Abstract. Ice growth from vapor deposition is an important process for the evolution of cirrus clouds, but the physics of depositional ice growth at the low temperatures (<235 K) characteristic of the upper troposphere and lower stratosphere is not well understood. Surface attachment kinetics, generally parameterized as a deposition coefficient αD, control ice crystal habit and also may limit growth rates in certain cases, but significant discrepancies between experimental measurements have not been satisfactorily explained. Experiments on single ice crystals have previously indicated the deposition coefficient is a function of temperature and supersaturation, consistent with growth mechanisms controlled by the crystal's surface characteristics. Here we use observations from cloud chamber experiments in the Aerosol Interactions and Dynamics in theAtmosphere (AIDA) aerosol and cloud chamber to evaluate surface kinetic models in realistic cirrus conditions. These experiments have rapidly changing temperature, pressure, and ice supersaturation such that depositional ice growth may evolve from diffusion limited to surface kinetics limited over the course of a single experiment. In Part 1, we describe the adaptation of a Lagrangian parcel model with the Diffusion Surface Kinetics Ice Crystal Evolution (DiSKICE) model (Zhang and Harrington, 2014) to the AIDA chamber experiments. We compare the observed ice water content and saturation ratios to that derived under varying assumptions for ice surface growth mechanisms for experiments simulating ice clouds between 180 and 235 K and pressures between 150 and 300 hPa. We found that both heterogeneous and homogeneous nucleation experiments at higher temperatures (>205 K) could generally be modeled consistently with either a constant deposition coefficient or the DiSKICE model assuming growth on isometric crystals via abundant surface dislocations. Lower-temperature experiments showed more significant deviations from any depositional growth model, with different ice growth rates for heterogeneous and homogeneous nucleation experiments.
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No anomalous supersaturation in ultracold cirrus laboratory experiments
Abstract. High-altitude cirrus clouds are climatically important: their formationfreeze-dries air ascending to the stratosphere to its final value, and theirradiative impact is disproportionately large. However, their formation andgrowth are not fully understood, and multiple in situ aircraft campaigns haveobserved frequent and persistent apparent water vapor supersaturations of5 %–25 % in ultracold cirrus (T<205 K), even in the presence of iceparticles. A variety of explanations for these observations have been putforth, including that ultracold cirrus are dominated by metastable ice whosevapor pressure exceeds that of hexagonal ice. The 2013 IsoCloud campaign atthe Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud andaerosol chamber allowed explicit testing of cirrus formation dynamics atthese low temperatures. A series of 28 experiments allows robust estimationof the saturation vapor pressure over ice for temperatures between 189 and235 K, with a variety of ice nucleating particles. Experiments are rapidenough (∼10 min) to allow detection of any metastable ice that mayform, as the timescale for annealing to hexagonal ice is hours or longer overthe whole experimental temperature range. We show that in all experiments,saturation vapor pressures are fully consistent with expected values forhexagonal ice and inconsistent with the highest values postulated formetastable ice, with no temperature-dependent deviations from expectedsaturation vapor pressure. If metastable ice forms in ultracold cirrusclouds, it appears to have a vapor pressure indistinguishable from that ofhexagonal ice to within about 4.5 %.
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- Award ID(s):
- 1743753
- NSF-PAR ID:
- 10284991
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 20
- Issue:
- 2
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 1089 to 1103
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Cirrus ice crystals are produced heterogeneously on ice‐nucleating particles (INPs) and homogeneously in supercooled liquid solution droplets. They grow by uptake of water molecules from the ice‐supersaturated vapor. The precursor particles, characterized by disparate ice nucleation abilities and number concentrations, compete for available vapor during ice formation events. We investigate cirrus formation events systematically in different temperature and updraft regimes, and for different INP number concentrations and time‐independent nucleation efficiencies. We consider vertical air motion variability due to mesoscale gravity waves and effects of supersaturation‐dependent deposition coefficients for water molecules on ice surfaces. We analyze ice crystal properties to better understand the dynamics of competing nucleation processes. We study the reduction of ice crystal numbers produced by homogeneous freezing due to INPs in both, individual simulations assuming constant updraft speeds and in ensemble simulations based on a stochastic representation of vertical wind speed fluctuations. We simulate and interpret probability distributions of total nucleated ice crystal number concentrations, showing signatures of homogeneous and heterogeneous nucleation. At typically observed, mean updraft speeds (≈15 cm s−1) competing nucleation should occur frequently, even at rather low INP number concentrations (<10 L−1). INPs increase cirrus occurrence and may alter cirrus microphysical properties without entirely suppressing homogeneous freezing events. We suggest to improve ice growth models, especially for low cirrus temperatures (<220 K) and low ice supersaturation (<0.3).
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Abstract This study investigates the evolution of temperature and lifetime of evaporating, supercooled cloud droplets considering initial droplet radius (
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-20-1089-2020
