scholarly journals Stratospheric impact on tropospheric ozone variability and trends: 1990–2009

2013 ◽  
Vol 13 (2) ◽  
pp. 649-674 ◽  
Author(s):  
P. G. Hess ◽  
R. Zbinden
Keyword(s):  
Tropospheric Ozone ◽  
Large Scale ◽  
Transport Model ◽  
Spatial Scales ◽  
Stratospheric Ozone ◽  
Atmospheric Model ◽  
Chemical Transport Model ◽  
Ozone Trends ◽  
Environmental Prediction

Abstract. The influence of stratospheric ozone on the interannual variability and trends in tropospheric ozone is evaluated between 30 and 90° N from 1990–2009 using ozone measurements and a global chemical transport model, the Community Atmospheric Model with chemistry (CAM-chem). Long-term measurements from ozonesondes, at 150 and 500 hPa, and the Measurements of OZone and water vapour by in-service Airbus aircraft programme (MOZAIC), at 500 hPa, are analyzed over Japan, Canada, the Eastern US and Northern and Central Europe. The measurements generally emphasize northern latitudes, although the simulation suggests that measurements over the Canadian, Northern and Central European regions are representative of the large-scale interannual ozone variability from 30 to 90° N at 500 hPa. CAM-chem is run with input meteorology from the National Center for Environmental Prediction; a tagging methodology is used to identify the stratospheric contribution to tropospheric ozone concentrations. A variant of the synthetic ozone tracer (synoz) is used to represent stratospheric ozone. Both the model and measurements indicate that on large spatial scales stratospheric interannual ozone variability drives significant tropospheric variability at 500 hPa and the surface. In particular, the simulation and the measurements suggest large stratospheric influence at the surface sites of Mace Head (Ireland) and Jungfraujoch (Switzerland) as well as many 500 hPa measurement locations. Both the measurements and simulation suggest the stratosphere has contributed to tropospheric ozone trends. In many locations between 30–90° N 500 hPa ozone significantly increased from 1990–2000, but has leveled off since (from 2000–2009). The simulated global ozone budget suggests global stratosphere-troposphere exchange increased in 1998–1999 in association with a global ozone anomaly. Discrepancies between the simulated and measured ozone budget include a large underestimation of measured ozone variability and discrepancies in long-term stratospheric ozone trends. This suggests the need for more sophisticated simulations including better representations of stratospheric chemistry and circulation.

scholarly journals Stratospheric impact on tropospheric ozone variability and trends: 1990–2009

2011 ◽  
Vol 11 (8) ◽  
pp. 22719-22770 ◽  
Author(s):  
P. G. Hess ◽  
R. Zbinden
Keyword(s):  
Interannual Variability ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Model Simulation ◽  
Spatial Scales ◽  
Stratospheric Ozone ◽  
Surface Ozone ◽  
High Mountain ◽  
Northern European ◽  
Ozone Trends

Abstract. We evaluate the influence of stratospheric ozone on the interannual variability and trends in tropospheric ozone from 30–90° N between 1990 and 2009 using ozone measurements and a global chemical transport model (the Community Atmospheric Model with chemistry) with input meteorology from the National Center for Environmental Prediction. The model simulation uses constant interannual emissions. Both the model and measurements indicate that on large spatial scales stratospheric interannual ozone variability drives significant tropospheric variability and contributes to long-term tropospheric ozone trends. To diagnose the measured variability we utilized measurements from ozonesondes and the Measurements of OZone and water vapour by in-service Airbus airCraft programme (MOZAIC) north of 30° N. We identify a regionally robust 150 hPa ozone signal from measurements over Canadian, Northern European and Central European regions and at 500 hPa over Canadian, Northern European and Eastern US regions. Averaged over these regions, the 150 hPa interannual ozone variability explains 69 % of the interannual variability at 500 hPa. The simulated stratospheric signal explains 81 % of the simulated variability over these same regions. Simulated and measured ozone are significantly correlated over these regions and the simulation suggests that the ozone record over these regions is representative of the overall hemispheric 500 hPa ozone record from 30–90° N. The measured 500 hPa trends averaged over these three regions between 1990 and 2000 and 1990 and 2009 are 0.73 (±0.51) ppbv yr−1 and 0.27 (±0.19) ppbv yr−1, respectively. The simulated trends in 1990–2000 and 1990–2009 are 0.29±0.10 ppbv yr−1 and 0.13±0.05 ppbv yr−1, respectively; however, these trends are substantially larger when the model is sampled for missing data exactly as the measurements are. Simulated stratospheric ozone accounts for 79 % of the simulated 500 hPa trend between 1990 and 2000 and 100 % of the simulated trend between 1990 and 2009. Due to the importance of local meteorology and emissions at the surface it is difficult to isolate the stratospheric component of measured surface ozone variability. Overall when averaged between 30–90° N simulated surface interannual ozone trends are 0.18 ppbv yr−1 and 0.07 ppbv yr−1 between 1990 and 1999, and between 1990 and 2009, respectively. We have identified a number of surface sites where the measured interannual ozone variability is correlated with the 150 hPa ozone signal. Most notably these sites include the high mountain sites over Europe and Macehead, Ireland. Over Macehead the measured 150 hPa ozone signal explains 40 % of the interannual variability of the unfiltered measured ozone record. The simulated and measured ozone are highly correlated over Macehead. The Macehead measured and simulated unfiltered ozone trends between 1990 and 2000 are 0.28 (±0.33) and 0.17 (±0.13) ppbv yr−1 respectively; between 1990 and 2009 the measured and simulated trends are 0.18 (±0.11) and 0.08 (±0.06) ppbv yr−1, respectively. Increases in the simulated stratospheric ozone component accounts for 53 % and 75 % of the overall modeled trend for the two periods at Macehead.

scholarly journals An exploration of ozone changes and their radiative forcing prior to the chlorofluorocarbon era

2002 ◽  
Vol 2 (5) ◽  
pp. 363-374 ◽  
Author(s):  
D. T. Shindell ◽  
G. Faluvegi
Keyword(s):  
Ozone Depletion ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Stratospheric Ozone ◽  
Data Sets ◽  
Independent Data ◽  
Spatial Coverage ◽  
Ozone Trends ◽  
Ozone Trend

Abstract. Using historical observations and model simulations, we investigate ozone trends prior to the mid-1970s onset of halogen-induced ozone depletion. Though measurements are quite limited, an analysis based on multiple, independent data sets (direct and indirect) provides better constraints than any individual set of observations. We find that three data sets support an apparent long-term stratospheric ozone trend of -7.2 ± 2.3 DU during 1957-1975, which modeling attributes primarily to water vapor increases. The results suggest that 20th century stratospheric ozone depletion may have been roughly 50% more than is generally supposed. Similarly, three data sets support tropospheric ozone increases over polluted Northern Hemisphere continental regions of 8.2 ± 2.1 DU during this period, which are mutually consistent with the stratospheric trends. As with paleoclimate data, which is also based on indirect proxies and/or limited spatial coverage, these results must be interpreted with caution. However, they provide the most thorough estimates presently available of ozone changes prior to the coincident onset of satellite data and halogen dominated ozone changes. If these apparent trends were real, the radiative forcing by stratospheric ozone since the 1950s would then have been -0.15 ± 0.05 W/m2, and -0.2 W/m2 since the preindustrial. For tropospheric ozone, it would have been 0.38 ± 0.10 W/m2 since the late 1950s. Combined with even a very conservative estimate of tropospheric ozone forcing prior to that time, this would be larger than current estimates since 1850 which are derived from models that are even less well constrained. These calculations demonstrate the importance of gaining a better understanding of historical ozone changes.

scholarly journals Clouds, photolysis and regional tropospheric ozone budgets

2009 ◽  
Vol 9 (3) ◽  
pp. 13889-13916 ◽  
Author(s):  
A. Voulgarakis ◽  
O. Wild ◽  
N. H. Savage ◽  
G. D. Carver ◽  
J. A. Pyle
Keyword(s):  
Tropospheric Ozone ◽  
Large Scale ◽  
Transport Model ◽  
Regional Scale ◽  
Three Dimensional ◽  
Global Scale ◽  
Chemical Production ◽  
Chemical Transport Model ◽  
Photolysis Rates ◽  
Boundary Layer Ozone

Abstract. We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity on regional scales.

scholarly journals Combined assimilation of IASI and MLS observations to constrain tropospheric and stratospheric ozone in a global chemical transport model

2013 ◽  
Vol 13 (8) ◽  
pp. 21455-21505
Author(s):  
E. Emili ◽  
B. Barret ◽  
S. Massart ◽  
E. Le Flochmoen ◽  
A. Piacentini ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Chemical Transport ◽  
Free Troposphere ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Global Chemical Transport Model ◽  
The Impact

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. In this study we examine the impact of assimilating ozone observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI) in a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE). The assimilation of the two instruments is performed by means of a variational algorithm (4-D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozone-sondes measurements to verify the presence of observations and model biases. It is found that the IASI Tropospheric Ozone Column (TOC, 1000–225 hPa) should be bias-corrected prior to assimilation and MLS lowermost level (215 hPa) excluded from the analysis. Furthermore, a longer analysis of 6 months (July–August 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (Root Mean Square Error, RMSE) of the modeled ozone columns from 30% to 15% in the Upper-Troposphere/Lower-Stratosphere (UTLS, 70–225 hPa) and from 25% to 20% in the free troposphere. The positive effect of assimilating IASI tropospheric observations is very significant at low latitudes (30° S–30° N), whereas it is not demonstrated at higher latitudes. Results are confirmed by a comparison with additional ozone datasets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be little sensitive to the assimilation parameters and the model chemical scheme, due to the high frequency of satellite observations compared to the average life-time of free-troposphere/low-stratosphere ozone.

scholarly journals ML-TOMCAT: machine-learning-based satellite-corrected global stratospheric ozone profile data set from a chemical transport model

2021 ◽  
Vol 13 (12) ◽  
pp. 5711-5729
Author(s):  
Sandip S. Dhomse ◽  
Carlo Arosio ◽  
Wuhu Feng ◽  
Alexei Rozanov ◽  
Mark Weber ◽  
...  
Keyword(s):  
Transport Model ◽  
Stratospheric Ozone ◽  
Chemical Transport ◽  
Data Sets ◽  
Chemical Transport Model ◽  
Profile Data ◽  
Data Set ◽  
Ozone Profile ◽  
Satellite Instruments

Abstract. High-quality stratospheric ozone profile data sets are a key requirement for accurate quantification and attribution of long-term ozone changes. Satellite instruments provide stratospheric ozone profile measurements over typical mission durations of 5–15 years. Various methodologies have then been applied to merge and homogenise the different satellite data in order to create long-term observation-based ozone profile data sets with minimal data gaps. However, individual satellite instruments use different measurement methods, sampling patterns and retrieval algorithms which complicate the merging of these different data sets. In contrast, atmospheric chemical models can produce chemically consistent long-term ozone simulations based on specified changes in external forcings, but they are subject to the deficiencies associated with incomplete understanding of complex atmospheric processes and uncertain photochemical parameters. Here, we use chemically self-consistent output from the TOMCAT 3-D chemical transport model (CTM) and a random-forest (RF) ensemble learning method to create a merged 42-year (1979–2020) stratospheric ozone profile data set (ML-TOMCAT V1.0). The underlying CTM simulation was forced by meteorological reanalyses, specified trends in long-lived source gases, solar flux and aerosol variations. The RF is trained using the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) data set over the time periods of the Microwave Limb Sounder (MLS) from the Upper Atmosphere Research Satellite (UARS) (1991–1998) and Aura (2005–2016) missions. We find that ML-TOMCAT shows excellent agreement with available independent satellite-based data sets which use pressure as a vertical coordinate (e.g. GOZCARDS, SWOOSH for non-MLS periods) but weaker agreement with the data sets which are altitude-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS). We find that at almost all stratospheric levels ML-TOMCAT ozone concentrations are well within uncertainties of the observational data sets. The ML-TOMCAT (V1.0) data set is ideally suited for the evaluation of chemical model ozone profiles from the tropopause to 0.1 hPa and is freely available via https://doi.org/10.5281/zenodo.5651194 (Dhomse et al., 2021).

The impact of iodine on ozone trends in the lower stratosphere

2020 ◽  
Author(s):  
Martyn Chipperfield ◽  
Wuhu Feng ◽  
Sandip Dhomse ◽  
Yajuan Li ◽  
Ryan Hossaini ◽  
...  
Keyword(s):  
Lower Stratosphere ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Ozone Layer ◽  
Small Contribution ◽  
Chemical Transport Model ◽  
Heterogeneous Processes ◽  
Ozone Trends ◽  
Phase Chemistry ◽  
The Impact

<p>Depletion of the stratospheric ozone layer by chlorine and bromine species has been a major environmental issue since the early 1970s. Following controls on the production of the long-lived halocarbons which transport chlorine and bromine to the stratosphere, the ozone layer is expected to recover over the course of this century. Decreases in the stratospheric loading of chlorine and bromine have been observed and there are signs of this resulting in an increase in ozone in the upper stratosphere and the Antarctic lower stratosphere. However, in contrast to this expectation of increasing stratospheric ozone, Ball et al. (ACP doi:10.5194/acp-18-1379-2018, 2018, ACP doi:10.5194/acp-19-12731-2019, 2019) have reported evidence for an ongoing decline in lower stratospheric ozone at extrapolar latitudes between 60°S and 60°N. Chipperfield et al. (GRL, doi:10.1029/2018GL078071, 2018) analysed these results using the TOMCAT 3-D chemical transport model (CTM). They reported that much of the observed ozone decrease could be explained by dynamical variability. Furthermore, they investigated the potential role for bromine and chlorine from very short-lived species (VSLS) but found only a small contribution.</p><p>Very recently, Koenig et al. (PNAS, doi:10.1073/pnas.1916828117, 2020) have reported quantitative observations of almost 1 pptv iodine in the lower stratosphere. They show that this iodine is an important contribution to the local iodine loss budget and speculate that a trend in iodine could therefore explain the observed downward trend in ozone.</p><p>Here we use an updated version of the TOMCAT CTM to investigate the impact of iodine on lower stratospheric ozone trends. We repeat the simulations of Chipperfield et al. (2018), using both ERA-Interim and ERA5 reanalyses (to compare the quantification of the dynamical contribution). We use assume trends in the stratospheric injection of iodine to quantify the possible impact of this on global ozone trends through both gas-phase chemistry and novel heterogeneous processes.</p><p> </p>

scholarly journals Tropospheric ozone variability in the tropics from ENSO to MJO and shorter timescales

2015 ◽  
Vol 15 (14) ◽  
pp. 8037-8049 ◽  
Author(s):  
J. R. Ziemke ◽  
A. R. Douglass ◽  
L. D. Oman ◽  
S. E. Strahan ◽  
B. N. Duncan
Keyword(s):  
Tropospheric Ozone ◽  
Large Scale ◽  
Climate Model ◽  
Transport Model ◽  
Southern Oscillation ◽  
Longwave Radiation ◽  
Chemical Transport Model ◽  
Enso Variability ◽  
Earth Observing System ◽  
The Tropics

Abstract. Aura OMI and MLS measurements are combined to produce daily maps of tropospheric ozone beginning October 2004. We show that El Niño-Southern Oscillation (ENSO) related inter-annual change in tropospheric ozone in the tropics is small in relation to combined intra-seasonal/Madden–Julian Oscillation (MJO) and shorter timescale variability by a factor of ~ 3–10 (largest in the Atlantic). Outgoing longwave radiation (OLR), taken as a proxy for convection, suggests that convection is a dominant driver of large-scale variability of tropospheric ozone in the Pacific from inter-annual (e.g., ENSO) to weekly periods. We compare tropospheric ozone and OLR satellite observations with two simulations: (1) the Goddard Earth Observing System (GEOS) chemistry-climate model (CCM) that uses observed sea surface temperatures and is otherwise free-running, and (2) the NASA Global Modeling Initiative (GMI) chemical transport model (CTM) that is driven by Modern Era Retrospective-Analysis for Research and Applications (MERRA) analyses. It is shown that the CTM-simulated ozone accurately matches measurements for timescales from ENSO to intra-seasonal/MJO and even 1–2-week periods. The CCM simulation reproduces ENSO variability but not shorter timescales. These analyses suggest that a model used to delineate temporal and/or spatial properties of tropospheric ozone and convection in the tropics must reproduce both ENSO and non-ENSO variability.

scholarly journals Stratospheric ozone intrusion events and their impacts on tropospheric ozone

2017 ◽  
Author(s):  
Jesse W. Greenslade ◽  
Simon P. Alexander ◽  
Robyn Schofield ◽  
Jenny A. Fisher ◽  
Andrew K. Klekociuk
Keyword(s):  
Southern Ocean ◽  
Southern Hemisphere ◽  
Tropospheric Ozone ◽  
Bandpass Filter ◽  
Transport Model ◽  
Meteorological Data ◽  
Stratospheric Ozone ◽  
Chemical Transport Model ◽  
Macquarie Island ◽  
Modelling Studies

Abstract. Stratosphere-to-troposphere transport (STT) provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the southern hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality and quantify the ozone transported across the tropopause over Davis (69° S), Macquarie Island (54° S), and Melbourne (38° S). STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile, and an analysis of the Brunt-Viäsälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter above all three sites. The majority of tropospheric ozone enhancements from STT events occur within 2.5 km, 3 km of the tropopause at Davis, and Macquarie Island. Events are more spread out at Melbourne, occurring frequently up to 7.5 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is 2–4 % at each site; however, during individual events over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, these are apparent during austral winter and spring, and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely resolved to distinguish STT events but is able to accurately simulate the seasonal cycle of tropospheric ozone columns over the three southern hemisphere sites. Combining the ozonesonde-derived STT event characteristics with the simulated tropospheric ozone columns from GEOS-Chem, we conservatively estimate that the annual tropospheric ozone flux over the Southern Ocean due to STT events is ~ 3.2 ×1016 molecules cm−2 yr−1. This value is significantly lower than expected from previous global estimates due to the conservative nature of several components of our calculation, in particular the contribution of STT to total tropospheric ozone during an event (STT impact). Using an assumed STT impact of 35 % based on prior modelling studies rather than our observational estimate of 2–4 % increases the estimated Southern Ocean flux by an order of magnitude. Despite lingering uncertainties in scaling ozonesonde measurements to regional values, ozonesonde datasets provide a useful tool for STT detection, and the analysis methods described in this paper could be applied to many existing long-term records.

scholarly journals Stratospheric ozone intrusion events and their impacts on tropospheric ozone in the Southern Hemisphere

2017 ◽  
Vol 17 (17) ◽  
pp. 10269-10290 ◽  
Author(s):  
Jesse W. Greenslade ◽  
Simon P. Alexander ◽  
Robyn Schofield ◽  
Jenny A. Fisher ◽  
Andrew K. Klekociuk
Keyword(s):  
Southern Hemisphere ◽  
Tropospheric Ozone ◽  
Bandpass Filter ◽  
Transport Model ◽  
Meteorological Data ◽  
Stratospheric Ozone ◽  
Austral Summer ◽  
Chemical Transport Model ◽  
Macquarie Island ◽  
Ozone Profile

Abstract. Stratosphere-to-troposphere transport (STT) provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the Southern Hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality of STT events and quantify the ozone transported across the tropopause over Davis (69° S, 2006–2013), Macquarie Island (54° S, 2004–2013), and Melbourne (38° S, 2004–2013). STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile and an analysis of the Brunt–Väisälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter for all three sites. The majority of tropospheric ozone enhancements owing to STT events occur within 2.5 and 3 km of the tropopause at Davis and Macquarie Island respectively. Events are more spread out at Melbourne, occurring frequently up to 6 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is  ∼ 1. 0–3. 5 % at each site; however, during individual events, over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low-pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, which are apparent during austral winter and spring and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely resolved to distinguish STT events but is able to accurately simulate the seasonal cycle of tropospheric ozone columns over the three southern hemispheric sites. Combining the ozonesonde-derived STT event characteristics with the simulated tropospheric ozone columns from GEOS-Chem, we estimate STT ozone flux near the three sites and see austral summer dominated yearly amounts of between 5. 7 and 8. 7 × 1017 molecules cm−2 a−1.

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