Sarah J. Masonis

An intercomparison of lidar-derived aerosol optical properties with airborne measurements near Tokyo during ACE-Asia

[1] During the ACE-Asia intensive observation period (IOP), an intercomparison experiment with ground-based lidars and aircraft observations was conducted near Tokyo. On 23 April 2001, four Mie backscatter lidars were simultaneously operated in the Tokyo region, while the National Center for Atmospheric Research C-130 aircraft flew a steppedascent profile between the surface and 6 km over Sagami Bay southwest of Tokyo. The C-130 observation package included a tracking Sun photometer and in situ packages measuring aerosol optical properties, aerosol size distribution, aerosol ionic composition, and SO2 concentration. The three polarization lidars suggested that the observed modest concentrations of Asian dust in the free troposphere extended up to an altitude of 8 km. We found a good agreement in the backscattering coefficient at 532 nm among lidars and in situ 180� backscatter nephelometer observations. The intercomparison indicated that the aerosol layer between 1.6 and 3.5 km was a remarkably stable and homogenous in mesoscale. We also found reasonable agreement between the aerosol extinction coefficients (sa � 0.03 km � 1 ) derived from the airborne tracking Sun photometer, in situ optical instruments, and those estimated from the lidars above the planetary boundary layer (PBL). We also found considerable vertical variation of the aerosol depolarization ratio (da) and a negative correlation between da and the backscattering coefficient (da) below 3.5 km. Airborne measurements of size-dependent optical parameters (e.g., the fine mode fraction of scattering) and of aerosol ionic compositions suggests that the mixing ratio of the accumulation-mode and coarse-mode (dust) aerosols was primarily responsible for the observed variation of da. Aerosol observations during the intercomparison period captured the following three types of layers in the atmosphere: a PBL (surface to 1.2–1.5 km) where fine (mainly sulfate) particles with a low da (<10%) dominated; an intermediate layer (between the top of the PBL and 3.5 km) where fine particles and dust particles were moderately externally mixed, giving moderate da; and an upper layer (above � 3.5 km) where dust dominated, giving a high da (30%). A substantial dust layer between 4.5 and 6.5 km was observed just west of Japan by the airborne instruments and found to have a lidar ratio of 50.4 ± 9.4 sr. This agrees well with nighttime Raman lidar measurements made later on this same dust layer as it passed over Tokyo, which found a lidar ratio of 46.5 ± 10.5 sr. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles

In situ measurement of the aerosol extinction-to-backscatter ratio at a polluted continental site

The extinction-to-backscatter ratio S is a crucial parameter for quantitative interpretation of lidar data, yet empirical knowledge of S for tropospheric aerosols is extremely limited. Here we review that knowledge and extend it using a recently developed in situ technique that employs a 180° backscatter nephelometer. This technique allows robust quantification of measurement uncertainties and permits correlations with other aerosol and meteorological properties to be explored. During 4 weeks of nearly continuous measurements in central Illinois, S was found to vary over a wide range, confirming previous indications that geographical location by itself is not necessarily a good predictor. The data suggest a modest dependence of S on relative humidity, but this explains only a small portion of the variation. Most variation was associated with changes between two dominant air mass types: rapid transport from the northwest and regional stagnation. The latter category displayed much higher aerosol concentrations and a systematically higher and more tightly constrained range of S. Averages and standard deviations were 64±4 sr for the stagnant category and 40±9 sr for the rapid transport category. Considering the 95% confidence precision uncertainty of the measurements, the difference between these averages is at least 13 sr and could be as large as 35 sr. The wavelength dependence of light scattering, as measured by a conventional nephelometer, is shown to have some discriminatory power with respect to S.

Measurement of the lidar ratio for atmospheric aerosols using a 180 degree-backscatter nephelometer

Laser radar (lidar) can be used to estimate atmospheric extinction coefficients that are due to aerosols if the ratio between optical extinction and 180 degrees backscatter (the lidar ratio) at the laser wavelength is known or if Raman or high spectral resolution data are available. Most lidar instruments, however, do not have Raman or high spectral resolution capability, which makes knowledge of the lidar ratio essential. We have modified an integrating nephelometer, which measures the scattering component of light extinction, by addition of a backward-pointing laser light source such that the detected light corresponds to integrated scattering over 176-178 degrees at a common lidar wavelength of 532 nm. Mie calculations indicate that the detected quantity is an excellent proxy for 180 degrees backscatter. When combined with existing techniques for measuring total scattering and absorption by particles, the new device permits a direct determination of the lidar ratio. A four-point calibration, run by filling the enclosed sample volume with particle-free gases of a known scattering coefficient, indicates a linear response and calibration reproducibility to within 4%. The instrument has a detection limit of 1.5 x 10(-7) m(-1) sr(-1) (approximately 10% of Rayleigh scattering by air at STP) for a 5-min average and is suitable for ground and mobile/airborne surveys. Initial field measurements yielded a lidar ratio of approximately 20 for marine aerosols and approximately 60-70 for continental aerosols, with an uncertainty of approximately 20%.

Sea-Salt Size Distributions from Breaking Waves: Implications for Marine Aerosol Production and Optical Extinction Measurements during SEAS*

The authors’ participation in the Shoreline Environment Aerosol Study (SEAS) involved measurements focused on the coastal aerosol size distribution and related optical measurements, including aerosol light scattering, visibility, and remote sensing of aerosol using lidar backscatter. Aerosol production from shoreline breaking waves and the more distant reef (;1 km) was characterized for dry sizes between 0.01 and 10 mm for both their contribution to the marine aerosol population and their influence on near-surface lidar extinction. Thermal volatility was used to extract the refractory sea-salt particles from the other constituents volatile at 360 8C. At 7 m ASL and 20 m inland from the water’s edge the production of sea-salt nuclei number was often in the range of 50‐100 cm23 above the open-ocean value of ;250 cm23. This number peak was near 0.03-mm dry diameter, while light scattering was dominated by a few particles larger than 1 mm. This indicates that production of sea salt from breaking waves contributes not only to aerosol mass and optical effects but also to nuclei mode particle number in remote regions. Separate studies of optical closure quantified links between the size distribution and optical scattering measurements, visibility, and extinction values for both nearshore breaking waves and openocean conditions. These data confirmed that extinction derived from coastal lidar measurements at 0.530 mm was accurate to better than the 25% uncertainty claimed for the lidar inversion.

A Study of the Extinction-to-Backscatter Ratio of Marine Aerosol during the Shoreline Environment Aerosol Study*

Abstract Ground-based aerosol optical measurements made at near-ambient relative humidity (RH) under clean marine sampling conditions are presented and compared to 1) almost identical optical measurements made at a polluted continental site and 2) optical properties calculated from measured size distributions and Mie theory. The use of Mie theory (which assumes homogeneous spheres) is justified based on the fact that the sea-salt aerosol was measured in a hydrated state. This study focuses on the extinction-to-backscatter ratio S, an optical property required to interpret remote measurements by elastic backscatter lidar. For clean marine conditions, S is found to be 25.4 ± 3.5 sr at 532 nm (central value ± 95% confidence uncertainty). Other optical properties reported include single-scattering albedo, wavelength dependence of scattering, fraction of scattering due to submicrometer particles, and hemispheric-backscatter fraction, as well as the extensive properties (e.g., scattering coefficient) upon which...