Abstract

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. The trace gas differential slant column densities (dSCDs), simulated by the forward models, are in good agreement, except for HCHO, where larger scatter is observed due to the increased spectral noise of the measurements in the UV. 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 (at 360 nm), and we show that the agreement strongly depends on the O4 scaling factor that is used in the analysis. The agreement for NO2 and HCHO near-surface concentrations is similar to the comparison of the integrated columns with slightly decreased correlation coefficients. The seasonal mean vertical profiles that are retrieved by MMF and MAPA are intercompared, and the seasonal variation in all species along with possible sources is discussed. 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 sun photometer and Brewer spectrophotometer 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 is the true aerosol profile 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 near-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 sun photometer and the Brewer spectrophotometer.

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

  • We intercompare the differential slant column densities (dSCDs) simulated by the forward models, the integrated columns (i.e., vertical column densities (VCDs) and aerosol optical depths (AODs) for trace gases and aerosols, respectively), the near-surface concentrations, and the seasonal mean vertical profiles between Mexican MAX-differential optical absorption spectroscopy (DOAS) Fit (MMF) and Mainz Profile Algorithm (MAPA)

  • In this study we have retrieved vertical profiles of aerosols, NO2, and HCHO for the first time in Thessaloniki, Greece, using MAX-DOAS observations by applying an optimal estimation method (OEM)-based inversion algorithm (MMF) and a parameterized algorithm (MAPA). Their performance is evaluated by intercomparing the dSCDs simulated by the forward models, the integrated columns (i.e., VCDs for trace gases and AODs for aerosols), the trace gas near-surface concentrations, and the seasonal mean vertical profiles derived by the two algorithms

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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 (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 vapor (H2O), ozone (O3), nitrous acid (HONO), iodine oxide (IO), glyoxal (CHOCHO), and bromine oxide (BrO).

Instrumentation
MAX-DOAS measurements and slant column retrieval settings
Retrieval of the vertical profile
Input parameters and settings
Ancillary data
CIMEL sun photometer
Brewer spectrophotometer
In situ
Results and discussion
Simulated dSCDs
Averaging kernels
Integrated columns
Surface concentrations
Seasonal mean vertical profiles
Validation
Aerosol extinction profiles
NO2 surface concentration
Summary and conclusions
Full Text
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