Abstract

Abstract. Mixed-phase clouds are frequently observed in high-latitude regions and have important impacts on the surface energy budget and regional climate. Marine organic aerosol (MOA), a natural source of aerosol emitted over ∼ 70 % of Earth's surface, may significantly modify the properties and radiative forcing of mixed-phase clouds. However, the relative importance of MOA as a source of ice-nucleating particles (INPs) in comparison to mineral dust, and MOA's effects as cloud condensation nuclei (CCN) and INPs on mixed-phase clouds are still open questions. In this study, we implement MOA as a new aerosol species into the Community Atmosphere Model version 6 (CAM6), the atmosphere component of the Community Earth System Model version 2 (CESM2), and allow the treatment of aerosol–cloud interactions of MOA via droplet activation and ice nucleation. CAM6 reproduces observed seasonal cycles of marine organic matter at Mace Head and Amsterdam Island when the MOA fraction of sea spray aerosol in the model is assumed to depend on sea spray biology but fails when this fraction is assumed to be constant. Model results indicate that marine INPs dominate primary ice nucleation below 400 hPa over the Southern Ocean and Arctic boundary layer, while dust INPs are more abundant elsewhere. By acting as CCN, MOA exerts a shortwave cloud forcing change of −2.78 W m−2 over the Southern Ocean in the austral summer. By acting as INPs, MOA enhances the longwave cloud forcing by 0.35 W m−2 over the Southern Ocean in the austral winter. The annual global mean net cloud forcing changes due to CCN and INPs of MOA are −0.35 and 0.016 W m−2, respectively. These findings highlight the vital importance for Earth system models to consider MOA as an important aerosol species for the interactions of biogeochemistry, hydrological cycle, and climate change.

Highlights

  • Ice crystals in clouds play a critical role in determining cloud phase, lifetime, electrification, and radiative properties

  • Given that a realistic representation of marine organic aerosol (MOA) emissions is a prerequisite for models to quantify its influence on ice nucleation, we evaluate three different MOA emission parameterizations

  • This study introduces MOA into Community Atmosphere Model version 6 (CAM6) as a new aerosol species and treats the chemistry, advection, and wet or dry deposition of MOA in the model

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Summary

Introduction

Ice crystals in clouds play a critical role in determining cloud phase, lifetime, electrification, and radiative properties. Cloud ice influences precipitation and cloud radiative forcing. To quantify the impact of ice crystals on the hydrologic cycle and energy budget of the Earth system, it is important to advance the process-based understanding of initiation and evolution of ice particles. Ice particles can be initialized by homogeneous freezing or by heterogeneous nucleation. Homogeneous freezing of cloud droplets and aerosol solution droplets happens when air temperature is below approximately −38 ◦C. In mixed-phase clouds in which air temperature is between −38 and 0 ◦C, ice is initialized only by heterogeneous nucleation on ice-nucleating particles (INPs) (Vali et al, 2015)

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