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Emmons, Louisa K.

Publications and source records attributed to Emmons, Louisa K..

Quantifying the Causes of Differences in Tropospheric OH Within Global Models

The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (Tau CH4) between these models. Annual average Tau CH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in Tau CH4 (Delta Tau CH4) result from variations in chemical mechanisms (Delta Tau CH4 = 0.46 years), the photolysis frequency (J) of O3 yields O(D-1) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The Delta Tau CH4 due to CTM differences in NO(x) (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NO(x). Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

Surface Measurements and Models

An Observationally Constrained Evaluation of the Oxidative Capacity in the Tropical Western Pacific Troposphere

Hydroxyl radical (OH) is the main daytime oxidant in the troposphere and determines the atmospheric lifetimes of many compounds. We use aircraft measurements of O3, H2O, NO, and other species from the Convective Transport of Active Species in the Tropics (CONTRAST) field campaign, which occurred in the tropical western Pacific (TWP) during January-February 2014, to constrain a photochemical box model and estimate concentrations of OH throughout the troposphere. We find that tropospheric column OH (OHCOL) inferred from CONTRAST observations is 12 to 40% higher than found in chemical transport models (CTMs), including CAM-chem-SD run with 2014 meteorology as well as eight models that participated in POLMIP (2008 meteorology). Part of this discrepancy is due to a clear-sky sampling bias that affects CONTRAST observations; accounting for this bias and also for a small difference in chemical mechanism results in our empirically based value of OHCOL being 0 to 20% larger than found within global models. While these global models simulate observed O3 reasonably well, they underestimate NOx (NO +NO2) by a factor of 2, resulting in OHCOL approx.30% lower than box model simulations constrained by observed NO. Underestimations by CTMs of observed CH3CHO throughout the troposphere and of HCHO in the upper troposphere further contribute to differences between our constrained estimates of OH and those calculated by CTMs. Finally, our calculations do not support the prior suggestion of the existence of a tropospheric OH minimum in the TWP, because during January-February 2014 observed levels of O3 and NO were considerably larger than previously reported values in the TWP.

Hydroxyl radical

Interpreting Space-Based Trends in Carbon Monoxide with Multiple Models

We use a series of chemical transport model and chemistry climate model simulations to investigate the observed negative trends in MOPITT CO over several regions of the world, and to examine the consistency of timedependent emission inventories with observations. We find that simulations driven by the MACCity inventory, used for the Chemistry Climate Modeling Initiative (CCMI), reproduce the negative trends in the CO column observed by MOPITT for 2000-2010 over the eastern United States and Europe. However, the simulations have positive trends over eastern China, in contrast to the negative trends observed by MOPITT. The model bias in CO, after applying MOPITT averaging kernels, contributes to the model-observation discrepancy in the trend over eastern China. This demonstrates that biases in a model's average concentrations can influence the interpretation of the temporal trend compared to satellite observations. The total ozone column plays a role in determining the simulated tropospheric CO trends. A large positive anomaly in the simulated total ozone column in 2010 leads to a negative anomaly in OH and hence a positive anomaly in CO, contributing to the positive trend in simulated CO. These results demonstrate that accurately simulating variability in the ozone column is important for simulating and interpreting trends in CO.

carbon monoxide

Asian Outflow and Trans-Pacific Transport of Carbon Monoxide and Ozone Pollution: An Integrated Satellite, Aircraft, and Model Perspective

Satellite observations of carbon monoxide (CO) from the Measurements of Pollution in the Troposphere (MOPITT) instrument are combined with measurements from the Transport and Chemical Evolution Over the Pacific (TRACE-P) aircraft mission over the northwest Pacific and with a global three-dimensional chemical transport model (GEOS-CHEM) to quantify Asian pollution outflow and its trans-Pacific transport during spring 2001. Global CO column distributions in MOPITT and GEOS-CHEM are highly correlated (R(exp 2) = 0.87), with no significant model bias. The largest regional bias is over Southeast Asia, where the model is 18% too high. A 60% decrease of regional biomass burning emissions in the model (to 39 Tg/yr) would correct the discrepancy; this result is consistent with TRACE-P observations. MOPITT and TRACE-P also give consistent constraints on the Chinese source of CO from fuel combustion (181 Tg CO/yr). Four major events of trans-Pacific transport of Asian pollution in spring 2001 were seen by MOPITT, in situ platforms, and GEOS-CHEM. One of them was sampled by TRACE-P (26-27 February) as a succession of pollution layers over the northeast Pacific. These layers all originated from one single event of Asian outflow that split into northern and southern plumes over the central Pacific. The northern plume (sampled at 6-8 km off California) had no ozone enhancement. The southern subsiding plume (sampled at 2-4 km west of Hawaii) contained a 8 - 17 ppbv ozone enhancement, driven by decomposition of peroxyacetylnitrate (PAN) to nitrogen oxides (NOx). This result suggests that PAN decomposition in trans-Pacific pollution plumes subsiding over the United States could lead to significant enhancements of surface ozone.

Heald, Colette L.

Measurements of the vertical profile, diurnal variation, and secular change of ClO in the stratosphere over Thule, Greenland, February-March, 1992

We report observations of stratospheric chlorine monoxide over the altitude range approx. 16 to 50 km at Thule, Greenland from Feb. 8 to Mar. 24, 1992. A new, more sensitive ground-based mm-wave spectrometer was employed for these measurements, similar in principle to that used earlier for the discovery of low altitude ClO in the Antarctic springtime. In this report, we discuss different aspects of vertical distribution, secular trends, and diurnal variation of ClO in the Arctic stratosphere, based on a preliminary analysis of our Thule data. We see no evidence for large (approx. 1.2-1.5 ppb) amounts of ClO in the lower stratosphere at any time during February or March, in agreement with UARS-MLS findings for this period, and in marked contrast to findings reported for the Arctic in January. We have some evidence for small enhancements (approx. 0.2-0.5 ppb) in the 18-30 km range in late February-early March, which might be associated with volcanic aerosol, rather than PSC, processing.

Dezafra, Robert L.

Observed changes in the vertical profile of stratopheric nitrous oxide at Thule, Greenland, February - March 1992

Using a ground-based mm-wave spectrometer, we have observed stratospheric N2O over Thule, Greenland (76.3 N, 68.4 W) during late February and March, 1992. Vertical profiles of mixing ratio ranging from 16 to 50 km were recovered from molecular emission spectra. The profiles of early March show an abrupt increase in the lower-stratosphere N2O mixing ratio similar to the spring-to-summer change associated with the break up of the Antarctic polar vortex. This increase is correlated with changes in potential vorticity, air temperature, and ozone mixing ratio.

Emmons, Louisa K.

Observation of a strong inverse temperature dependence for the opacity of atmospheric water vapor in the mm continuum near 280 GHz

Results are presented of the field measurements of atmospheric opacity at 278 GHz (9.3/cm) conducted at the McMurdo Station (Antarctica) during the austral springs of 1986 and 1987, in conjunction with balloon measurements of water vapor profile and total column density, showing a strong inverse temperature dependence when normalized to precipitable water vapor. The value of measured opacity per mm of precipitable water vapor (PWV) is roughly two times greater at -35 C than at -10 C and three times greater than measurements at +25 C reported by Zammit and Ade (1981). Various theories proposed to explain excess absorption in continuum regions are reviewed.

Emmons, Louisa K.