Abstract

In this study we focus on the retrieval of aerosol and trace gas vertical profiles from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations for the first time over Thessaloniki, Greece. We use two independent inversion algorithms for the profile retrievals: The Mexican MAX-DOAS Fit (MMF) and the Mainz Profile Algorithm (MAPA). The former is based on the Optimal Estimation Method (OEM), while the latter follows a parameterization approach. We evaluate the performance of MMF and MAPA and we validate their retrieved products with ancillary data measured by other co-located reference instruments. We find an excellent agreement between the tropospheric column densities of NO2 retrieved by MMF and MAPA (Slope = 1.009, Pearson's correlation coefficient R = 0.982) and a good correlation for the case of HCHO (R = 0.927). For aerosols, we find better agreement for the aerosol optical depths (AODs) in the visible (i.e., at 477 nm), compared to the UV (360 nm) and we show that the agreement strongly depends on the O4 scaling factor that is used in the analysis. The trace gas differential slant column densities (dSCDs), simulated by the forward models, are also in good agreement, except for HCHO, where larger scatter is observed due to the increased spectral noise of the measurements in the UV. The agreement for NO2 and HCHO surface concentrations is similar to the comparison of the integrated columns with slightly decreased correlation coefficients. The AODs retrieved by the MAX-DOAS are validated by comparing them with AOD values measured by a CIMEL sun-photometer and a Brewer spectrophotometer. Four different flagging schemes were applied to the data in order to evaluate their performance. Qualitatively, a generally good agreement is observed for both wavelengths, but we find a systematic bias from the CIMEL and Brewer measurements, due to the limited sensitivity of the MAX-DOAS in retrieving information at higher altitudes, especially in the UV. An in-depth validation of the aerosol vertical profiles retrieved by the MAX-DOAS is not possible since only in very few cases the true aerosol profile is known during the period of study. However, we examine four cases, where the MAX-DOAS provided a generally good estimation of the shape of the profiles retrieved by a co-located multi-wavelength lidar system. The NO2 surface concentrations are validated against in situ observations and the comparison of both MMF and MAPA revealed good agreement with correlation coefficients of R = 0.78 and R = 0.73, respectively. Finally, the effect of the O4 scaling factor is investigated by intercomparing the integrated columns retrieved by the two algorithms and also by comparing the AODs derived by MAPA for different values of the scaling factor with AODs measured by the CIMEL and the Brewer.

Highlights

  • The planetary boundary layer (PBL), called atmospheric boundary layer, is defined as the lowermost layer of the troposphere that is directly influenced by the terrestrial surface

  • The effect of the O4 scaling factor is investigated by intercomparing the integrated columns retrieved by the two algorithms and by comparing the aerosol optical depths (AODs) derived by Mainz Profile Algorithm (MAPA) for different values of the scaling factor with AODs measured by the CIMEL and the Brewer

  • The tropospheric column densities of NO2 are in excellent agreement, while for HCHO, even though a generally good correlation is found (R = 0.927), deviations from unity in the slopes are observed, which can be attributed to discrepancies between the HCHO differential slant column densities (dSCDs) simulated by the forward models of Mexican MAX-Differential Optical Absorption Spectroscopy 60 (DOAS) Fit (MMF) and MAPA

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Summary

Introduction

The planetary boundary layer (PBL), called atmospheric boundary layer, is defined as the lowermost layer of the troposphere that is directly influenced by the terrestrial surface. Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) is a well-established ground-based passive remote sensing technique that received considerable attention during the past decades (Hönninger and Platt, 2002; Hönninger et al., 2004; Wagner et al, 2004; Wittrock et al, 2004; Frieß et al, 2006; Irie et al, 2008) and is nowadays widely used in many studies in order to simultaneously detect trace gases and aerosols mainly in the PBL and in the lowermost free troposphere 55 (e.g., Clémer et al (2010); Irie et al (2011); Ma et al (2013); Pinardi et al (2013); Vlemmix et al (2015a, b); Wang et al (2017b); Chan et al (2019) and references therein) Such trace gases include NO2, HCHO, sulfur dioxide (SO2), water vapour (H2O), ozone (O3), nitrous acid (HONO), iodine oxide (IO), glyoxal (CHOCHO) and bromine oxide (BrO). The integration time at each elevation angle is ∼ 60 sec and a full measurement sequence for all azimuth directions lasts about one hour

MAX-DOAS measurements and slant column retrieval settings
Retrieval of the vertical profile
Input parameters and settings
CIMEL sun-photometer
In situ
Results and discussion
Integrated Columns
Simulated dSCDs
Conclusions
Full Text
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