding of the impact of the biomass burning and air pollutants on regional-to-global climate, hydrological and carbon cycles, and tropospheric chemistry in Asia.

Tsay, Si-Chee↗

NASA NTRS1990

ETO lidar studies of cirrostratus altocumulogenitus: Another role for supercooled liquid water in cirrus cloud formation

Cirrus clouds have traditionally been viewed as cold, wispy, or stratiform ice clouds, typically displaying optical phenomena such as haloes. A composition entirely of hexagonal ice crystals, of one habit or another could only have a transitory existence in cirrus, since the concentrations of ice nuclei (IN) measured by various techniques (at the surface or in the lower troposphere) indicate an enormous number of IN that should be active at cirrus cloud temperatures. In light of recent instrumental aircraft and polarization lidar studies of cirrus clouds, it is clear that highly supercooled cloud droplets can sometimes be a component of cirrus clouds. It remains to be determined if supercooled liquid water (SLW) is present abundantly enough in cirrus to play a significant role in earth's radiance balance, or is merely a curious, infrequent occurrence. To help evaluate this issue, the UH polarization lidar FIRE Extended Time Observation (ETO) of cirrus clouds are being utilized to compile, among other parameters, a climatological record of SLW clouds associated with and within cirrus.

Sassen, Kenneth↗

NASA NTRS2008

The GEOS Chemistry Climate Model: Implications of Climate Feedbacks on Ozone Depletion and Recovery

The Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) has been developed by combining the atmospheric chemistry and transport modules developed over the years at Goddard and the GEOS general circulation model, also developed at Goddard. The first version of the model was used in the CCMVal intercomparison exercises that contributed to the 2006 WMO/UNEP Ozone Assessment. The second version incorporates the updated version of the GCM (GEOS 5) and will be used for the next round of CCMVal evaluations and the 2010 Ozone Assessment. The third version, now under development, incorporates the combined stratosphere and troposphere chemistry package developed under the Global Modeling Initiative (GMI). We will show comparison to past observations that indicate that we represent the ozone trends over the past 30 years. We will also show the basic temperature, composition, and dynamical structure of the simulations. We will further show projections into the future. We will show results from an ensemble of transient and time-slice simulations, including simulations with fixed 1960 chlorine, simulations with a best guess scenario (Al), and simulations with extremely high chlorine loadings. We will discuss planned extensions of the model to include emission-based boundary conditions for both anthropogenic and biogenic compounds.

Stolarski, Richard S.↗

NASA NTRS2013

Improved Understanding of the Modeled QBO Using MLS Observations and MERRA Reanalysis

The Quasi-Biennial Oscillation (QBO) dominates the variability of the tropical stratosphere on interannual time scales. The QBO has been shown to extend its influence into the chemical composition of this region through dynamical mechanisms. We have started our analysis using the realistic QBO internally generated by the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 33 years. We will show targeted comparisons with observations from NASAs Aura satellite Microwave Limb Sounder (MLS) and the Modern Era Retrospective-Analysis for Research and Applications (MERRA) reanalysis to provide insight into the simulation of the primary and secondary circulations associated with the QBO. Using frequency spectrum analysis and multiple linear regression we can illuminate the resulting circulations and deduce the strengths and weaknesses in their modeled representation. Inclusion of the QBO in our simulation improves the representation of the subtropical barriers and overall tropical variability. The QBO impact on tropical upwelling is important to quantify when calculating trends in sub-decadal scale datasets.

MERRA↗

NASA NTRSDate not supplied

Generating Global CH4 NASA GEOS Product by Assimilating TROPOMI

Radiative properties of methane (CH4) significantly contribute to climate change and the recent acceleration of global CH4 growth requires thorough investigation into its causes. Examination of temporal and spatial CH4 variability is crucial for better understanding the shifts that are currently taking place. Integrating different CH4 observations to create a reliable, easily to use global atmospheric CH4 product could contribute to assessment of emissions processes, but remains challenging due to the lack of long satellite data records. Here we present the NASA Goddard Earth Observing System (GEOS) based global CH4 product constrained by atmospheric transport from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) and assimilated CH4 from the TROPOspheric Monitoring Instrument (TROPOMI). This product uses the Constituent Data Assimilation System (CoDAS) component of the GEOS capability, which has been expanded and generalized to assimilate any satellite, ground-based, or in situ observation of atmospheric composition that can be expressed as a vertical sounding or point sample. The product is similar to the one generated by assimilating carbon dioxide (CO2) data into GEOS from Orbiting Carbon Observatory 2 (OCO-2): OCO-2 GEOS Level 3 daily and monthly, 0.5x0.625 assimilated CO2 V10r. The preliminary product is investigated using a variety of quality check approaches with the help of in situ observations to examine bias correction, error inflation, and performance of the assimilation system. Potential applications of this approach include support for interpretation of high-resolution point source detection approaches, climate and greenhouse gas reanalyses, and boundary conditions for regional modeling approaches.

Nikolay Balashov↗

NASA NTRSDate not supplied

Dynamical Sensitivity in Response to a Wide Range of Abrupt CO 2 Forcings

An improved understanding of dynamical variability is important for projecting future changes in extratropical weather and the interaction between the extratropical troposphere and the tropics, stratosphere, cryosphere and ocean. Despite their simplicity, the abrupt 2x- and 4xCO 2 forcing simulations from the Coupled Model Intercomparison Project (CMIP) Phase 6 DECK experiments enable a mechanistic look into the forcing and feedback response characteristics of models that can be unambiguously attributed to an increase in carbon dioxide concentrations. Thus, while typically used to evaluate the climate sensitivity in models, with a primary focus on global surface temperature change, here we focus on several measures of extratropical variability, including projected changes in the storm tracks and in stratospheric polar vortex variability. Results are primarily based on simulations produced using low- and high-top versions of the NASA Goddard Institute for Space Studies Model (ModelE) but results are also presented from the larger CMIP6 multi-model ensemble. In addition to the 2x- and 4xCO 2 simulations, we also explore the linearity of the response of extratropical dynamical variability in ModelE to varying levels of CO 2 spanning the range 1/8-8xCO 2 . In particular, we show that the expansion of the jet streams varies nonlinearly with increasing CO 2 , especially in the Northern Hemisphere, and that this can be interpreted in terms of variations in ocean heat transport. The impact of composition feedbacks on changes in variability is also discussed.

dynamical variability↗

NASA NTRSDate not supplied

TPSAS-NF1676L-11382-DND

Long-range transport of ozone precursor species and carbonaceous aerosols emitted by wildfires may affect the atmospheric composition and regional climate far away from the location of the fires. Major outbreaks of fires occurred in 3 areas of Asia, Kazakhstan, Siberia, and Thailand, during the spring of 2008. Satellite and aircraft-based observations and trajectory studies have identified the transit of the plumes from these fires across the Pacific. We have conducted simulations of the effects of these fires on the atmospheric composition using the Real-time Air Quality Modeling System (RAQMS). RAQMS is a global scale meteorological and chemical modeling system with unified (stratosphere/troposphere) chemistry module. Model results, for example, indicate that increases of 10 ppbv in upper tropospheric ozone at 180W longitude and northern mid-latitudes in April, 2008 could be attributed to these fires. Large increases in aerosol optical depth due to carbonaceous aerosols are also seen nearer the fire location. Both tropospheric ozone and carbonaceous aerosols influence the atmospheric energy balance and climate. We use an off-line radiative transfer model along with the RAQMS chemical and aerosol analyses to calculate the direct radiative forcing during April, 2008, due to Asian wildfire emissions. Arctic indirect radiative forcing due to these emissions are evaluated using RAQMS aerosol extinction analyses in conjunction with MODIS retrievals of cloud liquid water and effective radius. We will discuss the radiative forcing results and the relative influences of the different fire events.

Murali Natarajan↗

NASA NTRSDate not supplied

The Roscoe Lidar: Initial Results from the Upward and Downward Looking Airborne Lidar from the ACCLIP and SABRE Campaigns

Backscatter lidars are a staple of airborne remote sensing and are primarily used in determining the altitude, vertical structure, and optical properties of clouds and aerosols. These airborne lidars typically observe in a downward direction which is sufficient for most tropospheric objectives. With more scientific attention being directed to upper tropospheric/lower stratospheric (UTLS) aerosols and recent volcanic and phrocumulonimbus events in the news, developing lidar instruments that can observe the UTLS will be vital in better understanding their composition and optical properties and determining their role in the planet's radiative balance. To meet this need, the downward and upward looking Roscoe lidar was developed and flown on two recent field campaigns: Stratospheric Aerosol processes, Budget, and Radiative Effects (SABRE) and Asian Summer Monsoon Chemical and CLimate Impact Project (ACCLIP) (both 2022). Building on its extensive Cloud Physics Lidar (CPL) heritage, we show that Roscoe can deliver CPL-like products in both the up and down-looking directions providing an unmatched vertical view of the atmosphere from an airborne platform. Future work can leverage Roscoe's updward looking view to quantify the optical properties and extinction of UTLS aerosols.

Kenneth Christian↗

NASA NTRS1994

The sensitivity of tropospheric chemistry to cloud interactions

Clouds, although only occupying a relatively small fraction of the troposphere volume, can have a substantial impact on the chemistry of the troposphere. In newly formed clouds, or in clouds with air rapidly flowing through, the chemistry is expected to be far more active than in aged clouds with stagnant air. Thus, frequent cycling of air through shortlived clouds, i.e. cumulus clouds, is likely to be a much more efficient media for altering the composition of the atmosphere than an extensive cloud cover i.e. frontal cloud systems. The impact of clouds is tested out in a 2-D channel model encircling the globe in a latitudinal belt from 30 to 60 deg N. The model contains a detailed gas phase chemistry. In addition physiochemical interactions between the gas and aqueous phases are included. For species as H2O2, CH2O, O3, and SO2, Henry's law equilibria are assumed, whereas HNO3 and H2SO4 are regarded as completed dissolved in the aqueous phase. Absorption of HO2 and OH is assumed to be mass-transport limited. The chemistry of the aqueous phase is characterized by rapid cycling of odd hydrogen, (H2O2, HO2, and OH). O2(-) (produced through dissociation of HO2) reacting with dissolved O3 is a major source of OH in the aqueous phase. This reaction can be a significant sink for O3 in the troposphere. In the interstitial cloud air, odd hydrogen is depleted, whereas NO(x) remains in the gas phase, thus reducing ozone production due to the reaction between NO and HO2. Our calculations give markedly lower ozone levels when cloud interactions are included. This may in part explain the overpredictions of ozone levels often experienced in models neglecting cloud chemical interactions. In the present study, the existence of clouds, cloud types, and their lifetimes are modeled as pseudo random variables. Such pseudo random sequences are in reality deterministic and may, given the same starting values, be reproduced. The effects of cloud interactions on the overall chemistry of the troposphere are discussed. In particular, tests are performed to determine the sensitivity of cloud frequencies and cloud types.

Jonson, Jan E.↗

NASA NTRS2002

Theoretical Studies of Stratospheric and Tropospheric Clouds and Aerosols in Support of SOLVE

We proposed a number of theoretical efforts to support NASA's SOLVE Mission which took place in Kiruna, Sweden in the winter of 1999-2000. We proposed to serve as one of the DC-8 project scientists, to work with various instrument teams to better understand the composition of polar stratospheric clouds, and their properties, and to help understand the physical conditions which lead to cloud formation in the polar winter.

Toon, Owen B.↗

DOE OSTI2026

Evaluation of UKESM aerosol size and composition using ATom measurements indicates missing marine aerosol formation mechanisms

Atmospheric aerosols influence climate through their interactions with radiation and clouds, yet large uncertainties remain in their simulation by global models. This study evaluates the United Kingdom Earth System Model version 1.1 (UKESM1.1) using global-scale aircraft observations from the Atmospheric Tomography (ATom) mission, focusing on aerosol lifecycle processes in the remote marine atmosphere. We assess model performance in simulating aerosol precursor vapours, number size distributions, chemical composition, and environmental conditions. Several process improvements are tested, including sulfuric acid-ammonia nucleation, ammonium nitrate scheme, methanesulfonic acid condensation, and low-temperature isoprene-derived secondary organic aerosol formation. Model biases differ significantly between the upper troposphere (UT) and the marine boundary layer (MBL). In the UT, UKESM1.1 overestimates nucleation and Aitken mode particles while underestimating accumulation mode, indicating insufficient growth. In the MBL, the model overestimates primary aerosols (e.g. seasalt) and precursor gases but underestimates nucleation and Aitken mode particles, even after incorporating updated nucleation and ammonium nitrate scheme. The persistence of low aerosol number concentrations, despite overestimated precursors, suggests missing formation pathways likely involving other species such as iodine, amines, and organic vapours. These limitations result in an unbalanced cloud condensation nuclei budget that over-relies on primary emissions. Sensitivity tests reveal that model outputs are strongly influenced by dimethyl sulfide emissions and vapour condensation schemes. Our results highlight the need for future model development to prioritise mechanistic representation of currently missing aerosol sources, rather than relying on empirical tuning, to improve aerosol-climate interaction estimates.

He, Xu-Cheng [Univ. of Cambridge (United Kingdom);↗

NASA NTRS2005

SVD analysis of Aura TES spectral residuals

Singular Value Decomposition (SVD) analysis is both a powerful diagnostic tool and an effective method of noise filtering. We present the results of an SVD analysis of an ensemble of spectral residuals acquired in September 2004 from a 16-orbit Aura Tropospheric Emission Spectrometer (TES) Global Survey and compare them to alternative methods such as zonal averages. In particular, the technique highlights issues such as the orbital variation of instrument response and incompletely modeled effects of surface emissivity and atmospheric composition.

spectra↗

NASA NTRS1993

Clouds, Hazes, and the Stratospheric Methane Abundance in Neptune

Analysis of high-spatial resolution methane band and continuum imagery of Neptune's relatively homogeneous Equatorial Region yields significant constraints on (1) the stratospheric gaseous methane mixing ratio, (2) the column abundances and optical properties of stratospheric and tropospheric hydrocarbon hazes, and (3) the wavelength-dependent single-scattering albedo of the 3-bar opaque cloud.

Neptune↗

NASA NTRS2020

Applying Orbital Multi-Angle Photopolarimetric Observations to Study Properties of Aerosols in the Earth's Atmosphere: Implications of Measurements in the 1.378 µm Spectral Channel to Retrieve Microphysical Characteristics and Composition of Stratospheric Aerosols

We analyze the possibilities of orbital photopolarimetric measurements to study properties of aerosols in the Earth's atmosphere. As an example, we consider the case when such measurements are performed within a narrow spectral channel centered at 1.378 µm that allows to retrieve microphysical characteristics of stratospheric aerosols separately from those of tropospheric aerosols. We consider the case of stratospheric aerosols caused by volcanic eruption, and adopt the model of the stratosphere in the form of a homogeneous plane-parallel layer composed of polydisperse spherical particles. We use numerically exact solutions of the vector radiative transfer equation to theoretically simulate measurements carried out at various numbers of scattering angles, including: (i) radiance measurements alone; (ii) polarization measurements alone; and (iii) radiance and polarization measurements together. The results of computations show that the simultaneous use of radiance and polarization measurements at a sufficiently large number of scattering angles enables one to retrieve the optical thickness, effective radius, and refractive index of aerosols with adequate accuracy. We demonstrate how the accuracy of the derived values of the optical parameters of aerosols depends on the accuracy of measurements of the intensity and polarization of the reflected light, optical thickness of aerosol layer itself, effective radius of aerosols, width of the particle size distribution, and number of viewing angles.

Aerosols↗