Temporal variations of aerosol, glyoxal, and formaldehyde at urban sites of Japan as observed by MAX-DOAS based on detailed error analysis
Friday, 19 December 2014
The degradation of volatile organic compounds (VOCs) results in the formation of ozone (O3) and secondary organic aerosols (SOA) in the troposphere. This process consists of the oxidation of VOCs by hydroxyl radical (OH), O3, and nitrate radical (NO3). Detailed understanding of the VOC degradation mechanism is challenged by the co-existence of vast variety of VOC species in the atmosphere. However, investigations on ubiquitous oxidation intermediates, e.g., formaldehyde (HCHO) and glyoxal (CHOCHO), can help us improve the current knowledge of the VOC sources and degradation pathways. We installed one ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) system in Meteorological Research Institute (MRI) located at Tsukuba, Japan (36.06N, 130.13E) in June 2010. In addition, two more systems were installed in Chiba University at Chiba, Japan (35.63N, 140.10E) in June and December 2012, respectively. Since then, we have retrieved lower-tropospheric vertical profile information for eight components; aerosol extinction coefficients at two wavelengths, 357 and 476 nm, and NO2, HCHO, CHOCHO, H2O, SO2, and O3 concentrations. For a detailed evaluation for the aerosol retrieval, which is a key step in the MAX-DOAS eight-component retrieval, simultaneous aerosol observations with the Cavity Ring-Down Spectroscopy (CRDS), lidar, and sky radiometer were conducted at Tsukuba on October 5-18, 2010. At Chiba, in addition to the comparison with sky radiometer data, a self-consistency test was performed by comparing results obtained from two MAX-DOAS systems operated at the same place. Through these detailed evaluations, our retrieval method was improved significantly, attaining excellent agreement with CRDS, lidar, and sky radiometer data. On the basis of these efforts, we find clear seasonal and diurnal temporal variations in HCHO and CHOCHO concentrations and their ratios (RGF) retrieved from MAX-DOAS systems. Using NO2 retrieved together with HCHO and CHOCHO, we find that HCHO and CHOCHO concentrations increased and the RGF decreased due to anthropogenic activities.