The effect of hygroscopicity on eddy covariance estimates of sea-spray aerosol fluxes: a comparison of high-rate and bulk correction methods

The eddy covariance technique is the most direct of the methods that have been used to measure the flux of sea-spray aerosol between the ocean and atmosphere, but has been applied in only a handful of studies. However, unless the aerosol is dried before the eddy covariance measurements are made, the hygroscopic nature of sea-spray may combine with a relative humidity flux to result in a bias in the calculated aerosol flux. "Bulk" methods have been presented to account for this bias, however, they rely on assumptions of the shape of the aerosol spectra which may not be valid for near-surface measurements of sea-spray. Here we describe a method of correcting aerosol spectra for relative humidity induced size variations at the high frequency (10 Hz) measurement timescale, where counting statistics are poor and the spectral shape cannot be well represented by a simple power law. Such a correction allows the effects of hygroscopicity and relative humidity flux on the aerosol flux to be explicitly evaluated and compared to the bulk corrections, both in their original form and once reformulated to better represent the measured mean aerosol spectra. In general, the bulk corrections - particularly when reformulated for the measured mean aerosol spectra - perform relatively well, producing flux corrections of the right sign and approximate magnitude. However, there are times when the bulk methods either significantly over- or underestimate the required flux correction. We conclude that, where possible, relative humidity corrections should be made at the measurement frequency.