Abstract. Plant canopies are an important source of biological particles aerosolized into the atmosphere. Certain aerosolized microorganisms are able to freeze slightly supercooled cloud droplets and therefore affect mixed-phase cloud development. Still, spatiotemporal variability of such biological ice-nucleating particles (INPs) is currently poorly understood. Here, we study this variability between late summer and leaf shedding on the scale of individual leaves collected about fortnightly from four temperate broadleaf tree species (Fagus sylvatica, Juglans regia, Prunus avium and Tilia platyphyllos) on a hillside (Gempen, 650 m a.s.l. (metres above sea level)) and in a vertical canopy profile of one Fagus sylvatica (Hölstein, 550 m a.s.l.) in north-western Switzerland. The cumulative concentration of INPs active at ≥-10 °C (INPs−10) did not vary significantly between the investigated tree species but, as inferred from leaf mass per area and leaf carbon isotopic ratios, seemed to be lower on sun leaves as compared with shade leaves. Between August and mid-November, the median INP concentration increased from 4 to 38 INP−10 cm−2 of leaf area and was positively correlated with mean relative humidity throughout 24 h prior to sampling (Spearman's r=0.52, p<0.0001, n=64). In 53 of the total 64 samples collected at the Gempen site, differential INP spectra between −3 and −10 °C exhibited clearly discriminable patterns: in 53 % of the spectra, the number of additionally activated INPs increased persistently with each 1 °C decrease in temperature; the remaining spectra displayed significant peaks in differential INP concentration above −9 °C, most frequently in the temperature interval between −8 and −9 °C (21 %) and between −7 and −8 °C (17 %). Interestingly, the three most frequent patterns in differential INP spectra on leaves in Gempen were also prevalent in similar fractions in air samples with clearly discriminable patterns at the high-altitude Jungfraujoch site (3580 m a.s.l., Switzerland) collected during summer in the previous year. These findings corroborate the idea that a large fraction of the airborne biological INP population above the Alps during summer originates from plant surfaces. Which parameter or set of parameters could affect biological INP populations on both scales – upwind airsheds of high-altitude sites as well as individual leaves – is an intriguing question for further exploration. A first guess is that leaf wetness duration plays a role.
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