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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]