Abstract

The reaction of sea salt (or biomass burning) particles with sulfuric acid and nitric acid leads to the displacement of chloride relative to sodium (or potassium). We have developed a new particle mass spectrometer to quantify non-refractory and refractory sulfate aerosols (referred to as refractory aerosol thermal desorption mass spectrometer: rTDMS). The combination of a graphite particle collector and a carbon dioxide laser enables high desorption temperature (up to 930 °C). Ion signals originating from evolved gas molecules are detected by a quadrupole mass spectrometer. Here we propose a new method to quantify the mass concentrations of sodium nitrate (NaNO3: SN), sodium chloride (NaCl: SC), sodium sulfate (Na2SO4: SS), potassium nitrate (KNO3: PN), potassium chloride (KCl: PC), and potassium sulfate (K2SO4 : PS) particles by using the rTDMS. Laboratory experiments were performed to test the sensitivities of the rTDMS to various types of particles. We measured ion signals originating from single-component particles for each compound, and found a good linearity (r2 > 0.8) between the major ion signals and mass loadings. We also measured ion signals originating from internally mixed SN + SC + SS (or PN + PC + PS) particles, and found that the temporal profiles of ion signals at m/z 23 (or 39) were characterized by three sequential peaks associated with the evolution of the desorption temperature. We tested potential interferences in the quantification of sea salt particles under real-world conditions by artificially generating "modified" sea salt particles from a mixture of diluted seawater and SS/SN solution. Based on these experimental results, the applicability of the rTDMS to ambient measurements of sea salt particles is discussed.

Highlights

  • IntroductionAerosols have large impacts on the Earth’s radiation budget by scattering and absorbing solar short-wave radiation

  • Aerosols have large impacts on the Earth’s radiation budget by scattering and absorbing solar short-wave radiation25 and by acting as cloud condensation nuclei (IPCC 2013)

  • We measured ion signals originating from internally mixed solution of NaNO3 (SN) + SC + SS particles, and found that the temporal profiles of ion signals at m/z 23 were characterized by three sequential peaks associated with the evolution of the desorption temperature

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Summary

Introduction

Aerosols have large impacts on the Earth’s radiation budget by scattering and absorbing solar short-wave radiation. 25 (direct effect) and by acting as cloud condensation nuclei (indirect effect) (IPCC 2013). The size and chemical composition of aerosol particles are important for quantitatively estimating the direct and indirect effects of aerosols. Aerosol particles emitted from sea spray and biomass burning make significant contributions to the global budget of aerosols. The reaction of sea salt (or biomass burning) particles with sulfuric acid (H2SO4) and nitric acid (HNO3) leads to the displacement of chloride relative to sodium (or potassium). Sea salt aerosols generally make the largest contribution to the budget of natural aerosols in the 30 troposphere (Seinfeld and Pandis, 2006; IPCC, 2013).

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