Ozone Lidar Measurements Research Articles

Microwave and Lidar Measurements of Ozone and Temperature Variations during Stratospheric Warmings of 2012–2015

Microwave and Lidar Measurements of Ozone and Temperature Variations during Stratospheric Warmings of 2012–2015

Vertical Profiles of Ozone Concentrations in the Lower Troposphere Downwind of New York City During LISTOS 2018–2019

AbstractWhile surface concentrations of ozone are routinely monitored, ozone aloft is infrequently measured, but critical for a full understanding of ozone production and transport. In this study, twenty‐six balloon‐borne ozonesondes were launched near the north shore of central Long Island in the summers of 2018 and 2019 as part of the Long Island Sound Tropospheric Ozone Study (LISTOS). The observed vertical ozone profiles are presented and analyzed with additional data sources and modeling tools, including lidar wind profiles from the New York State Mesonet, back trajectories based on 3 km resolution high‐resolution rapid refresh model data, and surface data, aircraft observations, sonde, and ozone lidar measurements from other LISTOS participants. Special attention is given to the region of interest for ozone pollution in the lower troposphere, from the surface to 2 km altitude. Cases analyzed in detail illustrate events with high ozone levels observed in the lower troposphere, often with pronounced vertical structure in the profile. Specifically, easily discernible layers are identified with ozone excursions of up to 40 ppb over short vertical distances. Analysis indicates that synoptic and local meteorological processes can combine to generate the observed vertical profiles. Hot, sunny days with high‐pressure systems are accompanied by high precursor emissions due to increased power demands, plentiful radiation for photochemistry, and stagnation of synoptic winds. Under these conditions, meso‐ and smaller‐scale flows like low‐level jets and sea/bay/land breeze circulations may dominate synoptic flow to produce shearing and the complex vertical layered structure observed.

Evaluation of the new DWD ozone and temperature lidar during the Hohenpeißenberg Ozone Profiling Study (HOPS) and comparison of results with previous NDACC campaigns

Abstract. A newly upgraded German Weather Service (DWD) ozone and temperature lidar (HOH) located at the Hohenpeißenberg Meteorological Observatory (47.8∘ N, 11.0∘ E) has been evaluated through comparison with the travelling standard lidar operated by NASA's Goddard Space Flight Center (NASA GSFC Stratospheric Ozone (STROZ) lidar), satellite overpasses from the Microwave Limb Sounder (MLS), the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), the Ozone Mapping and Profiler Suite (OMPS), meteorological radiosondes launched from Munich (65 km northeast), and locally launched ozonesondes. The “blind” evaluation was conducted under the framework of the Network for the Detection of Atmospheric Composition Change (NDACC) using 10 clear nights of measurements in 2018 and 2019. The campaign, referred to as the Hohenpeißenberg Ozone Profiling Study (HOPS), was conducted within the larger context of NDACC validation activities for European lidar stations. There was good agreement between all ozone lidar measurements in the range of 15 to 41 km with relative differences between co-located ozone profiles of less than ±10 %. Differences in the measured ozone number densities between the lidars and the locally launched ozone sondes were also generally less than 5 % below 30 km. The satellite ozone profiles demonstrated some differences with respect to the ground-based lidars which are due to sampling differences and geophysical variation. Both the original and new DWD lidars continue to meet the NDACC standard for lidar ozone profiles by exceeding 3 % accuracy between 16.5 and 43 km. Temperature differences for all instruments were less than ±5 K below 60 km, with larger differences present in the lidar–satellite comparisons above this region. Temperature differences between the DWD lidars met the NDACC accuracy requirements of ±1 K between 17 and 78 km. A unique cross-comparison between the HOPS campaign and a similar, recent campaign at Observatoire de Haute-Provence (Lidar Validation NDACC Experiment; LAVANDE) allowed for an investigation into potential biases in the NASA-STROZ reference lidar. The reference lidar may slightly underestimate ozone number densities above 43 km with respect to the French and German NDACC lidars. Below 20 km, the reference lidar temperatures profiles are 5 to 10 K cooler than the temperatures which are reported by the other instruments.

Effects of synoptic patterns on the vertical structure of ozone in Hong Kong using lidar measurement

Long-term ozone lidar routine measurements are sparse in China. In this study, we used one year of continuous ozone lidar measurements to systematically investigate the effects of synoptic patterns on the vertical structure of ozone during high ozone episodes in Hong Kong. The height of the near-surface ozone layer was identified and compared with that of the mixing layer. The results showed that Hong Kong was greatly affected by ozone transport from the Pearl River Delta region when a tropical cyclone (“C” pattern) or a trough (“T” pattern) existed. When a high-pressure center was located to the north (“H” pattern) or when both a high-pressure system and a tropical cyclone existed (“CH” pattern), Hong Kong was affected by ozone transport from southeastern or southern China. Substantial amounts of ozone were transported within a layer near the ground with an average height of 0.83, 0.75, 0.94, and 0.85 km under the C, H, CH, and T synoptic patterns, respectively. Variation in the near-surface ozone layer height was consistent with that of the mixing layer height. Weak vertical mixing resulted in a shallow near-surface ozone layer under the C and H synoptic patterns. Due to the combined effect of near-surface transport and suppressed vertical mixing, the ozone concentrations were extremely high near the ground but rapidly declined with height under the C synoptic pattern. Our investigations of the vertical structure of ozone contribute to filling the knowledge gap between synoptic patterns and the evolution of high surface ozone episodes.

The impact of Los Angeles Basin pollution and stratospheric intrusions on the surrounding San Gabriel Mountains as seen by surface measurements, lidar, and numerical models

Abstract. In this work, the impact of Los Angeles Basin pollution transport and stratospheric intrusions on the surface ozone levels observed in the San Gabriel Mountains is investigated based on a combination of surface and lidar measurements as well as WRF-Chem (Weather Research and Forecasting with Chemistry) and WACCM (Whole Atmosphere Community Climate Model) runs. The number of days with observed surface ozone levels exceeding the National Ambient Air Quality Standards exhibit a clear seasonal pattern, with a maximum during summer, when models suggest a minimum influence of stratospheric intrusions and the largest impact from Los Angeles Basin pollution transport. Additionally, measured and modeled surface ozone and PM10 were analyzed as a function of season, time of the day, and wind direction. Measurements and models are in good qualitative agreement, with maximum surface ozone observed for southwest and west winds. For the prevailing summer wind direction, slightly south of the ozone maximum and corresponding to south-southwest winds, lower ozone levels were observed. Back trajectories suggest that this is associated with transport from the central Los Angeles Basin, where titration limits the amount of surface ozone. A quantitative comparison of the lidar profiles with WRF-Chem and WACCM models revealed good agreement near the surface, with models showing an increasing positive bias as function of altitude, reaching 75 % at 15 km above sea level. Finally, three selected case studies covering the different mechanisms affecting the near-surface ozone concentration over the San Gabriel Mountains, namely stratospheric intrusions and pollution transport, are analyzed based on surface and ozone lidar measurements, as well as co-located ceilometer measurements and models.

Microwave and Lidar Measurements of Ozone and Temperature Variations During Stratospheric Warmings of 2012-2015

Microwave and Lidar Measurements of Ozone and Temperature Variations During Stratospheric Warmings of 2012-2015

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.

Very high stratospheric influence observed in the free troposphere over the northern Alps – just a local phenomenon?

Abstract. The atmospheric composition is strongly influenced by a change in atmospheric dynamics, which is potentially related to climate change. A prominent example is the doubling of the stratospheric ozone component at the Zugspitze summit station (2962 m a.s.l., Garmisch-Partenkirchen, Germany) between the mid-seventies and 2005, roughly from 11 to 23 ppb (43 %). Systematic efforts for identifying and quantifying this influence have been made since the late 1990s. Meanwhile, routine lidar measurements of ozone and water vapour carried out at Garmisch-Partenkirchen (German Alps) since 2007, combined with in situ and radiosonde data and trajectory calculations, have revealed that stratospheric intrusion layers are present on 84 % of the yearly measurement days. At Alpine summit stations the frequency of intrusions exhibits a seasonal cycle with a pronounced summer minimum that is reproduced by the lidar measurements. The summer minimum disappears if one looks at the free troposphere as a whole. The mid- and upper-tropospheric intrusion layers seem to be dominated by very long descent on up to hemispheric scale in an altitude range starting at about 4.5 km a.s.l. Without interfering air flows, these layers remain very dry, typically with RH ≤5 % at the centre of the intrusion. Pronounced ozone maxima observed above Garmisch-Partenkirchen have been mostly related to a stratospheric origin rather than to long-range transport from remote boundary layers. Our findings and results for other latitudes seem to support the idea of a rather high contribution of ozone import from the stratosphere to tropospheric ozone.

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.

Tropospheric NO<sub>2</sub>, SO<sub>2</sub>, and HCHO over the East China Sea, using ship-based MAX-DOAS observations and comparison with OMI and OMPS satellite data

Abstract. In this study, ship-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were performed in the East China Sea (ECS) area in June 2017. The tropospheric slant column densities (SCDs) of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) were retrieved from the measured spectra using the differential optical absorption spectroscopy (DOAS) technique. Using the simple geometric approach, the SCDs of different trace gases observed at a 15∘ elevation angle were adopted to convert into tropospheric vertical column densities (VCDs). During this campaign, the averaged VCDs of NO2, SO2, and HCHO in the marine environment over the ECS area are 6.50×1015, 4.28×1015, and 7.39×1015 molec cm−2, respectively. In addition, the ship-based MAX-DOAS trace gas VCDs were compared with satellite observations of the Ozone Monitoring Instrument (OMI) and Ozone Mapping and Profiler Suite (OMPS). The daily OMI NO2 VCDs agreed well with ship-based MAX-DOAS measurements showing the correlation coefficient R of 0.83. In addition, the good agreements of SO2 and HCHO VCDs between the OMPS satellite and ship-based MAX-DOAS observations were also found, with correlation coefficients R of 0.76 and 0.69. The vertical profiles of these trace gases are achieved from the measured differential slant column densities (DSCDs) at different elevation angles using the optimal estimation method. The retrieved profiles displayed the typical vertical distribution characteristics, which exhibit low concentrations of <3, <3, and <2 ppbv for NO2, SO2, and HCHO in a clean area of the marine boundary layer far from coast of the Yangtze River Delta (YRD) continental region. Interestingly, elevated SO2 concentrations can be observed intermittently along the ship routes, which is mainly attributed to the vicinal ship emissions in the view of the MAX-DOAS measurements. Combined with the on-board ozone lidar measurements, the ozone (O3) formation was discussed with the vertical profile of the HCHO∕NO2 ratio, which is sensitive to increases in NO2 concentration. This study provided further understanding of the main air pollutants in the marine boundary layer of the ECS area and also benefited the formulation of policies regulating the shipping emissions in such costal areas like the YRD region.

Airborne lidar measurements of aerosol and ozone above the Canadian oil sands region

Abstract. Aircraft-based lidar measurements of atmospheric aerosol and ozone were conducted to study air pollution from the oil sands extraction industry in northern Alberta. Significant amounts of aerosol were observed in the polluted air within the surface boundary layer, up to heights of 1 to 1.6 km above ground. The ozone mixing ratio measured in the polluted boundary layer air directly above the oil sands industry was equal to or less than the background ozone mixing ratio. On one of the flights, the lidar measurements detected a layer of forest fire smoke above the surface boundary layer in which the ozone mixing ratio was substantially greater than the background. Measurements of the linear depolarization ratio in the aerosol backscatter were obtained with a ground-based lidar and this aided in the discrimination between the separate emission sources from industry and forest fires. The retrieval of ozone abundance from the lidar measurements required the development of a method to account for the interference from the substantial aerosol content within the polluted boundary layer.

Characterizing the seasonal cycle and vertical structure of ozone in Paris, France using four years of ground based LIDAR measurements in the lowermost troposphere

Systematic ozone LIDAR measurements were completed during a 4 year period (2011–2014) in Paris, France to study the seasonal variability of the vertical structure of ozone in the urban boundary layer. In addition, we use in-situ measurements from the surface air quality network that is located in Paris (AIRPARIF). Specifically, we use ozone and NO2 measurements made at two urban stations: Paris13 (60 m ASL) and the Eiffel Tower (310 m ASL) to validate and interpret the LIDAR profiles. Remote sensed tropospheric NO2 integrated columns from the SAOZ instrument located in Paris are also used to interpret ozone measurements. Comparison between ozone LIDAR measurements averaged from 250 m to 500 m and the Eiffel Tower in-situ measurements shows that the accuracy of the LIDAR (originally ±14 μg·m−3) is significantly improved (±7 μg·m−3) when a small telescope with a wide angular aperture is used. Results for the seasonal cycle of the ozone vertical gradient are found to be similar using two methods: (1) measured differences between AIRPARIF stations with measurements at 60 m ASL and 310 m ASL and (2) using LIDAR profiles from 300 m to the top of the Planetary Boundary Layer (PBL). Ozone concentrations measured by the LIDAR increase with altitude within the PBL, with a steeper gradient in winter (60 μg·m−3·km−1) and a less strong gradient in summer (20 μg·m−3·km−1). Results show that in winter, there is a sharp positive gradient of ozone at the surface, which is explained by ozone titration by NO combined with increased atmospheric stability in winter. In the afternoon during summer, photochemistry and vertical mixing are large enough to compensate for ozone titration near the surface, where NOx is emitted, and there is no gradient in ozone observed. In contrast, in the summer during the morning, ozone has a sharper positive vertical gradient similar to the winter values. Comparison of the vertically averaged ozone concentrations up to (0–3 km) and urban layer (0–310 m) ozone concentrations shows that the ratio between these two quantities is the largest in summer (86%) and the lowest in winter (49%). We conclude that satellite measurements that represent the 0–3 km integrated ozone column are not necessarily a good proxy for surface ozone and may lead to incorrect conclusions about the surface ozone seasonal variability. The ratio between the urban layer NO2 average concentration and the boundary layer NO2 average concentration obtained from SAOZ NO2 tropospheric columns is always less than 50%, meaning NO2 does not decrease linearly in the PBL, but with a sharper decrease close to the surface.

Lidar Measurements of Tropospheric Ozone in the Arctic

This paper reports on differential absorption lidar (DIAL) measurements of tropospheric ozone in the Canadian Arctic during springtime. Measurements at Eureka Weather Station revealed that mountains have a significant effect on the vertical structure of ozone above Ellesmere Island. Ozone depletion events were observed when air that had spent significant time near to the frozen surface of the Arctic Ocean reached Eureka. This air arrived at Eureka by flowing over the surrounding mountains. Surface level ozone depletions were not observed during periods when the flow of air from over the sea ice was blocked by mountains. In the case of blocking there was an enhancement in the amount of ozone near the surface as air from the mid troposphere descended in the lee of the mountains. Three case studies will be shown in the presentation, while one is described in this paper.

Lidar Measurements of Ozone in the Upper Troposphere – Lower Stratosphere at Siberian Lidar Station in Tomsk

The paper presents the results of DIAL measurements of the vertical ozone distribution at the Siberian lidar station. Sensing is performed according to the method of differential absorption and scattering at wavelength pair of 299/341 nm, which are, respectively, the first and second Stokes components of SRS conversion of 4th harmonic of Nd:YAG laser (266 nm) in hydrogen. Lidar with receiving mirror 0.5 m in diameter is used to implement sensing of vertical ozone distribution in altitude range of 6-16 km. The temperature correction of zone absorption coefficients is introduced in the software to reduce the retrieval errors.

Combined Dial Sounding of Ozone, Water Vapour and Aerosol

Routine high-quality lidar measurements of ozone, water vapour and aerosol at Garmisch-Partenkirchen since 2007 have made possible more comprehensive atmospheric studies and lead to a growing insight concerning the most frequently occurring long-range transport pathways. In this contribution we present as examples results on stratospheric layers travelling in the free troposphere for extended periods of time without eroding. In particular, we present a case of an intrusion layer that subsided over as many as fifteen days and survived the interference by strong Canadian fires. These results impose a challenge on atmospheric modelling that grossly overestimates free-tropospheric mixing.

Airborne Lidar Measurements of Pollution above the Oil Sands Region in Northern Alberta

Lidar measurements of ozone and aerosol were conducted from a Twin Otter aircraft above the oil sands region of northern Alberta. For the majority of the flights, significant amounts of aerosol were observed within the boundary layer, up to an altitude of 2.0 km above sea level (ASL), while the ozone concentration remained at background levels (30-45 ppb) downwind of the industry. On August 24 th the lidar measured a separated layer of aerosol above the boundary layer, at a height of 2.0 km ASL, in which the ozone mixing ratio increased to 70 ppb. Backward trajectory calculations revealed that the air containing this separated aerosol layer had passed over an area of forest fires. Directly below the layer of forest fire smoke, pollution from the oil sands industry was observed. Measurements of the backscatter linear depolarization ratio were obtained with a ground based lidar operated by Environment Canada within the oil sands region. The depolarization measurements aided in discriminating between the separate sources of pollution from industry and forest fires. The depolarization ratio was 5-6% in forest fire smoke and 7-10% in the industrial pollution.

Stratospheric ozone in boreal fire plumes – the 2013 smoke season over central Europe

Abstract. In July 2013 very strong boreal fire plumes were observed at the northern rim of the Alps by lidar and ceilometer measurements of aerosol, ozone and water vapour for about 3 weeks. In addition, some of the lower-tropospheric components of these layers were analysed at the Global Atmosphere Watch laboratory at the Schneefernerhaus high-altitude research station (2650 m a.s.l., located a few hundred metres south-west of the Zugspitze summit). The high amount of particles confirms our hypothesis that fires in the Arctic regions of North America lead to much stronger signatures in the central European atmosphere than the multitude of fires in the USA. This has been ascribed to the prevailing anticyclonic advection pattern during favourable periods and subsidence, in contrast to warm-conveyor-belt export, rainout and dilution frequently found for lower latitudes. A high number of the pronounced aerosol structures were positively correlated with elevated ozone. Chemical ozone formation in boreal fire plumes is known to be rather limited. Indeed, these air masses could be attributed to stratospheric air intrusions descending from remote high-latitude regions, obviously picking up the aerosol on their way across Canada. In one case, subsidence from the stratosphere over Siberia over as many as 15–20 days without increase in humidity was observed although a significant amount of Canadian smoke was trapped. These coherent air streams lead to rather straight and rapid transport of the particles to Europe.

An overview of the 2013 Las Vegas Ozone Study (LVOS): Impact of stratospheric intrusions and long-range transport on surface air quality

The 2013 Las Vegas Ozone Study (LVOS) was conducted in the late spring and early summer of 2013 to assess the seasonal contribution of stratosphere-to-troposphere transport (STT) and long-range transport to surface ozone in Clark County, Nevada and determine if these processes directly contribute to exceedances of the National Ambient Air Quality Standard (NAAQS) in this area. Secondary goals included the characterization of local ozone production, regional transport from the Los Angeles Basin, and impacts from wildfires. The LVOS measurement campaign took place at a former U.S. Air Force radar station ∼45 km northwest of Las Vegas on Angel Peak (∼2.7 km above mean sea level, asl) in the Spring Mountains. The study consisted of two extended periods (May 19–June 4 and June 22–28, 2013) with near daily 5-min averaged lidar measurements of ozone and backscatter profiles from the surface to ∼2.5 km above ground level (∼5.2 km asl), and continuous in situ measurements (May 20–June 28) of O3, CO, (1-min) and meteorological parameters (5-min) at the surface. These activities were guided by forecasts and analyses from the FLEXPART (FLEXible PARTticle) dispersion model and the Real Time Air Quality Modeling System (RAQMS), and the NOAA Geophysical Research Laboratory (NOAA GFDL) AM3 chemistry-climate model. In this paper, we describe the LVOS measurements and present an overview of the results. The combined measurements and model analyses show that STT directly contributed to each of the three O3 exceedances that occurred in Clark County during LVOS, with contributions to 8-h surface concentrations in excess of 30 ppbv on each of these days. The analyses show that long-range transport from Asia made smaller contributions (<10 ppbv) to surface O3 during two of those exceedances. The contribution of regional wildfires to surface O3 during the three LVOS exceedance events was found to be negligible, but wildfires were found to be a major factor during exceedance events that occurred before and after the LVOS campaign. Our analyses also shows that ozone exceedances would have occurred on more than 50% of the days during the six-week LVOS campaign if the 8-h ozone NAAQS had been 65 ppbv instead of 75 ppbv.

First results of an integrated experiment on sounding the middle atmosphere in optical and millimeter wavelength ranges (over Tomsk)

Results of joint ground-based microwave and lidar measurements of ozone and temperature vertical profiles are presented. The importance of such observations for the study of the influence of different disturbances on the ozone layer is discussed. The results are compared with the MLS/AURA satellite data and model profiles.

The unusual persistence of an ozone hole over a southern mid-latitude station during the Antarctic spring 2009: a multi-instrument study

Abstract. Record-low ozone column densities (with a minimum of 212 DU) persisted over three weeks at the Río Gallegos NDACC (Network for the Detection of Atmospheric Composition Change) station (51.5° S, 69.3° W) in November 2009. Total ozone remained two standard deviations below the climatological mean for five consecutive days during this period. The statistical analysis of 30 years of satellite data from the Multi Sensor Reanalysis (MSR) database for Río Gallegos revealed that such a long-lasting low-ozone episode is a rare occurrence. The event is examined using height-resolved ozone lidar measurements at Río Gallegos, and observations from satellite and ground-based instruments. The computed relative difference between the measured total ozone and the climatological monthly mean shows reductions varying between 10 and 30% with an average decrease of 25%. The mean absolute difference of total ozone column with respect to climatological monthly mean ozone column is around 75 DU. Extreme values of the UV index (UVI) were measured at the ground for this period, with the daily maximum UVI of around 13 on 15 and 28 November. The high-resolution MIMOSA-CHIM (Modélisation Isentrope du transport Méso-échelle de l'Ozone Stratosphérique par Advection) model was used to interpret the ozone depletion event. An ozone decrease of about 2 ppmv was observed in mid-November at the 550 K isentropic level (~22 km). The position of Río Gallegos relative to the polar vortex was classified using equivalent latitude maps. During the second week of November, the vortex was over the station at all isentropic levels, but after 20 November and until the end of the month, only the 10 lower levels in the stratosphere were affected by vortex overpasses with ozone poor air masses. A rapid recovery of the ozone column density was observed later, due to an ozone rich filament moving over Río Gallegos between 18 and 24 km in the first two weeks of December 2009.