Abstract. Upper tropospheric observations outside and inside of cirrus clouds indicate water vapour mixing ratios sometimes exceeding water saturation. Relative humidities over ice (RH ice ) of up to and more than 200% have been reported from aircraft and balloon measurements in recent years.From these observations a lively discussion continues on whether there is a lack of understanding of ice cloud microphysics or whether the water measurements are tainted with large uncertainties or flaws.Here, RH ice in clear air and in ice clouds is investigated. Strict quality-checked aircraft in situ observations of RH ice were performed during 28 flights in tropical, mid-latitude and Arctic field experiments in the temperature range 183-240 K. In our field measurements, no supersaturations above water saturation are found. Nevertheless, super-or subsaturations inside of cirrus are frequently observed at low temperatures (<205 K) in our field data set. To explain persistent RH ice deviating from saturation, we analysed the number densities of ice crystals recorded during 20 flights. From the combined analysis -using conventional microphysics -of supersaturations and ice crystal numbers, we show that the high, persistent supersaturations observed inside of cirrus can possibly be explained by unexpected, frequent very low ice crystal numbers that could scarcely be caused by homogeneous ice nucleation. Heterogeneous ice formation or the suppression of freezing might better explain the observed ice crystal numbers.Correspondence to: M. Krämer (m.kraemer@fz-juelich.de) Thus, our lack of understanding of the high supersaturations, with implications for the microphysical and radiative properties of cirrus, the vertical redistribution of water and climate, is traced back to the understanding of the freezing process at low temperatures.

Supersaturations, microphysics and nitric acid partitioning in a very cold subvisible tropical cirrus cloud observed on 2 February 2006, during the field campaign CR-AVE, are studied by comparing a simulated set of possible cloud development scenarios with the in situ observations. The scenario that best matches the observations is a cirrus cloud forming by heterogeneous freezing of a small number of ice nuclei with subsequent unimpeded mass accommodation of water on ice. Variation of the freezing process, the accommodation coefficient or the amount of available water leads to simulated clouds that differ microphysically from the observed cloud in important respects. In particular, the simulations suggest that heterogeneous ice nucleation or another freezing mechanism producing only a low number of ice crystals could be an important process for cold cirrus cloud formation, possibly explaining the frequent observations of high supersaturations inside the cirrus cloud in this temperature regime.

Abstract. Upper tropospheric observations outside and inside of cirrus clouds of water vapour mixing ratios sometimes exceeding water saturation, yielding up to more than 200% relative humidities over ice (RHice) have been reported from aircraft and balloon measurements in recent years. From these observations a lively continuous discussion arose on whether there is a lack of understanding of ice cloud microphysics or if the water measurements are tainted with large uncertainties or flaws. Here, RHice in clear air and in ice clouds is investigated: strictly quality checked aircraft in-situ observations of RHice were performed during 28 flights in tropical, mid-latitude and Arctic field experiments in the temperature range 183–250 K. In our field measurements, no supersaturations above water saturation are found. Nevertheless, super- or subsaturations inside of cirrus are frequently observed at low temperatures (<205 K) in our field data set. To explain persistent RHice deviating from saturation, we analysed the number densities of ice crystals recorded during 20 flights. From the combined analysis – using conventional microphysics – of supersaturations and ice crystal numbers, we show that the high, persistent supersaturations observed inside of cirrus are caused by unexpected, frequent very low ice crystal numbers that could hardly be explained by homogeneous ice nucleation. Heterogeneous ice formation or the suppression of freezing might better explain the observed ice crystal numbers. Thus, our lack of understanding of the high supersaturations with implications to the microphysical and radiative properties of cirrus, the vertical redistribution of water and climate, is traced back to the understanding of the freezing process at low temperatures.

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A new method for stable carbon isotope ratio analysis of anhydrosugars from biomass burning aerosol particle source filter samples was developed by employing Thermal Desorption--2 Dimensional Gas Chromatography--Isotope Ratio Mass Spectrometry (TD-2DGC-IRMS). Compound specific isotopic measurements of levoglucosan, mannosan, and galactosan performed by TD-2DGC-IRMS in a standard mixture show good agreement with isotopic measurements of the bulk anhydrosugars, carried out by Elemental Analyzer--Isotope Ratio Mass Spectrometry (EA-IRMS). The established method was applied to determine the isotope ratios of levoglucosan, mannosan, and galactosan from source samples collected during combustion of hard wood, softwood, and crop residues. δ(13)C values of levoglucosan were found to vary between -25.6 and -22.2‰, being higher in the case of softwood. Mannosan and galactosan were detected only in the softwood samples showing isotope ratios of -23.5‰ (mannosan) and -25.7‰ (galactosan). The isotopic composition of holocellulose in the plant material used for combustion experiments was determined with δ(13)C values between -28.5 and -23.7‰. The difference in δ(13)C of levoglucosan in biomass burning aerosol particles compared to the parent fuel holocellulose was found to be -1.89 (±0.37)‰ for the investigated biomass fuels. Compound specific δ(13)C measurements of anhydrosugars should contribute to an improved source apportionment.