Abstract

Abstract. In situ observations of spectrally resolved aerosol extinction coefficients (300–700 nm at ∼ 0.8 nm resolution) from the May–June 2016 Korea–United States Ocean Color (KORUS-OC) oceanographic field campaign are reported. Measurements were made with the custom-built Spectral Aerosol Extinction (SpEx) instrument that previously has been characterized only using laboratory-generated aerosols of known size and composition. Here, the performance of SpEx under realistic operating conditions in the field was assessed by comparison to extinction coefficients derived from commercial instruments that measured scattering and filter-based absorption coefficients at three discrete visible wavelengths. Good agreement was found between these two sets of extinction coefficients with slopes near unity for all three wavelengths within the SpEx measurement error (± 5 Mm−1). The meteorological conditions encountered during the cruise fostered diverse ambient aerosol populations with varying sizes and composition at concentrations spanning 2 orders of magnitude. The sampling inlet had a 50 % size cut of 1.3 µm diameter particles such that the in situ aerosol sampling suite deployed aboard ship measured fine-mode aerosols only. The extensive hyperspectral extinction data set acquired revealed that nearly all measured spectra exhibited curvature in logarithmic space, such that Ångström exponent (α) power law fits could lead to large errors compared to measured values. This problem was particularly acute for α values calculated over only visible wavelengths and then extrapolated to the UV, highlighting the need for measurements in this wavelength range. Second-order polynomial fits to the logarithmically transformed data provided a much better fit to the measured spectra than the linear fits of power laws. Building on previous studies that used total column aerosol optical depth observations to examine the information content of spectral curvature, the relationship between α and the second-order polynomial fit coefficients (a1 and a2) was found to depend on the wavelength range of the spectral measurement such that any given α maps into a line in (a1, a2) coefficient space with a slope of −2LN(λch), where λch is defined as the single wavelength that characterizes the wavelength range of the measured spectrum (i.e., the “characteristic wavelength”). Since the curvature coefficient values depend on λch, it must be taken into account when comparing values from spectra obtained from measurement techniques with different λch. Previously published work has shown that different bimodal size distributions of aerosols can exhibit the same α yet have differing spectral curvature with different (a1, a2). This implies that (a1, a2) contain more information about size distributions than α alone. Aerosol size distributions were not measured during KORUS-OC, and the data reported here were limited to the fine fraction, but the (a1, a2) maps obtained from the SpEx data set are consistent with the expectation that (a1, a2) may contain more information than α – a result that will be explored further with future SpEx and size distribution data sets.

Highlights

  • Significant natural variability in the size and composition of atmospheric aerosols introduces uncertainty into the representation of their optical properties and radiative impacts in models and satellite retrievals

  • From 25 through 31 May the Transport/Haze period was characterized by air mass transport, overcast hazy conditions, and rapid local South Korean secondary production of inorganic aerosols resulting in the largest concentrations of the PM2.5 fraction of aerosols observed during the KORUS-AQ campaign (Peterson et al, 2019; Eck et al, 2020; Jordan et al, 2020)

  • The greatest σscat values observed aboard the R/V Onnuri were found during the first half of the Transport/Haze period while the ship was downwind of the Korean peninsula in the East Sea (Figs. 1a and b, and 2a)

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Summary

Introduction

Significant natural variability in the size and composition of atmospheric aerosols introduces uncertainty into the representation of their optical properties and radiative impacts in models and satellite retrievals. There is long-standing evidence that extinction and aerosol optical depth spectra in the ambient atmosphere exhibit curvature that is not fully captured by a power law (e.g., King and Byrne, 1976; King et al, 1978; Kaufman, 1993; Reid et al, 1999; Eck et al, 1999, 2001a, b, 2003a, b; O’Neill et al, 2001; Schuster et al, 2006; Kaskaoutis et al, 2010, 2011; Rao and Niranjan, 2012) This wavelength dependence of the aerosol extinction is thought to be driven primarily by the particle size distribution with only a minor contribution from the compositionally dependent aerosol absorption (Eck et al, 2001b; Schuster et al, 2006). This motivates the incorporation of recently developed, advanced instruments for measuring in situ, hyperspectral aerosol extinction into field campaigns that study the ambient atmosphere

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