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  1. 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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  2. Abstract. In situ measurements in the climatically important upper troposphere–lower stratosphere (UTLS) are critical for understanding controls on cloud formation, the entry of water into the stratosphere, and hydration–dehydration of the tropical tropopause layer.Accurate in situ measurement of water vapor in the UTLS however is difficult because of low water vapor concentrations (<5 ppmv) and a challenging low temperature–pressure environment.The StratoClim campaign out of Kathmandu, Nepal, in July and August 2017, which made the first high-altitude aircraft measurements in the Asian Summer Monsoon (ASM), also provided an opportunity to intercompare three in situ hygrometers mounted on the M-55 Geophysica: ChiWIS (Chicago Water Isotope Spectrometer), FISH (Fast In situ Stratospheric Hygrometer), and FLASH (Fluorescent Lyman-α Stratospheric Hygrometer).Instrument agreement was very good, suggesting no intrinsic technique-dependent biases: ChiWIS measures by mid-infrared laser absorption spectroscopy and FISH and FLASH by Lyman-α induced fluorescence.In clear-sky UTLS conditions (H2O<10 ppmv), mean and standard deviations of differences in paired observations between ChiWIS and FLASH were only (-1.4±5.9) % and those between FISH and FLASH only (-1.5±8.0) %.Agreement between ChiWIS and FLASH for in-cloud conditions is even tighter, at (+0.7±7.6) %.Estimated realized instrumental precision in UTLS conditions was 0.05, 0.2, and 0.1 ppmv for ChiWIS, FLASH, and FISH, respectively.This level of accuracy and precision allows the confident detection of fine-scale spatial structures in UTLS water vapor required for understanding the role of convection and the ASM in the stratospheric water vapor budget. 
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  3. null (Ed.)
    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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