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Emmons, Louisa

Publications and source records attributed to Emmons, Louisa.

Reconciling Observed and Predicted Tropical Rainforest OH Concentrations

We present OH observations made in Amazonas, Brazil during the Green Ocean Amazon campaign (GoAmazon2014/5) from February to March of 2014. The average diurnal variation of OH peaked with a midday (10:00–15:00) average of 1.0 × 10 6 (±0.6 × 10 6 ) molecules cm -3 . This was substantially lower than previously reported in other tropical forest photochemical environments (2–5 × 10 6 molecules cm -3 ) while the simulated OH reactivity was lower. The observational data set was used to constrain a box model to examine how well current photochemical reaction mechanisms can simulate observed OH. We used one near-explicit mechanism (MCM v3.3.1) and four condensed mechanisms (i.e., RACM2, MOZART-T1, CB05, CB6r2) to simulate OH. A total of 14 days of analysis shows that all five chemical mechanisms were able to explain the measured OH within instrumental uncertainty of 40% during the campaign in the Amazonian rainforest environment. Future studies are required using more reliable NO x and VOC measurements to further investigate discrepancies in our understanding of the radical chemistry in the tropical rainforest.

54 ENVIRONMENTAL SCIENCES↗

Understanding and improving model representation of aerosol optical properties for a Chinese haze event measured during KORUS-AQ

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM 2.5 , often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m 2 g –1 observed average) and light-scattering enhancement factor (ƒ(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm –3 in the model vs. observed average of 1.5 g cm –3 ) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.

54 ENVIRONMENTAL SCIENCES↗

Global and Regional Radiative Forcing from 20 Reductions in BC, OC and SO4 an HTAP2 Multi-Model Study

In the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise, a range of global atmospheric general circulation and chemical transport models performed coordinated perturbation experiments with 20% reductions in emissions of anthropogenic aerosols, or aerosol precursors, in a number of source regions. Here, we compare the resulting changes in the atmospheric load and vertically resolved profiles of black carbon (BC), organic aerosols (OA) and sulfate (SO4/ from 10 models that include treatment of aerosols. We use a set of temporally, horizontally and vertically resolved profiles of aerosol forcing efficiency (AFE) to estimate the impact of emission changes in six major source regions on global radiative forcing (RF) pertaining to the direct aerosol effect, finding values between. 51.9 and 210.8mW/sq m/Tg for BC, between -2.4 and -17.9mW/sq m/Tg for OA and between -3.6 and -10.3W/sq m/Tg for SO4. In most cases, the local influence dominates, but results show that mitigations in south and east Asia have substantial impacts on the radiative budget in all investigated receptor regions, especially for BC. In Russia and the Middle East, more than 80 % of the forcing for BC and OA is due to extra-regional emission reductions. Similarly, for North America, BC emissions control in east Asia is found to be more important than domestic mitigations, which is consistent with previous findings. Comparing fully resolved RF calculations to RF estimates based on vertically averaged AFE profiles allows us to quantify the importance of vertical resolution to RF estimates. We find that locally in the source regions, a 20% emission reduction strengthens the radiative forcing associated with SO4 by 25% when including the vertical dimension, as the AFE for SO4 is strongest near the surface. Conversely, the local RF from BC weakens by 37% since BC AFE is low close to the ground. The fraction of BC direct effect forcing attributable to intercontinental transport, on the other hand, is enhanced by one-third when accounting for the vertical aspect, because long-range transport primarily leads to aerosol changes at high altitudes, where the BC AFE is strong. While the surface temperature response may vary with the altitude of aerosol change, the analysis in the present study is not extended to estimates of temperature or precipitation changes.

profiles of aerosol forcing efficiency (AFE)↗

Exploring the Production of NOx by Lightning and Its Impact on Tropospheric Ozone

Our quantitative understanding of free tropospheric (FT) chemistry is quite poor. State-of-the-art regional air quality models (e.g., US EPA's CMAQ) perform very poorly in simulating FT chemistry, with Uniform ozone around 70 ppb throughout the FT in summer, while ozonesonde data show much higher levels of ozone and much spatial-temporal structure. Such models completely neglect lightning-NOx (LNOx) emissions (the most significant source of NOx in the FT), and also contain large uncertainties in the specifications of intercontinental transport, stratosphere-troposphere exchange (STE) and PBLFT exchange (PFTE). Global air chemistry models include LNOx, but in very crude fashion, with the frequency and distribution of lightning being based on modeled cloud parameters (hence large uncertainty), lightning energetics being assumed to be constant for all flashes (literature value, while in reality there is at least a two-orders of magnitude variability from flash-to-flash), and the production of NOx in the surrounding heated air, per Joule of heating, being assumed to be constant also (literature value, while in fact it is a non-linear function of the dissipated heat and local air density, p). This situation is commonly blamed on paucity of pertinent observational data, but for the USA, there is now a wealth of surface- and satellite-based data of lightning available to permit much improved observation-based estimation of LNOx emissions. In the FT, such NOx has a long residence time, and also the ozone production efficiency from NOx there is considerably higher than in the PBL. It is, therefore, of critical importance in FT chemistry. This paper will describe the approach and data products of an ongoing NSSTC project aimed at a much-improved quantification of not only LNOx production on the scale of continental USA based on local and regional lightning observations, but also of intercontinental transport, STE and PFTE, all in upgraded simulations of tropospheric transport and chemistry. In our approach for LNOx, (a) we utilize continuous observed lightning information from the NLDN ground network and from satellite imagers (OTD and LIS) to quantify lightning frequency and distribution at the spatial-temporal scales of models such as CMAQ; (b) we develop new methodologies to quantify flash-specific lightning energy dissipation as heat (epsilon) using data from the research-grade lightning measurement facility at NASA-KSC, and to parameterize epsilon based on regional lightning monitoring data (ground- and satellite-based); and, (c) we develop a new parameterization of NOx production as a function of epsilon and rho. Based on such observation-based information, we are working to develop a gridded, episodic LNOx emissions inventory for the USA for use in models like CMAQ. We are also developing approaches for global(MOZART)- regional(CMAQ) chemistry coupling to improve intercontinental transport and STE. Finally, we are developing new methodologies for assimilation of satellite-observed (GOES) clouds into meteorological modeling (MM5), to improve PFTE and to optimize co-location of cloud convection and observed lightning. We will incorporate these improvements in CMAQ simulations over the USA to better understand FT processes and chemistry, and its impact on ground-level ozone.

Gillani, Noor↗

Transport and Chemical Evolution over the Pacific (TRACE-P)Aircraft Mission: Design, Execution, and First Results

The NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission was conducted in February-April 2001 over the NW Pacific (1) to characterize the Asian chemical outflow and relate it quantitatively to its sources and (2) to determine its chemical evolution. It used two aircraft, a DC-8 and a P-3B, operating out of Hong Kong and Yokota Air Force Base (near Tokyo), with secondary sites in Hawaii, Wake Island, Guam, Okinawa, and Midway. The aircraft carried instrumentation for measurements of long-lived greenhouse gases, ozone and its precursors, aerosols and their precursors, related species, and chemical tracers. Five chemical transport models (CTMs) were used for chemical forecasting. Customized bottom-up emission inventories for East Asia were generated prior to the mission to support chemical forecasting and to serve as a priori for evaluation with the aircraft data. Validation flights were conducted for the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument and revealed little bias (6 plus or minus 2%) in the MOPITT measurements of CO columns. A major event of transpacific Asian pollution was characterized through combined analysis of TRACE-P and MOPITT data. The TRACE-P observations showed that cold fronts sweeping across East Asia and the associated warm conveyor belts (WCBs) are the dominant pathway for Asian outflow to the Pacific in spring. The WCBs lift both anthropogenic and biomass burning (SE Asia) effluents to the free troposphere, resulting in complex chemical signatures. The TRACE-P data are in general consistent with a priori emission inventories, lending confidence in our ability to quantify Asian emissions from socioeconomic data and emission factors. However, the residential combustion source in rural China was found to be much larger than the a priori, and there were also unexplained chemical enhancements (HCN, CH3Cl, OCS, alkylnitrates) in Chinese urban plumes. The Asian source of CCl4 was found to be much higher than government estimates. Measurements of HCN and CH3CN indicated a dominant biomass burning source and ocean sink for both gases. Large fractions of sulfate and nitrate were found to be present in dust aerosols. Photochemical activity in the Asian outflow was strongly reduced by aerosol attenuation of UV radiation, with major implications for the concentrations of HOx, radicals. New particle formation, apparently from ternary nucleation involving NH3, was observed in Chinese urban plumes.

Jacob, Daniel J.↗

Data archive for NO(y) from observations and construction and testing of airborne instrument for simultaneous measurement of NO, NO2, NO(y), and O3

The compilation and archiving of NO(x) and NO(y) measurements began in mid-March 1994. Since the submission of the first report, data summaries have been obtained for the TROPOZ 2, STRATOZ 3, OCTA and TOR/Schauinsland campaigns, and the full data sets will become a part of this archive in the near future. Climatologies of NO(x) and NO(y) have been developed from these and previously archived data sets, including the available GTE campaigns (ABLE-2A, B, -3A, B, CITE-2, -3, TRACE-A, PEM WEST-A) and AASE 1 and 2. The data have been grouped by season and altitude (boundary layer and 3 km ranges in the free troposphere). Maps showing median values of midday NO, NO(x) and NO(y) have been produced for each season for the boundary layer and 3 km ranges of the free troposphere. The statistics of the data (median, mean, and standard deviation, central 67% and 90%) have also been determined, and are shown in representative figures included in this report.

Carroll, Mary Anne↗

Procedure for computer-controlled milling of accurate surfaces of revolution for millimeter and far-infrared mirrors

A simple method for milling accurate off-axis parabolic mirrors with a computer-controlled milling machine is discussed. For machines with a built-in circle-cutting routine, an exact paraboloid can be milled with few computer commands and without the use of the spherical or linear approximations. The proposed method can be adapted easily to cut off-axis sections of elliptical or spherical mirrors.

Emmons, Louisa↗