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Global-scale distribution of ozone in the remote troposphere from ATom and HIPPO airborne field missions

Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

ATom, aircraft profiles, Atlantic pollution, ozone↗

Validation of OCO-2 and ACOS-GOSAT using HIPPO and TCCON

Consistent validation of satellite CO2 estimates is a prerequisite for using multiple satellite CO2measurements for joint flux inversion and establishing a long-term atmospheric CO2 data record. Wevalidate recent satellite observation of OCO-2 v7 and ACOS-GOSAT v7.3 using similar analysis as previouswork (Kulawik et al. (2016) and Frankenberg et al. (2106)) through comparisons to the HIAPER Pole-to-Pole Observations (HIPPO) and the Total Carbon Column Observing Network (TCCON) to estimate biasesand errors affecting the understanding of carbon cycle science. CarbonTracker RT is also compared tothe validation data, and additionally used to evaluate the mismatch between the HIPPO observationtimeframe and the OCO-2 record, which are offset by 3-7 years. Some key metrics that are validatedinclude the seasonal cycle phase and amplitude, latitudinal gradient by season, regional biases, anderrors with respect to averaging.

Kulawik, Susan S.↗

Views from the 6 Aircraft Campaigns: ACT-America, HIPPO, CONTRAIL, ATom, ORCAS, and ABoVE

This presentation describes the assimilation of airborne measurements of carbon dioxide (CO2) into the Goddard Earth Observing System (GEOS) general circulation model. The main goal is to construct observationally constrained fields of CO2 starting from the bottom of the atmosphere and extending through the entire vertical column. These fields can then be compared directly to retrievals of column CO2 (XCO2) from the Greenhouse Gases Observing Satellite (GOSAT) and the Orbiting Carbon Observatory 2 (OCO-2) by using the averaging kernel and a priori profile. This approach does not equire a direct satellite overpass, but rather an overpass of the much broader region impacted by the assimilation, which alleviates some of the jeopardy of coordinating flights with satellite tracks. Furthermore, checking if the story stays the same or if it changes when the unassimilated fields are compared to the satellite soundings allows us to separate model errors from retrieval errors. This work attempts to answer a number of questions including: What are the possible causes of systematic differences between model and satellite XCO2 over the Pacific Ocean? What is the contribution of tratospheric uncertainty to XCO2 errors? What is the impact of errors in boundary layer physics on modeled XCO2?

Weir, B.↗

High Pressure X-Ray Diffraction Studies of Nanocrystalline Materials

Experimental evidence obtained for a variety of nanocrystalline materials suggest that the crystallographic structure of a very small size particle deviates from that in the bulk crystals. In this paper we show the effect of the surface of nanocrystals on their structure by the analysis of generation and distribution of macro- and micro-strains at high pressures and their dependence on the grain size in nanocrystalline powders of Sic. We studied the structure of Sic nanocrystals by in-situ high-pressure powder diffraction technique using synchrotron and neutron sources and hydrostatic or isostatic pressure conditions. The diffraction measurements were done in HASYLAB at DESY using a Diamond Anvil Cell (DAC) in the energy dispersive geometry in the diffraction vector range up to 3.5 - 4/A and under pressures up to 50 GPa at room temperature. In-situ high pressure neutron diffraction measurements were done at LANSCE in Los Alamos National Laboratory using the HIPD and HIPPO diffractometers with the Paris-Edinburgh and TAP-98 cells, respectively, in the diffraction vector range up to 26 Examination of the response of the material to external stresses requires nonstandard methodology of the materials characterization and description. Although every diffraction pattern contains a complete information on macro- and micro-strains, a high pressure experiment can reveal only those factors which contribute to the characteristic diffraction patterns of the crystalline phases present in the sample. The elastic properties of powders with the grain size from several nm to micrometers were examined using three methodologies: (l), the analysis of positions and widths of individual Bragg reflections (used for calculating macro- and micro-strains generated during densification) [I], (2). the analysis of the dependence of the experimental apparent lattice parameter, alp, on the diffraction vector Q [2], and (3), the atomic Pair Distribution Function (PDF) technique [3]. The results of our studies show, that Sic nanocrystals have the features of two phases, each with its distinct elastic properties. and under pressures up to 8 GPa.

Palosz, B.↗

Magnitude and Seasonality of Wetland Methane Emissions from the Hudson Bay Lowlands (Canada)

The Hudson Bay Lowlands (HBL) is the second largest boreal wetland ecosystem in the world and an important natural source of global atmospheric methane. We quantify the HBL methane emissions by using the GEOS-Chem chemical transport model to simulate aircraft measurements over the HBL from the ARCTAS and pre-HIPPO campaigns in May-July 2008, together with continuous 2004-2008 surface observations at Fraserdale (southern edge of HBL) and Alert (Arctic background). The difference in methane concentrations between Fraserdale and Alert is shown to be a good indicator of HBL emissions, and implies a sharp seasonal onset of emissions in late May (consistent with the aircraft data), a peak in July-August, and a seasonal shut-off in September. The model, in which seasonal variation of emission is mainly driven by surface temperature, reproduces well the observations in summer but its seasonal shoulders are too broad. We suggest that this reflects the suppression of emissions by snow cover and greatly improve the model simulation by accounting for this effect. Our resulting best estimate for HBL methane emissions is 2.3 Tg/a, several-fold higher than previous estimates (Roulet et al., 1994; Worthy et al., 2000).

Pickett-Heaps, C. A.↗

Evaluating Global Emission Inventories of Biogenic Bromocarbons

Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs global oxidizing capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF (National Science Foundation) HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (38 %) to 0.78 (115 %) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24 %) to 1.25 (167 %) ppt. We also use aircraft observations made during the 2011 Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere (SHIVA) campaign, in the tropical western Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (Br(VSLS/y)). Our simulations show Br(VSLS/y) ranges from approximately 4.0 to 8.0 ppt depending on the inventory. We report an optimized estimate at the lower end of this range (approximately 4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.

bromocarbons↗

The Microwave Temperature Profiler (PERF)

The JPL developed Microwave Temperature Profiler (MTP) has recently participated in GloPac, HIPPO (I to V) and TORERO, and the ongoing ATTREX campaigns. The MTP is now capable of supporting the NASA Global Hawk and a new canister version supports the NCAR G-V. The primary product from the MTP is remote measurements of the atmospheric temperature at, above and below the flight path, providing for the vertical state of the atmosphere. The NCAR-MTP has demonstrated unprecedented instrument performance and calibration with plus or minus 0.2 degrees Kelvin flight level temperature error. Derived products include curtain plots, isentropes, lapse rate, cold point height and tropopause height.

airborne instruments↗

Global Carbon Monoxide Products from Combined AIRS, TES and MLS Measurements on A-Train Satellites

This study tests a novel methodology to add value to satellite data sets. This methodology, data fusion, is similar to data assimilation, except that the background modelbased field is replaced by a satellite data set, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these data sets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS-TES and AIRS-MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20-30% and above 20%, respectively) as compared with AIRS-only version 5 CO retrievals, and improved daily coverage compared with TES and MLS CO data.

combined AIRS↗

Evaluation of single-footprint AIRS CH4 Profile Retrieval Uncertainties Using Aircraft Profile Measurements

We evaluate the uncertainties of methane optimal estimation retrievals from single footprint thermal infrared observations from the Atmospheric Infrared Sounder (AIRS). These retrievals are primarily sensitive to atmospheric methane in the mid-troposphere through the lower stratosphere (~2 to ~17 km). We compare to in situ observations made from aircraft during the Hiaper Pole to Pole Observations (HIPPO), the NASA Atmospheric Tomography Mission (ATom) campaigns, and from the NOAA ESRL aircraft network, between the surface and 5-13 km, across a range of years, latitudes between 60 S to 80 N, and over land and ocean. After a global, pressure dependent bias correction, we find that the land and ocean have similar biases and that the reported observation error (combined measurement and interference errors) of ~27 ppb is consistent with the standard deviation between aircraft and individual AIRS observations. A single measurement has measurement (noise related) uncertainty of ~17 ppb, a ~20 ppb uncertainty from radiative interferences (e.g. from water, temperature, etc.), and ~ 30 ppb due to “smoothing error”, which is partially removed when making comparisons to in situ measurements or models in a way that account for this regularization. We estimate a 16 ppb validation error because the aircraft typically did not measure methane at altitudes where the AIRS measurements have some sensitivity, e.g. the stratosphere. Daily averaged AIRS measurements of at least 9 observations over spatio-temporal domains of < 1 degree and 1 hour have a standard deviation of ~17 ppb versus aircraft, likely because the observation errors from temperature and water vapor (for example) are only partly reduced through averaging. Seasonal averages can reduce this ~17 ppb uncertainty further to ~10 ppb, as determined through comparison with NOAA aircraft, likely because uncertainties related to radiative effects of temperature and water vapor can be reduced when averaged over a season.

Susan Kulawik↗

Observations of the Age of Air from the Northern Hemisphere Midlatitude Surface

Understanding and modeling the interhemispheric transport (IHT) of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. One IHT measure -- the mean age since air was last at the Northern Hemisphere (NH) midlatitude surface – represents a fundamental property of tropospheric transport that can be estimated from measurements of sulfur hexafluoride (SF6). Here we use SF6 measurements obtained from the recent NASA Atmospheric Tomography Mission (ATom) to construct observational estimates of the mean age throughout the troposphere. We compare the ATom based ages, which span all four seasons during the period 2016-2018 over both the Pacific and Atlantic Oceans, with previous in situ-based estimates obtained from the HIAPER Pole‐to‐Pole Observations (HIPPO) project, which are available only for the Pacific. In order to interpret the observed variations in mean age and their relationship with the large-scale flow we use simulations of the Goddard Earth Observing System (GEOS) general circulation model, constrained with meteorological fields derived from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), performed over the entire MERRA-2 period (including ATom). We confirm results from previous studies showing that the model ages are biased old compared to the observational estimates. However, we also show that this model bias is reduced in more recent years, which we interpret in terms of changes in the latitudinal distribution of SF6 emissions over the 2000s.

interhemispheric transport (IHT)↗