Vertical Profiles Of NO2 Research Articles

Impacts of transportation emissions on horizontal and vertical distributions of air pollutants in Shanghai: Insights from emission reduction in COVID-19 lockdown

Transportation is a major sector of anthropogenic emissions in urban areas and deteriorates air quality. The surface and vertical observational data were combined with the model results to reveal its impact on the horizontal and vertical variations of pollutants during the COVID-19 lockdown period. The evident reductions in ambient PM2.5 (∼30%) and NO2 (∼50%) concentrations but a ∼25% increase in O3 concentration were observed at the transportation sites. On the vertical scale, a uniform decrease of ∼28% in PM2.5 concentrations was observed within 600 m. However, the vertical profiles of NO2 and O3 exhibited increasing vertical variation rates with concentrations varying significantly within 400 m. Meanwhile, Ox shared a similar pattern of vertical profile with O3, with a uniform increase (∼5%) within 600 m in the urban area. The WRF-CMAQ model reproduced the variations, and revealed that the reduction of transportation emissions was the key factor contributing to the increase of urban O3 and Ox due to the weakened NO titration effect. The simulated vertical profile of NO2 was featured by a decreasing curve, while that of O3 exhibited the opposite trend. We find that the transportation emissions impact vertical concentrations of NO2 and O3 within at most 400 m. The process analysis revealed that the vertical transport and horizontal transport from bay areas contributed to O3 in the urban area, while chemical processes mainly consumed it. The reduction in transportation emissions weakened the consumption and resulted in O3 accumulation during rush hours and at night. The variation of planetary boundary layer height also favored the rise of urban O3 by promoting vertical transport at daytime and trapping it at night. The reduction in NOx emissions from the transportation enhanced O3 pollution, suggesting that collaborative reductions in VOCs from multiple sectors should be conducted. This study also indicated that regional collaborations in emission reductions were necessary for comprehensive air pollution prevention.

Observations of HONO and its precursors between urban and its surrounding agricultural fields: The vertical transports, sources and contribution to OH

The insufficient study on vertical observations of main atmospheric reactive nitrogen oxides (NO2 and HONO) posed a great challenge to evaluate their intertransport between urban and agricultural areas, and to further learn the atmospheric nitrogen chemistry and the atmospheric oxidation capacity at high altitudes. A stereoscopic measurement campaign (satellite remote sensing, hyperspectral unmanned aerial vehicle (UAV) remote sensing and MAX-DOAS observation) was performed in a typical inland city Hefei and its surrounding agricultural fields from June to October 2022. Average aerosol vertical profiles exhibited a Gaussian shape above 100 m with maximum values of 0.67 km−1 and 0.55 km−1 at 300–400 m layer at Anhui University (AHU) and Changfeng (CF), respectively. The distinct layered structure was mainly attributed to regional transport. Average H2O and NO2 vertical profiles all showed a Gaussian shape and an exponential shape at AHU and CF, respectively. Moreover, the diurnal evolution of H2O profiles performed one peak and bi-peak patterns at AHU and CF, respectively, whereas the diurnal evolution of NO2 at two stations all exhibited bi-peak patterns attributed to vehicle emissions. Average HONO vertical profiles showed an exponential shape and a Gaussian shape at AHU and CF, respectively. Higher HONO (> 0.05 ppb) above 1.0 km at 14:00–16:00 was observed at CF. The transport flux analysis showed that the northern transport flux always larger than southern transport flux for aerosol and H2O. The maximum northern transport fluxes appeared at 300 m and surface for aerosol and H2O, respectively. It indicated that surrounding agricultural fields was an important source of atmospheric H2O of city. The southern transport flux was larger than northern transport flux for NO2, with a maximum net transport flux of 9.20 ppb m s−1 at 100 m. It demonstrated that NO2 transported from urban areas was an important source of NO2 in agricultural fields. For HONO, the southern transport flux was larger than northern transport flux under 100 m, whereas it was opposite above 100 m. It indicated that the HONO distributed at high altitudes at agricultural fields had potential to enhance the atmospheric oxidation capacity of urban area. The net horizontal transport fluxes of HONO of our defined cropland were 5.25 μg m−2 s−1 and -3.65 μg m−2 s−1 during non-fertilization and fertilization periods, respectively. It indicated that the cropland could obviously export HONO to surrounding atmosphere during the fertilization period. Deducing the contribution of direct emission, heterogeneous process was a major source of HONO at urban and agricultural areas. The average surface conversion rate of NO2-to-HONO (CHONO) was 0.01467 h−1, and this value decreased with the increase of height at urban station. While average surface CHONO was 0.0322 h−1 at agricultural fields, which was ~1.2–2.8 times higher than that at urban area. The CHONO at agricultural fields significantly increased with the increase of height. The average CHONO at 1.0 km was ~2.0–3.6 times higher than that at surface. That suggested that the heterogeneous process was the main HONO source at high altitudes at CF, and this process obviously correlated with aerosol and H2O. The higher OH production from HONO (P(OH)HONO) occurred at 0–200 m and 100–400 m with averaged values of 0.31 ppb h−1 and 0.39 ppb h−1 at AHU and CF, respectively. The high P(OH)HONO above 1.0 km at CF from September to October was strongly correlated with high O3 (> 80 ppb). This study emphasized the importance of the stereoscopic of HONO on the analysis of its distribution, evolution, source and atmospheric oxidizing contribution.

MAX-DOAS Measurements of Tropospheric NO2 and HCHO Vertical Profiles at the Longfengshan Regional Background Station in Northeastern China

The vertical profiles of nitrogen dioxide (NO2) and formaldehyde (HCHO) in the troposphere at the Longfengshan (LFS) regional atmospheric background station (127°36' E, 44°44' N, 330.5 m above sea level) from 24 October 2020 to 13 October 2021 were retrieved from solar scattering spectra by multi-axis differential optical absorption spectroscopy (MAX-DOAS). We analyzed the temporal variations of NO2 and HCHO as well as the sensitivity of ozone (O3) production to the concentration ratio of HCHO to NO2. The largest NO2 volume mixing ratios (VMRs) occur in the near-surface layer for each month, with high values concentrated in the morning and evening. HCHO has an elevated layer around the altitude of 1.4 km consistently. The means ± standard deviations of vertical column densities (VCDs) and near-surface VMRs were 4.69 ± 3.72 ×1015 molecule·cm-2 and 1.22 ± 1.09 ppb for NO2, and they were 1.19 ± 8.35 × 1016 molecule·cm-2 and 2.41 ± 3.26 ppb for HCHO. The VCDs and near-surface VMRs for NO2 were high in the cold months and low in the warm months, while HCHO presented the opposite. The larger near-surface NO2 VMRs appeared in the condition associated with lower temperature and higher humidity, but this relationship was not found between HCHO and temperature. We also found the O3 production at the Longfengshan station was mainly in the NOx-limited regime. This is the first study presenting the vertical distributions of NO2 and HCHO in the regional background atmosphere of northeastern China, which are significant to enhancing the understanding of background atmospheric chemistry and regional ozone pollution processes.

Validation of Sentinel-5P TROPOMI tropospheric NO2 products by comparison with NO2 measurements from airborne imaging DOAS, ground-based stationary DOAS, and mobile car DOAS measurements during the S5P-VAL-DE-Ruhr campaign

Abstract. Airborne imaging differential optical absorption spectroscopy (DOAS), ground-based stationary DOAS, and car DOAS measurements were conducted during the S5P-VAL-DE-Ruhr campaign in September 2020. The campaign area is located in the Rhine-Ruhr region of North Rhine-Westphalia, western Germany, which is a pollution hotspot in Europe comprising urban and large industrial sources. The DOAS measurements are used to validate spaceborne NO2 tropospheric vertical column density (VCD) data products from the Sentinel-5 Precursor (S5P) TROPOspheric Monitoring Instrument (TROPOMI). Seven flights were performed with the airborne imaging DOAS instrument for measurements of atmospheric pollution (AirMAP), providing measurements that were used to create continuous maps of NO2 in the layer below the aircraft. These flights cover many S5P ground pixels within an area of 30 km × 35 km and were accompanied by ground-based stationary measurements and three mobile car DOAS instruments. Stationary measurements were conducted by two Pandora, two Zenith-DOAS, and two MAX-DOAS instruments. Ground-based stationary and car DOAS measurements are used to evaluate the AirMAP tropospheric NO2 VCDs and show high Pearson correlation coefficients of 0.88 and 0.89 and slopes of 0.90 ± 0.09 and 0.89 ± 0.02 for the stationary and car DOAS, respectively. Having a spatial resolution of about 100 m × 30 m, the AirMAP tropospheric NO2 VCD data create a link between the ground-based and the TROPOMI measurements with a nadir resolution of 3.5 km × 5.5 km and are therefore well suited to validate the TROPOMI tropospheric NO2 VCD. The observations on the 7 flight days show strong NO2 variability, which is dependent on the three target areas, the day of the week, and the meteorological conditions. The AirMAP campaign data set is compared to the TROPOMI NO2 operational offline (OFFL) V01.03.02 data product, the reprocessed NO2 data using the V02.03.01 of the official level-2 processor provided by the Product Algorithm Laboratory (PAL), and several scientific TROPOMI NO2 data products. The AirMAP and TROPOMI OFFL V01.03.02 data are highly correlated (r=0.87) but show an underestimation of the TROPOMI data with a slope of 0.38 ± 0.02 and a median relative difference of −9 %. With the modifications in the NO2 retrieval implemented in the PAL V02.03.01 product, the slope and median relative difference increased to 0.83 ± 0.06 and +20 %. However, the modifications resulted in larger scatter and the correlation decreased significantly to r=0.72. The results can be improved by not applying a cloud correction for the TROPOMI data in conditions with high aerosol load and when cloud pressures are retrieved close to the surface. The influence of spatially more highly resolved a priori NO2 vertical profiles and surface reflectivity are investigated using scientific TROPOMI tropospheric NO2 VCD data products. The comparison of the AirMAP campaign data set to the scientific data products shows that the choice of surface reflectivity database has a minor impact on the tropospheric NO2 VCD retrieval in the campaign region and season. In comparison, the replacement of the a priori NO2 profile in combination with the improvements in the retrieval of the PAL V02.03.01 product regarding cloud heights can further increase the tropospheric NO2 VCDs. This study demonstrates that the underestimation of the TROPOMI tropospheric NO2 VCD product with respect to the validation data set has been and can be further significantly improved.

Tropospheric NO2 vertical profiles over South Korea and their relation to oxidant chemistry: implications for geostationary satellite retrievals and the observation of NO2 diurnal variation from space

Abstract. Nitrogen oxides (NOx≡ NO + NO2) are of central importance for air quality, climate forcing, and nitrogen deposition to ecosystems. The Geostationary Environment Monitoring Spectrometer (GEMS) is now providing hourly NO2 satellite observations over East Asia, offering the first direct measurements of NO2 diurnal variation from space to guide understanding of NOx emissions and chemistry. The NO2 retrieval requires independent vertical profile information from a chemical transport model (CTM) to compute the air mass factor (AMF) that relates the NO2 column measured along the line of sight to the NO2 vertical column. Here, we use aircraft observations from the Korea-United States Air Quality (KORUS-AQ) campaign over the Seoul metropolitan area (SMA) and around the Korean Peninsula in May–June 2016 to better understand the factors controlling the NO2 vertical profile, its diurnal variation, the implications for the AMFs, and the ability of the GEOS-Chem CTM to compute the NO2 vertical profiles used for AMFs. Proper representation of oxidant chemistry is critical for the CTM simulation of NO2 vertical profiles and is achieved in GEOS-Chem through new model developments, including aerosol nitrate photolysis, reduced uptake of hydroperoxy (HO2) radicals by aerosols, and accounting for atmospheric oxidation of volatile chemical products (VCPs). We find that the tropospheric NO2 columns measured from space in the SMA are mainly contributed by the planetary boundary layer (PBL) below 2 km altitude, reflecting the highly polluted conditions. Repeated measurements of NO2 vertical profiles over the SMA at different times of day show that diurnal change in mixing depth affecting the NO2 vertical profile induces a diurnal variation in AMFs of comparable magnitude to the diurnal variation in the NO2 column. GEOS-Chem captures this diurnal variation in AMFs and more generally the variability in the AMFs for the KORUS-AQ NO2 vertical profiles (2.7 % mean bias, 7.6 % precision), with some outliers in the morning due to errors in the timing of mixed-layer growth.

Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements

Abstract. Satellite-based retrievals of tropospheric NO2 columns are widely used to infer NOx (≡ NO + NO2) emissions. These retrievals rely on model information for the vertical distribution of NO2. The free tropospheric background above 2 km is particularly important because the sensitivity of the retrievals increases with altitude. Free tropospheric NOx also has a strong effect on tropospheric OH and ozone concentrations. Here we use observations from three aircraft campaigns (SEAC4RS, DC3, and ATom) and four atmospheric chemistry models (GEOS-Chem, GMI, TM5, and CAMS) to evaluate the model capabilities for simulating NOx in the free troposphere and attribute it to sources. NO2 measurements during the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convective Clouds and Chemistry (DC3) campaigns over the southeastern U.S. in summer show increasing concentrations in the upper troposphere above 10 km, which are not replicated by the GEOS-Chem, although the model is consistent with the NO measurements. Using concurrent NO, NO2, and ozone observations from a DC3 flight in a thunderstorm outflow, we show that the NO2 measurements in the upper troposphere are biased high, plausibly due to interference from thermally labile NO2 reservoirs such as peroxynitric acid (HNO4) and methyl peroxy nitrate (MPN). We find that NO2 concentrations calculated from the NO measurements and NO–NO2 photochemical steady state (PSS) are more reliable to evaluate the vertical profiles of NO2 in models. GEOS-Chem reproduces the shape of the PSS-inferred NO2 profiles throughout the troposphere for SEAC4RS and DC3 but overestimates NO2 concentrations by about a factor of 2. The model underestimates MPN and alkyl nitrate concentrations, suggesting missing organic NOx chemistry. On the other hand, the standard GEOS-Chem model underestimates NO observations from the Atmospheric Tomography Mission (ATom) campaigns over the Pacific and Atlantic oceans, indicating a missing NOx source over the oceans. We find that we can account for this missing source by including in the model the photolysis of particulate nitrate on sea salt aerosols at rates inferred from laboratory studies and field observations of nitrous acid (HONO) over the Atlantic. The median PSS-inferred tropospheric NO2 column density for the ATom campaign is 1.7 ± 0.44 × 1014 molec. cm−2, and the NO2 column density simulated by the four models is in the range of 1.4–2.4 × 1014 molec. cm−2, implying that the uncertainty from using modeled NO2 tropospheric columns over clean areas in the retrievals for stratosphere–troposphere separation is about 1 × 1014 molec. cm−2. We find from GEOS-Chem that lightning is the main primary NOx source in the free troposphere over the tropics and southern midlatitudes, but aircraft emissions dominate at northern midlatitudes in winter and in summer over the oceans. Particulate nitrate photolysis increases ozone concentrations by up to 5 ppbv (parts per billion by volume) in the free troposphere in the northern extratropics in the model, which would largely correct the low model bias relative to ozonesonde observations. Global tropospheric OH concentrations increase by 19 %. The contribution of the free tropospheric background to the tropospheric NO2 columns observed by satellites over the contiguous U.S. increases from 25 ± 11 % in winter to 65 ± 9 % in summer, according to the GEOS-Chem vertical profiles. This needs to be accounted for when deriving NOx emissions from satellite NO2 column measurements.

Diagnosis of Ozone Formation Sensitivities in Different Height Layers via MAX‐DOAS Observations in Guangzhou

AbstractDiagnosing the vertical distributions of ozone formation sensitivities within the boundary layers is the prerequisite for formulating proper ozone control strategies. From 1 January 2020, to 20 August 2021, a multi‐function MAX‐DOAS instrument was set up in Guangzhou to detect the NO2 and HCHO vertical profiles. The ozone formation sensitivities in different height layers were diagnosed using the FNRsec, which was defined as the ratio of secondary HCHO to NO2 VMRs (HCHOsec/NO2). The secondary sources in ambient HCHO participate in the photochemical reactions directly, and the FNRsec can indicate the ozone formation sensitivities more accurately. Therefore, the secondary source was separated from ambient HCHO via a multi‐linear regression method, and its relative contribution was approximately 66.9 ± 6.3%. The sensitivity thresholds of ozone formation were determined by the slope of the linear regression analysis for O3 versus the normalized secondary HCHO or NO2 mixing ratios for different FNRsec ranges, which were 0.22 and 0.36. For the ground layer, the VOC‐limited, transitional, and NOx‐limited regimes accounted for 40.66%, 32.42%, and 26.92%, respectively. Diurnally, the ground layer was usually in the VOC‐limited regime in morning, but in the transitional regime in noon and afternoon. Vertically, the ozone formation sensitivity changed with altitude from VOC‐limited (0.02–0.22 km) to transitional (0.22–0.42 km) to NOx‐limited (0.42–2.02 km). These findings can help formulate proper ozone control strategies in time according to the varying local conditions.

Three decades of remote sensing of NO2 vertical distribution and column content at the A. M. Obukhov Institute of Atmospheric Physics

The paper reviews the results of 30-year spectrometric measurements of vertical distribution and column content of NO2 at the Zvenigorod Scientific Station (ZSS) of the A. M. Obukhov Institute of Atmospheric Physics and presents analysis of NO2 long-term trends and interannual variations. The station is located in the western Moscow region. It is part of the Network for the Detection of Atmospheric Composition Change (NDACC). Measurements are done in the morning and evening twilight by zenith-scattered visible solar radiation. Vertical NO2 profiles are retrieved and column NO2 contents are calculated by profile integration. Long term trends and inter-annual variations of NO2 are analysed by multivariate regression method taking into account autocorrelation of data in a wide range of time scales. Seasonally dependent estimates of NO2 trends and interannual variations due to the quasi-biennial oscillation, El Nino–Southern oscillation, North Atlantic Oscillation, and the 11-year solar cycle are obtained. Most pronounced (in per cent units) trends and circulation and solar cycle effects are peculiar to the winter–spring period of the year. Mutual influence is assessed between the estimates of the trend and the solar cycle effect in stratospheric NO2.

Temporal Variation of NO2 and HCHO Vertical Profiles Derived from MAX-DOAS Observation in Summer at a Rural Site of the North China Plain and Ozone Production in Relation to HCHO/NO2 Ratio

We performed a comprehensive and intensive field experiment including ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurement at Raoyang (115°44′ E, 38°14′ N; 20 m altitude) in summer (13 June–20 August) 2014. The NO2 and HCHO profiles retrieved by MAX-DOAS take on different vertical distribution shapes, with the former declining with the increasing altitude and the latter having an elevated layer. The average levels of vertical column densities (VCDs) and near-surface volume mixing ratios (VMRs) were 1.02 ± 0.51 × 1016 molec·cm−2 and 3.23 ± 2.70 ppb for NO2 and 2.32 ± 0.56 × 1016 molec·cm−2 and 5.62 ± 2.11 ppb for HCHO, respectively. The NO2 and HCHO levels are closely connected with meteorological conditions, with the larger NO2 VCDs being associated with lower temperature, higher relative humidity (RH) and lower planetary boundary layer height (PBLH). With respect to the diurnal variations of vertical distribution, the NO2 in the residual layer gradually disappeared from 1.2 km height to the surface during the period of 7:00–11:00 Beijing time (BJ), and the near-surface NO2 had larger VMRs in the early morning and evening than in the later morning and afternoon. An elevated HCHO layer was observed to occur persistently with the lifted layer height rising from ~0.5 km to ~1.0 km before 10:00 BJ; the near-surface HCHO VMRs gradually increased and peaked around 10:00 BJ. The ratios of HCHO to NO2 (RHCHO-NO2) were generally larger than two in the boundary layer from 11:00 BJ until 19:00 BJ, the time period when ozone photochemistry was most active. Thus, ozone (O3) production was mainly in the NOx-limited regime during the observation campaign, which was closely related to relatively high temperatures and low RH. The O3 production regimes also changed with the wind’s direction. These results are significant to reveal the formation mechanism of O3 pollution and develop strategies for controlling the O3 photochemical pollution over the North China Plain.

Variations of Urban NO2 Pollution during the COVID-19 Outbreak and Post-Epidemic Era in China: A Synthesis of Remote Sensing and In Situ Measurements

Since the COVID-19 outbreak in 2020, China’s air pollution has been significantly affected by control measures on industrial production and human activities. In this study, we analyzed the temporal variations of NO2 concentrations during the COVID-19 lockdown and post-epidemic era in 11 Chinese megacities by using satellite and ground-based remote sensing as well as in situ measurements. The average satellite tropospheric vertical column density (TVCD) of NO2 by TROPOMI decreased by 39.2–71.93% during the 15 days after Chinese New Year when the lockdown was at its most rigorous compared to that of 2019, while the in situ NO2 concentration measured by China National Environmental Monitoring Centre (CNEMC) decreased by 42.53–69.81% for these cities. Such differences between both measurements were further investigated by using ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) remote sensing of NO2 vertical profiles. For instance, in Beijing, MAX-DOAS NO2 showed a decrease of 14.19% (versus 18.63% by in situ) at the ground surface, and 36.24% (versus 36.25% by satellite) for the total tropospheric column. Thus, vertical discrepancies of atmospheric NO2 can largely explain the differences between satellite and in situ NO2 variations. In the post-epidemic era of 2021, satellite NO2 TVCD and in situ NO2 concentrations decreased by 10.42–64.96% and 1.05–34.99% compared to 2019, respectively, possibly related to the reduction of the transportation industry. This study reveals the changes of China’s urban NO2 pollution in the post-epidemic era and indicates that COVID-19 had a profound impact on human social activities and industrial production.

Research of NO2 vertical profiles with look-up table method based on MAX-DOAS

Obtaining the vertical distribution profile of trace gas is of great significance for studying the diffusion procedure of air pollution. In this article, a look-up table method based on multi-axis differential optical absorption spectroscopy (MAXDOAS) technology is established for retrieving the tropospheric NO2 vertical distribution profiles. This method retrieves the aerosol extinction profiles with minimum cost function. Then, the aerosol extinction profiles and the atmospheric radiation transfer model (RTM) are employed to establish the look-up table for retrieving the NO2 vertical column densities (VCDs) and profiles. The measured NO2 differential slant column densities (DSCDs) are compared with the NO2 DSCDs simulated by the atmospheric RTM, and the NO2 VCDs, the weight factor of NO2 in the boundary layer, and the boundary layer height are obtained by the minimization process. The look-up table is established to retrieve NO2 VCDs based on MAX-DOAS measurements in Huaibei area, and the results are compared with the data from Copernicus Atmospheric Monitoring Service(CAMS) model. It isfound that there are nearly consistent and the correlation coefficient R2 is morethan 0.86. The results show that this technology provides a more convenient and accurate retrieval method for the stereoscopic monitoring ofatmospheric environment.

Evaluation and Evolution of MAX-DOAS-observed Vertical NO2 Profiles in Urban Beijing

Multiaxis differential absorption spectroscopy (MAX-DOAS) is a newly developed advanced vertical profile detection method, but the vertical nitrogen dioxide (NO2) profiles measured by MAX-DOAS have not yet been fully verified. In this study, we perform MAX-DOAS and tower gradient observations to simultaneously acquire tropospheric NO2 observations in the Beijing urban area from 1 April to 31 May 2019. The average values of the tropospheric NO2 vertical column densities measured by MAX-DOAS and the tropospheric monitoring instrument are 15.8 × 1015 and 12.4 × 1015 molecules cm−2, respectively, and the correlation coefficient R reaches 0.87. The MAX-DOAS measurements are highly consistent with the tower-based in situ measurements, and the correlation coefficients R from the ground to the upper air are 0.89 (60 m), 0.87 (160 m), and 0.76 (280 m). MAX-DOAS accurately measures the trend of NO2 vertical profile changes, although a large underestimation occurs by a factor of two. By analyzing the NO2 vertical profile, the NO2 concentration reveals an exponential decrease with height. The NO2 vertical profile also coincides with the evolution of the boundary layer height. The study shows that the NO2 over Beijing mainly originates from local sources and occurs in the boundary layer, and its vertical evolution pattern has an important guiding significance to better understand nitrate production and ozone pollution.

Prediction of Vertical Profile of NO₂ Using Deep Multimodal Fusion Network Based on the Ground-Based 3-D Remote Sensing

The vertical distribution profiles of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> are essential for understanding the mechanisms, detecting near-surface emissions, and tracking pollutant transportation at high altitude. However, most of the published NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> studies are based on the surface 2-D measurements. The ground-based 3-D remote-sensing stations were recently built to measure vertical distribution profiles of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> . However, the stations were spatially sparse due to the high cost and could not make the measurements without sunlight. In this study, we first developed a multimodel fusion network (MF-net) based on the sparse vertical observations from the Jing-Jin-Ji region. We achieved the 3-D profile prediction of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> in the range of 39.005–41.405N and 115.005–117.905E with 24-h coverage. The MF-net significantly surpassed the conventional WRF-CHEM model and provided a more accurate evaluation of the NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> transmission between Beijing and the neighboring cities. Besides, the MF-net covers the monitoring of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> to the whole study area and extends the monitoring time to the entire day (24 h), making it serviceable for continuous spatial-temporal estimation of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> and its transmission in pollution events. The MF-net provides more robust data support to formulate reasonable and effective pollution prevention and control measures.

Vertically increased NO3 radical in the nocturnal boundary layer

In the nocturnal boundary layer, nitrate radical (NO3) has an important contribution to atmospheric chemistry through oxidation of nitrogen oxides and hydrocarbons. Vertical distributions of NO2, O3 and NO3 were measured by four differential optical absorption spectroscopy instruments at meteorological tower in Beijing from June 1 to July 22, 2019. The results show the mean diurnal variations of NO2, O3, and NO3 display a single peak (up to 65.0 ppbv, 196.8 ppbv and 317.5 pptv, respectively) in time. O3 and NO3 mixing ratios generally increased against heights, which is opposite to NO2, suggesting the contribution of O3 to NO3 production at higher altitude. According to the correlation coefficients between NO3 production rates (PNO3) and NO2 or O3 levels, PNO3 was sensitive to NO2 mixing ratio at higher altitude but to O3 near the ground. Averaged NO3 lifetimes (τNO3) of lowest, middle, upper and highest layer intervals were 104, 118, 164 and 213 s, respectively, which indicates τNO3 increase against height and explains why NO3 mixing ratios are larger at higher altitude to some extent. Main control factors of NO3 removal changed from gas-phase reactions to N2O5 hydrolysis with height increase. When relative humidity (RH) exceeded 70% or PM2.5 level exceeded 50 μg·m−3, τNO3 was almost less than 300 s with mixing ratio lower than 70 pptv. The clear negative dependence of τNO3 on RH and PM2.5 reveals the influencing factors on indirect loss. Under polluted conditions, vertical profiles of NO2, O3 and NO3 varied drastically. Stable atmosphere (low nocturnal boundary layer height and thermal inversion), RH level and RH gradient are the main reason for the evident difference in NO3 gradient. Vertically increased NO3 radicals may imply the formation of nitrate aerosols and further increase the nitrate content in high- altitude particulate matter.

Vertical distributions of tropospheric formaldehyde, nitrogen dioxide, ozone and aerosol in southern China by ground-based MAX-DOAS and LIDAR measurements during PRIDE-GBA 2018 campaign

As the development of megacities, combined air pollution has been of increasing concern in China, which is composed by primary pollution, such as Nitrogen dioxide (NO2), and the followed secondary pollution under certain meteorology circumstances and high concentration of precursors, such as tropospheric ozone, formaldehyde (HCHO) and fine particles. During PRIDE-GBA 2018 Campaign (Particles, Radicals, Intermediates from oxiDation of primary Emissions in Great Bay Area), we performed the high resolution vertical observations of pollution gases and aerosol, which are significant but scarce indexes in studying the mechanisms of tropospheric pollution, using remote sensing techniques. NO2 and HCHO column densities and vertical profiles are reconstructed from data of multi-axis differential optical absorption spectroscopy (MAX-DOAS). Tropospheric ozone profile and aerosol extinction are retrieved by the differential absorption light detection and ranging (LIDAR) system. In order to verifying the accuracy, we evaluated the consistency and reliability of MAX-DOAS and LIDAR measurements. The results showed reasonable agreement with in-situ and off-line observations at Canton Tower. A typical combined pollution process from Sep 29 to Oct 10 was analyzed in detail. More than 200 μg/m3 tropospheric ozone in this case was considered from the anthropogenic sources, including industry, power plant, residential and transportation. The high emission from local industry and polluted air transport from northeast brought the main precursors of this pollution process. The photochemical formation of tropospheric ozone was turned into a VOC-limited regime on polluted days.

Observation of vertical profiles of NO, O&lt;SUB&gt;3&lt;/SUB&gt;, and VOCs to estimate their sources and sinks by inverse modeling in a Japanese larch forest

Observation of vertical profiles of NO, O&lt;SUB&gt;3&lt;/SUB&gt;, and VOCs to estimate their sources and sinks by inverse modeling in a Japanese larch forest

Full-azimuthal imaging-DOAS observations of NO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; and O&amp;lt;sub&amp;gt;4&amp;lt;/sub&amp;gt; during CINDI-2

Abstract. A novel imaging-DOAS (differential optical absorption spectroscopy) instrument IMPACT (Imaging MaPper for AtmospheriC observaTions) is presented combining full-azimuthal pointing (360∘) with a large vertical coverage (∼41∘). Complete panoramic scans are acquired at a temporal resolution of ∼15 min, enabling the retrieval of NO2 vertical profiles over the entire panorama around the measurement site. IMPACT showed excellent agreement (correlation &gt;99 %) with coincident multiaxis DOAS (MAX-DOAS) measurements during the Second Cabauw Intercomparison of Nitrogen Dioxide measuring Instruments (CINDI-2) campaign. The temporal variability of NO2 slant columns within a typical MAX-DOAS vertical scanning sequence could be resolved and was as large as 20 % in a case study under good viewing conditions. The variation of corresponding profiles and surface concentrations was even larger (40 %). This variability is missed when retrieving trace gas profiles based on standard MAX-DOAS measurements. The azimuthal distribution of NO2 around the measurement site showed inhomogeneities (relative differences) up to 120 % (on average 35 %) on short timescales (individual panoramic scans). This is more than expected for the semirural location. We explain this behavior by the transport of pollution. Exploiting the instrument's advantages, the plume's trajectory during a prominent transport event could be reconstructed. Finally, the potential for retrieving information about the aerosol phase function from O4 slant columns along multiple almucantar scans of IMPACT is demonstrated, with promising results for future studies.

Vertical profiles of NO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;, SO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;, HONO, HCHO, CHOCHO and aerosols derived from MAX-DOAS measurements at a rural site in the central western North China Plain and their relation to emission sources and effects of regional transport

Abstract. A multi-axis differential optical absorption spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18∘ N, 114.36∘ E) in the suburban area of Xingtai, which is one of the most polluted cities in the North China Plain (NCP), during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) experiment and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with the coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ∼3.5 ppb. Underestimations of MAX-DOAS results compared to in situ measurements of NO2 (∼60 %) and SO2 (∼20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2 and SO2 are reasonably consistent with those measured by a collocated Raman lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ∼1.4 km) than NO2, SO2 and HONO did (with 75 % integrated column below ∼0.5 km) under polluted conditions. Lifted layers were systematically observed for all species (except HONO), indicating accumulation, secondary formation or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2, SO2 and HONO but occurred at around noon for aerosols, HCHO and CHOCHO, mainly dominated by photochemistry, characteristic upslope–downslope circulation and planetary boundary layer (PBL) dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with the backward propagation approach based on HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution was observed from the southern areas such as industrialized Wu'an. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations in HCHO, CHOCHO and aerosols. It needs to be noted that although several MAX-DOAS measurements of trace gases and aerosols in the NCP area have been reported in previous studies, this study is the first work to derive a comprehensive set of vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols from measurements of one MAX-DOAS instrument. Also, so far, the validation of MAX-DOAS profile results by comparison with various surface in situ measurements as well as profile measurements from lidar and aircraft is scarce. Moreover, the backward propagation approach for characterizing the contributions of regional transport of pollutants from different regions was applied to the MAX-DOAS results of trace gases and aerosols for the first time.

Changes in Vertical Distribution and Column Content of NO2 under the Influence of Sudden Stratospheric Warmings

Characteristic features of changes in the vertical distribution and column content of NO2, total ozone, and stratospheric temperature have been revealed as a result of major sudden stratospheric warmings (SSWs). Strong negative anomalies of column NO2, total ozone and stratospheric temperature are caused by the displacement of the stratospheric circumpolar vortex aside from the pole. Strong positive anomalies of column NO2 and total ozone are observed more frequently under SSWs accompanied by splitting of the stratospheric circumpolar vortex and are caused by the transport of stratospheric air from the low latitudes. Major SSWs can lead to significant changes in the vertical profile of NO2. The changes in different stratospheric layers can be opposite to each other when the edge of the polar vortex is over a site of ground-based observations.

GOME-2A retrievals of tropospheric NO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; in different spectral ranges – influence of penetration depth

Abstract. In this study, we present a novel nitrogen dioxide (NO2) differential optical absorption spectroscopy (DOAS) retrieval in the ultraviolet (UV) spectral range for observations from the Global Ozone Monitoring Instrument 2 on board EUMETSAT's MetOp-A (GOME-2A) satellite. We compare the results to those from an established NO2 retrieval in the visible (vis) spectral range from the same instrument and investigate how differences between the two are linked to the NO2 vertical profile shape in the troposphere.As expected, radiative transfer calculations for satellite geometries show that the sensitivity close to the ground is higher in the vis than in the UV spectral range. Consequently, NO2 slant column densities (SCDs) in the vis are usually higher than in the UV if the NO2 is close to the surface. Therefore, these differences in NO2 SCDs between the two spectral ranges contain information on the vertical distribution of NO2 in the troposphere. We combine these results with radiative transfer calculations and simulated NO2 fields from the TM5-MP chemistry transport model to evaluate the simulated NO2 vertical distribution.We investigate regions representative of both anthropogenic and biomass burning NO2 pollution. Anthropogenic air pollution is mostly located in the boundary layer close to the surface, which is reflected by large differences between UV and vis SCDs of ∼ 60 %. Biomass burning NO2 in contrast is often uplifted into elevated layers above the boundary layer. This is best seen in tropical Africa south of the Equator, where the biomass burning NO2 is well observed in the UV, and the SCD difference between the two spectral ranges is only ∼ 36 %. In tropical Africa north of the Equator, however, the biomass burning NO2 is located closer to the ground, reducing its visibility in the UV.While not enabling a full retrieval of the vertical NO2 profile shape in the troposphere, our results can help to constrain the vertical profile of NO2 in the lower troposphere and, when analysed together with simulated NO2 fields, can help to better interpret the model output.