Mary M. Kleb

Pacific Exploratory Mission in the Tropical Pacific: PEM-Tropics B, March-April 1999

The Pacific Exploratory Mission - Tropics B (PEM-Tropics B) was conducted by the NASA Global Tropospheric Experiment (GTE) over the tropical Pacific Ocean in March-April 1999. It used the NASA DC-8 and P-3B aircraft equipped with extensive instrumentation for measuring numerous chemical compounds and gases. Its central objective was to improve knowledge of the factors controlling ozone, OH, aerosols, and related species over the tropical Pacific. Geographical coverage ranged from 38°N to 36°S and 148°W to 76°E. Major deployment sites included Hilo, Hawaii, Christmas Island, Tahiti, Fiji, and Easter Island. PEM-Tropics B was a sequel to PEM-Tropics A, which was conducted in September-October 1996 and encountered considerable biomass burning. PEM-Tropics B, conducted in the wet season of the southern tropics, observed an exceedingly clean atmosphere over the South Pacific but a variety of pollution influences over the tropical North Pacific. Photochemical ozone loss over both the North and the South Pacific exceeded local photochemical production by about a factor of 2, implying a major deficit in the tropospheric ozone budget. Dedicated flights investigated the sharp air mass transitions at the Intertropical Convergence Zone (ITCZ) and the South Pacific Convergence Zone (SPCZ). Extensive OH observations permitted the first large-scale comparisons with photochemical model predictions. High concentrations of oxygenated organics were observed ubiquitously in the tropical Pacific atmosphere and may have important implications for global HOx and NOx budgets. Extensive equatorial measurements of dimethyl sulfide and OH suggest that important aspects of marine sulfur chemistry are still poorly understood.

Response of middle atmosphere chemistry and dynamics to volcanically elevated sulfate aerosol: Three‐dimensional coupled model simulations

The NASA Langley Research Center Interactive Modeling Project for Atmospheric Chemistry and Transport (IMPACT) model has been used to examine the response of the middle atmosphere to a large tropical stratospheric injection of sulfate aerosol, such as that following the June 1991 eruption of Mount Pinatubo. The influence of elevated aerosol on heterogeneous chemical processing was simulated using a three-dimensional climatology of surface area density (SAD)developed using observations made from the Halogen Occultation Experiment, Stratospheric Aerosol and Gas Experiment II, and Stratospheric Aerosol Measurement satellite instruments beginning in June 1991. Radiative effects of the elevated aerosol were represented by monthly mean zonally averaged heating perturbations obtained from a study conducted with the European Center/Hamburg (ECHAM4) general circulation model combined with an observationally derived set of aerosol parameters. Two elevated-aerosol simulations were integrated for 31/2 years following the volcanic injection. One simulation included only the aerosol radiative perturbation, and one simulation included both the radiative perturbation and the elevated SAD. These perturbation simulations are compared with multiple-year control simulations to isolate relative contributions of transport and heterogeneous chemical processing. Significance of modeled responses is assessed through comparison with interannual variability. Dynamical and photochemical contributions to ozone decreases are of comparable magnitude. Important stratospheric chemical/dynamical feedback effects are shown, as ozone reductions modulate aerosol-induced heating by up to 10% in the lower stratosphere and 25% in the middle stratosphere. Dynamically induced changes in chemical constituents which propagate into the upper stratosphere are still pronounced at the end of the simulations.

Dynamical climatology of the NASA Langley Research Center Interactive Modeling Project for Atmospheric Chemistry and Transport (IMPACT) model

A comparison of the NASA Langley Research Center (LaRC) Interactive Modeling Project for Atmospheric Chemistry and Transport (IMPACT) models dynamical characteristics with assimilated data sets and observations is presented to demonstrate the ability of the model to represent the dynamical characteristics of Earths troposphere and stratosphere. The LaRC IMPACT model is a coupled chemical/dynamical general circulation model (GCM) of the Earths atmosphere extending from the surface to the lower mesosphere. It has been developed as a tool for assessing the effects of chemical, dynamical, and radiative coupling in the stratosphere on the Earths climate. The LaRC IMPACT model winds and temperatures are found to be in fairly good agreement with Upper Atmospheric Research Satellite (UARS) United Kingdom Meteorological Office (UKMO) assimilated winds and temperatures in the lower stratosphere. The model upper stratospheric zonal mean temperatures are also in good agreement with the UARS-UKMO climatology except for a cold winter pole which results from the upward extension of the cold vortex temperatures and an elevated winter stratopause in the model. The cold pole bias is consistent with the overprediction of the winter stratospheric jet strength, and is characteristic of stratospheric GCMs in general. The model northern and southern hemisphere stratospheric eddy heat and momentum fluxes are within the expected interannual variability of the UARS-UKMO climatology. The combined effects of water vapor transport, radiative, convective, and planetary boundary layer parameterizations are shown to produce tropospheric winds and circulation statistics that are in good agreement with the UARS-UKMO climatology, although the model tropopause and upper tropospheric temperatures are generally cold relative to the UARS-UKMO temperatures. Comparisons between the model and UARS-UKMO climatology indicate that the model does a reasonable job in reproducing the frequency of observed synoptic-scale storms during the northern and southern hemisphere winters. Generally good agreement is found between the model and observations in the distribution of outgoing longwave radiation and precipitable water. However, the model precipitation and cloud distributions are influenced by spectral truncation errors which indicate that the T32 spectral resolution of the model is probably not adequate to accurately represent coupling between localized convection and large-scale water vapor transport. The agreement between the observed and model stratospheric circulation and temperatures, reasonableness of the model stratospheric wave driving, and stability of the model climatology provides confidence that the LaRC IMPACT model is appropriate for multiyear coupled radiation/chemistry/dynamics studies of the stratosphere.

Large biogenic contribution to boundary layer O3‐CO regression slope in summer

Strong correlation between O3 and CO was observed during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) aircraft experiment in July 2011 over the Washington-Baltimore area. The observed correlation does not vary significantly with time or altitude in the boundary layer. The observations are simulated well by a regional chemical transport model. We analyze the model results to understand the factors contributing to the observed O3-CO regression slope, which has been used in past studies to estimate the anthropogenic O3 production amount. We trace separately four different CO sources: primary anthropogenic emissions, oxidation of anthropogenic volatile organic compounds, oxidation of biogenic isoprene, and transport from the lateral and upper model boundaries. Modeling analysis suggests that the contribution from biogenic isoprene oxidation to the observed O3-CO regression slope is as large as that from primary anthropogenic CO emissions. As a result of decrease of anthropogenic primary CO emissions during the past decades, biogenic CO from oxidation of isoprene is increasingly important. Consequently, observed and simulated O3-CO regression slopes can no longer be used directly with an anthropogenic CO emission inventory to quantify anthropogenic O3 production over the United States. The consistent enhancement of O3 relative to CO observed in the boundary layer, as indicated by the O3-CO regression slope, provides a useful constraint on model photochemistry and emissions.