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The evaluation of chemical transport models, CTMs, is essential for the assessment of their performance regarding the physical and chemical parameterizations used. While regional CTMs have been widely used and evaluated over Europe, their validation over Greece is limited. In this study, we investigate the performance of the Long Term Ozone Simulation European Operational Smog (LOTOS-EUROS) v2.2.001 regional chemical transport model in simulating nitrogen dioxide, NO 2 , over Greece from June to December 2018. In situ NO 2 measurements obtained from 14 stations of the National Air Pollution Monitoring Network are compared with surface simulations over the two major cities of Greece, Athens and Thessaloniki. Overall the LOTOS-EUROS NO 2 surface simulations compare very well to the in situ measurements showing a mild underestimation of the measurements with a mean relative bias of ∼-10 %, a high spatial correlation coefficient of 0.86 and an average temporal correlation of 0.52. The CTM underestimates the NO 2 surface concentrations during daytime by ∼-50 ± 15 %, while it slightly overestimates during night-time ∼ 10 ± 35 %. Furthermore, the LOTOS-EUROS tropospheric NO 2 columns are evaluated against ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) NO 2 measurements in Athens and Thessaloniki. We report that the CTM tropospheric NO 2 column simulations over both urban and rural locations represent the diurnal patterns and hourly levels for both summer and winter seasons satisfactorily. The relative biases range between ∼ - 2 % and - 35 %, depending on season and relative NO 2 load observed. Finally, the CTM was assessed also against space-borne Sentinel-5 Precursor (S5P) carrying the Tropospheric Monitoring Instrument (TROPOMI) tropospheric NO 2 observations. We conclude that LOTOS-EUROS simulates extremely well the tropospheric NO 2 patterns over the region with very high spatial correlation of 0.82 on average, ranging between 0.66 and 0.95, with negative biases in the summer and positive in the winter. Updated emissions for the simulations and model improvements when extreme values of boundary layer height are encountered are further suggested. [ABSTRACT FROM AUTHOR]

In this study, we report on the retrieval of aerosol extinction profiles from ground-based scattered sunlight multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, carried out at Athens, Greece. It is the first time that aerosol profiles are retrieved from MAX-DOAS measurements in Athens. The reported aerosol vertical distributions at 477 nm are derived from the oxygen dimer (O4) differential-slant-column-density observations at different elevation angles by applying the BRemen Optimal estimation REtrieval for Aerosol and trace gaseS (BOREAS) retrieval algorithm. Four case studies have been selected for validation purposes; the retrieved aerosol profiles and the corresponding aerosol optical depths (AODs) from the MAX-DOAS are compared with lidar extinction profiles and with sun-photometric measurements (Aerosol Robotic Network, AERONET, observations), respectively. Despite the different approach of each method regarding the retrieval of the aerosol information, the comparison with the lidar measurements at 532 nm reveals a very good agreement in terms of vertical distribution, with r>0.90 in all cases. The AODs from the MAX-DOAS and the sun photometer (the latter at 500 nm) show a satisfactory correlation (with 0.45 < r < 0.7 in three out of the four cases). The comparison indicates that the MAX-DOAS systematically underestimates the AOD in the cases of large particles (small Ångström exponent) and for measurements at small relative azimuthal angles between the viewing direction and the sun. Better agreement is achieved in the morning, at large relative azimuthal angles. Overall, the aerosol profiles retrieved from MAX-DOAS measurements are of good quality; thus, new perspectives are opened up for assessing urban aerosol pollution on a long-term basis in Athens from continuous and uninterrupted MAX-DOAS measurements. [ABSTRACT FROM AUTHOR]

In this study, we report on the retrieval of aerosol extinction profiles from ground-based scattered sunlight multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, carried out at Athens, Greece. It is the first time that aerosol profiles are retrieved from MAX-DOAS measurements in Athens. The reported aerosol vertical distributions at 477 nm are derived from the oxygen dimer (O4) differential slant column density observations at different elevation angles by applying the BOREAS retrieval algorithm. Four case studies have been selected for validation purposes; the retrieved aerosol profiles and the corresponding aerosol optical depths (AODs) from the MAX-DOAS are compared with lidar extinction profiles and with sun photometric measurements (AERONET observations), respectively. Despite the different approach of each method regarding the retrieval of the aerosol information, the comparison with the lidar measurements at 532 nm reveals a very good agreement in terms of vertical distribution, with r > 0.85 in all cases. The AODs from the MAX-DOAS and the sun-photometer (the latter at 500 nm) show a satisfactory correlation (with r ≈ 0.6 in three out of the four cases). The comparison indicates that the MAX-DOAS systematically underestimates the AOD in the cases of large particles (small Ångström exponent) and for measurements at small relative azimuthal angles between the viewing direction and the Sun. Better agreement is achieved in the morning, at large relative azimuthal angles. Overall, the aerosol profiles retrieved from MAX-DOAS measurements are of good quality; thus, new perspectives are opened up for assessing urban aerosol pollution on a long term-basis in Athens from continuous and uninterrupted MAX-DOAS measurements. [ABSTRACT FROM AUTHOR]

Long-term nitrogen dioxide (NO2) slant column density measurements using the MAX-DOAS (multi-axis differential optical absorption spectroscopy) technique were analyzed in order to demonstrate the temporal and horizontal variability of the trace gas in Athens for the period October 2012–July 2017. The synergy with in situ measurements and model simulations was exploited for verifying the MAX-DOAS technique and its ability to assess the spatiotemporal characteristics of NO2 pollution in the city. Tropospheric NO2 columns derived from ground-based MAX-DOAS observations in two horizontal and five vertical viewing directions were compared with in situ chemiluminescence measurements representative of urban, urban background and suburban conditions; a satisfactory correlation was found for the urban (r ≈ 0.55) and remote areas (r ≈ 0.40). Mean tropospheric slant columns retrieved from measurements at the lowest elevation over the urban area ranged from 0.1 to 32 × 1016 molec cm−2. The interannual variability showed a rate of increase of 0.3 × 1016 molec cm−2 per year since 2012 in the urban area, leading to a total increase of 20%. The retrieved annual cycles captured the seasonal variability with lower NO2 levels in summer, highly correlated (r ≈ 0.85) with the urban background and suburban in situ observations. The NO2 diurnal variation for different seasons exhibited varied patterns, indicating the different role of photochemistry and anthropogenic activities in the different seasons. Compared to in situ observations, the MAX-DOAS NO2 morning peak occurred with a one-hour delay and decayed less steeply in winter. Measurements at different elevation angles are shown as a primary indicator of the vertical distribution of NO2 at the urban environment; the vertical convection of the polluted air masses and the enhanced NO2 near-surface concentrations are demonstrated by this analysis. The inhomogeneity of the NO2 spatial distribution was shown using a relevant inhomogeneity index; greater variability was found during the summer period. Comparisons with city-scale model simulations demonstrated that the horizontal light path length of MAX-DOAS covered a distance of 15 km. An estimation of urban sources' contribution was also made by applying two simple methodologies on the MAX-DOAS measurements. The results were compared to NO2 predictions from the high resolution air quality model to infer the importance of vehicle emissions for the urban NO2 levels; 20–35% of the urban NO2 was found to be associated with road transport. [ABSTRACT FROM AUTHOR]

Slant column (SC) densities of nitrogen dioxide (NO 2 ), formaldehyde (HCHO), glyoxal (CHOCHO) and oxygen dimer (O 4 ) were successfully retrieved for the first time in Athens, by using spectral measurements from a ground-based multi-azimuth Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) system. The data span the period from October 2012 to March 2014 and measurements were conducted at NOA's (National Observatory of Athens) station in Penteli (38.0°N, 23.9°E, 527 m a.s.l.) at eight azimuth angles and eight off-axis elevation angles. The SC NO2 , SC HCHO and SC CHOCHO measurements at +1 ο elevation angle, pointing towards the urban area, range from 0.6 to 24·10 16 , 0.8–9.6·10 16 and 0.3–5.2·10 15 molec cm −2 (mean daily values throughout the whole period), respectively. Seasonal modulation characterised by summertime maximum and wintertime minimum was observed for HCHO and CHOCHO, while for NO 2 the maximum values were recorded during winter. Changes in the diurnal variability of all trace gases with season and day of the week are investigated suggesting a strong link to primary anthropogenic sources for NO 2 and a weaker one, compared to photochemistry, for HCHO and CHOCHO. In addition, the impact of the reduced anthropogenic emissions during weekends on the measured SC values was quantified and 30%–50% lower SC NO2 values were found during weekends. The contribution of local urban emissions to the overall recorded amounts of the selected species was assessed. Using meteorological data from NOA's station in Penteli, the impact of the local circulation patterns on the SC levels was estimated, and a strong relation between western wind direction, which is related to the industrial area, and enhanced SC measurements was found. [ABSTRACT FROM AUTHOR]