Constraining Upper Troposphere/Lower Stratosphere Aerosol Physical Processes with High-Altitude Aircraft Measurements

Interest in a more complete understanding of the sources, composition and microphysics of stratospheric aerosol particles has intensified during recent years for several reasons: (1) small volcanic eruptions have been recognized as a driver of short-term changes in climate forcing; (2) emissions of sulfur dioxide (SO2) and other aerosol precursors have shifted to south Asia and other low latitude regions with intense vertical transport; (3) organic material has been recognized as a key contributor to lower stratospheric aerosol mass; and (4) interest in possible solar radiation management (geoengineering) through significant enhancements in stratospheric aerosols has intensified. To address stratospheric aerosol science issues, we are proposing a NASA Earth Ventures mission to NASA to provide extensive high-altitude aircraft measurements of critical gas-phase and aerosol properties at multiple locations across the planet. In this presentation, we will discuss the objectives of the proposed campaign, the measurements provided, the sampling strategy, and the modeling and analysis approaches that would be used to address specific science questions

Modelling the Inorganic Bromine Partitioning in the Tropical Tropopause over the Pacific Ocean

The stratospheric inorganic bromine burden (Bry) arising from the degradation of brominated very short-lived organic substances (VSL org ), and its partitioning between reactive and reservoir species, is needed for a comprehensive assessment of the ozone depletion potential of brominated trace gases. Here we present modelled inorganic bromine abundances over the Pacific tropical tropopause based on aircraft observations of VSL org of two campaigns of the Airborne Tropical TRopopause EXperiment (ATTREX 2013 carried out over eastern Pacific and ATTREX 2014 carried out over the western Pacific) and chemistry-climate simulations (along ATTREX flight tracks) using the specific meteorology prevailing. Using the Community Atmosphere Model with Chemistry (CAM-Chem), we model that BrO and Br are the daytime dominant species. Integrated across all ATTREX flights BrO represents ~ 43 % and 48 % of daytime Bry abundance at 17 km over the Western and Eastern Pacific, respectively. The results also show zones where Br/BrO >1 depending on the solar zenith angle (SZA), ozone concentration and temperature. On the other hand, BrCl and BrONO 2 were found to be the dominant night-time species with ~ 61% and 56 % of abundance at 17 km over the Western and Eastern Pacific, respectively. The western-to-eastern differences in the partitioning of inorganic bromine are explained by different abundances of ozone (O3), nitrogen dioxide (NO2) , and total inorganic chlorine (Cly).Fil: Navarro, María A.. University of Miami; Estados UnidosFil: Saiz-lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; EspañaFil: Cuevas, Carlos Alberto. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; EspañaFil: Fernandez, Rafael Pedro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; ArgentinaFil: Atlas, Elliot. University of Miami; Estados UnidosFil: Rodriguez Lloeveras, Xavier. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; EspañaFil: Kinnison, Douglas E.. National Center For Atmospheric Research. Amospheric Chemistry División; Estados UnidosFil: Lamarque, Jean Francois. National Center For Atmospheric Research. Amospheric Chemistry División; Estados UnidosFil: Tilmes, Simone. National Center For Atmospheric Research. Amospheric Chemistry División; Estados UnidosFil: Thornberry, Troy. State University of Colorado at Boulder; Estados Unidos. Earth System Research Laboratory; Estados UnidosFil: Rollins, Andrew. State University of Colorado at Boulder; Estados Unidos. Earth System Research Laboratory; Estados UnidosFil: Elkins, James W.. Earth System Research Laboratory; Estados UnidosFil: Hintsa, Eric J.. State University of Colorado at Boulder; Estados Unidos. Earth System Research Laboratory; Estados UnidosFil: Moore, Fred L.. State University of Colorado at Boulder; Estados Unidos. Earth System Research Laboratory; Estados Unido

Photochemical production of nitrous acid on glass sample manifold surface

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/94760/1/grl15858.pd

Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

We report measurements of CH4 (measured in situ by the Harvard University Picarro Cavity Ringdown Spectrometer (HUPCRS) and NOAA Unmanned Aircraft System Chromatograph for Atmospheric Trace Species (UCATS) instruments), O3 (measured in situ by the NOAA dual-beam ultraviolet (UV) photometer), NO2, BrO (remotely detected by spectroscopic UV-visible (UV-vis) limb observations; see the companion paper of Stutz et al., 2016), and of some key brominated source gases in whole-air samples of the Global Hawk Whole Air Sampler (GWAS) instrument within the subtropical lowermost stratosphere (LS) and the tropical upper troposphere (UT) and tropopause layer (TTL). The measurements were performed within the framework of the NASA-ATTREX (National Aeronautics and Space Administration - Airborne Tropical Tropopause Experiment) project from aboard the Global Hawk (GH) during six deployments over the eastern Pacific in early 2013. These measurements are compared with TOMCAT/SLIMCAT (Toulouse Off-line Model of Chemistry And Transport/Single Layer Isentropic Model of Chemistry And Transport) 3-D model simulations, aiming at improvements of our understanding of the bromine budget and photochemistry in the LS, UT, and TTL.Changes in local O3 (and NO2 and BrO) due to transport processes are separated from photochemical processes in intercomparisons of measured and modeled CH4 and O3. After excellent agreement is achieved among measured and simulated CH4 and O3, measured and modeled [NO2] are found to closely agree with ≤ 15ppt in the TTL (which is the detection limit) and within a typical range of 70 to 170ppt in the subtropical LS during the daytime. Measured [BrO] ranges between 3 and 9ppt in the subtropical LS. In the TTL, [BrO] reaches 0.5±0.5ppt at the bottom (150hPa/355K/14km) and up to about 5ppt at the top (70hPa/425K/18.5km; see Fueglistaler et al., 2009 for the definition of the TTL used), in overall good agreement with the model simulations. Depending on the photochemical regime, the TOMCAT/SLIMCAT simulations tend to slightly underpredict measured BrO for large BrO concentrations, i.e., in the upper TTL and LS. The measured BrO and modeled BrO/Bryinorg ratio is further used to calculate inorganic bromine, Bryinorg. For the TTL (i.e., when [CH4] ≥ 1790ppb), [Bryinorg] is found to increase from a mean of 2.63±1.04ppt for potential temperatures (θ) in the range of 350-360K to 5.11±1.57ppt for θ = 390 - 400 K, whereas in the subtropical LS (i.e., when [CH4] ≤ 1790ppb), it reaches 7.66±2.95ppt for θ in the range of 390-400K. Finally, for the eastern Pacific (170-90[deg]W), the TOMCAT/SLIMCAT simulations indicate a net loss of ozone of -0.3ppbvday-1 at the base of the TTL (θ = 355K) and a net production of +1.8ppbvday-1 in the upper part (θ = 383K)

AIITS: Preliminary light scattering data from Tropical Tropopause Layer cirrus

The new optical particle spectrometer AIITS (Aerosol Ice Interface Transition Spectrometer) is the next instrument in the Small Ice Detector (SID) family. Like SID3, it acquires two-dimensional forward scattering patterns from particles in the size range from about one to a few hundred micrometers (depending on variable settings). The patterns allow quantifying the phase, habit and fine surface features of large aerosol and ice crystals, which are frequently too small to be adequately characterised using traditional imaging techniques.Two 2D-forward scattering patterns are recorded per particle using two high-resolution cameras. The cameras fire simultaneously, recording the scattering pattern via a beamsplitter. AIITS can be configured such that the cameras measure either perpendicular polarisations (i.e. P-polarisation with one camera, S-polarisation with the other) or to have a different gain setting on each camera to encompass a larger dynamic range. The incident beam can be either circularly or linearly polarised. Backscatter depolarisation is also measured. The camera and beam configuration must be selected pre-flight.The probe was deployed on board the NASA Global Hawk aircraft during a recent ATTREX/CAST campaign over the tropical eastern Pacific. We present preliminary results from a case study from the 5th of March 2015 which showed the existence of a variety of particles, including rough surfaced ice crystals, some regular, hexagonal ones, as well as particles with smooth, curved surfaces (but not spherical). We compare AIITS data with co-located particle imaging from the SPEC Hawkeye probe.The Hawkeye probe combines a 2D-Stereo optical array probe, a Cloud Particle Imager (CPI), and a Fast Cloud Droplet Probe (FCDP) to provide high resolution images (2.3 micron pixel resolution) and particle size distributions of concentration, area, and mass for particles with diameter between one micron and a few centimeters.The TTL is known to be of importance due to the presence of subvisual cirrus, which contributes to net climate radiative feedback. Knowledge of the processes involved in the creation and persistence of such clouds is limited due to sparse observational data.Non peer reviewe

Variability of Ice Supersaturation, Nucleation, and Cirrus in TTL Vertical Layers

No abstract availabl

Physical Processes Controlling the Spatial Distributions of Relative Humidity in the Tropical Tropopause Layer over the Pacific

The spatial distribution of relative humidity with respect to ice (RHI) in the boreal wintertime tropical tropopause layer (TTL, is asymptotically Equal to 14-18 km) over the Pacific is examined with the measurements provided by the NASA Airborne Tropical TRopopause EXperiment. We also compare the measured RHI distributions with results from a transport and microphysical model driven by meteorological analysis fields. Notable features in the distribution of RHI versus temperature and longitude include (1) the common occurrence of RHI values near ice saturation over the western Pacific in the lower to middle TTL; (2) low RHI values in the lower TTL over the central and eastern Pacific; (3) common occurrence of RHI values following a constant mixing ratio in the middle to upper TTL (temperatures between 190 and 200 K); (4) RHI values typically near ice saturation in the coldest airmasses sampled; and (5) RHI values typically near 100% across the TTL temperature range in air parcels with ozone mixing ratios less than 50 ppbv. We suggest that the typically saturated air in the lower TTL over the western Pacific is likely driven by a combination of the frequent occurrence of deep convection and the predominance of rising motion in this region. The nearly constant water vapor mixing ratios in the middle to upper TTL likely result from the combination of slow ascent (resulting in long residence times) and wave-driven temperature variability. The numerical simulations generally reproduce the observed RHI distribution features, and sensitivity tests further emphasize the strong influence of convective input and vertical motions on TTL relative humidity

Physical Processes Controlling the Distribution of Relative Humidity in the Tropical Tropopause Layer over the Pacific

The distribution of relative humidity with respect to ice (RHI) in the Boreal wintertime Tropical Tropopause Layer (TTL - about 14-19 km) over the Pacific is examined with the extensive dataset of measurements from the NASA Airborne Tropical TRopopause EXperiment (ATTREX). Multiple deployments of the Global Hawk during ATTREX provided hundreds of vertical profiles spanning the Pacific with accurate measurements of temperature, pressure, water vapor concentration, ozone concentration, and cloud properties. We also compare the measured RHI distributions with results from a transport and microphysical model driven by meteorological analysis fields. Notable features in the distribution of RHI versus temperature and longitude include (1) the common occurrence of RHI values near ice saturation over the western Pacific in the lower TTL (temperatures greater than 200 K) and in airmasses with low ozone concentrations indicating recent detrainment from deep convection; (2) low RHI values in the lower TTL over the eastern Pacific where deep convection is infrequent; (3) RHI values following a constant H2O mixing ratio in the upper TTL (temperatures below about 195 degrees Kelvin), particularly for samples with ozone mixing ratios greater than about 50-100 parts-per-billion-volume indicating mixtures of tropospheric and stratospheric air, and (4) RHI values typically near ice saturation in the coldest airmasses sampled (temperatures less than about 190 degrees Kelvin). We find that the typically saturated air in the lower TTL over the western Pacific is largely driven by the frequent occurrence of deep convection in this region. The nearly-constant water vapor mixing ratios in the upper TTL result from the combination of slow ascent (resulting in long residence times) and wave-driven temperature variability on a range of time scales (resulting in most air parcels having experienced low temperature and dehydration)

UAS Chromatograph for Atmospheric Trace Species (UCATS) – a versatile instrument for trace gas measurements on airborne platforms

UCATS (the UAS Chromatograph for Atmospheric Trace Species) was designed and built for observations of important atmospheric trace gases from unmanned aircraft systems (UAS) in the upper troposphere and lower stratosphere (UTLS). Initially it measured major chlorofluorocarbons (CFCs) and the stratospheric transport tracers nitrous oxide (N2O) and sulfur hexafluoride (SF6), using gas chromatography with electron capture detection. Compact commercial absorption spectrometers for ozone (O3) and water vapor (H2O) were added to enhance its capabilities on platforms with relatively small payloads. UCATS has since been reconfigured to measure methane (CH4), carbon monoxide (CO), and molecular hydrogen (H2) instead of CFCs and has undergone numerous upgrades to its subsystems. It has served as part of large payloads on stratospheric UAS missions to probe the tropical tropopause region and transport of air into the stratosphere; in piloted aircraft studies of greenhouse gases, transport, and chemistry in the troposphere; and in 2021 is scheduled to return to the study of stratospheric ozone and halogen compounds, one of its original goals. Each deployment brought different challenges, which were largely met or resolved. The design, capabilities, modifications, and some results from UCATS are shown and described here, including changes for future missions.Support was provided for HIPPO by NSF award no. AGS-0628452, for ATTREX by NASA Earth Venture program award no. NNA11AA55I, and for ATom by NASA award no. NNH17AE26I; additional support was provided by NASA Upper Atmosphere Research Program award no. NNH13AV69I. This work was also supported in part by the NOAA Cooperative Agreement with CIRES, NA17OAR4320101