Ship-borne observations of sea fog and rain chemistry over the North and South Pacific Ocean

Abstract

Clouds, fogs, and rain can serve as useful integrators of both atmospheric aerosols and soluble trace gases. To better understand the chemical characteristics of sea fog and rain in the North and South Pacific Ocean, fog and rain were measured aboard the R/V ARAON in 2012 and 2014, respectively, as part of the Ship-borne Pole-to-Pole Observations (SHIPPO) project. The mean sea fog pH (3.59) was lower than the mean rain pH (4.54), reflecting greater inputs of non-sea-salt (nss)-SO₄^2?. For the collected rain, nss-Ca²⁺ and nss-Mg²⁺ from mineral dust particles were the major contributors to acidity neutralization. NO₃^? concentrations, which are derived from scavenging of gaseous nitric acid and aerosol nitrate, were higher than NH₄⁺ concentrations, indicating that terrestrial and/or local anthropogenic NO₃^? sources outweighed contributions from anthropogenic or biological oceanic NH₃/NH₄⁺ sources. The ratio of Cl^?/Na⁺ in the sea fog was slightly lower than that in the sea water due to HCl volatilization from scavenged sea-salt particles. The ratio of NH₄⁺/ nss-Ca²⁺ was lower in the rain than in the sea fog, revealing the influence of mineral dust particles at altitudes above the sea fog layer. The average sea fog water TOC concentration, 13.2 ppmC, was much higher than the measured TOC concentrations in marine fogs and clouds in other remote environments, likely due to continental influence; the TN and TOC concentrations in the fog water were much higher than those in the rain. The sea fog and rain chemical properties measured during research cruises like these enhance our understanding of wet deposition and cloud condensation nuclei sources and processes in the Pacific Ocean.