Aerosol optical properties along the northeast coast of North America during the New England Air Quality Study–Intercontinental Transport and Chemical Transformation 2004 campaign and the influence of aerosol composition

[1] Optical and hygroscopic properties of submicrometer diameter aerosol particles were measured on board the NOAA R/V Ronald H. Brown as part of the NEAQS-ITCT field campaign. The campaign occurred along the northeast coast of North America during the summer of 2004. A scanning relative humidity (RH) nephelometry system (humidograph) measured total light scattering and backscattering coefficients (σsp and σbsp, respectively) at three wavelengths (λs) and RH = 26% and while RH was scanned between 40% and 85%. These measurements were combined with aerosol light absorption and composition measurements to describe σsp, σbsp, single scattering albedo (ω), Angstrom exponent (a), and hemispheric backscatter fraction (b) at a low reference RH of 26 ± 4% and the aerosol's hygroscopic properties based on its optical response up to 85% RH. Humidogram curve structure was dominated by hygroscopic growth without hysteresis (76% frequency). Dependence of the aerosol's σsp values with changes in RH, fσsp(RH, 26), was observed to decrease with increasing mass fraction of particulate organic matter (POM, FO). Statistical analyses indicated that increasing FO resulted in a less hygroscopic aerosol, while increasing molar equivalence ratio (ER) resulted in lower hysteresis factors based on the aerosols' optical responses at a 0.95 confidence level. ω showed little RH dependence while a and b decreased with increasing RH values. Values for a(λ1, λ2), b, and fσsp(82, 26) increased with increasing λ values. Sensitivities of top of the atmosphere aerosol radiative forcing to changes in ω, b, and σsp with RH were also estimated.