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Ozone trends, derived from 1979-1996 Dobson spectrophotometer total ozone data obtained at five U.S. mainland midlatitude stations, averaged -3.4, -4.9, -2.6, -1.9, and -3.3%/decade for winter, spring, summer, and autumn months, and on an annual basis, respectively. At the lower latitude stations of Mauna Loa and Samoa, corresponding-period annual ozone trends were -0.4 and -1.3%/decade, respectively, while at Huancayo, Peru, the 1979-1991 annual trend was -0.9%/decade. A linear trend approximation to ozone changes that occurred since 1978 during austral daylight times at Amundsen-Scott (South Pole) station, Antarctica, yielded a value of -12%/decade. By combining 1979-1996 annual trend data for three U.S. mainland stations with trends for the sites derived from 1963-1978 data, it is estimated that the ozone decrease at U.S. midlatitudes through 1996, relative to ozone present in the mid-1960s, was -6.7%. Similar analyses incorporating South Pole data obtained since 1963 yielded an ozone change at South Pole (daylight observations) through 1996 of approximately -25%. South Pole October total ozone values in 1996 were lower than mid-1960s October ozone values by a factor of two. Trend data are also presented for several shorter record period stations, including the foreign cooperative stations of Haute Provence, France; Lauder, New Zealand; and Perth, Australia.
Carbon monoxide (CO) mixing ratios were measured in air samples collected weekly at eight locations. The air was collected as part of the CMDL/NOAA cooperative flask sampling program (Climate Monitoring and Diagnostics Laboratory, formerly Geophysical Monitoring for Climatic Change, Air Resources Laboratory/National Oceanic and Atmospheric Administration) at Point Barrow, Alaska (71°N), Niwot Ridge, Colorado (40°N), Mauna Loa and Cape Kumakahi, Hawaii (19°N), Guam, Marianas Islands (13°N), Christmas Island (2°N), Ascension Island (8°S) and American Samoa (14°S). Half-liter or 3-L glass flasks fitted with glass piston stopcocks holding teflon O rings were used for sample collection. CO levels were determined within several weeks of collection using gas chromatography followed by mercuric oxide reduction detection, and mixing ratios were referenced against the CMDL/NOAA carbon monoxide standard scale. During the period of study (mid-1988 through December 1990) CO levels were greatest in the high latitudes of the northern hemisphere (mean mixing ratio from January 1989 to December 1990 at Point Barrow was approximately 154 ppb) and decreased towards the south (mean mixing ratio at Samoa over a similar period was 65 ppb). Mixing ratios varied seasonally, the amplitude of the seasonal cycle was greatest in the north and decreased to the south. Carbon monoxide levels were affected by both local and regional scale processes. The difference in CO levels between northern and southern latitudes also varied seasonally. The greatest difference in CO mixing ratios between Barrow and Samoa was observed during the northern winter (about 150 ppb). The smallest difference, 40 ppb, occurred during the austral winter. The annually averaged CO difference between 71°N and 14°S was approximately 90 ppb in both 1989 and 1990; the annually averaged interhemispheric gradient from 71°N to 41°S is estimated as approximately 95 ppb.
We present a comprehensive estimate of nitrous oxide (N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. The Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected discrete air samples in flasks and in situ measurements from remote sites across the globe and analyzed them for a suite of species including N2O. In addition to these major networks, we include in situ and aircraft measurements from the National Institute of Environmental Studies (NIES) and flask measurements from the Tohoku University and Commonwealth Scientific and Industrial Research Organization (CSIRO) networks. All measurements show increasing atmospheric mole fractions of N2O, with a varying growth rate of 0.1–0.7% per year, resulting in a 7.4% increase in the background atmospheric mole fraction between 1979 and 2011. Using existing emission inventories as well as bottom-up process modeling results, we first create globally gridded a priori N2O emissions over the 37 years since 1975. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions for five source sectors from 13 regions in the world. This is the first time that all of these measurements from multiple networks have been combined to determine emissions. Our inversion indicates that global and regional N2O emissions have an increasing trend between 1995 and 2008. Despite large uncertainties, a significant increase is seen from the Asian agricultural sector in recent years, most likely due to an increase in the use of nitrogenous fertilizers, as has been suggested by previous studies.
SF6 total columns were successfully retrieved from FTIR (Fourier transform infrared) measurements (Saint Denis and Maïdo) on Reunion Island (21°â€¯S, 55°â€¯E) between 2004 and 2016 using the SFIT4 algorithm: the retrieval strategy and the error budget were presented. The FTIR SF6 retrieval has independent information in only one individual layer, covering the whole of the troposphere and the lower stratosphere. The trend in SF6 was analysed based on the FTIR-retrieved dry-air column-averaged mole fractions (XSF6) on Reunion Island, the in situ measurements at America Samoa (SMO) and the collocated satellite measurements (Michelson Interferometer for Passive Atmospheric Sounding, MIPAS, and Atmospheric Chemistry Experiment Fourier Transform Spectrometer, ACE-FTS) in the southern tropics. The SF6 annual growth rate from FTIR retrievals is 0.265â€¯±â€¯0.013â€¯pptvâ€†year−1 for 2004–2016, which is slightly weaker than that from the SMO in situ measurements (0.285â€¯±â€¯0.002â€¯pptvâ€†year−1) for the same time period. The SF6 trend in the troposphere from MIPAS and ACE-FTS observations is also close to the ones from the FTIR retrievals and the SMO in situ measurements.
Profiles of CFC-11 (CCl3F), CFC-12 (CCl2F2) and HCFC-22 (CHF2Cl) have been obtained from Fourier transform infrared (FTIR) solar absorption measurements above the Saint-Denis (St Denis) and Maïdo sites at Réunion Island (21°â€¯S, 55°â€¯E) with low vertical resolution. FTIR profile retrievals are performed by the well-established SFIT4 program and the detail retrieval strategies along with the systematic/random uncertainties of CFC-11, CFC-12 and HCFC-22 are discussed in this study. The FTIR data of all three species are sensitive to the whole troposphere and the lowermost stratosphere, with the peak sensitivity between 5 and 10â€¯km.
The ground-based FTIR data have been compared with the collocated Michelson Interferometer for Passive Atmospheric Sounding (MIPAS/ENVISAT) data and found to be in good agreement: the observed mean relative biases and standard deviations of the differences between the smoothed MIPAS and FTIR partial columns (6–30â€¯km) are (−4.3 and 4.4â€¯%), (−2.9 and 4.6â€¯%) and (−0.7 and 4.8â€¯%) for CFC-11, CFC-12 and HCFC-22, respectively, which are within the combined error budgets from both measurements. The season cycles of CFC-11, CFC-12 and HCFC-22 from FTIR measurements and MIPAS data show a similar variation: concentration is highest in February–April and lowest in August–October.
The trends derived from the combined St Denis and Maïdo FTIR time series are −0.86â€¯±â€¯0.12 and 2.84â€¯±â€¯0.06â€¯% year−1 for CFC-11 and HCFC-22, respectively, for the period 2004 to 2016, and −0.76â€¯±â€¯0.05â€¯% year−1 for CFC-12 for 2009 to 2016. These measurements are consistent with the trends observed by the National Oceanic and Atmospheric Administration (NOAA) Global Monitoring Division's (GMD) Halocarbons & other Atmospheric Trace Species Group (HATS) measurements at Samoa (14.2°â€¯S, 170.5°â€¯W) for CFC-11 (−0.87â€¯±â€¯0.04â€¯% year−1), but slightly weaker for HCFC-22 (3.46â€¯±â€¯0.05â€¯%) year−1 and stronger for CFC-12 (−0.60â€¯±â€¯0.02â€¯% year−1).