Vertical Ozone Profiles Research Articles

Comparison of ozone vertical profiles in the upper troposphere–stratosphere measured over Tomsk, Russia (56.5° N, 85.0° E) with DIAL, MLS, and IASI

ABSTRACT Laser ranging methods employing light detection and ranging (LiDAR) technology are widely used for studying the atmosphere and monitoring its state. The purpose of this work is to measure the ozone vertical distribution (OVD) in the upper troposphere–stratosphere by differential absorption LiDAR (DIAL) at 299–341 nm and 308–353 nm and to compare the results with satellite data. А LiDAR complex for measuring the OVD in the altitude range approximately 5–45 km has been created. Here, we analyse the results of ozone LiDAR measurements at wavelengths of 299–341 nm and 308–353 nm between 2017 and 2018 at Siberian LiDAR Station (SLS) and compare them with satellite (Microwave Limb Sounder (MLS)/Aura and Infrared Atmospheric Sounding Interferometer (IASI)/MetOp) measurements of OVD. The retrieved LiDAR OVD profiles in the upper troposphere–stratosphere in comparison with MLS/Aura and IASI/MetOp profiles, as well as the stitched OVD profile in comparison with the mid-latitude Krueger model, confirm the prospects of using the pairs of ozone sounding wavelengths 299–341 nm and 308–353 nm. The average relative difference between LiDAR and MLS/Aura measurements is negative in the altitude range 16–38 km and attains –49.81% at 38 km, and also, the average relative difference between LiDAR and IASI/MetOp measurements is positive in the altitude ranges 6 and 7.40 to 18 km, where it attains 43.68% at 16.80 km, and is negative in the altitude range 6–7.30 km, where it attains – 43.86% at 6.20 km.

Stratosphere–Troposphere Exchange and O3 Variability in the Lower Stratosphere and Upper Troposphere over the Irene SHADOZ Site, South Africa

This study aims to investigate the Stratosphere-Troposphere Exchange (STE) events and ozone changes over Irene (25.5° S, 28.1° E). Twelve years of ozonesondes data (2000–2007, 2012–2015) from Irene station operating in the framework of the Southern Hemisphere Additional Ozonesodes (SHADOZ) was used to study the troposphere (0–16 km) and stratosphere (17–28 km) ozone (O3) vertical profiles. Ozone profiles were grouped into three categories (2000–2003, 2004–2007 and 2012–2015) and average composites were calculated for each category. Fifteen O3 enhancement events were identified over the study period. These events were observed in all seasons (one event in summer, four events in autumn, five events in winter and five events in spring); however, they predominantly occur in winter and spring. The STE events presented here are observed to be influenced by the Southern Hemisphere polar vortex. To strengthen the investigation into STE events, advected potential vorticity maps were used, which were assimilated using Modélisation Isentrope du transport Méso–échelle de l’Ozone Stratosphérique par Advection (MIMOSA) model for the 350 K (~12–13 km) isentropic level. These maps indicated transport of high latitude air masses responsible for the reduction of the O3 mole fractions at the lower stratosphere over Irene which coincides with the enhancement of ozone in the upper troposphere. In general, the stratosphere is dominated by higher Modern Retrospective Analysis for Research Application (MERRA-2) potential vorticity (PV) values compared to the troposphere. However, during the STE events, higher PV values from the stratosphere were observed to intrude the troposphere. Ozone decline was observed from 12 km to 24 km with the highest decline occurring from 14 km to 18 km. An average decrease of 6.0% and 9.1% was calculated from 12 to 24 km in 2004–2007 and 2012–2015 respectively, when compared with 2000–2003 average composite. The observed decline occurred in the upper troposphere and lower stratosphere with winter and spring showing more decline compared with summer and autumn.

Compact and movable ozone differential absorption lidar system based on an all-solid-state, tuning-free laser source.

The differential absorption lidar (DIAL) has been proposed as an effective method for detecting polluted gases in the atmosphere. In this paper, we present a compact and movable ozone differential absorption (O3-DIAL) based on an all-solid-state and tuning-free laser source. For the first time, solid-state stimulated Raman scattering technology is used in the emitting source of the lidar for wavelength conversion. A high repetition frequency Innoslab laser is used for pumping SrWO4 crystals to get yellow lasers which can achieve up to 70% light-to-light conversion efficiency. Our results demonstrate that using the SrWO4 crystal as the Raman frequency-shifting media of the lidar laser source for obtaining the vertical profiles of tropospheric ozone in the Planetary Boundary Layer (PBL) is a suitable choice. As a compact movable lidar system, the results demonstrate the reliability and stability.

Development and utilization of hexacopter unmanned aerial vehicle platform to characterize vertical distribution of boundary layer ozone in wintertime

Vertical observations of ozone play vital roles in understanding various atmospheric chemical processes in the boundary layer, particularly in winter. In this study, we attempted to measure vertical profiles of boundary layer ozone in the winter of 2018 over the Yangtze River Delta region of China, using a hexacopter unmanned aerial vehicle (UAV) platform. A commercial portable ozone monitor mounted in a thermal insulation box was attached to the UAV platform to conduct vertical ozone measurements. The results showed that the UAV platform could effectively capture the vertical variations of boundary layer ozone in wintertime. During the field campaign, surface ozone was in relatively low levels due to weak photochemical production. In the daytime, the ozone was well mixed within the boundary layer. At nighttime, uniform vertical distribution patterns and stratified distribution patterns were frequently obtained in ozone profiles below 500 m. Backward trajectories and wind profiles were used to investigate the horizontal and vertical transport of ozone. The stratified distribution patterns of ozone were closely associated with strong contemporary advection transport of ozone that was accompanied by enhanced winds aloft. Besides, strong wind shear enhanced the downward transport of ozone from the free troposphere into the boundary layer, leading to uniform vertical distribution patterns of boundary layer ozone and the elevated nocturnal surface ozone levels. The results of this study could provide insights into the understanding of the spatial variations and evolution patterns of boundary layer ozone in wintertime and constructing suitable boundary layer schemes in atmospheric chemical models.

Implementation of the CMIP6 Forcing Data in the IPSL‐CM6A‐LR Model

AbstractThe implementation of boundary conditions is a key aspect of climate simulations. We describe here how the Climate Model Intercomparison Project Phase 6 (CMIP6) forcing data sets have been processed and implemented in Version 6 of the Institut Pierre‐Simon Laplace (IPSL) climate model (IPSL‐CM6A‐LR) as used for CMIP6. Details peculiar to some of the Model Intercomparison Projects are also described. IPSL‐CM6A‐LR is run without interactive chemistry; thus, tropospheric and stratospheric aerosols as well as ozone have to be prescribed. We improved the aerosol interpolation procedure and highlight a new methodology to adjust the ozone vertical profile in a way that is consistent with the model dynamical state at the time step level. The corresponding instantaneous and effective radiative forcings have been estimated and are being presented where possible.

Advanced Ultraviolet Radiation and Ozone Retrieval for Applications—Surface Ultraviolet Radiation Products

AURORA (Advanced Ultraviolet Radiation and Ozone Retrieval for Applications) is a three-year project supported by the European Union in the frame of its H2020 Call (EO-2-2015) for “Stimulating wider research use of Copernicus Sentinel Data”. The project addresses key scientific issues relevant for synergistic exploitation of data acquired in different spectral ranges by different instruments on board the atmospheric Sentinels. A novel approach, based on the assimilation of geosynchronous equatorial orbit (GEO) and low Earth orbit (LEO) fused products by application of an innovative algorithm to Sentinel-4 (S-4) and Sentinel-5 (S-5) synthetic data, is adopted to assess the quality of the unique ozone vertical profile obtained in a context simulating the operational environment. The first priority is then attributed to the lower atmosphere with calculation of tropospheric columns and ultraviolet (UV) surface radiation from the resulting ozone vertical distribution. Here we provide details on the surface UV algorithm of AURORA. Both UV index (UVI) and UV-A irradiance are provided from synthetic satellite measurements, which in turn are based on atmospheric scenarios from MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, Version 2) re-analysis. The UV algorithm is implemented in a software tool integrated in the technological infrastructure developed in the context of AURORA for the management of the synthetic data and for supporting the data processing. This was closely linked to the application-oriented activities of the project, aimed to improve the performance and functionality of a downstream application for personal UV dosimetry based on satellite data. The use of synthetic measurements from MERRA-2 gives us also a “ground truth”, against which to evaluate the performance of our UV model with varying inputs. In this study we both describe the UV algorithm itself and assess the influence that changes in ozone profiles, due to the fusion and assimilation, can cause in surface UV levels.

Measurements of Ozone Vertical Profiles in the Upper Troposphere–Stratosphere over Western Siberia by DIAL, MLS, and IASI

The purpose of this work is to measure the ozone vertical distribution (OVD) in the upper troposphere–stratosphere by differential absorption lidar (DIAL) at 299/341 nm and 308/353 nm and to compare and analyze the results against satellite data. А lidar complex for measuring the OVD in the altitude range ≈(5–45) km has been created. Here we analyze the results of ozone lidar measurements at wavelengths of 299/341 nm and 308/353 nm in 2018 at Siberian Lidar Station (SLS) and compare them with satellite (MLS/Aura and IASI/MetOp) measurements of OVD. The retrieved lidar OVD profiles in the upper troposphere–stratosphere in comparison with MLS/Aura and IASI/MetOp profiles, as well as the stitched OVD profile in comparison with the mid-latitude Krueger model, confirm the prospects of using the pairs of ozone sounding wavelengths 299/341 and 308/353 nm.

Ozone Lidar Observations in the City of Paris: Seasonal Variability and Role of The Nocturnal Low Level Jet

Ozone lidar measurements have been carried out in Paris during 4 years to characterize the seasonal variability of the vertical gradient within the urban planetary boundary layer (PBL). The interaction between NOx emission and thermal stability of the PBL is the main driver of the winter strong positive O3 gradient, while summer neutral gradient is related to weaker thermal stability and photochemical ozone production at the regional scale. Simultaneous lidar measurements of ozone and wind vertical profiles during 36 hours in September 2014 also show that the nocturnal low level jet (NLLJ) plays a significant role in the early morning ozone increase.

Vertical Characteristics of Winter Ozone Distribution within the Boundary Layer in Shanghai Based on Hexacopter Unmanned Aerial Vehicle Platform

Ozone is an important secondary air pollutant and plays different significant roles in regulating the formation of secondary organic aerosols. However, the characteristics of winter vertical ozone distributions have rarely been studied. In the winter of 2017, field experiments were performed in Shanghai, China using hexacopter unmanned aerial vehicle (UAV) platforms. The vertical profiles of ozone were obtained from 0–1200 m above the ground level. Results show that the UAV observations were reliable to capture the vertical variations of ozone. Vertical ozone profiles in the winter are classified into four categories: (1) well-mixed profile, (2) altitudinal increasing profile, (3) stratification profile, and (4) spike profile. Results show that although the average surface ozone level was relatively low, strong ozone variability and high ozone concentrations occurred at the upper air. The maximum observed ozone concentration was 220 ppb. In addition, using meteorological profiles and backward trajectories, we found that the ozone elevation aloft can be attributed to the downward transport of air flow from higher altitudes. Furthermore, ozone accumulation in the winter could be influenced by the horizontal transport of air masses for the northern part of China. This study successfully used hexacopter UAV platforms to perform vertical observations within the boundary layer. This provides systematic classification of winter ozone distribution within the boundary layer.

Intercomparison of Ground- and Satellite-Based Total Ozone Data Products at Marambio Base, Antarctic Peninsula Region

This study aims to compare the ground-based Brewer spectrophotometer total ozone column measurements with the Dobson spectrophotometer and various satellite overpass data available at Marambio Base during the period 2011–2013. This station provides a unique opportunity to study ozone variability near the edge of the southern polar vortex; therefore, many institutions, such as the National Meteorological Service of Argentina, the Finnish Meteorological Institute and the Czech Hydrometeorological Institute, have been carrying out various scientific activities there. The intercomparison was performed using total ozone column data sets retrieved from the ground-based instruments and from Ozone Monitoring Instrument (OMI)—Total Ozone Mapping Spectrometer (TOMS), OMI–Differential Optical Absorption Spectroscopy (DOAS), Global Ozone Monitoring Experiment 2 (GOME2), and Scanning Imaging Absorption Spectrophotometer for Atmospheric Cartography (SCIAMACHY) satellite observations. To assess the quality of the selected data products, comparisons with reference to the Brewer spectrophotometer single observations were made. The performance of the satellite observational techniques was assessed against the solar zenith angle and effective temperature, as well as against the actual shape of the vertical ozone profiles, which represent an important input parameter for the satellite ozone retrievals. The ground-based Dobson observations showed the best agreement with the Brewer data set (R2 = 1.00, RMSE = 1.5%); however, significant solar zenith angle (SZA) dependency was found. The satellite overpass data confirmed good agreement with the Brewer observations but were, however, overestimated in all cases except for the OMI(TOMS), when the mean bias differed from −0.7 DU in the case of the OMI(TOMS) to 6.4 DU for the SCIAMACHY. The differences in satellite observational techniques were further evaluated using statistical analyses adapted for depleted and non-depleted conditions over the ozone hole period.

Evaluation of NASA's high-resolution global composition simulations: Understanding a pollution event in the Chesapeake Bay during the summer 2017 OWLETS campaign

Recirculation of pollutants due to a bay breeze effect is a key meteorological mechanism impacting air quality near urban coastal areas, but regional and global chemical transport models have historically struggled to capture this phenomenon. We present a case study of a high ozone (O3) episode observed over the Chesapeake Bay during the NASA Ozone Water-Land Environmental Transition Study (OWLETS) in summer 2017. OWLETS included a complementary suite of ground-based and airborne observations, with which we characterize the meteorological and chemical context of this event and develop a framework to evaluate model performance. Two publicly-available NASA global high-resolution coupled chemistry-meteorology models (CCMMs) are investigated: GEOS-CF and MERRA2-GMI. The GEOS-CF R2 value for comparisons between the NASA Sherpa C-23 aircraft measurements to the GEOS-CF resulted in good agreement (R2: 0.67) on July 19th and fair agreement (R2: 0.55) for July 20th. Compared to surface observations, we find the GEOS-CF product with a 25 × 25 km2 grid box, at an hourly (R2: 0.62 to 0.87) and 15-min (R2: 0.64 to 0.87) interval for six regional sites outperforms the hourly nominally 50 × 50 km2 gridded MERRA2-GMI (R2: 0.53 to 0.76) for four of the six sites, suggesting it is better capable of simulating complex chemical and meteorological features associated with ozone transport within the Chesapeake Bay airshed. When the GEOS-CF product was compared to the TOLNet LiDAR observations at both NASA Langley Research Center (LaRC) and the Chesapeake Bay Bridge Tunnel (CBBT), the median differences at LaRC were −6 to 8% and at CBBT were ±7% between 400 and 2000 m ASL. This indicates that, for this case study, the GEOS-CF is able to simulate surface level ozone diurnal cycles and vertical ozone profiles at small scales between the surface level and 2000 m ASL. Evaluating global chemical model simulations at sub-regional scales will help air quality scientists understand the complex processes occurring at small spatial and temporal scales within complex surface terrain changes, simulating nighttime chemistry and deposition, and the potential to use global chemical transport simulations in support of regional and sub-regional field campaigns.

Variations in the vertical profile of ozone at four high-latitude Arctic sites from 2005 to 2017

Abstract. Understanding variations in atmospheric ozone in the Arctic is difficult because there are only a few long-term records of vertical ozone profiles in this region. We present 12 years of ozone profiles from February 2005 to February 2017 at four sites: Summit Station, Greenland; Ny-Ålesund, Svalbard, Norway; and Alert and Eureka, Nunavut, Canada. These profiles are created by combining ozonesonde measurements with ozone profile retrievals using data from the Microwave Limb Sounder (MLS). This combination creates a high-quality dataset with low uncertainty values by relying on in situ measurements of the maximum altitude of the ozonesondes (∼30 km) and satellite retrievals in the upper atmosphere (up to 60 km). For each station, the total column ozone (TCO) and the partial column ozone (PCO) in four atmospheric layers (troposphere to upper stratosphere) are analyzed. Overall, the seasonal cycles are similar at these sites. However, the TCO over Ny-Ålesund starts to decline 2 months later than at the other sites. In summer, the PCO in the upper stratosphere over Summit Station is slightly higher than at the other sites and exhibits a higher standard deviation. The decrease in PCO in the middle and upper stratosphere during fall is also lower over Summit Station. The maximum value of the lower- and middle-stratospheric PCO is reached earlier in the year over Eureka. Trend analysis over the 12-year period shows significant trends in most of the layers over Summit and Ny-Ålesund during summer and fall. To understand deseasonalized ozone variations, we identify the most important dynamical drivers of Arctic ozone at each level. These drivers are chosen based on mutual selected proxies at the four sites using stepwise multiple regression (SMR) analysis of various dynamical parameters with deseasonalized data. The final regression model is able to explain more than 80 % of the TCO and more than 70 % of the PCO in almost all of the layers. The regression model provides the greatest explanatory value in the middle stratosphere. The important proxies of the deseasonalized ozone time series at the four sites are tropopause pressure (TP) and equivalent latitude (EQL) at 370 K in the troposphere, the quasi-biennial oscillation (QBO) in the troposphere and lower stratosphere, the equivalent latitude at 550 K in the middle and upper stratosphere, and the eddy heat flux (EHF) and volume of polar stratospheric clouds throughout the stratosphere.

Assessing the role of planetary and gravity waves in the vertical structure of ozone over midlatitudinal Europe

Abstract. Planetary and gravity waves play an important role in the dynamics of the atmosphere. They are present in the atmospheric distribution of temperature, wind, and ozone content. These waves are detectable also in the vertical profile of ozone and they cause its undulation. One of the structures occurring in the vertical ozone profile is laminae, which are narrow layers of enhanced or depleted ozone concentrations in the vertical ozone profile. They are connected with the total amount of ozone in the atmosphere and with the activity of the planetary and gravity waves. The aim of this paper is to quantify these processes in midlatitudinal Europe. We compare the occurrence of laminae induced by planetary waves (PL) with the occurrence of these induced by gravity waves (GL). We show that the PL are 10–20 times more frequent than that of GL. There is a strong annual variation of PL, while GL exhibit only a very weak variation. With the increasing lamina size the share of GL decreases and the share of PL increases. The vertical profile of lamina occurrence is different for PL and GL smaller than 2 mPa. For laminae greater than 2 mPa this difference is smaller.

Ozone Measurements Using the Refurbished Eureka Stratospheric Differential Absorption Lidar

The Stratospheric Ozone Differential Absorption Lidar (DIAL) located at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut (80°N, 86°W) has been a powerful tool for the measurement of stratospheric ozone vertical profiles in the Canadian High Arctic since 1993. The lidar ozone profiles measured during the 2017 Canadian Arctic Atmospheric Chemistry Experiment (ACE) and Optical Spectrograph and InfraRed Imaging System (OSIRIS) Validation Campaign were compared to coincident ozonesonde, ACE-FTS, ACE-MAESTRO and OSIRIS profiles. The results show the lidar overestimates the ozone by ∼10% in the 10 km–20 km altitude range on average in comparison with the ozonesonde. Above 20 km the profiles agree within 10%. The OSIRIS ozone agrees within 10% with DIAL ozone between 15 km and 41 km. A strong stratospheric ozone depletion event was seen on March 3, 2017, during which the ozone concentration dropped below 1012 molecules cm–3 at the 15.5 km and below 6 × 1012 molecules cm–3 at 16 km as measured by the ozonesonde and the lidar correspondingly. Laminated structures were observed in the ozonesonde profiles near the polar vortex edge regions. This together with non-optimal temporal and spatial coincidences between the measurements conducted by different instruments can affect validation accuracy.

Detection and classification of laminae in balloon-borne ozonesonde profiles: application to the long-term record from Boulder, Colorado

Abstract. We quantify ozone variability in the upper troposphere and lower stratosphere (UTLS) by investigating lamination features in balloon measurements of ozone mixing ratio and potential temperature. Laminae are defined as stratified variations in ozone that meet or exceed a 10 % threshold for deviations from a basic state vertical profile of ozone. The basic state profiles are derived for each sounding using smoothing methods applied within a vertical coordinate system relative to the World Meteorological Organization (WMO) tropopause. We present results of this analysis for the 25-year record of ozonesonde measurements from Boulder, Colorado. The mean number of ozone laminae identified per sounding is about 9±2 (1σ). The root-mean-square relative amplitude is 20 %, and laminae with much larger amplitudes (>40 %) are seen in ∼ 2 % of the profiles. The vertical scale of detected ozone laminae typically ranges between 0.5 and 1.2 km. The lamina occurrence frequency varies significantly with altitude and is largest within ∼2 km of the tropopause. Overall, ozone laminae identified in our analysis account for more than one-third of the total intra-seasonal variability in ozone. A correlation technique between ozone and potential temperature is used to classify the subset of ozone laminae that are associated with gravity wave (GW) phenomena, which accounts for 28 % of all laminar ozone features. The remaining 72 % of laminae arise from non-gravity wave (NGW) phenomena. There are differences in both the vertical distribution and seasonality of GW versus NGW ozone laminae that are linked to the contrast in main generating mechanisms for each laminae type.

A mobile differential absorption lidar for simultaneous observations of tropospheric and stratospheric ozone over Tibet.

We developed a mobile ozone differential absorption lidar system to simultaneously measure the vertical profiles of tropospheric and stratospheric ozone from an altitude of ~5 to 50 km. The system emits four laser beams at wavelength of 289 nm, 299 nm, 308 nm and 355 nm and receives their corresponding Mie/Rayleigh backscattering return signals, and two N2 Raman return signals at 332 nm and 387 nm shifted from 308 nm and 355 nm, respectively. An assembled telescope array with four 1.25-m telescopes (effective diameter > 2 m) collects the Rayleigh and Raman backscattering signals at 308/332 and 355/387 nm. This system is currently deployed at the Yangbajing Observatory in Tibet (~4300 m elevation) and has begun observations in regular campaign mode since October 2017. The lidar results agree very well with those observed by the Aura/MLS satellite. This novel ozone lidar system operates at the highest elevation of any such system in the world. The higher elevation and larger receiver aperture of this system yield a higher signal-to-noise ratio and lower statistical uncertainty.

Validation of the TOLNet lidars: the Southern California Ozone Observation Project (SCOOP)

Abstract. The North America-based Tropospheric Ozone Lidar Network (TOLNet) was recently established to provide high spatiotemporal vertical profiles of ozone, to better understand physical processes driving tropospheric ozone variability and to validate the tropospheric ozone measurements of upcoming spaceborne missions such as Tropospheric Emissions: Monitoring Pollution (TEMPO). The network currently comprises six tropospheric ozone lidars, four of which are mobile instruments deploying to the field a few times per year, based on campaign and science needs. In August 2016, all four mobile TOLNet lidars were brought to the fixed TOLNet site of JPL Table Mountain Facility for the 1-week-long Southern California Ozone Observation Project (SCOOP). This intercomparison campaign, which included 400 h of lidar measurements and 18 ozonesonde launches, allowed for the unprecedented simultaneous validation of five of the six TOLNet lidars. For measurements between 3 and 10 km a.s.l., a mean difference of 0.7 ppbv (1.7 %), with a root-mean-square deviation of 1.6 ppbv or 2.4 %, was found between the lidars and ozonesondes, which is well within the combined uncertainties of the two measurement techniques. The few minor differences identified were typically associated with the known limitations of the lidars at the profile altitude extremes (i.e., first 1 km above ground and at the instruments' highest retrievable altitude). As part of a large homogenization and quality control effort within the network, many aspects of the TOLNet in-house data processing algorithms were also standardized and validated. This thorough validation of both the measurements and retrievals builds confidence as to the high quality and reliability of the TOLNet ozone lidar profiles for many years to come, making TOLNet a valuable ground-based reference network for tropospheric ozone profiling.

Influence of vertical mixing and nighttime transport on surface ozone variability in the morning in Paris and the surrounding region

Vertical profiles of ozone (O3), aerosols, and winds in Paris, France have been measured via remote sensing (Lidar) during a 36 h intensive observation period (IOP) on 9–10 September 2014. The measurements show an ozone poor layer (ozone concentrations as low as 40 μg.m−3) is present above the nocturnal boundary layer (NBL) during the IOP (∼400 m AGL, 10 Sept. 2014 06:00 LT). This ozone poor layer is reincorporated in the morning into the developing daytime boundary layer, resulting in lower measured surface ozone concentrations in Paris. Specifically, the surface ozone concentration at 12:30 LT is 33 μg.m−3 smaller on 10 Sept. 2014 than on 9 Sept. 2014 in Paris. This ozone poor layer is also co-located with a nocturnal low-level jet (NLLJ), which transports air away from the Paris region, resulting in lower ozone concentrations downwind of Paris the following day. We track transport and dispersion of this airmass using the regional Weather Research and Forecasting (WRF) model combined with the FLEXible PARTicle dispersion model (FLEXPART-WRF). This dataset demonstrates that clean air masses above the NBL have the ability to impact “next-day” ozone concentrations in cities and the surrounding areas. Our analysis shows that vertical mixing and incorporation of ozone located above the boundary layer in the morning is a significant factor that can control daytime surface ozone concentrations in Paris and the surrounding area.

Impact of time-dependent chemical boundary conditions on tropospheric ozone simulation with WRF-Chem: An experiment over the Metropolitan Area of São Paulo

WRF-Chem (Weather Research and Forecasting with Chemistry Model) is being used to perform air quality forecast over the southeast Brazil with a domain centered in the Metropolitan Area of São Paulo (MASP). The simulations are used to understand the pollutants behavior concerning the fluxes to and from the urban areas, to examine the formation of secondary pollutants (e.g., tropospheric ozone), and to validate the efficacy of air quality policies implementation, particularly the ones that are related to the vehicular fuel used in the region. One important factor to improve the air quality simulations is the configuration of suited inflow boundary conditions for the chemical species. In that context, the objective of this study is to assess the impacts of using time-dependent Chemical Lateral Boundary Conditions (CBC) on tropospheric ozone simulations with WRF-Chem. Two simulations were carried out using Carbon-Bond Mechanism version Z (CBMZ). The first simulation was a set-up to run with WRF-Chem default CBC, and the second one using time-dependent CBC obtained from MOZART-4 (Model for Ozone and Related chemical Tracers, version 4) simulations. The period of study was from May 15 to May 18 and from October 30 to November 1, 2006, when a comprehensive experiment with ozonesondes launching and surface measurements was performed. Results show that using MOZART-4 CBC reduced mean bias, RMSE and slightly improved correlation coefficients for ground level ozone as well as ozone vertical profile above 3 km. These improvements were more significant during periods with lower photochemical activity. However, underestimation of ozone concentration peaks was also observed in this period, which can be an issue for operational air quality forecasting.

Vertical Profiles of Tropospheric Ozone From MAX‐DOAS Measurements During the CINDI‐2 Campaign: Part 1—Development of a New Retrieval Algorithm

AbstractGround‐based measurements of tropospheric ozone (O3) are valuable for studies of atmospheric chemistry, air pollution, climate change, and for satellite validation. The Multi Axis Differential Optical Absorption Spectroscopy (MAX‐DOAS) technique has been widely used to derive vertical profiles of trace gases and aerosols in the troposphere. However, tropospheric O3 has not yet been satisfactorily derived from MAX‐DOAS measurements due to the influence of stratospheric O3 absorption. In this study, we developed two new retrieval approaches for tropospheric O3 from MAX‐DOAS measurements. In method 1, stratospheric O3 profiles from external data sources are considered in the retrieval. In method 2, stratospheric and tropospheric O3 are separated based on the temperature‐dependent differences between tropospheric and stratospheric O3 absorption structures in the UV spectral range. The feasibility of both methods is first verified by applying them to synthetic spectra. Then they are applied to real MAX‐DOAS measurements recorded during the CINDI‐2 campaign in Cabauw, the Netherlands (September 2016). The obtained results are compared with independent O3 measurements and global chemical transport model simulations. Good agreement of the near‐surface O3 concentrations with the independent data sets is found for both methods. However, tropospheric O3 profiles are only reasonably derived using method 1, while they are significantly overestimated at altitudes above 1 km using method 2, probably due to the approximation of the ring spectra used to correct the rotational Raman scattering structures in the DOAS fit. Advantages and disadvantages of both methods are discussed and improvement directions are suggested for further studies.