[1] Continuous observations of aerosols in China and Japan were made by polarization lidars during March to May 2001, corresponding with the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) field campaign period. Lidars in Beijing, Nagasaki, and Tsukuba were continuously operated regardless of weather conditions. Scatterers in the atmosphere were categorized for all vertical profiles, and occurrence frequencies of dust, spherical aerosols, and clouds up to 6 km were calculated. The frequency of dust was highest in Beijing for the whole height range. There was a peak of dust occurrence near the ground in Nagasaki. Dust was frequently detected in the free troposphere in Tsukuba. The contributions of dust and spherical aerosols to the total backscattering coefficient were estimated from the depolarization ratio with the assumption of the external mixture of both kinds of aerosols. Vertical profiles of backscattering by dust and by spherical aerosols represented the different characteristics of these aerosols. The monthly averaged backscattering coefficients by dust near the surface were 0.003/km/sr in Beijing, 0.001-0.002/km/sr in Nagasaki, and 0.0006/km/sr in Tsukuba. The backscattering coefficients by spherical aerosols near the surface were 0.002-0.004/km/sr at all three observatories. We compared the derived backscattering coefficients with aerosol mass concentrations calculated by a numerical model, Chemical Weather Forecasting System (CFORS). CFORS reproduced well the vertical structures of the tall dust events and the enhancements of spherical aerosols throughout the observation period. A specific dust event on 16-19 May 2001 was analyzed by using five lidars in Japan, and its fine structure is described.

[1] It has recently been suggested that some organic aerosols can absorb solar radiation, especially at the shorter visible and UV wavelengths. Although quantitative characterization of the optical properties of secondary organic aerosols (SOAs) is required in order to confirm the effect of SOAs on the atmospheric radiation balance, the light absorption of SOAs has not yet been thoroughly investigated. In this study, we conducted laboratory experiments to measure the optical properties of SOAs generated during the photooxidation of toluene in the presence of NO x and the ozonolysis of a-pinene. Extinction and scattering coefficients of the SOAs were measured by a cavity ring-down aerosol extinction spectrometer and an integrating nephelometer, respectively. Refractive indices of the SOAs were determined so that the measured particle size dependence of the extinction and scattering efficiencies could be reproduced by calculations using Mie scattering theory. As a result, significant light absorption was found at 355 nm for the toluene SOAs. In contrast, no significant absorption was found either at 355 or 532 nm for the a-pinene SOAs. Using the obtained refractive index, mass absorption cross-section values of the toluene SOAs were calculated to be 0.3-3 m 2 g −1 at 355 nm. The results indicate that light absorption by the SOAs formed from the photooxidation of aromatic hydrocarbons have a potential to influence the total aerosol light absorption, especially at UV wavelengths.Citation: Nakayama, T., Y. Matsumi, K. Sato, T. Imamura, A. Yamazaki, and A. Uchiyama (2010), Laboratory studies on optical properties of secondary organic aerosols generated during the photooxidation of toluene and the ozonolysis of a-pinene,

Recently, secondary organic aerosols (SOAs) generated from anthropogenic volatile organic compounds have been proposed as a possible source of light-absorbing organic compounds, "brown carbon," in the urban atmosphere. However, the atmospheric importance of these SOAs remains unclear due to limited information about their optical properties. In this study, the complex refractive index (RI, m = nki) values at 405, 532, and 781 nm of the SOAs generated during the photooxidation of toluene (toluene-SOAs) under a variety of initial nitrogen oxide (NO x = NO + NO 2 ) conditions were examined by photoacoustic spectroscopy (PAS) and cavity ring-down spectroscopy (CRDS). The complex RI-values obtained in the present study and reported in the literature indicate that the k-value, which represents the light absorption of the toluene-SOAs, increased to shorter wavelengths at <532 nm, and the n-value also increased to shorter wavelengths from 781 to 355 nm. The k-values at 405 nm were found to increase from 0.0018 to 0.0072 with increasing initial NO x concentration from 109 to 571 ppbv. The nitrate to organics ratio of the SOAs determined using a high-resolution time-of-flight aerosol mass spectrometer (H-ToF-AMS) also increased with increasing initial NO x concentration. The RI-values of the SOAs generated during the photooxidation of 1,3,5-trimethylbenzene in the presence of NO x (1,3,5-TMB-SOAs) were also determined to investigate the influence of the chemical structure of the precursor on the optical properties of the SOAs, and it was found that the light absorption of the 1,3,5-TMB-SOAs is negligible at all of the wavelengths investigated (405, 532, and 781 nm). These results can be reasonably explained by the hypothesis that ni-troaromatic compounds, such as nitrocresols, are the major contributors to the light absorption of the toluene-SOAs. Using the obtained RI-values, mass absorption cross sections of the toluene-SOAs at 405 nm were estimated to be 0.08-0.52 m 2 g −1 under typical conditions in an urban atmosphere during the daytime. These results indicate that light absorption by the SOAs potentially contributes to the radiation balance at ultraviolet wavelengths below ∼400 nm, specifically when the mass concentrations of the anthropogenic SOAs are significant compared with other light-absorbing particles.

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Abstract. This study compares the aerosol optical and physical properties simultaneously measured by a SKYNET PREDE skyradiometer and AERONET/PHOTONS CIMEL sunphotometer at a location in Beijing, China. Aerosol optical properties (AOP) including the Aerosol Optical Depth (AOD), Angstrom exponent (α), volume size distribution, single scattering albedo (ω) and the complex refractive index were compared. The difference between the two types of instruments was less than 1.3% for the AOD and less than 4% for the single scattering albedo below the wavelength of 670 nm. There is a difference between the volume size distribution patterns derived from two instruments, which is probably due to difference of measurement protocols and inversion algorithms for the respective instruments.AOP under three distinct weather conditions (background, haze, and dust days) over Beijing were compared by using the retrieved skyradiometer and sunphotometer data combined with MODIS satellite results, pyranometer measurements, PM 10 measurements, and backtrajectory analysis. The results show that the significant difference of AOP under background, haze, and dust days over Beijing is probably due to different aerosol components under distinct weather conditions.

Laboratory experiments were conducted for characterizing the performance of two commercially available instruments employed for the measurement of light absorption and scattering coefficients of aerosols at λ = 405, 532, and 781 nm (using three-wavelength photoacoustic soot spectrometer; PASS-3) as well as at 375 nm (using photoacoustic extinctiometer; PAX) based on photoacoustic spectroscopy and reciprocal nephelometry, respectively. The calibration factors (conversion factors from the readout to real values) associated with scattering measurements, estimated using gaseous molecules, mono-disperse polystyrene latex and ammonium sulfate particles, and/or polydisperse ammonium sulfate particles, are in good agreement with one another, typically within 5 %, 5 %, and 10 % at 375, 405, and 781 nm, respectively. In contrast, a significant particle size dependency was observed for the calibration factors at 532 nm, which is possibly because of a combination of differences in the polarization states of the lasers relative to the scattering planes and large truncation angle. Considering the estimated effective truncation angle, the typical uncertainties in calibration factors for scattering when measuring non-or weakly light-absorbing particles, with volume-based geometrical diameters of less than 700 nm, were estimated to be 12 %, 7 %, 34 %, and 17 %, at 375, 405, 532, and 781 nm, respectively. The typical uncertainties in the calibration factors for absorption measurements, which were determined using poly-disperse propane soot particles, were estimated to be 6 %, 4 %, 8 %, and 11 %, at 375, 405, 532, and 781 nm, respectively. The calibration factors for absorption determined by the poly-disperse soot particles at 375 and 405 nm were 48 % and 36 % smaller than those by light absorption of NO 2 molecules possibly because of NO 2 photolysis, although good agreement was observed at 532 nm. These results suggest that the photolysis effect should be taken into account when light absorption by NO 2 is used for calibration at 375 and 405 nm.

[1] Collocated aircraft observations of microstructure and radiative properties of winter boundary layer clouds over the East China Sea and the Japan Sea have been carried out in January 1999 within the Japanese Cloud and Climate Study (JACCS) program. The first part of the paper describes the in situ measured microphysical and optical properties for two cases of boundary layer winter stratocumulus clouds, which concern, first, a rather uniform, supercooled water cloud contaminated by aerosols and, second, a highly heterogeneous, mixed-phase stratiform cloud. Using the Polar Nephelometer, a new instrument for measuring, in situ, the scattering phase function of cloud droplets and ice particles, the polluted, continental-type stratocumulus cloud can be optically regarded as a liquid water cloud because the measured scattering phase functions fitted very well with those calculated from Mie theory for the directly measured FSSP size distributions. In mixed-phase cloud, the measured scattering phase function shows that ice particles strongly affect optical properties of the cloud, where large number of liquid water droplets with higher extinction coefficient and asymmetry factor values were converted into a much smaller number of large ice crystals with lower extinction coefficient and asymmetry factor. Furthermore, a quasi-stable liquid-topped cloud layer with precipitating ice particles was noticed; the layer may, first, affect the cloud radiative properties and, second, seriously restrict the interpretation of satellite cloud composition retrievals.

Atmospheric aerosol particles play an important role in climate change by scattering and absorbing solar radiation. To quantify the direct influence of aerosols on the atmospheric radiation balance, a detailed understanding of the complex refractive index (RI) for a variety of aerosols is required. The wavelength dependence of the RI values for secondary organic aerosols (SOAs) generated during the ozonolysis and photooxidation of α-pinene, which is a major biogenic volatile organic compound (BVOC), was investigated using a photoacoustic soot spectrometer (PASS) and a cavity ring-down spectrometer (CRDS). The real part of the RI values for SOAs generated from both ozonolysis and photooxidation was found to lie between 1.4 and 1.5 at 405, 532, and 781 nm, and to slightly increase with decreasing wavelength. Additionally, the imaginary part of the RI values for these SOAs was found to be negligible (< 0.003) at all of the wavelengths studied (405, 532, and 781 nm). The obtained complex RI values were also compared with values reported in the literature and the chemical properties of the SOAs, which were measured using a high resolution time-of-flight aerosol mass spectrometer (H-ToF-AMS).