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AbstractWe have conducted a study to determine the influence of Asian pollution plumes on free tropospheric ozone above the west coast of the United States during spring. We also explored the additional impact of North American emissions on east coast free tropospheric ozone. Long-term ozone monitoring sites in the United States are few, but we obtained ozonesonde profiles from Trinidad Head on the west coast, Huntsville, Alabama, in the southeast, and Wallops Island, Virginia, on the east coast. Additional east coast ozone profiles were measured by the MOZAIC commercial aircraft at Boston, New York City, and Philadelphia. Kilometer-averaged ozone was compared between Trinidad Head and the three east coast sites (MOZAIC, Wallops Island, and Huntsville). Only in the 0-1 km layer did the MOZAIC site have a statistically significant greater amount of ozone than Trinidad Head. Likewise only the 0-1 and 1-2 km layers had greater ozone at Wallops Island and Huntsville in comparison to Trinidad Head. While Wallops Island did show greater ozone than Trinidad Head at 6-9 km, this excess ozone was attributed to a dry air mass sampling bias. A particle dispersion model was used to determine the surface source regions for each case, and the amount of anthropogenic NOx tracer that would have been emitted into each air mass. Transport times were limited to 20 days to focus on the impact of direct transport of pollution plumes from the atmospheric boundary layer. As expected, the amount of NOx tracer emitted into the east coast profiles was much greater in the lower and mid troposphere than at the west coast. At various altitudes at both coasts there existed a significant positive correlation between ozone and the NOx tracer, but the explained variance was generally less than 30%. On the east coast, Wallops Island had the weakest relationship between ozone and the NOx tracer, while Huntsville had the strongest. During spring, differences in photochemistry and transport pathways in the lowest 2 km of the troposphere results in an extra 5-14 ppbv of ozone on the east coast in comparison to Trinidad Head. However, despite differing amounts of NOx tracer from Asia and North America in the free troposphere, we found no significant difference in free tropospheric ozone between the east and west coasts of the United States during spring.
AbstractField measurements of a wide suite of trace gases and aerosols were carried out during April and May 2002, along with extensive chemical transport modeling, as part of the NOAA Intercontinental Transport and Chemical Transformation study. Here, we use a combination of in-situ ground-based measurements from Trinidad Head, CA, chemical transport modeling, and backward trajectory analysis to examine the impact of long-range transport from Asia on the composition of air masses arriving at the California coast at the surface. The impact of Asian emissions is explored in terms of both episodic enhancements and contribution to background concentrations. We find that variability in CO concentrations at the ground site was largely driven by North American emissions, and that individual Asian plumes did not cause any observable pollution enhancement episodes at Trinidad Head. Despite this, model simulations suggest that Asian emissions were responsible for 33% of the CO observed at Trinidad Head, providing a larger mean contribution than direct emissions from any other region of the globe. Surface ozone levels were found to depend primarily on local atmospheric mixing, with surface deposition leading to low concentrations under stagnant conditions. Model simulations suggested that on average 4 ± 1 ppb of ozone (10% of observed) at Trinidad Head was transported from Asia.
AbstractMulti-scale tracer and full-chemistry simulations with the STEM atmospheric chemistry model are used to analyze the effects of transported background ozone (O3) from the eastern Pacific on California air quality during the ARCTAS-CARB experiment conducted in June 2008. Previous work has focused on the importance of long-range transport of O3 to North America air quality in springtime. However during this summer experiment the long-range transport of O3 is also shown to be important. Simulated and observed O3 transport patterns from the coast to inland northern California are shown to vary based on meteorological conditions and the oceanic O3 profiles, which are strongly episodically affected by Asian inflows. Analysis of the correlations of O3 at various altitudes above the coastal site at Trinidad Head and at a downwind surface site in northern California, show that under long-range transport events, high O3 air-masses (O3>60 ppb) at altitudes between about 2 and 4 km can be transported inland and can significantly influence surface O3 20–30 h later. These results show the importance of characterizing the vertical structure of the lateral boundary conditions (LBC) needed in air quality simulations. The importance of the LBC on O3 prediction during this period is further studied through a series of sensitivity studies using different forms of LBC. It is shown that the use of the LBC downscaled from RAQMS global model that assimilated MLS and OMI data improves the model performance. We also show that the predictions can be further improved through the use of LBC based on NASA DC-8 airborne observations during the ARCTAS-CARB experiment. These results indicate the need to develop observational strategies to improve the representation of the vertical and temporal variations in the air over the eastern Pacific.
AbstractThe emissions of halogenated gases from the West Coast region of the United States are estimated from measurements from 1995 to 2003 at the Advanced Global Atmospheric Gases Experiment site at Trinidad Head, California. The emissions estimation procedure uses pollution events combined with population densities integrated along back trajectories, and the estimates are constrained by independent estimates of CH4 and N2O emissions from the U. S. West Coast region. The best fit, average emissions of CH4 and N2O and the average chloroform emissions in California, Oregon, and Washington combined from 1996 to 2002 are 44, 3.7, and 0.07 kg person(-1) yr(-1), respectively. The emissions per person of CFC-11 (CCl3F), CFC-2 (CCl2F2), CFC-113 (CCl2FCClF2), and methyl chloroform (CH3CCl3) from California in 1996-1998 are calculated to be factors of approximately 2.2, 1.3, 0.7, and 1.6, respectively, less (more for CFC-113) than those reported for the northeastern United States by Barnes et al. (2003). The emission per person of all these gases in the U. S. West Coast region decreased from 1998 to 1999 by a factor of 2 or more, but from 1999 to 2002 the estimated emissions of all four gases have remained fairly constant and are 0.016, 0.048, 0.002, and 0.006 kg person(-1) yr(-1), respectively. The methyl chloroform estimates suggest a delay of up to 1 year in the decline of the emissions from 1996 to 1998, but otherwise, and in 1999-2000, in contrast to the Millet and Goldstein (2004) results, they are in agreement with the average methyl chloroform emissions per person for the United States based on the UNEP country by country consumption figures (A. McCulloch, private communication, 2004). Averaging the Trinidad Head and the Barnes et al. (2003) per person estimates and multiplying by the U. S. population suggests average methyl chloroform emissions in the United States of 18 Gg yr(-1) in 1996 to 1998. In 2001-2002, if the ratio of the emissions per person in these two regions was the same as in 1996-1998, we estimate U. S. emissions of 2.2 Gg yr(-1), which is one half of the Millet and Goldstein (2004) estimate.
AbstractSeasonal cycles in the mixing ratios of tropospheric nitrous oxide (N[subscript 2]O) are derived by detrending long-term measurements made at sites across four global surface monitoring networks. The detrended monthly data display large interannual variability, which at some sites challenges the concept of a "mean" seasonal cycle. In the Northern Hemisphere, correlations between polar winter lower stratospheric temperature and detrended N[subscript 2]O data, around the month of the seasonal minimum, provide empirical evidence for a stratospheric influence, which varies in strength from year to year and can explain much of the interannual variability in the surface seasonal cycle. Even at sites where a strong, competing, regional N[subscript 2]O source exists, such as from coastal upwelling at Trinidad Head, California, the stratospheric influence must be understood to interpret the biogeochemical signal in monthly mean data. In the Southern Hemisphere, detrended surface N[subscript 2]O monthly means are correlated with polar spring lower stratospheric temperature in months preceding the N[subscript 2]O minimum, providing empirical evidence for a coherent stratospheric influence in that hemisphere as well, in contrast to some recent atmospheric chemical transport model (ACTM) results. Correlations between the phasing of the surface N[subscript 2]O seasonal cycle in both hemispheres and both polar lower stratospheric temperature and polar vortex break-up date provide additional support for a stratospheric influence. The correlations discussed above are generally more evident in high-frequency in situ data than in data from weekly flask samples. Furthermore, the interannual variability in the N[subscript 2]O seasonal cycle is not always correlated among in situ and flask networks that share common sites, nor do the mean seasonal amplitudes always agree. The importance of abiotic influences such as the stratospheric influx and tropospheric transport on N[subscript 2]O seasonal cycles suggests that, at sites remote from local sources, surface N[subscript 2]O mixing ratio data by themselves are unlikely to provide information about seasonality in surface sources, e.g., for atmospheric inversions, unless the ACTMs employed in the inversions accurately account for these influences. An additional abioitc influence is the seasonal ingassing and outgassing of cooling and warming surface waters, which creates a thermal signal in tropospheric N[subscript 2]O that is of particular importance in the extratropical Southern Hemisphere, where it competes with the biological ocean source signal
AbstractWe report ozonesonde observations from the following four locations across the United States: Trinidad Head, California; Boulder, Colorado; Huntsville, Alabama; and Wallops Island, Virginia. These ozone profiles clearly indicate evidence of stratosphere-troposphere exchange, boundary layer pollution, and strong seasonal variations. Significant variation at the shortest interlaunch frequencies (typically weekly) appears in all seasons, at all stations throughout the troposphere. Activity near the tropopause dominates in the winter and spring, while boundary layer ozone maximizes in the summer. The vertical extent and maximum values of boundary layer ozone are larger at the eastern stations. Comparisons to the TOMS overpasses indicate agreement to within 2% for the total-column ozone at all stations, with station-to-station mean biases less than 2%. The seasonal variation of the total ozone column is essentially identical at Trinidad Head and Wallops Island, while the summertime values at Boulder are significantly smaller by comparison, and the amplitude of the annual cycle at Huntsville is smaller than the amplitude of the other three stations. The longitudinal character of upper tropospheric ozone shows amounts generally increasing westward from Huntsville, and in the lower troposphere, ozone decreases westward from Huntsville in all seasons. Values to the east of Huntsville increase at all altitudes and seasons, with the possible exception of August when Huntsville's boundary layer and free-tropospheric ozone dominate.
AbstractDuring April 2008, as part of the International Polar Year (IPY), a number of ground-based and aircraft campaigns were carried out in the North American Arctic region (e.g., ARCTAS, ARCPAC). The widespread presence during this period of biomass burning effluent, both gaseous and particulate, has been reported. Unusually high ozone readings for this time of year were recorded at surface ozone monitoring sites from northern Alaska to northern California. At Barrow, Alaska, the northernmost point in the United States, the highest April ozone readings recorded at the surface (hourly average values >55 ppbv) in 37 years of observation were measured on April 19, 2008. At Denali National Park in central Alaska, an hourly average of 79 ppbv was recorded during an 8-h period in which the average was over 75 ppbv, exceeding the ozone ambient air quality standard threshold value in the U.S. Elevated ozone (>60 ppbv) persisted almost continuously from April 19–23 at the monitoring site during this event. At a coastal site in northern California (Trinidad Head), hourly ozone readings were >50 ppbv almost continuously for a 35-h period from April 18–20. At several sites in northern California, located to the east of Trinidad Head, numerous occurrences of ozone readings exceeding 60 ppbv were recorded during April 2008. Ozone profiles from an extensive series of balloon soundings showed lower tropospheric features at 1–6 km with enhanced ozone during the times of elevated ozone amounts at surface sites in western Canada and the U.S. Based on extensive trajectory calculations, biomass burning in regions of southern Russia was identified as the likely source of the observed ozone enhancements. Ancillary measurements of atmospheric constituents and optical properties (aerosol optical thickness) supported the presence of a burning plume at several locations. At two coastal sites (Trinidad Head and Vancouver Island), profiles of a large suite of gases were measured from airborne flask samples taken during probable encounters with burning plumes. These profiles aided in characterizing the vertical thickness of the plumes, as well as confirming that the plumes reaching the west coast of North America were associated with biomass burning events.
AbstractAn analysis of surface ozone measurements at a west coast site in northern California (Trinidad Head) demonstrates that this location is well situated to sample air entering the west coast of the US from the Pacific Ocean. During the seasonal maximum in the spring, this location regularly observes hourly average ozone mixing ratios >= 50 ppbv in air that is uninfluenced by the North American continent. Mean daytime values in the spring exceed 40 ppbv. A location in southern California (Channel Islands National Park) demonstrates many of the characteristics during the Spring as Trinidad Head in terms of air flow patterns and ozone amounts suggesting that background levels of ozone entering southern California from the Pacific Ocean are similar to those in northern California. Two inland locations (Yreka and Lassen Volcanic National Park) in northern California with surface ozone data records of 20 years or more are More difficult to interpret because of possible influences of local or regional changes. They show differing results for the long-term trend during the Spring. The 10-year ozone vertical profile measurements obtained with weekly ozonesondes at Trinidad Head show no significant longer-term change in tropospheric ozone. Published by Elsevier Ltd.
Abstract[ 1] As part of the Transport and Chemical Evolution over the Pacific (TRACE-P) mission, ozonesondes were used to make ozone vertical profile measurements at nine locations in the North Pacific. At most of the sites there is a multiyear record of observations. From locations in the western Pacific ( Hong Kong; Taipei; Jeju Island, Korea; and Naha, Kagoshima, Tsukuba, and Sapporo, Japan), a site in the central Pacific ( Hilo, Hawaii), and a site on the west coast of the United States ( Trinidad Head, California) both a seasonal and event specific picture of tropospheric ozone over the North Pacific emerges. Ozone profiles over the North Pacific generally show a prominent spring maximum throughout the troposphere. This maximum is tied to the location of the jet stream and its influence on stratosphere-troposphere exchange and the increase in photochemical ozone production through the spring. Prominent layers of enhanced ozone in the middle and upper troposphere north of about 30degrees N seem to be more closely tied to stratospheric intrusions while biomass burning leads to layers of enhanced ozone in the lower and upper troposphere at Hong Kong (22 degreesN) and Taipei (25 degreesN). The lower free tropospheric layers at Hong Kong are associated with burning in SE Asia, but the upper layer may be associated with either equatorial Northern Hemisphere burning in Africa or SE Asian biomass burning. In the boundary layer at Taipei very high mixing ratios of ozone were observed that result from pollution transport from China in the spring and local urban pollution during the summer. At the ozonesonde site near Tokyo ( Tsukuba, 36 degreesN) very large enhancements of ozone are seen in the boundary layer in the summer that are characteristic of urban air pollution. At sites in the mid and eastern Pacific the signature of transport of polluted air from Asia is not readily identifiable from the ozonesonde profile. This is likely due to the more subtle signal and the fact that from the ozone profile and meteorological data by themselves it is difficult to identify such a signal. During the TRACE-P intensive campaign period (February - April 2001), tropospheric ozone amounts were generally typical of those seen in the long-term records of the stations with multiyear soundings. The exception was the upper troposphere over Hong Kong and Taipei where ozone amounts were lower in 2001.
AbstractOzone sondes launched from Trinidad Head, California provide a measure of background O3 transported ashore, and allow an evaluation of the impact of this transport on air quality in California's Northern Sacramento Valley. A strong summertime vertical O3 gradient and correlation analysis indicate that O3-rich air from above the marine boundary layer is transported to the surface. Surface O3 is found to increase proportionally to the transported background. At the surface site experiencing the highest O3 concentrations, the mean maximum daily 8-h average (MDA8) O3 on exceedance days (i.e. those days when MDA8 O3 exceeds 75 ppbv) is 20 ppbv higher than on non-exceedance days. The transported background O3, as measured 22 h earlier by the Trinidad Head sondes, accounts for more than half (11 ppbv) of this difference. This finding contrasts with conclusions from model calculations that indicate the US policy relevant O3 background is generally 15–35 ppbv, and that it is lower, rather than higher, during pollution episodes. The present work indicates that O3 transported on hemispheric scales substantially impacts air quality in some areas of the US.
HCFC-22 (CHClF2, chlorodifluoromethane) is an ozone-depleting substance (ODS) as well as a significant greenhouse gas (GHG). HCFC-22 has been used widely as a refrigerant fluid in cooling and air-conditioning equipment since the 1960s, and it has also served as a traditional substitute for some chlorofluorocarbons (CFCs) controlled under the Montreal Protocol. A low frequency record on tropospheric HCFC-22 since the late 1970s is available from measurements of the Southern Hemisphere Cape Grim Air Archive (CGAA) and a few Northern Hemisphere air samples (mostly from Trinidad Head) using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. Since the 1990s high-frequency, high-precision, in situ HCFC-22 measurements have been collected at these AGAGE stations. Since 1992, the Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected flasks on a weekly basis from remote sites across the globe and analyzed them for a suite of halocarbons including HCFC-22. Additionally, since 2006 flasks have been collected approximately daily at a number of tower sites across the US and analyzed for halocarbons and other gases at NOAA. All results show an increase in the atmospheric mole fractions of HCFC-22, and recent data show a growth rate of approximately 4% per year, resulting in an increase in the background atmospheric mole fraction by a factor of 1.7 from 1995 to 2009. Using data on HCFC-22 consumption submitted to the United Nations Environment Programme (UNEP), as well as existing bottom-up emission estimates, we first create globally-gridded a priori HCFC-22 emissions over the 15 yr since 1995. 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. Our inversion indicates that the global HCFC-22 emissions have an increasing trend between 1995 and 2009. We further find a surge in HCFC-22 emissions between 2005 and 2009 from developing countries in Asia – the largest emitting region including China and India. Globally, substantial emissions continue despite production and consumption being phased out in developed countries currently.
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.
 The tropospheric seasonal cycles of N2O, CFC-11 (CCl3F), and CFC-12 (CCl2F2) are influenced by atmospheric dynamics. The interannually varying summertime minima in mole fractions of these trace gases have been attributed to interannual variations in mixing of stratospheric air (depleted in CFCs and N2O) with tropospheric air with a few months lag. The amount of wave activity that drives the stratospheric circulation and influences the winter stratospheric jet and subsequent mass transport across the tropopause appears to be the primary cause of this interannual variability. We relate the observed seasonal minima of species at three Northern Hemisphere sites (Mace Head, Ireland; Trinidad Head, U.S.; and Barrow, Alaska) with the behavior of the winter stratospheric jet. As a result, a good correlation is obtained between zonal winds in winter at 10 hPa, 58°N–68°N, and the detrended seasonal minima in the stratosphere-influenced tracers. For these three tracers, individual Pearson correlation coefficients (r) between 0.51 and 0.71 were found, with overall correlations of between 0.67 and 0.77 when “composite species” were considered. Finally, we note that the long-term observations of CFCs and N2O in the troposphere provide an independent monitoring method complementary to satellite data. Furthermore, they could provide a useful observational measure of the strength of stratosphere-troposphere exchange and, thus, could be used to monitor any long-term trend in the Brewer-Dobson circulation which is predicted by climate models to increase over the coming decades.
Much attention has been focused on the transport of ozone (O3) to the western U.S., particularly given the latest revision of the National Ambient Air Quality Standard to 70 parts per billion by volume (ppbv) of O3. This makes quantifying the contributions of stratosphere-to-troposphere exchange, local pollution, and pollution transport to this region essential. To evaluate free-tropospheric and surface O3 in the western U.S., we use self-organizing maps to cluster 18 years of ozonesonde profiles from Trinidad Head, CA. Three of nine O3 mixing ratio profile clusters exhibit thin laminae of high O3 above Trinidad Head. The high O3 layers are located between 1 and 6 km above mean sea level and reside above an inversion associated with a northern location of the Pacific subtropical high. Ancillary data (reanalyses, trajectories, and remotely sensed carbon monoxide) help identify the high O3 sources in one cluster, but distinguishing mixed influences on the elevated O3 in other clusters is difficult. Correlations between the elevated tropospheric O3 and surface O3 at high-altitude monitors at Lassen Volcanic and Yosemite National Parks, and Truckee, CA, are marked and long lasting. The temporal correlations likely result from a combination of transport of baseline O3 and covarying meteorological parameters. Days corresponding to the high O3 clusters exhibit hourly surface O3 anomalies of +5–10 ppbv compared to a climatology; the positive anomalies can last up to 3 days after the ozonesonde profile. The profile and surface O3 links demonstrate the importance of regular ozonesonde profiling at Trinidad Head.
High precision measurements of three chlorofluorocarbons (CFCs), three hydrochlorofluorocarbons (HCFCs), six hydrofluorocarbons (HFCs), three perfluorocarbons (PFCs), and sulfur hexafluoride (SF6) were made at five Chinese background stations from January 2011 to December 2012. Their station means in the background air were 239.5 ± 0.69 parts-per-trillion dry-air mole fraction mixing ratios (ppt) for CFC-11, 536.5 ± 1.49 ppt for CFC-12, 74.66 ± 0.09 ppt for CFC-113, 232.1 ± 4.77 ppt for HCFC-22, 23.78 ± 0.29 ppt for HCFC-141b, 22.92 ± 0.42 ppt for HCFC-142b, 11.75 ± 0.43 ppt for HFC-125, 71.32 ± 1.35 ppt for HFC-134a, 13.62 ± 0.43 ppt for HFC-143a, 9.10 ± 1.26 ppt for HFC-152a, 25.45 ± 0.1 ppt for HFC-23, 7.28 ± 0.48 ppt for HFC-32, 4.32 ± 0.03 ppt for PFC-116, 0.63 ± 0.04 ppt for PFC-218, 1.36 ± 0.01 ppt for PFC-318, and 7.67 ± 0.03 ppt for SF6, respectively, which were comparable with those measured at the two Northern Hemisphere (NH) AGAGE stations: Mace Head, Ireland (MHD) and Trinidad Head, California, USA (THD). Compared with our results for earlier years from in-situ measurement at SDZ, background-air mixing ratios of CFCs are now declining, while those for HCFCs, HFCs, PFCs, and SF6 are still increasing. The ratios of the number of sampling events in which measured mixing ratios were elevated above background (pollution events) relative to the total sample frequency (POL/SUM) for CFCs, HCFCs, and HFCs were found to be station dependent, generally LAN > SDZ > LFS > XGL > WLG. The enhancement (â–³, polluted mixing ratios minus background mixing ratios) generally show distinct patterns, with HCFCs (40.7–175.4 ppt) > HFCs (15.8–66.3 ppt)> CFCs (15.8–33.8 ppt)> PFCs (0.1–0.9 ppt) at five stations, especially for HCFC-22 ranging from 36.9 ppt to 138.2 ppt. Combining with the molecular weights, our findings imply biggest emissions of HCFCs in the regions around these Chinese sites compared to HFCs and CFCs, while the smallest of PFCs, consistent with CFCs being phased out and replaced with HCFCs in China. In addition, relative emission strengths (emission was expressed by mole fractions) of these halocarbons in China were inferred as HCFC-22 > HCFC-141b > HFC-134a > HCFC-142b for the Yangtze River Delta (YRD) and as HCFC-22 > HCFC-142b > HCFC-141b ≈ HFC-134a in the North China Plain (NCP).