Abstract

Abstract. Determining the dominant ice nucleation mode in cirrus is still an open research question that impacts the ability to assess the climate impact of these clouds in numerical models. Homogeneous nucleation is generally well understood. More uncertainty surrounds heterogeneous nucleation due to a weaker understanding of the complex physio-chemical properties (e.g., ice nucleation efficiency and atmospheric abundance) of ice nucleating particles (INPs). This hampers efforts to simulate their interactions with cirrus, which is crucial in order to assess the effect these clouds have on the climate system. Kärcher and Marcolli (2021) introduced a new deterministic heterogeneous ice nucleation parameterization based on the differential activated fraction (AF), which describes the number of INPs that activate ice within a specified temperature or ice saturation ratio interval. They argued that this new approach with explicit INP budgeting, which removes INPs from the total population after they nucleate ice, could help to correct a potential overprediction of heterogeneous nucleation within cirrus when budgeting is not considered. We formulated a general circulation model (GCM)-compatible version of the differential AF parameterization for simulating only deposition nucleation within in situ cirrus and compared it to the method currently employed in the ECHAM6.3-HAM2.3 GCM that is based on cumulative AF. This default cumulative AF approach does not use explicit INP budgeting but instead implicitly budgets for INPs that nucleated ice using a differential ice crystal number concentration variable to calculate whether new ice formation should be added to the pre-existing concentration. In a series of box model simulations that were based on the cirrus sub-model from ECHAM, we found that the cumulative approach likely underpredicts heterogeneous nucleation in cirrus, as it does not account for interstitial INPs remaining from the previous GCM time step. However, as the cases that we simulated in the box model were rather extreme, we extended our analysis to compare the differential and cumulative AF approaches in two simulations in ECHAM-HAM. We find that choosing between these two approaches impacts ice nucleation competition within cirrus in our model. However, based on our 5-year simulations, the small and insignificant difference in the top-of-atmosphere radiative balance of 0.02±0.35 Wm−2 means that the overall climate impact is negligible. We argue that while our GCM-compatible differential AF parameterization is closer to first principles, the default approach based on cumulative AF is simpler due to the lack of additional tracers required. Finally, our new approach could be extended to assess the impact of explicit versus implicit INP budgeting on the ice crystal number concentration produced by immersion freezing of mineral dust particles, as this is also an important mechanism in cirrus.

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