Jennifer A. Logan

Tropospheric Aerosol Optical Thickness from the GOCART Model and Comparisons with Satellite and Sun Photometer Measurements

The Georgia Institute of Technology‐Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model is used to simulate the aerosol optical thickness t for major types of tropospheric aerosols including sulfate, dust, organic carbon (OC), black carbon (BC), and sea salt. The GOCART model uses a dust emission algorithm that quantifies the dust source as a function of the degree of topographic depression, and a biomass burning emission source that includes seasonal and interannual variability based on satellite observations. Results presented here show that on global average, dust aerosol has the highest t at 500 nm (0.051), followed by sulfate (0.040), sea salt (0.027), OC (0.017), and BC (0.007). There are large geographical and seasonal variations of t, controlled mainly by emission, transport, and hygroscopic properties of aerosols. The model calculated total ts at 500 nm have been compared with the satellite retrieval products from the Total Ozone Mapping Spectrometer (TOMS) over both land and ocean and from the Advanced Very High Resolution Radiometer (AVHRR) over the ocean. The model reproduces most of the prominent features in the satellite data, with an overall agreement within a factor of 2 over the aerosol source areas and outflow regions. While there are clear differences among the satellite products, a major discrepancy between the model and the satellite data is that the model shows a stronger variation of t from source to remote regions. Quantitative comparison of model and satellite data is still difficult, due to the large uncertainties involved in deriving the t values by both the model and satellite retrieval, and by the inconsistency in physical and optical parameters used between the model and the satellite retrieval. The comparison of monthly averaged model results with the sun photometer network [Aerosol Robotics Network (AERONET)] measurements shows that the model reproduces the seasonal variations at most of the sites, especially the places where biomass burning or dust aerosol dominates.

Three-dimensional climatological distribution of tropospheric OH: Update and evaluation

A global climatological distribution of tropospheric OH is computed using observed distributions of O3, H2O, NOt (NO2 +NO + 2N2O5 + NO3 + HNO2 +HNO4), CO, hydrocarbons, temperature, and cloud optical depth. Global annual mean OH is 1.16×106 molecules cm−3 (integrated with respect to mass of air up to 100 hPa within ±32° latitude and up to 200 hPa outside that region). Mean hemispheric concentrations of OH are nearly equal. While global mean OH increased by 33% compared to that from Spivakovsky et al. [1990], mean loss frequencies of CH3CCl3 and CH4 increased by only 23% because a lower fraction of total OH resides in the lower troposphere in the present distribution. The value for temperature used for determining lifetimes of hydrochlorofluorocarbons (HCFCs) by scaling rate constants [Prather and Spivakovsky, 1990] is revised from 277 K to 272 K. The present distribution of OH is consistent within a few percent with the current budgets of CH3CCl3 and HCFC-22. For CH3CCl3, it results in a lifetime of 4.6 years, including stratospheric and ocean sinks with atmospheric lifetimes of 43 and 80 years, respectively. For HCFC-22, the lifetime is 11.4 years, allowing for the stratospheric sink with an atmospheric lifetime of 229 years. Corrections suggested by observed levels of CH2Cl2 (annual means) depend strongly on the rate of interhemispheric mixing in the model. An increase in OH in the Northern Hemisphere by 20% combined with a decrease in the southern tropics by 25% is suggested if this rate is at its upper limit consistent with observations of CFCs and 85Kr. For the lower limit, observations of CH2Cl2 imply an increase in OH in the Northern Hemisphere by 35% combined with a decrease in OH in the southern tropics by 60%. However, such large corrections are inconsistent with observations for 14CO in the tropics and for the interhemispheric gradient of CH3CCl3. Industrial sources of CH2Cl2 are sufficient for balancing its budget. The available tests do not establish significant errors in OH except for a possible underestimate in winter in the northern and southern tropics by 15–20% and 10–15%, respectively, and an overestimate in southern extratropics by ∼25%. Observations of seasonal variations of CH3CCl3, CH2Cl2, 14CO, and C2H6 offer no evidence for higher levels of OH in the southern than in the northern extratropics. It is expected that in the next few years the latitudinal distribution and annual cycle of CH3CCl3 will be determined primarily by its loss frequency, allowing for additional constraints for OH on scales smaller than global.

Global gridded inventories of anthropogenic emissions of sulfur and nitrogen

Two sets of global inventories of anthropogenic emissions of both oxides of sulfur and oxides of nitrogen for circa 1985 have been produced under the umbrella of the Global Emissions Inventory Activity (GEIA) of the International Global Atmospheric Chemistry Program. The two sets of inventories have different temporal, sectoral, and vertical resolution. Both were compiled using the same data sets; default data sets of global emissions have been refined via the use of more detailed regional data sets. This article reports on the compilation of the annual, one-vertical-level inventories, called version 1A; the inventory files are available to the scientific community via anonymous file transform protocol (FTP). Existing global inventories and regional inventories have been updated and combined on a 1° × 1° longitude/latitude grid. The resulting global anthropogenic emissions are 65 Tg S yr−1 and 21 Tg N yr−1; qualitative uncertainty estimates have been assigned on a regional basis. Emissions of both SOx and NOx are strongly localized in the highly populated and industrialized areas of eastern North America and across Europe; other smaller regions of large emissions are associated with densely populated areas with developed industries or in connection with exploitation of fuels or mineral reserves. The molar ratio of nitrogen to sulfur emissions reflects the overall character of sources; its value is generally between 0.33 and 10 for industrialized and heavily populated areas but varies over a wide range for other areas. We suggest that those requiring sulfur or nitrogen emission inventories standardize on the GEIA inventories, which we believe are authoritative and which are freely available to all users by anonymous FTP.

An assessment of biofuel use and burning of agricultural waste in the developing world

[1] We present an assessment of biofuel use and agricultural field burning in the developing world. We used information from government statistics, energy assessments from the World Bank, and many technical reports, as well as from discussions with experts in agronomy, forestry, and agro-industries. We estimate that 2060 Tg biomass fuel was used in the developing world in 1985; of this, 66% was burned in Asia, and 21% and 13% in Africa and Latin America, respectively. Agricultural waste supplies about 33% of total biofuel use, providing 39%, 29%, and 13% of biofuel use in Asia, Latin America, and Africa, and 41% and 51% of the biofuel use in India and China. We find that 400 Tg of crop residues are burned in the fields, with the fraction of available residue burned in 1985 ranging from 1% in China, 16–30% in the Middle East and India, to about 70% in Indonesia; in Africa about 1% residue is burned in the fields of the northern drylands, but up to 50% in the humid tropics. We distributed this biomass burning on a spatial grid with resolution of 1 1, and applied emission factors to the amount of dry matter burned to give maps of trace gas emissions in the developing world. The emissions of CO from biofuel use in the developing world, 156 Tg, are about 50% of the estimated global CO emissions from fossil fuel use and industry. The emission of 0.9 Pg C (as CO2) from burning of biofuels and field residues together is small, but nonnegligible when compared with the emissions of CO2 from fossil fuel use and industry, 5.3 Pg C. The biomass burning source of 10 Tg/yr for CH4 and 2.2 Tg N/yr of NOx are relatively small when compared with total CH4 and NOx sources; this source of NOx may be important on a regional basis. INDEX TERMS: 1610 Global Change: Atmosphere (0315, 0325); 1803 Hydrology: Anthropogenic effects; 1615 Global Change: Biogeochemical processes (4805); KEYWORDS: biofuel use, global biofuel burning, agricultural waste burning, biofuel emissions

An analysis of ozonesonde data for the troposphere: Recommendations for testing 3‐D models and development of a gridded climatology for tropospheric ozone

I present an analysis of ozonesonde data, synthesizing what is known about the distribution of tropospheric ozone. Major features of the distribution are highlighted, and recommendations are given for testing three-dimensional models of tropospheric chemistry and transport with these data. The data are analyzed on pressure surfaces and relative to the height of the thermal tropopause. A minimum of 20 soundings are required for 95% confidence intervals of the ozone monthly means to be less than ±30% near the extratropical tropopause. Twenty soundings also ensures means reliable to better than ±15% for 800–500 hPa for the extratropics and for 800–100 hPa in the tropics. Ozone variability is higher in the upper troposphere for subtropical locations than for tropical locations, and 35 soundings are required for 400–100 hPa for the means to be defined to better than ±15%. For northern middle and high latitudes, the broad summer maximum in ozone in the middle troposphere extends all the way up to the tropopause. Median concentrations at the tropopause are highest in June and July, typically 125–200 ppb, and are a factor of 2 smaller in winter. Highest values of ozone are in spring 2 km above the tropopause. The change in the phase of the annual cycle of ozone between the tropopause and the region immediately above it, and the steep concentration gradients across the tropopause, suggest that high vertical resolution (∼1 km) will be required in models to simulate this behavior. Mean ozone values in the middle troposphere are approximately constant from 30° to 75° in the winter in both hemispheres, while there is a maximum from 35° to 50°N in summer. In the northern subtropics, there is a summer minimum in middle tropospheric ozone over the Pacific and a summer maximum over the Atlantic which appear to be related to differences in circulation. Mean ozone values over Samoa are similar to those measured 20–30 years ago over Panama. Ozone is higher over the tropical South Atlantic (Natal) than over the western Pacific (Samoa) all year from about 800 hPa to the tropopause; ozone is most similar in May and June over the Atlantic and Pacific, the months with minimum burning in the tropics. The ozone maximum at Samoa in the middle and upper troposphere in October is caused by long-range transport of ozone and its precursors from biomass burning, with the peak lagging that at Natal by about a month. The secondary peak in ozone in January and December at South Atlantic sites reflects transport of biomass burning effluents from the Northern Hemisphere. The sonde data were used in combination with surface and satellite data to derive a gridded climatology for tropospheric ozone.

Global simulation of tropospheric O3-NOx-hydrocarbon chemistry: 1. Model formulation

We describe a global three-dimensional model for tropospheric O3-NOx-hydrocarbon chemistry with synoptic-scale resolution. A suite of 15 chemical tracers, including O3, NOx, PAN, HNO3, CO, H2O2, and various hydrocarbons, is simulated in the model. For computational expediency, chemical production and loss of tracers are parameterized as polynomial functions to fit the results of a detailed O3-NOx-hydrocarbon mechanism. The model includes state-of-the-art inventories of anthropogenic emissions and process-based formulations of natural emissions and deposition that are tied to the model meteorology. Improvements are made to existing schemes for computing biogenic emissions of isoprene and NO. Our best estimates of global emissions include among others 42 Tg N yr−1 for NOx (21 Tg N yr−1 from fossil fuel combustion, 12 Tg N yr−1 from biomass burning, 6 Tg N yr−1 from soils, and 3 Tg N yr−1 from lightning), and 37 Tg C yr−1 for acetone (1 Tg C yr−1 from industry, 9 Tg C yr−1 from biomass burning, 15 Tg C yr−1 from vegetation, and 12 Tg C yr−1 from oxidation of propane and higher alkanes).

Rociletinib in EGFR-mutated non-small-cell lung cancer.

BACKGROUND Non-small-cell lung cancer (NSCLC) with a mutation in the gene encoding epidermal growth factor receptor (EGFR) is sensitive to approved EGFR inhibitors, but resistance develops, mediated by the T790M EGFR mutation in most cases. Rociletinib (CO-1686) is an EGFR inhibitor active in preclinical models of EGFR-mutated NSCLC with or without T790M. METHODS In this phase 1-2 study, we administered rociletinib to patients with EGFR-mutated NSCLC who had disease progression during previous treatment with an existing EGFR inhibitor. In the expansion (phase 2) part of the study, patients with T790M-positive disease received rociletinib at a dose of 500 mg twice daily, 625 mg twice daily, or 750 mg twice daily. Key objectives were assessment of safety, side-effect profile, pharmacokinetics, and preliminary antitumor activity of rociletinib. Tumor biopsies to identify T790M were performed during screening. Treatment was administered in continuous 21-day cycles. RESULTS A total of 130 patients were enrolled. The first 57 patients to be enrolled received the free-base form of rociletinib (150 mg once daily to 900 mg twice daily). The remaining patients received the hydrogen bromide salt (HBr) form (500 mg twice daily to 1000 mg twice daily). A maximum tolerated dose (the highest dose associated with a rate of dose-limiting toxic effects of less than 33%) was not identified. The only common dose-limiting adverse event was hyperglycemia. In an efficacy analysis that included patients who received free-base rociletinib at a dose of 900 mg twice daily or the HBr form at any dose, the objective response rate among the 46 patients with T790M-positive disease who could be evaluated was 59% (95% confidence interval [CI], 45 to 73), and the rate among the 17 patients with T790M-negative disease who could be evaluated was 29% (95% CI, 8 to 51). CONCLUSIONS Rociletinib was active in patients with EGFR-mutated NSCLC associated with the T790M resistance mutation. (Funded by Clovis Oncology; ClinicalTrials.gov number, NCT01526928.).

Effect of rising Asian emissions on surface ozone in the United States

The effect of increasing fossil fuel combustion in eastern Asia on surface O3 air pollution in the United States is examined with a global three-dimensional tropospheric chemistry model. Tripling of Asian anthropogenic emissions from 1985 to 2010 is expected to increase monthly mean O3 concentrations by 2–6 ppbv in the western United States and by 1–3 ppbv in the eastern United States, the maximum effect being in April–June. This increase would more than offset the benefits of 25% domestic reductions in anthropogenic emissions of NOx and hydrocarbons in the western United States. Asian influence may be less under the stagnant conditions leading to violations of the U.S. air quality standard. Nevertheless, our results suggest that a global perspective is necessary when designing a strategy to meet regional O3 air quality objectives.

Origin of ozone and NOx in the tropical troposphere: A photochemical analysis of aircraft observations over the South Atlantic basin

The photochemistry of the troposphere over the South Atlantic basin is examined by modeling of aircraft observations up to 12-km altitude taken during the TRACE A expedition in September–October 1992. A close balance is found in the 0 to 12-km column between photochemical production and loss of O3, with net production at high altitudes compensating for weak net loss at low altitudes. This balance implies that O3 concentrations in the 0–12 km column can be explained solely by in situ photochemistry; influx from the stratosphere is negligible. Simulation of H2O2, CH3OOH, and CH2O concentrations measured aboard the aircraft lends confidence in the computations of O3 production and loss rates, although there appears to be a major gap in current understanding of CH2O chemistry in the marine boundary layer. The primary sources of NOx over the South Atlantic Basin appear to be continental (biomass burning, lightning, soils). There is evidence that NOx throughout the 0 to 12-km column is recycled from its oxidation products rather than directly transported from its primary sources. There is also evidence for rapid conversion of HNO3 to NOx in the upper troposphere by a mechanism not included in current models. A general representation of the O3 budget in the tropical troposphere is proposed that couples the large-scale Walker circulation and in situ photochemistry. Deep convection in the rising branches of the Walker circulation injects NOx from combustion, soils, and lightning to the upper troposphere, leading to O3 production; eventually, the air subsides and net O3 loss takes place in the lower troposphere, closing the O3 cycle. This scheme implies a great sensitivity of the oxidizing power of the atmosphere to NOx emissions in the tropics.

Climate forcings in Goddard Institute for Space Studies SI2000 simulations

[1] We define the radiative forcings used in climate simulations with the SI2000 version of the Goddard Institute for Space Studies (GISS) global climate model. These include temporal variations of well-mixed greenhouse gases, stratospheric aerosols, solar irradiance, ozone, stratospheric water vapor, and tropospheric aerosols. Our illustrations focus on the period 1951–2050, but we make the full data sets available for those forcings for which we have earlier data. We illustrate the global response to these forcings for the SI2000 model with specified sea surface temperature and with a simple Q-flux ocean, thus helping to characterize the efficacy of each forcing. The model yields good agreement with observed global temperature change and heat storage in the ocean. This agreement does not yield an improved assessment of climate sensitivity or a confirmation of the net climate forcing because of possible compensations with opposite changes of these quantities. Nevertheless, the results imply that observed global temperature change during the past 50 years is primarily a response to radiative forcings. It is also inferred that the planet is now out of radiation balance by 0.5 to 1 W/m 2 and that additional global warming of about 0.5� C is already ‘‘in the pipeline.’’ INDEX TERMS: 1620 Global Change: Climate dynamics (3309); 1635 Global Change: Oceans (4203); 1650 Global Change: Solar variability;