Stratosphere-troposphere Exchange Research Articles

Distribution of ozone, carbon monoxide and oxides of nitrogen over an urban location in the foothills of the North-Western Himalayas

Increasing anthropogenic activities and biomass burning events over the Northern Indian region severely affect the pristine environment of North-Western Himalayas. To investigate their influence in this data sparse region, continuous monitoring of O3, CO and NOx are made during January 2018 to December 2019 over Dehradun, an urban location in the foothills of North-western Himalayas. Ozone shows daytime broad peak and CO and NOx show two peaks during morning and evening hours. The maximum daytime ozone is observed during spring with 58.2 ± 2.0 ppbv (56.2 ± 2.7 ppbv) during 2018 (2019). CO and NOx show maximum value during winter and minimum during summer-monsoon. Their concentrations are found to be influenced from stubble burning and forest fire emissions during late spring. WRF-Chem simulations are made with and without biomass burning emissions to quantify the contribution of these emissions on the variability of these gases over Dehradun. Sensitivity simulations reveal that biomass burning over northern Indian region contributed 43 ppbv, 79 ppbv and 1.2 ppbv increase in O3, CO and NOx mixing ratios over Dehradun. In addition, dust storm event in June 2018 contributed for lower ozone levels in 2018 (16.1 ± 9.3 ppbv) and stratosphere troposphere exchange process enhanced surface ozone in June 2019 (53.6 ± 22.3 ppbv).

Impact of stratospheric intrusions on surface ozone enhancement in Hong Kong in the lower troposphere: Implications for ozone control strategy

Understanding the impact of stratospheric intrusion (SI) is crucial for elucidating atmospheric complexities and implications for ozone (O3) control. However, current studies have not focused on the influence of SI on surface O3, thus limiting the effectiveness of control strategies. This study delves into an SI event that occurred from March 5 to 12, 2022, employing a comprehensive integration of the Weather Research and Forecasting model coupled with Chemistry and multi-reanalysis data. The lower tropospheric O3 enhancement in Hong Kong has been noticed, despite the absence of SIs in the upper troposphere. This study employed a comprehensive methodology, integrating the use of a box model to estimate the stratosphere–troposphere exchange (STE) O3 flux, integrated process rate (IPR) analysis to quantify the contributions from individual physical and chemical processes, and tracer methods to detect stratospheric O3. During the deep SI episode, the STE flux peaked at −81.33 × 10−8 kg m−2·s−1, surpassing the monthly average by 15.2-fold. The IPR results indicate that vertical transport within the 0–16 km range contributes between 18.4 and 39.0 ppbv h−1 during the SI event, whereas horizontal advection shows a negative contribution. Stratospheric O3 tagging revealed that SI contributes 15.5–31.3 ppb (29.6–50.2%, respectively, of surface O3) when stratospheric O3 mixes down. Five emission reduction paths were designed in response to the negative impacts of SI. The “anthropogenic VOC (AVOC) only” path was the most efficient; however, when SI contributed 31 ppb on March 9, the “NOx only” path required a 69% reduction, while the “AVOC only” path required an 85% reduction for efficiency. This research not only elucidates the complex interplay between SI and surface O3 concentrations but also emphasizes the significance of refining existing emission reduction paths.

Lifetimes and timescales of tropospheric ozone

The lifetime of tropospheric O3 is difficult to quantify because we model O3 as a secondary pollutant, without direct emissions. For other reactive greenhouse gases like CH4 and N2O, we readily model lifetimes and timescales that include chemical feedbacks based on direct emissions. Here, we devise a set of artificial experiments with a chemistry-transport model where O3 is directly emitted into the atmosphere at a quantified rate. We create 3 primary emission patterns for O3, mimicking secondary production by surface industrial pollution, that by aviation, and primary injection through stratosphere–troposphere exchange (STE). The perturbation lifetimes for these O3 sources includes chemical feedbacks and varies from 6 to 27 days depending on source location and season. Previous studies derived lifetimes around 24 days estimated from the mean odd-oxygen loss frequency. The timescales for decay of excess O3 varies from 10 to 20 days in northern hemisphere summer to 30 to 40 days in northern hemisphere winter. For each season, we identify a single O3 chemical mode applying to all experiments. Understanding how O3 sources accumulate (the lifetime) and disperse (decay timescale) provides some insight into how changes in pollution emissions, climate, and stratospheric O3 depletion over this century will alter tropospheric O3. This work incidentally found 2 distinct mistakes in how we diagnose tropospheric O3, but not how we model it. First, the chemical pattern of an O3 perturbation or decay mode does not resemble our traditional view of the odd-oxygen family of species that includes NO2. Instead, a positive O3 perturbation is accompanied by a decrease in NO2. Second, heretofore we diagnosed the importance of STE flux to tropospheric O3 with a synthetic “tagged” tracer O3S, which had full stratospheric chemistry and linear tropospheric loss based on odd-oxygen loss rates. These O3S studies predicted that about 40% of tropospheric O3 was of stratospheric origin, but our lifetime and decay experiments show clearly that STE fluxes add about 8% to tropospheric O3, providing further evidence that tagged tracers do not work when the tracer is a major species with chemical feedbacks on its loss rates, as shown previously for CH4.

Measurement report: The Palau Atmospheric Observatory and its ozonesonde record – continuous monitoring of tropospheric composition and dynamics in the tropical western Pacific

Abstract. The tropical western Pacific is recognized as an important region for stratosphere–troposphere exchange but lies in a data-sparse location that had a measurement gap in the global ozone sounding network. The Palau Atmospheric Observatory (PAO, approx. 7.3∘ N, 134.5∘ E) was established to study the atmospheric composition above the remote tropical western Pacific with a comprehensive instrumental setup. Since 2016, two laboratory containers in Palau host a Fourier transform infrared spectrometer; a lidar (micro-lidar until 2016, cloud and aerosol lidar from 2018); a Pandora 2S photometer; and laboratory space for weather balloon soundings with ozone, water vapor, aerosol, and radiosondes. In this analysis, we focus on the continuous, fortnightly ozone sounding program with electrochemical concentration cell (ECC) ozonesondes. The aim of this study is to introduce the PAO and its research potential, present the first observation of the typical seasonal cycle of tropospheric ozone in the tropical western Pacific based on a multiannual record of in situ observations, and investigate major drivers of variability and seasonal variation from January 2016 until December 2021​​​​​​​ related to the large-scale atmospheric circulation. We present the PAO ozone (O3) volume mixing ratios (VMR) and relative humidity (RH) time series complemented by other observations. The site is exposed to year-round high convective activity reflected in dominating low O3 VMR and high RH. In 2016, the impact of the strong El Niño is evident as a particularly dry, ozone-rich episode. The main modulator of annual tropospheric O3 variability is identified as the movement of the Intertropical Convergence Zone (ITCZ), with the lowest O3 VMR in the free troposphere during the ITCZ position north of Palau. An analysis of the relation of O3 and RH for the PAO and selected sites from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network reveals three different regimes. Palau's O3 / RH distribution resembles the one in Fiji, Java and American Samoa but is unique in its seasonality and its comparably narrow Gaussian distribution around low O3 VMR and the evenly distributed RH. A previously found bimodal distribution of O3 VMR and RH could not be seen for the full Palau record but only during specific seasons and years. Due to its unique remote location, Palau is an ideal atmospheric background site to detect changes in air dynamics imprinted on the chemical composition of the tropospheric column. The efforts to establish, run and maintain the PAO have succeeded to fill an observational gap in the remote tropical western Pacific and give good prospects for ongoing operations. The ECC sonde record will be integrated into the SHADOZ database in the near future.

Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes

Abstract. Ozone (O3) pollution research and management in China have mainly focused on anthropogenic emissions, while the importance of natural processes is often overlooked. With the increasing frequency of extreme weather events, the role of natural processes in exacerbating O3 pollution is gaining attention. In September 2022, the Pearl River Delta (PRD) in southern China experienced an extended period (25 d) of regional O3 exceedances and high temperatures (second highest over last 2 decades) due to extreme weather conditions influenced by the subtropical high and typhoon peripheries. Employing an integrated approach involving field measurements, machine learning and numerical model simulations, we investigated the impact of weather-induced natural processes on O3 pollution by considering meteorological factors, natural emissions, chemistry pathways and atmospheric transport. The hot weather intensified the emission of biogenic volatile organic compounds (BVOCs) by ∼10 %. Isoprene and biogenic formaldehyde accounted for 47 % of the in situ O3 production, underscoring the predominant role of BVOC emissions in natural processes. The chemical pathway of isoprene contributing to O3 formation was further explored, with O3 production more attributable to the further degradation of early generation isoprene oxidation products (contributed 64.5 %) than the direct isoprene oxidation itself (contributed 35.5 %). Besides, it was found that the hot weather significantly promoted regional photochemical reactions, with meteorological factors contributing to an additional 10.8 ppb of O3 levels compared to normal conditions. Temperature was identified as the dominant meteorological factor. Furthermore, the typhoon nearing landfall significantly enhanced the cross-regional transport of O3 from northern to southern China through stratosphere–troposphere exchange (STE). The CAM-Chem model simulations revealed that the STE-induced O3 on the PRD surface could reach a maximum of ∼8 ppb, highlighting the non-negligible impact of STE. This study highlights the importance of natural processes exacerbated by extreme weather events in O3 pollution and provides valuable insights into O3 pollution control under global warming.

Atmospheric fallout of 7Be in bulk precipitation at the Adriatic coast, Croatia

ABSTRACT Atmospheric fallout of naturally occurring cosmic radionuclide 7Be was monitored in bulk precipitation over a year (July 2018 to June 2019) at a coastal station (Martinska) of the Adriatic Sea, Croatia. The monthly depositional fluxes varied between 25.08 and 78.97 Bq m−2 month−1 (average: 49.18 ± 19.17 Bq m−2 month−1) and showed a significant correlation with precipitation (r = 0.92). The highest seasonal flux observed in winter (172 ± 4.31 Bq m−2 season−1) coincides with the highest amount of precipitation (190 mm), suggesting an important role of precipitation in the scavenging process of 7Be deposition to the surface. The monthly volume-weighted activities of 7Be varied from 0.63 to 5.74 Bq L−1 (average: 1.96 ± 1.7 Bq L−1) with the highest value corresponding to the summer season. The precipitation-normalised enrichment factor (α) indicates a higher depositional flux of 7Be in the summer season than the desired value due to the stratosphere-troposphere exchange and the contribution of dry deposition. The annual bulk depositional flux of 7Be was 590 Bq m−2 y−1, which is comparable with several Mediterranean coastal stations. The annual bulk depositional fluxes of 7Be in the 30°N - 50°N latitude band showed a good correlation with precipitation and established that the atmospheric fallout of this radionuclide is mainly governed by precipitation in that given latitude band.

Ozone at Mace Head, Ireland from 1987 to 2021: Declining baselines, phase-out of European regional pollution, COVID-19 impacts

Just under three hundred thousand hourly O3 observations from the Mace Head, Ireland atmospheric monitoring station have been assembled into a complete dataset covering the thirty five-year period from April 1, 1987 through to May 31, 2022. Of these, seventy thousand hourly observations were assigned to baseline air masses over the 422 months in the study. Annual mean baseline mixing ratios rose from 34 ppb in 1988 to a peak of 42 ppb in 1999 before declining to 39 ppb in 2021. Monthly mean baseline mixing ratios reached a peak of 53 ppb in April 1999. Baseline O3 mixing ratios exhibit a marked seasonal cycle, with maxima in April and minima in August. A detailed examination of the differences between the baseline and complete monthly mean O3 mixing ratios revealed a set of monthly differences with some striking long-term changes. Wintertime differences were dominated by a series of O3 depletion events in which, during the early years of the study, reduced ozone to near zero in long-range transport events. European NOx emission reductions have reduced significantly the number and severity of these wintertime O3 depletion events. Summertime differences were dominated by a series of regional photochemical episodes. In the early years of the record, the regional photochemical episodes were intense enough to raise the monthly means in the complete record above the baseline means. European volatile organic compound (VOC) and NOx precursor emission reductions have dramatically reduced the number and intensity of these events. Episodic peak O3 levels have also fallen steadily as a result of concerted, European action on regional VOC and NOx emissions. Subsets of the baseline and complete ozone datasets between 2017 and 2022 were scrutinised for possible COVID-19 impacts. Baseline ozone levels were lower than expected during 2020 and 2021 but the statistical significance of these impacts is difficult to judge, and reduced stratosphere-troposphere exchange rather than COVID-19 emission reductions may be the cause.

The effects of gravity waves on ozone over the Tibetan Plateau

The ozone valley over the Tibetan Plateau (TP) has an important effect on global weather and climate. As a significant source of atmospheric gravity waves (GWs), TP is also a key area of global stratosphere-troposphere exchange (STE), yet the exploration of the causes of low ozone values over the TP has been scarce from the perspective of GW. In this paper, we used the hyperspectral Atmospheric Infrared Sounder (AIRS) data to extract GWs and deep convection over the TP and analyzed the statistical characteristics of ozone for corresponding events. The results show that: (1) The GWs observed by AIRS mainly occur in the mid-latitude region, with a maximum frequency of >10%, and their intensity varies with longitude. Three large-value regions have been identified on the coast of Southeast Asia, Central America, and Central Africa. (2) Most deep convection occurs in the Intertropical Convergence Zone (ITCZ), with three large value centers in the East Asian monsoon region, Central America and Central Africa. Among them, the Indian monsoon region, the Northwest Pacific region to the east of the Philippines, and the western side of the South China Sea (SCS) are the large-value areas within the East Asian monsoon region, with the maximum occurrence frequency exceeding 15%. (3) TP is a region with a large frequency of convective gravity waves. In most areas of the southern foothills of the TP, the frequency of GWs related to convection is 30%–50%. Almost all deep convection over the TP and its adjacent areas are accompanied by GWs, with a frequency of 60–90%. (4) The composite analysis results show that the occurrence of GWs or deep convection is accompanied by negative anomalies of ozone in most areas of the southern foothills of the TP, indicating a decrease in the integrated column amount of ozone. (5) By analyzing the anomaly distribution of meteorological elements such as cloud fraction, cloud top height, tropopause height, and outgoing longwave radiation (OLR), the results show a dual effect in the presence of GWs or deep convection. The effect involves not only an increased generation of clouds, conducive to convection but also elevated cloud top height, promoting the formation of high clouds, some even beyond the tropopause. In addition, the occurrence of GW or deep convection can also affect the tropopause height, strengthen convective activity, and facilitate the upward transfer of low-concentration ozone from the lower layer to the upper layer, thereby causing a decrease in the integrated column amount of ozone.

Tropospheric Gravity Waves Increase the Likelihood of Double Tropopauses

AbstractThe tropopause region is crucial for the stratosphere‐troposphere exchange (STE) and acts as an indicator of climate change. Double tropopauses (DTs) act to increase the STE process but their driving mechanisms remain an open question. The present assessment offers for the first time the linkage between tropospheric gravity waves (GWs) and DT events by exploring a global data set of multi‐year radiosonde measurements. In the extratropics, the occurrence frequency of DT events keeps a remarkably consistent spatial‐temporal structure with GW total energy. Under the DT scenario, GW total energy has increased by 37.67% compared to single tropopause events. Based on a statistical assessment, the upward propagating GWs throughout the second tropopause region can probably raise Kelvin‐Helmholtz instability or turbulence, leading permanent irregularities in thermodynamic structure, and consequently, increasing the likelihood of DT.

Global trends of tropopause folds in recent decades

Tropopause folds represent a primary mechanism for stratosphere-troposphere exchange. This study employs a 3D labeling method with ERA5 reanalysis data spanning from 1979 to 2020 to elucidate the spatiotemporal variations of tropopause folds. The results reveal distinct seasonal and regional variations in trends of tropopause folds. Notably, tropopause folds exhibit an increasing trend, with the magnitude varying seasonally. Significant increasing trends of tropopause folds are observed in northern spring, summer, and winter, primarily along subtropical jets. Further analysis reveals that the increase in tropopause folds is related to the strengthening of frontogenesis due to enhanced atmospheric baroclinicity, while the intensification of meridional potential temperature gradients enhances secondary circulations and may further promote an increase in folds activities.摘要对流层顶折卷是平流层-对流层物质交换的主要机制. 本研究采用三维标记方法, 利用1979-2020年间的ERA5再分析数据, 分析了对流层顶折卷的时空变化特征及机理. 研究结果表明, 全球对流层顶折卷的多年变化趋势存在明显的季节性和区域性差异. 总体上, 对流层顶折卷呈增加趋势, 其中北半球的春季,夏季和冬季, 对流层顶折卷主要沿副热带急流区呈现明显增加的趋势. 进一步分析表明, 对流层顶折卷发生频率的增加与大气斜压性增大导致的锋生增强有关, 而经向位温梯度的增大使得次级环流增强, 也可能促进了对流层顶折卷活动的增多.

The impact of tropopause fold event on surface ozone concentration over Tibetan Plateau in July

Tropopause fold events are one of the major processes in stratosphere-troposphere exchange (STE) in the mid-latitudes. The Tibetan Plateau (TP) is a hotspot of STE in the world. It has been proved that the tropopause fold events over the TP could impact on tropospheric ozone concentration in summer, yet most of these studies only focus on tropopause fold events at individual stations. In this study, we use ozone soundings data over Minle County (38.41°N, 100.65°E) and surface observations in the TP to verify the effect of tropopause fold events on surface ozone concentration. The stratospheric ozone tracers (O3S) simulation by the WACCM model and the passive tracers simulation by the WRF model indicate that the tropopause fold event observed on 11 July 2020 contributed to surface ozone in the northern regions of TP. In addition, we identified all the tropopause fold events that occurred over the TP in each July from 2015 to 2020 and quantified their impacts on surface ozone concentration. The results show that the average increase in surface ozone concentration is 15.94 ppbv during the period affected by the tropopause fold events. The site most affected by tropopause fold events is Shannan City, followed by Nyingchi City. This study revealed the importance of the influence of tropopause fold event on surface ozone concentration in the TP in summer.

Simulations of 7Be and 10Be with the GEOS-Chem global model v14.0.2 using state-of-the-art production rates

Abstract. The cosmogenic radionuclides 7Be and 10Be are useful tracers for atmospheric transport studies. Combining 7Be and 10Be measurements with an atmospheric transport model can not only improve our understanding of the radionuclide transport and deposition processes but also provide an evaluation of the transport process in the model. To simulate these aerosol tracers, it is critical to evaluate the influence of radionuclide production uncertainties on simulations. Here we use the GEOS-Chem chemical transport model driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) reanalysis to simulate 7Be and 10Be with the state-of-the-art production rate from the CRAC:Be (Cosmic Ray Atmospheric Cascade: Beryllium) model considering realistic spatial geomagnetic cutoff rigidities (denoted as P16spa). We also perform two sensitivity simulations: one with the default production rate in GEOS-Chem based on an empirical approach (denoted as LP67) and the other with the production rate from the CRAC:Be but considering only geomagnetic cutoff rigidities for a geocentric axial dipole (denoted as P16). The model results are comprehensively evaluated with a large number of measurements including surface air concentrations and deposition fluxes. The simulation with the P16spa production can reproduce the absolute values and temporal variability of 7Be and 10Be surface concentrations and deposition fluxes on annual and sub-annual scales, as well as the vertical profiles of air concentrations. The simulation with the LP67 production tends to overestimate the absolute values of 7Be and 10Be concentrations. The P16 simulation suggests less than 10 % differences compared to P16spa but a significant positive bias (∼18 %) in the 7Be deposition fluxes over East Asia. We find that the deposition fluxes are more sensitive to the production in the troposphere and downward transport from the stratosphere. Independent of the production models, surface air concentrations and deposition fluxes from all simulations show similar seasonal variations, suggesting a dominant meteorological influence. The model can also reasonably simulate the stratosphere–troposphere exchange process of 7Be and 10Be by producing stratospheric contribution and 10Be/7Be ratio values that agree with measurements. Finally, we illustrate the importance of including the time-varying solar modulations in the production calculation, which significantly improve the agreement between model results and measurements, especially at mid-latitudes and high latitudes. Reduced uncertainties in the production rates, as demonstrated in this study, improve the utility of 7Be and 10Be as aerosol tracers for evaluating and testing transport and scavenging processes in global models. For future GEOS-Chem simulations of 7Be and 10Be, we recommend using the P16spa (versus default LP67) production rate.

The Impact of Meteorological Conditions and Emissions on Tropospheric Column Ozone Trends in Recent Years

Based on OMI/MLS data (2005–2020) and Community Earth System Model (CESM2) simulated results (2001–2020), annual variation trends of tropospheric column ozone (TCO) in the recent two decades are explored, and the separate impacts of meteorological conditions and emissions on TCO are quantified. The stratospheric ozone tracer (O3S) is used to quantify the contribution of stratospheric ozone to the trend of TCO. The evaluation shows that the simulated results capture the spatial-temporal distributions and the trends of tropospheric column ozone well. Over the East Asia and Southeast Asia regions, TCO is increasing, with a rate of ~0.2 DU/yr, which is primarily attributed to the emission changes in ozone precursors, nitrogen oxide (NOx) and volatile organic chemicals (VOCs). But the changes in meteorological conditions weaken the increase in TCO, even leading to a decrease in East Asia in spring and summer. TCO is decreasing in the middle and high latitudes of the southern hemisphere, which is mainly attributed to the changes in meteorological conditions. The increasing rates are the highest in autumn, especially over North America, East Asia, Europe and South of East Asia, with rate values of 0.20, 0.31, 0.17, and 0.32 DU/yr, respectively. Over the equatorial region, the contribution of stratospheric ozone to TCO is below 10 DU, and shows a weak positive trend of ~0.2 DU/yr. In the latitude of ~30°N/S, the stratospheric contribution is high, ~25 DU, and is affected by the sinking branch of the Brewer–Dobson circulation and stratosphere–troposphere exchange in the vicinity of tropical jet stream. The stratospheric contribution to TCO in the north of 30°N is significantly decreasing (~0.6 DU/yr) under the influence of meteorological conditions. Changes in emissions weaken the decrease in stratospheric contributions in the north of 30°N and enhance the increase in 30°S–30°N significantly. The trends of stratospheric contributions on TCO partly explain the trends of TCO which are mostly affected by the change in emissions. To control the increasing TCO, actions to reduce emissions are urgently needed.

Influence of stratosphere-troposphere exchange on long-term trends of surface ozone in CMIP6

Surface ozone, which is a major air pollutant, has gained widespread public attention due to its significant harm to human health and ecosystems. Here we find that long-term trends of surface ozone are largely influenced by stratosphere-troposphere exchange (STE) using the historical simulations in the CMIP6 multi-model ensemble. It is found that STE contributes up to 39.5% of climatological surface ozone in the extratropics of the winter hemisphere. In the Southern Hemisphere (SH), prominent stratospheric ozone depletion tends to reduce tropospheric and surface ozone due to STE over 1960–1997, which has been reversed during 1997–2014. In the Northern Hemisphere (NH), STE enhances surface ozone during both ozone depletion and recovery periods. About 29.5% of the positive trends of surface ozone over 1960–2014 can be attributed to STE processes in boreal winter in the NH extratropics. The enhancement of STE is related to the changes in atmospheric circulation associated with global warming. Our results suggest that STE will further worsen surface ozone pollution in the future associated with the stratospheric ozone recovery and global warming.

Tropopause folds over the Tibetan Plateau and their impact on water vapor in the upper troposphere-lower stratosphere

As one of the most important greenhouse gases, water vapor in the upper troposphere and lower stratosphere (UTLS) has a significant impact on the global earth-atmosphere system. The Tibetan Plateau (TP) is an important high terrain which exerts a profound impact on the change of weather and climate, and mass exchange. Tropopause folds occur frequently over the TP due to the impact of the subtropical westerly jet, which affects water vapor transport between the stratosphere and the troposphere. In this paper, the spatial and temporal distribution characteristics of tropopause folds over the TP are examined by applying an improved three-dimensional (3D) labeling algorithm to the ERA5 reanalysis data (1979 to 2019). The effects of different fold depths in various regions over the TP on the variations of UTLS water vapor are further studied. The results of a case study (25 February 2008) suggest that there is a good continuity in identification of the fold depth for the same fold event using the improved 3D labeling algorithm. The fold depth and height are consistent with the results of radiosonde data and ERA5 reanalysis data. The fold frequency over the TP shows an increasing trend in the last 41 years, with slightly lower frequency of medium folds than that of shallow folds, and lowest frequency of deep folds. There is increasing water vapor in the UTLS over the TP due to tropopause folds. The results indicate that tropopause folds enhance the horizontal divergence of water vapor in the UTLS and increase the vertical water vapor flux in the UTLS region. The folding over the plateau leads to increased moisture in the UTLS. It is argued that vertical velocity anomalies in the vicinity of the fold and subgrid perturbations have a significant impact on the increase of UTLS water vapor over the TP. The results of this work provide a scientific basis for a better understanding of the stratosphere-troposphere exchanges due to tropopause folds over the TP.

Variability and trends of the tropical tropopause derived from a 1980–2021 multi-reanalysis assessment

As the tropopause plays a key role in regulating the entry of air from the troposphere into the stratosphere and in controlling stratosphere-troposphere exchange, variation of the tropopause impacts the atmospheric dynamics, circulation patterns, and the distribution of greenhouse gases in the upper troposphere and lower stratosphere (UTLS). Therefore, it is of particular interest to investigate the climatological characteristics and trends of the tropopause. Previous studies have investigated the tropopause characteristics using reanalyses and multi-source observations. This study extends the analysis of long-term variability and trends of tropical tropopause characteristics in earlier studies from 1980 up to 2021 using the modern ERA5 reanalysis and compares the results with those of other reanalyses, including ERA-Interim, MERRA-2, and NCEP1/2. Our analysis reveals a general rise and cooling of the tropical tropopause between 1980 and 2021. The geopotential height has increased by approximately 0.06 ± 0.01 km/decade (at a 95% confidence level), while the temperature has decreased by −0.09 ± 0.03 K/decade (at a 95% confidence level) for both the lapse rate tropopause and the cold point tropopause in ERA5. However, from 2006 to 2021, ERA5 shows a warming tropical tropopause (0.10 ± 0.11 K/decade) along with a slower rise in tropopause height (0.05 ± 0.02 km/decade) (at a 95% confidence level). Furthermore, our analysis demonstrates a decline in the rise and cooling of the tropical tropopause since the late 1990s, based on moving 20-year window trends in ERA5. Similar trends are observed in other investigated reanalyses. In addition, this study evaluated the variability of the width of the tropical belt based on tropopause height data from the reanalyses. The ERA5 data show a narrowing tropical belt (−0.16 ± 0.11°/decade) for the time period 1980–2021 according to the relative threshold method. It reveals a tropical widening (0.05 ± 0.22°/decade) for the period between 1980 and 2005, followed by a tropical narrowing (−0.17 ± 0.42°/decade) after 2006. However, the large uncertainties pose a challenge in drawing definitive conclusions on the change of tropical belt width. Despite the many challenges involved in deriving the characteristics and trends of the tropopause from reanalysis data, this study and the open reanalysistropopause data sets provided to the community will help to better inform future assessments of stratosphere-troposphere exchange and studies of chemistry and dynamics of the upper troposphere and lower stratosphere region.

O3 and PAN in southern Tibetan Plateau determined by distinct physical and chemical processes

Abstract. Tropospheric ozone (O3) and peroxyacetyl nitrate (PAN) are both photochemical pollutants harmful to the ecological environment and human health. In this study, measurements of O3 and PAN as well as their precursors were conducted from May to July 2019 at Nam Co station (NMC), a highly pristine high-altitude site in the southern Tibetan Plateau (TP), to investigate how distinct transport processes and photochemistry contributed to their variations. Results revealed that, despite highly similar diurnal variations with steep morning rises and flat daytime plateaus that were caused by boundary layer development and downmixing of free-tropospheric air, day-to-day variations in O3 and PAN were in fact controlled by distinct physicochemical processes. During the dry spring season, air masses rich in O3 were associated with high-altitude westerly air masses that entered the TP from the west or the south, which frequently carried high loadings of stratospheric O3 to NMC. During the summer monsoon season, a northward shift of the subtropical jet stream shifted the stratospheric downward entrainment pathway also to the north, leading to direct stratospheric O3 entrainment into the troposphere of the northern TP, which traveled southwards to NMC within low altitudes via northerly winds in front of ridges or closed high pressures over the TP. Westerly and southerly air masses, however, revealed low O3 levels due to the overall less stratospheric O3 within the troposphere of low-latitude regions. PAN, however, was only rich in westerly or southerly air masses that crossed over polluted regions such as northern India, Nepal or Bangladesh before entering the TP and arriving at NMC from the south during both spring and summer. Overall, the O3 level at NMC was mostly determined by stratosphere–troposphere exchange (STE), which explained 77 % and 88 % of the observed O3 concentration in spring and summer, respectively. However, only 0.1 % of the springtime day-to-day O3 variability could be explained by STE processes, while 22 % was explained during summertime. Positive net photochemical formation was estimated for both O3 and PAN based on observation-constrained box modeling. Near-surface photochemical formation was unable to account for the high O3 level observed at NMC, nor was it the determining factor for the day-to-day variability of O3. However, it was able to capture events with elevated PAN concentrations and explain its day-to-day variations. O3 and PAN formation were both highly sensitive to NOx levels, with PAN being also quite sensitive to volatile organic compound (VOC) concentrations. The rapid development of transportation networks and urbanization within the TP may lead to increased emissions and loadings in NOx and VOCs, resulting in strongly enhanced O3 and PAN formation in downwind pristine regions, which should be given greater attention in future studies.

Changes in Stratosphere‐Troposphere Exchange of Air Mass and Ozone Concentration in CCMI Models From 1960 to 2099

AbstractThis study investigates changes in stratosphere‐troposphere exchange (STE) of air masses and ozone concentrations from 1960 to 2099 using multiple model simulations from Chemistry Climate Model Initiative (CCMI) under climate change scenario RCP6.0. We employ a lowermost stratosphere mass budget approach with dynamic isentropic surfaces fitted to the tropical tropopause as the upper boundary of lowermost stratosphere. The multi‐model mean (MMM) trends of air mass STEs are all small over all regions, which are within 0.3 (0.1) % decade−1 for 1960–2000 (2000–2099). The MMM trends of ozone STE for 1960–2000 are 0.3%, −2.7%, 3.4%, −0.9%, and −2.7% decade−1 over the Northern hemisphere (NH) extratropics, Southern hemisphere (SH) extratropics, tropics, extratropics, and globe, respectively. The corresponding ozone STE trends for 2000–2099 are 3.0%, 4.3%, 0.8%, 3.5%, and 4.7% decade−1. Changes in ozone STEs are dominated by ozone concentration changes, driven by climate‐induced changes and ozone‐depleting substance (ODS) changes. For 1960–2000, small changes in ozone STEs in the NH extratropics are due to a cancellation between effects of climate‐induced changes and ODS increases, while the ODS effect dominates in the SH extratropics, leading to a large ozone STE magnitude decrease. Increased ozone transport from tropical troposphere to stratosphere for 1960–2000 is due to increased tropospheric ozone. A decreased global ozone STE magnitude for 1960–2000 was largely caused by ODS‐induced ozone loss that is partly compensated by climate‐induced ozone changes. For 2000–2099, about two‐thirds of global ozone STE magnitude increases are caused by ozone increases in the extratropical lower stratosphere due to climate‐induced changes. The remaining one‐third is caused by ozone recovery due to the phaseout of ODS.

The Different Characteristics of the Mass Transport between the Stratosphere and the Troposphere in Two Types of Cyclonic Rossby Wave-Breaking Events

Using the ERA5 reanalysis data and trajectory analysis provided by Hysplit4, a comparative analysis was conducted on the primary pathways of air particles and the dominant weather systems in two distinct cases of equatorward and poleward cyclonic Rossby wave-breaking (CWB) events. Subsequently, the characteristics of mass exchange between the stratosphere and troposphere in both CWBs were estimated and discussed. CWB events are frequently associated with the development of an upper front in subtropics and a ridge or blocking in mid-latitudes, leading to a tropopause anomaly characterized by a downward depression in the subtropics and an upward bulge in the mid-latitudes. High potential vorticity (PV) particles exhibit negligible vertical motion and are instead controlled by the circulation of the ridge or blocking, leading to a significant poleward transport. In contrast, low PV particles display noticeable vertical motion, with approximately one fourth of them ascending on the north side of the upper-level jet exit region. After CWB occurrence, approximately 25% of low PV particles moved southward and sank below 500 hPa with the downstream trough’s cold air. Most high PV particles remained in the stratosphere, and low PV particles predominantly remained in the troposphere. Only a small proportion (2% to 6%) of particles underwent stratosphere–troposphere exchange (STE). In equatorward CWB, STE manifested as transport from stratosphere to troposphere, occurring mainly in 24–48 h post breaking with a maximum mass transport of approximately 1.54 × 1013 kg. In poleward CWB, STE involved transport from troposphere to stratosphere, occurring mainly within 0–18 h post breaking with a maximum mass transport of approximately 1.48 × 1013 kg.

Determination of the chemical equator from GEOS-Chem model simulation: a focus on the tropical western Pacific region

Abstract. The tropical western Pacific (TWP) plays an important role in global stratosphere–troposphere exchange and is an active region of the interhemispheric transport (IHT). Common indicators for transport between the hemispheres like the tropical rain belt are too broad or lack precision in the TWP. In this paper, we provide a method to determine the atmospheric chemical equator (CE), which is a boundary for air mass transport between the two hemispheres in the tropics. This method used the model output from an artificial passive tracer simulated by the chemical transport model GEOS-Chem in the troposphere. We investigated the movement of the CE in the tropics, which indicates the migration of atmospheric circulation systems and air mass origins. Our results show the CE on different timescales, suggesting that the different features of the IHT in different regions are highly related to the variation in the circulation systems. We compared the CE with the tropical wind fields, indicating that the region of IHT does not coincide with the convergence of the 10 m wind fields in the tropical land sectors and the TWP region. We compared the CE with the atmospheric composition such as satellite data of CH4 and model simulation of sulfur hexafluoride (SF6). The results show that the CE and north–south gradient of CH4 in the Indian Ocean in January are well consistent with each other, which indicates the CE has good potential to estimate the IHT inferred by observations. We discussed the vertical extent and the meridional extent of the IHT. We find that the vertical structure above 2 km has a slight northern tilt in the Northern Hemisphere (NH) winter season and a southern tilt in the NH summer, meaning the seasonality of the migration of the CE at the lower altitude is larger than that at the higher altitude. The meridional extent of the CE indicates a narrow transition zone where IHT happens throughout the year. We find that the meridional extent above South America is larger compared to other regions. The distribution of the land–sea contrast plays an important role in the meridional extent of IHT. We focus on the TWP region and further compared the tropical rain belt with the CE. There is a broad region of high precipitation occurring in the TWP region, and it is difficult to determine the IHT by the rain belt. In the NH winter, the CE is not consistent with the tropical rain belt in the TWP but is confined to the southern branch of the peak of the rain belt. For the other seasons, both indicators of IHT agree.