Stratospheric Intrusions Research Articles

Measurements of Humidity in the Atmosphere and Validation Experiments (MOHAVE)-2009: overview of campaign operations and results

Abstract. The Measurements of Humidity in the Atmosphere and Validation Experiment (MOHAVE) 2009 campaign took place on 11–27 October 2009 at the JPL Table Mountain Facility in California (TMF). The main objectives of the campaign were to (1) validate the water vapor measurements of several instruments, including, three Raman lidars, two microwave radiometers, two Fourier-Transform spectrometers, and two GPS receivers (column water), (2) cover water vapor measurements from the ground to the mesopause without gaps, and (3) study upper tropospheric humidity variability at timescales varying from a few minutes to several days. A total of 58 radiosondes and 20 Frost-Point hygrometer sondes were launched. Two types of radiosondes were used during the campaign. Non negligible differences in the readings between the two radiosonde types used (Vaisala RS92 and InterMet iMet-1) made a small, but measurable impact on the derivation of water vapor mixing ratio by the Frost-Point hygrometers. As observed in previous campaigns, the RS92 humidity measurements remained within 5% of the Frost-point in the lower and mid-troposphere, but were too dry in the upper troposphere. Over 270 h of water vapor measurements from three Raman lidars (JPL and GSFC) were compared to RS92, CFH, and NOAA-FPH. The JPL lidar profiles reached 20 km when integrated all night, and 15 km when integrated for 1 h. Excellent agreement between this lidar and the frost-point hygrometers was found throughout the measurement range, with only a 3% (0.3 ppmv) mean wet bias for the lidar in the upper troposphere and lower stratosphere (UTLS). The other two lidars provided satisfactory results in the lower and mid-troposphere (2–5% wet bias over the range 3–10 km), but suffered from contamination by fluorescence (wet bias ranging from 5 to 50% between 10 km and 15 km), preventing their use as an independent measurement in the UTLS. The comparison between all available stratospheric sounders allowed to identify only the largest biases, in particular a 10% dry bias of the Water Vapor Millimeter-wave Spectrometer compared to the Aura-Microwave Limb Sounder. No other large, or at least statistically significant, biases could be observed. Total Precipitable Water (TPW) measurements from six different co-located instruments were available. Several retrieval groups provided their own TPW retrievals, resulting in the comparison of 10 different datasets. Agreement within 7% (0.7 mm) was found between all datasets. Such good agreement illustrates the maturity of these measurements and raises confidence levels for their use as an alternate or complementary source of calibration for the Raman lidars. Tropospheric and stratospheric ozone and temperature measurements were also available during the campaign. The water vapor and ozone lidar measurements, together with the advected potential vorticity results from the high-resolution transport model MIMOSA, allowed the identification and study of a deep stratospheric intrusion over TMF. These observations demonstrated the lidar strong potential for future long-term monitoring of water vapor in the UTLS.

Regional and global modeling estimates of policy relevant background ozone over the United States

Abstract Policy Relevant Background (PRB) ozone, as defined by the US Environmental Protection Agency (EPA), refers to ozone concentrations that would occur in the absence of all North American anthropogenic emissions. PRB enters into the calculation of health risk benefits, and as the US ozone standard approaches background levels, PRB is increasingly important in determining the feasibility and cost of compliance. As PRB is a hypothetical construct, modeling is a necessary tool. Since 2006 EPA has relied on global modeling to establish PRB for their regulatory analyses. Recent assessments with higher resolution global models exhibit improved agreement with remote observations and modest upward shifts in PRB estimates. This paper shifts the paradigm to a regional model (CAMx) run at 12 km resolution, for which North American boundary conditions were provided by a low-resolution version of the GEOS-Chem global model. We conducted a comprehensive model inter-comparison, from which we elucidate differences in predictive performance against ozone observations and differences in temporal and spatial background variability over the US. In general, CAMx performed better in replicating observations at remote monitoring sites, and performance remained better at higher concentrations. While spring and summer mean PRB predicted by GEOS-Chem ranged 20–45 ppb, CAMx predicted PRB ranged 25–50 ppb and reached well over 60 ppb in the west due to event-oriented phenomena such as stratospheric intrusion and wildfires. CAMx showed a higher correlation between modeled PRB and total observed ozone, which is significant for health risk assessments. A case study during April 2006 suggests that stratospheric exchange of ozone is underestimated in both models on an event basis. We conclude that wildfires, lightning NOx and stratospheric intrusions contribute a significant level of uncertainty in estimating PRB, and that PRB will require careful consideration in the ozone standard setting process.

Attributes of dynamical events to tropospheric ozone distribution over equatorial africa

Volcanic activity, biological decay, forest fi res, thunderstorm events and stratospheric intrusions are key sources that introduce atmospheric traces to the troposphere. Ozone is one of such traces which can be found in very high concentration than its normal level due to natural factors. Upper and middle tropospheric ozone act as a green house gas while ozone found in high concentration at lower troposphere is a pollutant that harms living organisms. In few ozone and relative humidity data records by measurements of ozone by airbus in service aircraft (MOZAIC), spikes were observed at a fl ying altitude of 250‐200 hPa at equatorial Africa. Equatorial Africa is one of the three thunderstorm hot spot regions (South America, Equatorial Africa and Southeast Asia) of the world. This work discusses how ozone of stratospheric origin produced enhanced ozone over the troposphere of equatorial Africa and its redistribution due to dynamical events. To understand the events that attribute to spiky MOZAIC ozone and relative humidity observations, in addition to MOZAIC ozone and relative humidity, data sets from different sources were used for diagnosis. Meridional cross-section of potential vorticity over the region of interest showed high potential vorticity (PV) intrusion below the tropopause level that induced enhanced ozone into upper troposphere. Vertical wind fi elds in the regions of low outgoing long wave radiation (OLR), very high latent heat and cloud liquid water content transport have indicated presence of convection and thunderstorm events. Enhanced ozone of stratospheric origin, as revealed by GOME satellite data produced during stratospheric intrusion, transported from the stratosphere all the way down to the boundary layer. Convective erosion was found to scavenge ozone concentration mainly at the boundary layers between 1000 and 700 hPa and enhanced ozone volume mixing ratio (VMR) of 60‐100 ppbv which exceeds the WHO guideline limit of 60 ppbv were observed. These events have led to ozone pollution.

The impact of transported ozone-rich air on the atmospheric ozone content following the 26 January 2001 and 7 March 2006 Gujarat earthquakes

The contribution of transport processes to the observed ozone concentration following the 26 January 2001 and 7 March 2006 earthquakes in the Kutch region of Gujarat is presented. The analysis of back trajectories at different altitudes and vertical pressure velocities at the tropopause indicated the transport of ozone-rich air from higher latitudes in the tropospheric and lower stratospheric regions apart from stratospheric intrusion of ozone into the troposphere along the path of the back trajectory and its transport to the epicentre during these earthquakes.

Ozone Air Pollution: How Low Can You Go?

Ozone Air Pollution: How Low Can You Go?

The importance of stratospheric–tropospheric transport in affecting surface ozone concentrations in the western and northern tier of the United States

Stratospheric–tropospheric exchange (STE) processes contribute at both high and low-elevation monitoring sites to background ozone (O3) concentrations. This study addresses the importance of stratospheric intrusions contributing to enhanced hourly average surface O3 concentrations (i.e., ≥50 ppb) at 12 O3 monitoring stations in the western and northern tier of the US for 2006, 2007, and 2008. The Lagrangian Analysis Tool (LAGRANTO) trajectory model identified specific days when stratosphere-to-troposphere transport was optimal to elevate surface O3 levels. The coincidences between the number of days with a daily maximum hourly average O3 concentration ≥ 50 ppb and stratosphere-to-troposphere transport to surface (STT-S > 0) were quantified. The high-elevation site at Yellowstone National Park (NP) in Wyoming exhibited the most coincidences (i.e., more than 19 days a month) during the spring and summer for hourly average O3 concentrations ≥ 50 ppb with STT-S > 0 of the 12 monitoring sites. At this site, the daily maximum hourly springtime average O3 concentrations were usually in the 60–70 ppb range. The maximum daily 8-h average concentrations mostly ranged from 50 to 65 ppb. At many of the lower-elevation sites, there was a preference for O3 enhancements to be coincident with STT-S > 0 during the springtime, although summertime occurrences were sometimes observed. When statistically significant coincidences occurred, the daily maximum hourly average concentrations were mostly in the 50–65 ppb range and the daily maximum 8-h average concentrations were usually in the 50–62 ppb range. For many cases, the coincidences between the enhancements and the STT-S events occurred over a continuous multiday period. Supplementary observations, such as (1) the greater frequency of O3 concentration enhancements occurring during the springtime versus other times of the year, (2) the elevation dependency of the frequency of enhancements, (3) the year-to-year variability, (4) the timing of the hour-by-hour occurrences of the O3 concentration enhancements within and across monitoring sites, and (5) the detailed analyses of O3 enhancement events at specific sites, provide additional support for our modeling and statistical results. Our analysis provides an important step in better understanding the variability of natural background O3 concentrations. The study has provided insight into stratospheric intrusions, with emphasis on the combined role of quasi-isentropic large-scale advection and mesoscale boundary layer turbulence for stratospheric air influencing enhanced surface O3.

Transport analysis of ozone enhancement in Southern Ontario during BAQS-Met

Abstract. Twice-daily ozonesondes were launched from Harrow, in southwestern Ontario, Canada, during the BAQS-Met (Border Air Quality and Meteorology Study) field campaign in June and July of 2007. A co-located radar windprofiler measured tropopause height continuously. These data, in combination with continuous surface ozone measurements and geo-statistical interpolation of satellite ozone observations, present a consistent picture and indicate that a number of significant ozone enhancements in the troposphere were observed that were the result of stratospheric intrusion events. The combined observations have also been compared with results from two Environment Canada numerical models, the operational weather prediction model GEM (as input to FLEXPART), and a new version of the regional air quality model AURAMS, in order to examine the ability of these models to accurately represent sporadic cross-tropopause ozone transport events. The models appear to reproduce intrusion events with some skill, implying that GEM dynamics (which also drive AURAMS) are able to represent such events well. There are important differences in the quantitative comparison, however; in particular, the poor vertical resolution of AURAMS around the tropopause causes it to bring down too much ozone in individual intrusions. These campaign results imply that stratospheric intrusions are important to the ozone budget of the mid-latitude troposphere, and appear to be responsible for much of the variability of ozone in the free troposphere. GEM-FLEXPART calculations indicate that stratospheric ozone intrusions contributed significantly to surface ozone on several occasions during the BAQS-Met campaign, and made a moderate but significant contribution to the overall tropospheric ozone budget.

Transport pathways and signatures of mixing in the extratropical tropopause region derived from Lagrangian model simulations

[1] Model simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) driven by wind fields of the National Center for Environmental Prediction (NCEP) were performed in the midlatitude tropopause region in April 2008 to study two research flights conducted during the START08 campaign. One flight targeted a deep tropospheric intrusion and another flight targeted a deep stratospheric intrusion event, both of them in the vicinity of the subtropical and polar jet. Air masses with strong signatures of mixing between stratospheric and tropospheric air masses were identified from measured CO-O3 correlations, and the characteristics were reproduced by CLaMS model simulations. CLaMS simulations in turn complement the observations and provide a broader view of the mixed region in physical space. Using artificial tracers of air mass origin within CLaMS yields unique information about the transport pathways and their contribution to the composition in the mixed region from different transport origins. Three different regions are examined to categorize dominant transport processes: (1) on the cyclonic side of the polar jet within tropopause folds where air from the lowermost stratosphere and the cyclonic side of the jet is transported downward into the troposphere, (2) on the anticyclonic side of the polar jet around the 2 PVU surface air masses, where signatures of mixing between the troposphere and lowermost stratosphere were found with large contributions of air masses from low latitudes, and (3) in the lower stratosphere associated with a deep tropospheric intrusion originating in the tropical tropopause layer (TTL). Moreover, the time scale of transport from the TTL into the lowermost stratosphere is in the range of weeks whereas the stratospheric intrusions occur on a time scale of days.

Non-Convective High Winds Associated with Extratropical Cyclones

Non-convective high winds are a damaging and potentially life-threatening weather phenomenon that occurs in the absence of thunderstorms, tornadoes and tropical cyclones. The vast majority of non-convective high wind events develop in association with extratropical cyclones in mid-latitude regions. Interest in non-convective high winds is growing due to their societal impact, gaps in the scientific understanding of the triggering mechanisms for these events, and possible future changes in their frequency and intensity caused by climate change. In this article, non-convective high winds are examined first in terms of their historical and cultural significance and climatological characteristics. Then, four possible mechanisms for the development of non-convective high winds in extratropical cyclones are discussed and critiqued: topography; the isallobaric wind; tropopause folds associated with stratospheric intrusions and dry slots; and sting jets associated with marine frontal cyclones. Evidence for past and future trends in non-convective high wind event frequency and intensity is also briefly examined. New avenues for future work in this emerging area of research are suggested that unite applied and basic research as well as climatological and case-study perspectives.

Seasonal stratospheric intrusion of ozone in the upper troposphere over India

Abstract. The Model for Ozone and Related chemical Tracers-2 (MOZART-2) is used to examine the evolution of pollutant O3 in the upper troposphere over the Indian region. Vertical profiles of ozone mixing ratio retrieved from Microwave Limb Sounder (MLS) aboard Earth Observing System (EOS) AURA satellite for the period 2005–2009 and Tropospheric Emission Spectrometer (TES) aboard (EOS) AURA for the period 2006–2007 has been analyzed. The satellite observations reveal the evidence of downward propagation of ozone (100–200 ppb) due to stratospheric intrusion during the winter and pre-monsoon seasons. The regular feature of enhancement of ozone in the upper troposphere over India is presented. Results obtained by the MOZART-2 simulations (for years 2000–2005) confirm the observations and indicate stratospheric intrusion of O3 during winter and pre-monsoon seasons. Observed enhanced O3 mixing ratio in the upper troposphere is explained by, variation of Potential Vorticity (PV), tropopause pressure, relative humidity and CO-O3 correlation.

A deep stratospheric intrusion event down to the earth’s surface of the megacity of Athens

This case study investigates a stratospheric intrusion event down to the earth’s surface (near sea-level pressure) of the greater area of Athens (23.43°E 37.58°N), which occurred on 9 October 2003 and caused a remarkable increase in surface ozone concentrations not related to photochemical production. This event is among the rare case studies investigating, on the one hand, a deep stratospheric intrusion down to the earth’s surface at near sea-level pressure and, on the other, an event affecting the near surface ozone of a megacity such as Athens. The synoptic situation is described by a deep upper lever trough at 300 and 500 hPa extending over Greece, which is related to a deep tropopause fold as revealed by vertical cross sections of potential vorticity, relative humidity, divergence and vertical velocity. The analysis of potential vorticity at several isentropic levels indicates a hook-shaped streamer of high PV values (greater than 4 pvu at the 315 K isentropic level) over southeast Europe, which coincides with a streamer of dry air as observed from satellite images of water vapor. The aforementioned structure characterizes a textbook case study of stratosphere-to-troposphere transport. The Lagrangian particle dispersion model FLEXPART was used to calculate the trajectories of air particles reaching the receptor site and the fraction of particles with stratospheric origin. It reveals an important direct stratospheric impact within 1 day related to the tropopause fold described in this study with the fraction of stratospheric particles reaching maximum values of 1.9 and 4.5% for threshold values of the dynamical tropopause 2 and 1.5 pvu, respectively. Furthermore, a larger indirect aged stratospheric contribution is also revealed 4 to 5 days prior to the release, related to stratospheric intrusion events at the western Atlantic Ocean, reaching maximum values of 2.5 and 6.9% of particles crossing the 2 and 1.5 pvu potential vorticity surfaces, respectively.

Descent of deep stratospheric intrusions during the IONS August 2006 campaign

Deep stratosphere‐to‐troposphere transport (STT) conveying ozone‐rich stratospheric air to the lower troposphere in the extratropics can episodically increase ozone concentrations in the lower troposphere. However, dynamical aspects of the descent, including dispersion and mixing with the surrounding tropospheric air and necessary conditions for reaching the lower troposphere, are not clearly understood yet. This study focuses on August 2006, as daily balloon sonde measurements were made from many sites covering North America within the Intercontinental Chemical Transport Experiment Ozonesonde Network Study campaign. During this period, four profiles were found with clear signs of deep STT. A mesoscale model was used together with trajectory calculation to represent these events. Over 10 days, 20 distinct clusters of trajectories were identified as significant deep STT events, including three observed. The four largest clusters carried 41, 35, 25, and 16 × 1012 kg of mass of air, respectively. A dynamical analysis was performed on the three observed events that were captured numerically. The descents showed three distinct phases: (1) crossing of the tropopause, (2) free descent, and (3) quasi‐horizontal dispersion in the lower troposphere. Clusters are rapidly sliding down sloping isentropes while being slowly diabatically cooled (approximately −1 K d−1). The tilt in the isentropes along the descent is due to an approximately equal combination of a negative potential temperature anomaly at the tropopause during phase 1 and a nearby baroclinic zone at the ground. The combination of these two conditions appears to be necessary for reaching the lower troposphere. In the three cases, the clusters stayed compact until they reach the lower troposphere, and it is estimated that approximately 80% of the ozone of stratospheric origin is released directly in the lower troposphere.

Acetone in the upper troposphere/lowermost stratosphere measured by the CARIBIC passenger aircraft: Distribution, seasonal cycle, and variability

Mass‐spectrometric measurements of acetone (CH3COCH3) have been performed monthly using a Lufthansa Airbus A340‐600 passenger aircraft between February 2006 and December 2008. In total, 106 measurement flights (4 per month) were conducted between Germany and South America, North America, South Asia, and East Asia. Here measurements collected between 33°N and 56°N in the upper troposphere (UT) and lowermost stratosphere (LMS) at 9–12 km altitude are analyzed. By integrating data collected at 12 ozonesonde stations, ozone concentrations measured on flight are translated into a representative (mixing‐based) altitude above the thermal tropopause. A strong seasonal variation of acetone occurs at the midlatitude tropopause with maxima of ∼900 parts per 1012 vol (pptv) in summer and minima of ∼200 pptv in midwinter. This seasonality propagates into the LMS in approximately 6 weeks with rapidly decreasing concentrations and increasing phase shifts reaching 2 km above the tropopause. Throughout the year, acetone and ozone are highly negatively correlated in the LMS with a mean linear correlation coefficient (R) of −0.93. This linear relationship marks the O3–acetone‐based extratropical tropopause mixing layer (exTL). A “stratospheric intrusion height of acetone” (Zacetone) is defined that concurs with the vertical depth of the O3–CO‐based exTL, namely, averaging ∼2.2 km but with slightly lower values in winter. Probability density functions (PDFs) and the course of the seasonal variation of acetone relative to the tropopause are interpreted regarding the in‐mixing and subsequent dispersion of acetone in the LMS.

Tropospheric ozone variations at the Nepal Climate Observatory-Pyramid (Himalayas, 5079 m a.s.l.) and influence of deep stratospheric intrusion events

Abstract. The paper presents the first 2 years of continuous surface ozone (O3) observations and systematic assessment of the influence of stratospheric intrusions (SI) at the Nepal Climate Observatory at Pyramid (NCO-P; 27°57' N, 86°48' E), located in the southern Himalayas at 5079 m a.s.l.. Continuous O3 monitoring has been carried out at this GAW-WMO station in the framework of the Ev-K2-CNR SHARE and UNEP ABC projects since March 2006. Over the period March 2006–February 2008, an average O3 value of 49±12 ppbv (±1δ) was recorded, with a large annual cycle characterized by a maximum during the pre-monsoon (61±9 ppbv) and a minimum during the monsoon (39±10 ppbv). In general, the average O3 diurnal cycles had different shapes in the different seasons, suggesting an important interaction between the synoptic-scale circulation and the local mountain wind regime. Short-term O3 behaviour in the middle/lower troposphere (e.g. at the altitude level of NCO-P) can be significantly affected by deep SI which, representing one of the most important natural input for tropospheric O3, can also influence the regional atmosphere radiative forcing. To identify days possibly influenced by SI at the NCO-P, a specially designed statistical methodology was applied to the time series of observed and modelled stratospheric tracers. On this basis, during the 2-year investigation, 14.1% of analysed days were found to be affected by SI. The SI frequency showed a clear seasonal cycle, with minimum during the summer monsoon (1.2%) and higher values during the rest of the year (21.5%). As suggested by back-trajectory analysis, the position of the subtropical jet stream could play an important role in determining the occurrence of deep SI transport on the southern Himalayas. We estimated the fraction of O3 due to SI at the NCO-P. This analysis led to the conclusion that during SI O3 significantly increased by 27.1% (+13 ppbv) with respect to periods not affected by such events. Moreover, the integral contribution of SI (O3S) to O3 at the NCO-P was also calculated, showing that up to 13.7% of O3 recorded at the measurement site could be possibly attributed to SI. On a seasonal basis, the lowest SI contributions were found during the summer monsoon (less than 0.1%), while the highest were found during the winter period (up to 24.2%). Even considering the rather large uncertainty associated with these estimates, the obtained results indicated that, during non-monsoon periods, high O3 levels could affect NCO-P during SI, thus influencing the variability of tropospheric O3 over the southern Himalayas.

A study of tropospheric ozone column enhancements over North America using satellite data and a global chemical transport model

Tropospheric ozone columns (TCOs) have been calculated from the differences between the Aura Ozone Monitoring Instrument (OMI) Total Ozone Mapping System (TOMS) total ozone (level 2 version 3) and the Aura Microwave Limb Sounding (MLS) measurements of stratospheric ozone (version 2.2). These OMI‐MLS TCOs were compared against ozonesonde measurements from the Intercontinental Chemical Transport Experiment (INTEX) Ozonesonde Network Study (IONS) campaign over North America in spring and summer, 2006. The OMI‐MLS potential vorticity mapped TCOs are smaller than IONS TCOs by 5.9 DU (9.9 ppb when expressed as volume mixing ratio) with a standard deviation of the differences of 8.4 DU (14.4 ppb) and a standard error of the mean differences of approximately 0.5 DU (0.7 ppb). Compared to previously published versions, these OMI‐MLS TCOs are an additional 2 DU smaller relative to ozonesonde measurements. The extra 2 DU arises from changes in OMI (∼−3 to −6 DU) and MLS (−1 to 3 DU), giving a net change of −2 DU. OMI‐MLS TCOs derived using OMI Differential Optical Absorption Spectroscopy (DOAS) show similar differences in summer, but these TCOs are smaller than the sondes by only 2 DU (5 ppb) in spring. OMI‐MLS TCOs derived from TOMS total ozone retrievals lead to better results when validated against IONS data, with less noise and a better seasonal consistency. Tropospheric ozone columns were also compared to those from GEOS‐Chem model simulations in main distribution features. In the spring and summer of 2005 and 2006, the most dominant enhancement features are a tongue of enhancement stretching from around Yellow Sea northeastward into the Pacific and an enhancement band over the North America centered over the eastern United States and the adjacent ocean. The OMI‐MLS TCO enhancements over the western Pacific and over the eastern United States increased from March to June and then decreased. In the GEOS‐Chem model simulations, the monthly variation tendency is similar to that of satellite data over the west Pacific but the decrease tendency from June into August over eastern United States is less dramatic. A springtime TCO enhancement event of a few days duration over coastal California was investigated to demonstrate the ability of OMI‐MLS mapped TCO columns in capturing ozone enhancements associated with stratospheric intrusions and trans‐Pacific transport. Tagged ozone model simulations support the stratospheric contributions to the high TCOs over coastal California and over the Baja peninsula, and meteorological fields indicate that the stratospheric intrusions are associated with Rossby wave breaking events. Furthermore, back trajectory studies and comparisons of GEOS‐Chem standard simulations and sensitivity runs with Asia anthropogenic emissions turned off provide evidence that the high tropospheric ozone columns over coastal California near Santa Barbara, California, has been influenced by cross‐Pacific transport. Two‐day‐average maps of tropospheric ozone columns from Aura OMI‐MLS TCOs also indicate cross‐Pacific propagating features.

What causes the springtime tropospheric ozone maximum over Northeast Asia?

Scientists have long debated the relative importance of tropospheric photochemical production versus stratospheric influx as causes of the springtime tropospheric ozone maximum over northern mid-latitudes. This paper investigates whether or not stratospheric intrusion and photochemistry play a significant role in the springtime ozone maximum over Northeast Asia, where ozone measurements are sparse. We examine how tropospheric ozone seasonalities over Naha (26°N, 128°E), Kagoshima (31°N, 131°E), and Pohang (36°N, 129°E), which are located on the same meridional line, are related to the timing and location of the jet stream. The ozone seasonality shows a gradual increase from January to the maximum ozone month, which corresponds to April at Naha, May at Kagoshima, and June at Pohang. In order to examine the occurrence of stratospheric intrusion, we analyze a correlation between jet stream activity and tropospheric ozone seasonality. From these analyses, we did not find any favorable evidence supporting the hypothesis that the springtime enhancement may result from stratospheric intrusion. According to trajectory analysis for vertical and horizontal origins of the airmass, a gradual increasing tendency in ozone amounts from January until the onset of monsoon was similar to the increasing ozone formation tendency from winter to spring over mainland China, which has been observed during the build-up of tropospheric ozone over Central Europe in the winter-spring transition period due to photochemistry. Overall, the analyses suggest that photochemistry is the most important contributor to observed ozone seasonality over Northeast Asia.

Winter- and summertime continental influences on tropospheric O<sub>3</sub> and CO observed by TES over the western North Atlantic Ocean

Abstract. The distributions of tropospheric ozone (O3) and carbon monoxide (CO), and the synoptic factors regulating these distributions over the western North Atlantic Ocean during winter and summer were investigated using profile retrievals from the Tropospheric Emission Spectrometer (TES) for 2004–2006. Seasonal composites of TES retrievals, reprocessed to remove the influence of the a priori on geographical and seasonal structure, exhibited strong seasonal differences. At the 681 hPa level during winter months of December, January and February (DJF) the composite O3 mixing ratios were uniformly low (~45 ppbv), but continental export was evident in a channel of enhanced CO (100–110 ppbv) flowing eastward from the US coast. In summer months June, July, and August (JJA) O3 mixing ratios were variable (45–65 ppbv) and generally higher due to increased photochemical production. The summer distribution also featured a channel of enhanced CO (95–105 ppbv) flowing northeastward around an anticyclone and exiting the continent over the Canadian Maritimes around 50° N. Offshore O3-CO slopes were generally 0.15–0.20 mol mol−1 in JJA, indicative of photochemical O3 production. Composites for 4 predominant synoptic patterns or map types in DJF suggested that export to the lower free troposphere (681 hPa level) was enhanced by the warm conveyor belt airstream of mid-latitude cyclones while stratospheric intrusions increased TES O3 levels at 316 hPa. A major finding in the DJF data was that offshore 681 hPa CO mixing ratios behind cold fronts could be enhanced up to >150 ppbv likely by lofting from the surface via shallow convection resulting from rapid destabilization of cold air flowing over much warmer ocean waters. In JJA composites for 3 map types showed that the general export pattern of the seasonal composites was associated with a synoptic pattern featuring the Bermuda High. However, weak cyclones and frontal troughs could enhance offshore 681 hPa CO mixing ratios to >110 ppbv with O3-CO slopes >0.50 mol mol−1 south of 45° N. Intense cyclones, which were not as common in the summer, enhanced export by lofting of boundary layer pollutants from over the US and also provided a possible mechanism for transporting pollutants from boreal fire outflow southward to the US east coast. Overall, for winter and summer the TES retrievals showed substantial evidence of air pollution export to the western North Atlantic Ocean with the most distinct differences in distribution patterns related to strong influences of mid-latitude cyclones in winter and the Bermuda High anticyclone in summer.

Changes in seasonal and diurnal cycles of ozone and temperature in the eastern U.S.

The pollutant tropospheric ozone causes human health problems, and environmental degradation and acts as a potent greenhouse gas. Using long-term hourly observations at five US air quality monitoring surface stations we studied the seasonal and diel cycles of ozone concentrations and surface air temperature to examine the temporal evolution over the past two decades. Such an approach allows visualizing the impact of natural and anthropogenic processes on ozone; nocturnal inversion development, photochemistry, and stratospheric intrusion. Analysis of the result provides an option for determining the duration for a regulatory ozone season. The application of the method provides independent confirmation of observed changes and trends in the ozone and temperature data records as reported elsewhere. The results provide further evidence supporting the assertion that ozone reductions can be attributed to emission reductions as opposed to weather variation. Despite a (∼0.5 °C decade −1) daytime warming trend, ozone decreased by up to 6 ppb decade −1 during times of maximum temperature in the most polluted locations. Ozone also decreased across the emission reduction threshold of 2002 by 6–10 ppb indicating that emission reductions have been effective where and when it is most needed. Longer time series, and coupling with other data sources, may allow for the direct investigation of climate change influence on regional ozone air pollution formation and destruction over annual and daily time scales.

Midlatitude stratosphere – troposphere exchange as diagnosed by MLS O<sub>3</sub> and MOPITT CO assimilated fields

Abstract. This paper presents a comprehensive characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14° N, 1.19° W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Météo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Météo-France using a variational 3-D-FGAT (First Guess at Appropriate Time) method. The validation of O3 and CO assimilated fields is done using self-consistency diagnostics and by comparison with independent observations such as MOZAIC (O3 and CO), AIRS (CO) and OMI (O3). It particularly shows in the upper troposphere and lower stratosphere region that the assimilated fields are closer to MOZAIC than the free model run. The O3 bias between MOZAIC and the analyses is −11.5 ppbv with a RMS of 22.4 ppbv and a correlation coefficient of 0.93, whereas between MOZAIC and the free model run, the corresponding values are 33 ppbv, 38.5 ppbv and 0.83, respectively. In the same way, for CO, the bias, RMS and correlation coefficient between MOZAIC and the analyses are −3.16 ppbv, 13 ppbv and 0.79, respectively, whereas between MOZAIC and the free model they are 6.3 ppbv, 16.6 ppbv and 0.71, respectively. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the STE event well. Assimilated MOPITT CO allows a better qualitative description of the stratospheric intrusion event. The MOPITT CO analyses appear more promising than the MLS O3 analyses in terms of their ability to capture a deep STE event. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies.

Forecasted deep stratospheric intrusions over Central Europe: case studies and climatologies

Abstract. Based on daily predictions of stratospheric air intrusions, obtained from trajectory calculations by ETH Zürich with wind fields from ECMWF forecasts, a high number of measurements with the ozone lidar at IMK-IFU (Garmisch-Partenkirchen, Germany) were carried out in 2001. The lidar measurements show a large variety of rather different cases reflecting the full complexity of intrusion episodes that is not visible in classical case studies. In part, tropopause folds could be fully captured. The frequency of intrusion cases forecasted and verified by vertical sounding or in the in-situ data recorded at the nearby Zugspitze summit (2962 m a.s.l.) exceed that in previous work by more than a factor of two. Three cases mapped with the lidar were selected to validate the results for the corresponding time periods extracted from a one-year run with the new hemispheric version of the chemistry-transport model EURAD. Due to the high spatial resolution chosen for these simulations the agreement with the lidar measurements is satisfactory. The Zugspitze ozone data from 1978 to 2004 were recently filtered by applying different criteria for stratospheric air, based on the 7Be and humidity measurements. Here, by using the daily model forecasts during the time period 2001–2005, we examine three criteria and determine how well they represent the stratospheric air intrusions reaching the mountain site. Seasonal cycles for the period 2001–2005 were derived for the forecasts as well as the intrusion frequency per month for the forecasted intrusions and each of the criteria, distinguishing eight different characteristic transport pathways. In most cases a winter maximum and a summer minimum was obtained, but in the case of cyclonic arrival of intrusions starting over Greenland a late-spring maximum is seen. Two of the filtering criteria examined, based on combining a relative-humidity (RH) threshold of 60% with either a 7Be threshold of 5.5 mBq m−3 or the requirement for RH≤30% within ±6 h, rather reliably predict periods of deep intrusions reaching the Zugspitze station. An "or" combination of both these criteria yields slightly more cases and covers 77.9% of the intrusions identified. The lack of observations in the complementary 22.1% are mostly explained by overpasses. In this way the long-term trend of stratospheric ozone observed at this site as well as the corresponding ozone budget may be derived on the basis of measurements only. This effort will be the subject of a subsequent publication.