Abstract. The microphysical and radiative properties of cirrus clouds continue to be beyond understanding and thus still represent one of the largest uncertainties in the prediction of the Earth's climate (IPCC, 2013). Our study aims to provide a guide to cirrus microphysics, which is compiled from an extensive set of model simulations, covering the broad range of atmospheric conditions for cirrus formation and evolution. The model results are portrayed in the same parameter space as field measurements, i.e., in the Ice Water ContentTemperature (IWC-T) parameter space. We validate this cirrus analysis approach by evaluating cirrus data sets from 17 aircraft campaigns, conducted in the last 15 years, spending about 94 h in cirrus over Europe, Australia, Brazil as well as South and North America. Altogether, the approach of this study is to track cirrus IWC development with temperature by means of model simulations, compare with observations and then assign, to a certain degree, cirrus microphysics to the observations. Indeed, the field observations show characteristics expected from the simulated Cirrus Guide. For example, high (low) IWCs are found together with high (low) ice crystal concentrations N ice .An important finding from our study is the classification of two types of cirrus with differing formation mechanisms and microphysical properties: the first cirrus type forms directly as ice (in situ origin cirrus) and splits in two subclasses, depending on the prevailing strength of the updraft: in slow updrafts these cirrus are rather thin with lower IWCs, while in fast updrafts thicker cirrus with higher IWCs can form. The second type consists predominantly of thick cirrus originating from mixed phase clouds (i.e., via freezing of liquid droplets -liquid origin cirrus), which are completely glaciated while lifting to the cirrus formation temperature region (< 235 K). In the European field campaigns, slow updraft in situ origin cirrus occur frequently in low-and high-pressure systems, while fast updraft in situ cirrus appear in conjunction with jet streams or gravity waves. Also, liquid origin cirrus mostly related to warm conveyor belts are found. In the US and tropical campaigns, thick liquid origin cirrus which are formed in large convective systems are detected more frequently.

Simultaneous in situ measurements of the concentrations of OH, HO(2), ClO, BrO, NO, and NO(2) demonstrate the predominance of odd-hydrogen and halogen free-radical catalysis in determining the rate of removal of ozone in the lower stratosphere during May 1993. A single catalytic cycle, in which the rate-limiting step is the reaction of HO(2) with ozone, accounted for nearly one-half of the total O(3) removal in this region of the atmosphere. Halogen-radical chemistry was responsible for approximately one-third of the photochemical removal of O(3); reactions involving BrO account for one-half of this loss. Catalytic destruction by NO(2), which for two decades was considered to be the predominant loss process, accounted for less than 20 percent of the O(3) removal. The measurements demonstrate quantitatively the coupling that exists between the radical families. The concentrations of HO(2) and ClO are inversely correlated with those of NO and NO(2). The direct determination of the relative importance of the catalytic loss processes, combined with a demonstration of the reactions linking the hydrogen, halogen, and nitrogen radical concentrations, shows that in the air sampled the rate of O(3) removal was inversely correlated with total NOx, loading.

Abstract. The radiative role of ice clouds in the atmosphere is known to be important, but uncertainties remain concerning the magnitude and net effects. However, through measurements of the microphysical properties of cirrus clouds, we can better characterize them, which can ultimately allow for their radiative properties to be more accurately ascertained. Recently, two types of cirrus clouds differing by formation mechanism and microphysical properties have been classified -in situ and liquid origin cirrus. In this study, we present observational evidence to show that two distinct types of cirrus do exist. Airborne, in situ measurements of cloud ice water content (IWC), ice crystal concentration (N ice ), and ice crystal size from the 2014 ML-CIRRUS campaign provide cloud samples that have been divided according to their origin type. The key features that set liquid origin cirrus apart from the in situ origin cirrus are higher frequencies of high IWC ( > 100 ppmv), higher N ice values, and larger ice crystals. A vertical distribution of N ice shows that the in situ origin cirrus clouds exhibit a median value of around 0.1 cm −3 , while the liquid origin concentrations are slightly, but notably higher. The median sizes of the crystals contributing the most mass are less than 200 µm for in situ origin cirrus, with some of the largest crystals reaching 550 µm in size. The liquid origin cirrus, on the other hand, were observed to have median diameters greater than 200 µm, and crystals that were up to 750 µm. An examination of these characteristics in relation to each other and their relationship to temperature provides strong evidence that these differences arise from the dynamics and conditions in which the ice crystals formed. Additionally, the existence of these two groups in cirrus cloud populations may explain why a bimodal distribution in the IWC-temperature relationship has been observed. We hypothesize that the low IWC mode is the result of in situ origin cirrus and the high IWC mode is the result of liquid origin cirrus.