F. S. Rowland

Bio: F. S. Rowland is an academic researcher from University of California, Irvine. The author has contributed to research in topics: Troposphere & Methylene. The author has an hindex of 31, co-authored 54 publications receiving 7381 citations.

Stratospheric sink for chlorofluoromethanes: chlorine atomc-atalysed destruction of ozone

Abstract: Chlorofluoromethanes are being added to the environment in steadily increasing amounts. These compounds are chemically inert and may remain in the atmosphere for 40–150 years, and concentrations can be expected to reach 10 to 30 times present levels. Photodissociation of the Chlorofluoromethanes in the stratosphere produces significant amounts of chlorine atoms, and leads to the destruction of atmospheric ozone.

Chlorofluoromethanes in the Environment

Abstract: A study is presented on the photoprocesses of atmospheric chlorofluoromethanes, including their ultimate sinks. Topics covered include: current inventories of atmospheric trichlorofluoromethane and dichlorodifluoromethane, absorption cross-sections for photodissociation of chlorofluoromethanes, mechanisms and quantum yields for photodissociation of CF/sub 2/Cl/sub 2/ and CFCl/sub 3/, solar irradiation flux versus wavelength and altitude, atmospheric diffusion models, chain reactions in the ozone layer, the chloroxyl chains for decomposition of O/sub 3/, abstraction reactions by thermal chlorine atoms, release of Cl atoms by hydroxyl radical attack on hydrogen chloride, methane concentrations at 50 km, rate constants for ClO/sub x/ reactions with O/sub 3/ and oxygen atoms, chain terminating reactions, the importance of symmetrical dioxychloride in the stratosphere, fluorine atom chains, possible removal of chlorofluoromethanes by electron capture and/or ionic reaction, possible chlorofluoromethane removal by reaction with singlet oxygen, hydrolysis of chlorofluoromethanes, possible reactions of chlorofluoromethanes with aerosol particles in the stratosphere, calculated O/sub 3/ depletion by chlorine-containing species, multi-dimensional calculations, feedback in the ozone depletion calculation, increased odd oxygen production with O/sub 3/ depletion, time delay effects in the appearance of O/sub 3/ depletion, time concentration patterns with a one year stepfunction injection of CF/sub 2/Cl/sub 2/ and for several hypothetical models of chlorofluoromethane releasemore » stratospheric concentrations from CF/sub 2/Cl/sub 2/ injected by 1975, estimates of consequences for two different manufacturing patterns for CF/sub 2/Cl/sub 2/ between 1975 and 1990, current stratospheric levels of chlorine-containing compounds, possible biological and climatological effects of stratospheric O/sub 3/ depletion, and observable trends in the average O/sub 3/ concentration of the atmosphere.« less

Potential impact of iodine on tropospheric levels of ozone and other critical oxidants

Abstract: A new analysis of tropospheric iodine chemistry suggests that under certain conditions this chemistry could have a significant impact on the rate of destruction of tropospheric ozone. In addition, it suggests that modest shifts could result in the critical radical ratio HO2/OH. This analysis is based on the first ever observations of CH3I in the middle and upper free troposphere as recorded during the NASA Pacific Exploratory Mission in the western Pacific. Improved evaluations of several critical gas kinetic and photochemical rate coefficients have also been used. Three iodine source scenarios were explored in arriving at the above conclusions. These include: (1) the assumption that the release of CH3I from the marine environment was the only iodine source with boundary layer levels reflecting a low-productivity source region, (2) same as scenario 1 but with an additional marine iodine source in the form of higher molecular weight iodocarbons, and (3) source scenario 2 but with the release of all iodocarbons occurring in a region of high biological productivity. Based on one-dimensional model simulations, these three source scenarios resulted in estimated Ix (Ix = I + IO + HI + HOI + 2I2O2 + INOx) yields for the upper troposphere of 0.5, 1.5, and 7 parts per trillion by volume (pptv), respectively. Of these, only at the 1.5 and 7 pptv level were meaningful enhancements in O3 destruction estimated. Total column O3 destruction for these cases averaged 6 and 30%, respectively. At present we believe the 1.5 pptv Ix source scenario to be more typical of the tropical marine environment; however, for specific regions of the Pacific (i.e., marine upwelling regions) and for specific seasons of the year, much higher levels might be experienced. Even so, significant uncertainties still remain in the proposed iodine chemistry. In particular, much uncertainty remains in the magnitude of the marine iodine source. In addition, several rate coefficients for gas phase processes need further investigating, as does the efficiency for removal of iodine due to aerosol scavenging processes.

Characterization of trace gases measured over Alberta oil sands mining operations: 76 speciated C 2 –C 10 volatile organic compounds (VOCs), CO 2 , CH 4 , CO, NO, NO 2 , NO y , O 3 and SO 2

Abstract: . Oil sands comprise 30% of the world's oil reserves and the crude oil reserves in Canada's oil sands deposits are second only to Saudi Arabia. The extraction and processing of oil sands is much more challenging than for light sweet crude oils because of the high viscosity of the bitumen contained within the oil sands and because the bitumen is mixed with sand and contains chemical impurities such as sulphur. Despite these challenges, the importance of oil sands is increasing in the energy market. To our best knowledge this is the first peer-reviewed study to characterize volatile organic compounds (VOCs) emitted from Alberta's oil sands mining sites. We present high-precision gas chromatography measurements of 76 speciated C2–C10 VOCs (alkanes, alkenes, alkynes, cycloalkanes, aromatics, monoterpenes, oxygenated hydrocarbons, halocarbons and sulphur compounds) in 17 boundary layer air samples collected over surface mining operations in northeast Alberta on 10 July 2008, using the NASA DC-8 airborne laboratory as a research platform. In addition to the VOCs, we present simultaneous measurements of CO2, CH4, CO, NO, NO2, NOy, O3 and SO2, which were measured in situ aboard the DC-8. Carbon dioxide, CH4, CO, NO, NO2, NOy, SO2 and 53 VOCs (e.g., non-methane hydrocarbons, halocarbons, sulphur species) showed clear statistical enhancements (1.1–397×) over the oil sands compared to local background values and, with the exception of CO, were greater over the oil sands than at any other time during the flight. Twenty halocarbons (e.g., CFCs, HFCs, halons, brominated species) either were not enhanced or were minimally enhanced ( In addition to the emission of many trace gases, the natural drawdown of OCS by vegetation was absent above the surface mining operations, presumably because of the widespread land disturbance. Unexpectedly, the mixing ratios of α-pinene and β-pinene were much greater over the oil sands (up to 217 pptv and 610 pptv, respectively) than over vegetation in the background boundary layer (20±7 pptv and 84±24 pptv, respectively), and the pinenes correlated well with several industrial tracers that were elevated in the oil sands plumes. Because so few independent measurements from the oil sands mining industry exist, this study provides an important initial characterization of trace gas emissions from oil sands surface mining operations.

Boreal forest fire emissions in fresh Canadian smoke plumes: C 1 -C 10 volatile organic compounds (VOCs), CO 2 , CO, NO 2 , NO, HCN and CH 3 CN

Abstract: . Boreal regions comprise about 17 % of the global land area, and they both affect and are influenced by climate change. To better understand boreal forest fire emissions and plume evolution, 947 whole air samples were collected aboard the NASA DC-8 research aircraft in summer 2008 as part of the ARCTAS-B field mission, and analyzed for 79 non-methane volatile organic compounds (NMVOCs) using gas chromatography. Together with simultaneous measurements of CO2, CO, CH4, CH2O, NO2, NO, HCN and CH3CN, these measurements represent the most comprehensive assessment of trace gas emissions from boreal forest fires to date. Based on 105 air samples collected in fresh Canadian smoke plumes, 57 of the 80 measured NMVOCs (including CH2O) were emitted from the fires, including 45 species that were quantified from boreal forest fires for the first time. After CO2, CO and CH4, the largest emission factors (EFs) for individual species were formaldehyde (2.1 ± 0.2 g kg−1), followed by methanol, NO2, HCN, ethene, α-pinene, β-pinene, ethane, benzene, propene, acetone and CH3CN. Globally, we estimate that boreal forest fires release 2.4 ± 0.6 Tg C yr−1 in the form of NMVOCs, with approximately 41 % of the carbon released as C1-C2 NMVOCs and 21 % as pinenes. These are the first reported field measurements of monoterpene emissions from boreal forest fires, and we speculate that the pinenes, which are relatively heavy molecules, were detected in the fire plumes as the result of distillation of stored terpenes as the vegetation is heated. Their inclusion in smoke chemistry models is expected to improve model predictions of secondary organic aerosol (SOA) formation. The fire-averaged EF of dichloromethane or CH2Cl2, (6.9 ± 8.6) × 10−4 g kg−1, was not significantly different from zero and supports recent findings that its global biomass burning source appears to have been overestimated. Similarly, we found no evidence for emissions of chloroform (CHCl3) or methyl chloroform (CH3CCl3) from boreal forest fires. The speciated hydrocarbon measurements presented here show the importance of carbon released by short-chain NMVOCs, the strong contribution of pinene emissions from boreal forest fires, and the wide range of compound classes in the most abundantly emitted NMVOCs, all of which can be used to improve biomass burning inventories in local/global models and reduce uncertainties in model estimates of trace gas emissions and their impact on the atmosphere.

The Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2)

Abstract: The Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), is the latest atmospheric reanalysis of the modern satellite era produced by NASA’s Global Modeling and Assimilation Office (GMAO). MERRA-2 assimilates observation types not available to its predecessor, MERRA, and includes updates to the Goddard Earth Observing System (GEOS) model and analysis scheme so as to provide a viable ongoing climate analysis beyond MERRA’s terminus. While addressing known limitations of MERRA, MERRA-2 is also intended to be a development milestone for a future integrated Earth system analysis (IESA) currently under development at GMAO. This paper provides an overview of the MERRA-2 system and various performance metrics. Among the advances in MERRA-2 relevant to IESA are the assimilation of aerosol observations, several improvements to the representation of the stratosphere including ozone, and improved representations of cryospheric processes. Other improvements in the quality of M...

Anthropogenic and Natural Radiative Forcing

Abstract: This chapter should be cited as: Myhre, G., D. Shindell, F.-M. Bréon, W. Collins, J. Fuglestvedt, J. Huang, D. Koch, J.-F. Lamarque, D. Lee, B. Mendoza, T. Nakajima, A. Robock, G. Stephens, T. Takemura and H. Zhang, 2013: Anthropogenic and Natural Radiative Forcing. In: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change [Stocker, T.F., D. Qin, G.-K. Plattner, M. Tignor, S.K. Allen, J. Boschung, A. Nauels, Y. Xia, V. Bex and P.M. Midgley (eds.)]. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA. Coordinating Lead Authors: Gunnar Myhre (Norway), Drew Shindell (USA)

Emission of trace gases and aerosols from biomass burning

Abstract: A large body of information on emissions from the various types of biomass burning has been accumulated over the past decade, to a large extent as a result of International Geosphere-Biosphere Programme/International Global Atmospheric Chemistry research activities. Yet this information has not been readily accessible to the atmospheric chemistry community because it was scattered over a large number of publications and reported in numerous different units and reference systems. We have critically evaluated the presently available data and integrated these into a consistent format. On the basis of this analysis we present a set of emission factors for a large variety of species emitted from biomass fires. Where data were not available, we have proposed estimates based on appropriate extrapolation techniques. We have derived global estimates of pyrogenic emissions for important species emitted by the various types of biomass burning and compared our estimates with results from inverse modeling studies.

Couplings between changes in the climate system and biogeochemistry

Abstract: Couplings Between Changes in the Climate System and Biogeochemistry Coordinating Lead Authors: Kenneth L. Denman (Canada), Guy Brasseur (USA, Germany) Lead Authors: Amnat Chidthaisong (Thailand), Philippe Ciais (France), Peter M. Cox (UK), Robert E. Dickinson (USA), Didier Hauglustaine (France), Christoph Heinze (Norway, Germany), Elisabeth Holland (USA), Daniel Jacob (USA, France), Ulrike Lohmann (Switzerland), Srikanthan Ramachandran (India), Pedro Leite da Silva Dias (Brazil), Steven C. Wofsy (USA), Xiaoye Zhang (China) Contributing Authors: D. Archer (USA), V. Arora (Canada), J. Austin (USA), D. Baker (USA), J.A. Berry (USA), R. Betts (UK), G. Bonan (USA), P. Bousquet (France), J. Canadell (Australia), J. Christian (Canada), D.A. Clark (USA), M. Dameris (Germany), F. Dentener (EU), D. Easterling (USA), V. Eyring (Germany), J. Feichter (Germany), P. Friedlingstein (France, Belgium), I. Fung (USA), S. Fuzzi (Italy), S. Gong (Canada), N. Gruber (USA, Switzerland), A. Guenther (USA), K. Gurney (USA), A. Henderson-Sellers (Switzerland), J. House (UK), A. Jones (UK), C. Jones (UK), B. Karcher (Germany), M. Kawamiya (Japan), K. Lassey (New Zealand), C. Le Quere (UK, France, Canada), C. Leck (Sweden), J. Lee-Taylor (USA, UK), Y. Malhi (UK), K. Masarie (USA), G. McFiggans (UK), S. Menon (USA), J.B. Miller (USA), P. Peylin (France), A. Pitman (Australia), J. Quaas (Germany), M. Raupach (Australia), P. Rayner (France), G. Rehder (Germany), U. Riebesell (Germany), C. Rodenbeck (Germany), L. Rotstayn (Australia), N. Roulet (Canada), C. Sabine (USA), M.G. Schultz (Germany), M. Schulz (France, Germany), S.E. Schwartz (USA), W. Steffen (Australia), D. Stevenson (UK), Y. Tian (USA, China), K.E. Trenberth (USA), T. Van Noije (Netherlands), O. Wild (Japan, UK), T. Zhang (USA, China), L. Zhou (USA, China) Review Editors: Kansri Boonpragob (Thailand), Martin Heimann (Germany, Switzerland), Mario Molina (USA, Mexico) This chapter should be cited as: Denman, K.L., G. Brasseur, A. Chidthaisong, P. Ciais, P.M. Cox, R.E. Dickinson, D. Hauglustaine, C. Heinze, E. Holland, D. Jacob, U. Lohmann, S Ramachandran, P.L. da Silva Dias, S.C. Wofsy and X. Zhang, 2007: Couplings Between Changes in the Climate System and Biogeochemistry. In: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change [Solomon, S., D. Qin, M. Manning, Z. Chen, M. Marquis, K.B. Averyt, M.Tignor and H.L. Miller (eds.)]. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA.