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The Asian Summer Monsoon (ASM) convection transports aerosols and their precursors from the boundary layer to the upper troposphere and lower stratosphere (UTLS). This process forms an annually recurring aerosol layer near the tropopause. Recent observations have revealed a distinct property of the aerosol layer over the ASM region, it is nitrate‐rich. We present a newly implemented aerosol formation algorithm that enhances the representation of nitrate aerosol in the Community Aerosol and Radiation Model for Atmospheres (CARMA) coupled with the Community Earth System Model (CESM). The simulated aerosol chemical composition, as well as vertical distributions of aerosol size and mass, are evaluated using in situ and remote sensing observations. The simulated concentrations (ammonium, nitrate, and sulfate) and size distributions are generally within the error bars of data. We find nitrate, organics, and sulfate contribute significantly to the UTLS aerosol concentration between 15°–45°N and 0°–160°E. The two key formation mechanisms of nitrate‐containing aerosols in the ATAL are ammonium neutralization to form ammonium nitrate in regions where convection is active, and condensation of nitric acid in regions of cold temperature. Furthermore, including nitrate formation in the model doubles the surface area density in the tropical tropopause region between 15°–45°N and 0°–160°E, which alters the chlorine partitioning and subsequently impacts the rate of ozone depletion. Plain Language Summary: The Asian Summer Monsoon can efficiently transport pollutants into the upper troposphere and form a layer of aerosols called the Asian Tropopause Aerosol Layer (ATAL). This research investigates the two key formation mechanisms for nitrate aerosol in the ATAL: one is due to cold temperature, and one is due to ammonium neutralization. The simulations are validated against in situ measurements. It also found that O3 chemistry inside ATAL is influenced by nitrate aerosol. Key Points: A new nitrate aerosol formation algorithm is implemented for the community model CARMA to represent the Asian Tropopause Aerosol LayerThe simulated aerosol size distributions and compositions are within error bars of observationsIncluding the new nitrate formation scheme doubles the simulated surface area, changing the chlorine partitioning and ozone depletion [ABSTRACT FROM AUTHOR]

Aviation is a rapidly growing source of climate forcing, and the non-CO2 effective radiative forcing of aviation is approximately twice that of aviation CO2. However, considerable uncertainty remains regarding aviation's non-CO2 effects because the radiative forcing of aviation aerosol-cloud interactions, especially with cirrus clouds, is poorly known. Here, we use a large eddy simulation model to quantify the impact of ice crystal number concentration (ICNC) perturbations on the water budget and microphysics of pre-existing cirrus clouds. These perturbations aim to represent the second half of the chain of effects linking aircraft aerosol emissions to changes in ICNC and ice water path. We examine two types of cirrus: warm conveyor belt outflow and gravity wave cirrus, which represent different updraft regimes and formation mechanisms. In both cases, the primary effect of an idealised increase in ICNC is to extend cloud lifetime, with the increase proportional to the magnitude of the ICNC perturbation applied. The effect is more pronounced in the gravity wave cirrus case than in the warm conveyor belt outflow cirrus case because the latter has lower initial ICNC and ice water contents. Quantitatively, the sensitivity of ice water path (IWP) to changes in ICNC, expressed as ∆ln(IWP)/∆ln(ICNC), is 0.06 for gravity wave cirrus and 0.35 for warm conveyor belt outflow cirrus when calculated 45 minutes after imposing the ICNC perturbation. These results suggest that aviation has the potential to increase the lifetime and radiative effects of pre-existing cirrus clouds. [ABSTRACT FROM AUTHOR]

The cloud particle size distribution (PSD) is a key parameter for the retrieval of microphysical and optical properties from remote-sensing instruments, which in turn are necessary for determining the radiative effect of clouds. Current representations of PSDs for ice clouds rely on parameterizations that were largely based on aircraft in situ measurements where the distribution of small ice crystals were uncertain. This makes current parameterizations deficient to simulate remote-sensing observations sensitive to small ice, such as from lidar and thermal infrared instruments. In this study we fit the in situ PSDs of ice crystals from the JULIA (JÜLich In situ Aircraft data set) database, which consists of 11 campaigns covering the tropics, midlatitudes and the Arctic, consistently processed and considered more robust in their measurements of small ice. For the fitting, we implement an established approach to PSD parameterizations, which consists of finding an adequate set of parameters for a modified gamma function after normalization of both PSD axes. These parameters are constrained to match in situ measurements when predicting microphysical properties from the PSDs, via a cost function minimization method. We selected the ice water content and the ice crystal number concentration, which are currently key parameters for modern satellite retrievals and model microphysics schemes. We found that a bimodal parameterization yields better results than a monomodal one. The bimodal parameterization has a lower spread for almost all ice crystal sizes over the entire range of analyzed temperatures and fits better the observations, especially for particles between 20 and about 110 µ m at temperatures between -60 and -20 ∘ C. For this temperature range, the root mean square error for the retrieved Nice is reduced from 0.36 to 0.20. This demonstrates a clear advantage to considering the bimodality of PSDs, e.g., for satellite retrievals. [ABSTRACT FROM AUTHOR]

Despite their proven importance for the atmospheric radiative energy budget, the effect of cirrus on climate and the magnitude of their modification by human activity is not well quantified. Besides anthropogenic pollution sources on the ground, aviation has a large local effect on cirrus microphysical and radiative properties via the formation of contrails and their transition to contrail cirrus. To investigate the anthropogenic influence on natural cirrus, we compare the microphysical properties of cirrus measured at mid-latitude (ML) regions (<60 ∘ N) that are often affected by aviation and pollution with cirrus measured in the same season in comparatively pristine high latitudes (HLs; ≥60 ∘ N). The number concentration, effective diameter, and ice water content of the observed cirrus are derived from in situ measurements covering ice crystal sizes between 2 and 6400 µm collected during the CIRRUS-HL campaign (Cirrus in High Latitudes) in June and July 2021. We analyse the dependence of cirrus microphysical properties on altitude and latitude and demonstrate that the median ice number concentration is an order of magnitude larger in the measured mid-latitude cirrus, with 0.0086 cm-3 , compared to the high-latitude cirrus, with 0.001 cm-3. Ice crystals in mid-latitude cirrus are on average smaller than in high-latitude cirrus, with a median effective diameter of 165 µm compared to 210 µm , and the median ice water content in mid-latitude cirrus is higher (0.0033 gm-3) than in high-latitude cirrus (0.0019 gm-3). In order to investigate the cirrus properties in relation to the region of formation, we combine the airborne observations with 10 d backward trajectories to identify the location of cirrus formation and the cirrus type, i.e. in situ or liquid origin cirrus, depending on whether there is only ice or also liquid water present in the cirrus history, respectively. The cirrus formed and measured at mid-latitudes (M–M) have a particularly high ice number concentration and low effective diameter. This is very likely a signature of contrails and contrail cirrus, which is often observed in the in situ origin cirrus type. In contrast, the largest effective diameter and lowest number concentration were found in the cirrus formed and measured at high latitudes (H–H) along with the highest relative humidity over ice (RHi). On average, in-cloud RHi was above saturation in all cirrus. While most of the H–H cirrus were of an in situ origin, the cirrus formed at mid-latitudes and measured at high latitudes (M–H) were mainly of liquid origin. A pristine Arctic background atmosphere with relatively low ice nuclei availability and the extended growth of few nucleated ice crystals may explain the observed RHi and size distributions. The M–H cirrus are a mixture of the properties of M–M and H–H cirrus (preserving some of the initial properties acquired at mid-latitudes and transforming under Arctic atmospheric conditions). Our analyses indicate that part of the cirrus found at high latitudes is actually formed at mid-latitudes and therefore affected by mid-latitude air masses, which have a greater anthropogenic influence. [ABSTRACT FROM AUTHOR]

During the StratoClim Geophysica campaign, air with total water mixing ratios up to 200 ppmv and ozone up to 250 ppbv was observed within the Asian summer monsoon anticyclone up to 1.7 km above the local cold-point tropopause (CPT). To investigate the temporal evolution of enhanced water vapor being transported into the stratosphere, we conduct forward trajectory simulations using both a microphysical and an idealized freeze-drying model. The models are initialized at the measurement locations and the evolution of water vapor and ice is compared with satellite observations of MLS and CALIPSO. Our results show that these extremely high water vapor values observed above the CPT are very likely to undergo significant further freeze-drying due to experiencing extremely cold temperatures while circulating in the anticyclonic "dehydration carousel". We also use the Lagrangian dry point (LDP) of the merged back-and-forward trajectories to reconstruct the water vapor fields. The results show that the extremely high water vapor mixed with the stratospheric air has a negligible impact on the overall water vapor budget. The LDP mixing ratios are a better proxy for the large-scale water vapor distributions in the stratosphere during this period. [ABSTRACT FROM AUTHOR]

Aviation has a large impact on the Earth's atmosphere and climate by various processes. Line-shaped contrails and contrail cirrus clouds lead to changes in the natural cirrus cloud cover and have a major contribution to the effective radiative forcing from aviation. In addition, aviation-induced aerosols might also change the microphysical properties and optical properties of naturally formed cirrus clouds. Latter aerosol–cloud interactions show large differences in the resulting effective radiative forcing, and our understanding on how aviation-induced aerosols affect cirrus cloud properties is still poor. Up to now, observations of this aviation-induced aerosol effect have been rare. In this study, we use combined airborne lidar and in situ ice cloud measurements to investigate differences in the microphysical and optical properties of naturally formed cirrus clouds, which formed in regions that are highly affected by aviation-induced aerosol emissions and, of those, which formed in regions rather unaffected by aviation. Urbanek et al. (2018) showed that those cirrus clouds, which are more affected by aviation-induced soot emission, are characterized by larger values of the particle linear depolarization ratio (PLDR). In this follow-on study we relate collocated lidar measurements performed aboard HALO during the ML-CIRRUS mission of the particle linear depolarization ratio with in situ cloud probe measurements of the number concentration and effective diameter of the ice particles. In situ measurements for both cloud types (high-PLDR-mode – aviation-affected – and low-PLDR-mode – pristine – cirrus) can be reliably compared in a temperature range between 210 and 215 K. Within this temperature range we find that high-PLDR-mode cirrus clouds tend to show larger effective ice particle diameters with a median value of 61.4 compared to 50.7 µ m for low-PLDR-mode pristine cirrus clouds. Larger effective ice particles in aviation-influenced (high-PLDR-mode) cirrus are connected to lower ice particle number concentration with a median value of 0.05 compared to 0.11 cm -3 (low-PLDR-mode), which evolved in more pristine regions with only little impact from aviation. We suspect that a suppression of homogeneous ice formation by the heterogeneously freezing soot aerosol particles included in the areas affected by air traffic is the cause of the reduced ice crystal concentrations. [ABSTRACT FROM AUTHOR]

The cloud particle size distribution (PSD) is a key parameter for the retrieval of micro-physical and optical properties from remote sensing instruments, which in turn are necessary for determining the radiative effect of clouds. Current representations of PSDs for ice clouds rely on parameterizations that were largely based on in situ measurements where the distribution of small ice crystals were uncertain. This makes current parameterizations deficient to simulate remote sensing observations sensitive to small ice, such as from lidar and thermal infrared instruments. In this study we fit the in situ PSDs of ice crystals from the JULIA (JÜLich In situ Aircraft data set) database, which consists of 11 campaigns covering the tropics, mid-latitudes and the Arctic, consistently processes and considered more robust in their measurements of small ice. For the fitting, we implement an established approach to PSD parameterizations, which consists in finding an adequate set of parameters for a modified gamma function after normalization of both PSD axes. These parameters are constrained to match in-situ mea surements when predicting microphysical properties from the PSDs, via a cost function minimization method. We selected the ice water content and the ice crystal number concentration, which are currently key parameters for modern satellite retrievals and model microphysics schemes. We found that a bimodal parameterization yields better results than a monomodal one. The bimodal parameterization has a lower spread for almost all ice crystal sizes over the entire range of analyzed temperatures and fits better the observations, especially for particles between 20 and about 110 μm at temperatures between −60 and −20 °C. For this temperature range, the root mean square error for the retrieved Nice is reduced from 0.36 to 0.20. This demonstrates a clear advantage to considering the bimodality of PSDs, e.g. for satellite retrievals. [ABSTRACT FROM AUTHOR]

Despite their proven significance for the atmospheric radiative energy budget, the effect of cirrus on climate and the magnitude of their modification by human activity is not well quantified. Besides anthropogenic pollution sources on the ground, aviation has a large local effect on cirrus microphysical and radiative properties via the formation of contrails and their transition to contrail cirrus. To investigate the anthropogenic influence on natural cirrus, we compare the microphysical properties of cirrus measured at mid-latitude regions (ML, < 60° N) that are often affected by aviation and pollution with cirrus measured in the same season in comparatively pristine high latitudes (HL, ≥ 60° N). The number concentration, effective diameter, and ice water content of the observed cirrus are derived from in situ measurements covering ice crystal sizes between between 2 and 6400 µm collected during the CIRRUS-HL campaign (CIRRUS in High Latitudes) in June and July 2021. We analyse the dependence of cirrus microphysical properties on altitude and latitude and demonstrate that the median ice number concentration is by an order of magnitude larger in the measured mid-latitude cirrus with 0.0086 cm-3 compared to 0.001 cm-3 in high-latitude cirrus. Ice crystals in mid-latitude cirrus are on average smaller than in high-latitude cirrus, with a median effective diameter of 165 µm compared to 210 µm and the median ice water content in mid-latitude cirrus is higher (0.0033 g m-3) than in high-latitude cirrus (0.0019 g m-3). In order to investigate the cirrus properties in relation to the region of formation, we combine the airborne observations with 10-day backward trajectories to identify the location of cirrus formation and the cirrus type: in situ or liquid origin cirrus, depending on whether there is only ice or also liquid water present in the cirrus history, respectively. The cirrus formed and measured at mid-latitudes (M-M) have particularly high ice number concentration and low effective diameter. This is very likely a signature of contrails and contrail cirrus, which is often observed in the in situ origin cirrus type. In contrast, the largest effective diameter and lowest number concentration were found in the cirrus formed and measured at high latitudes (H-H) along with the highest relative humidity over ice (RHi). On average, in-cloud RHi was above saturation in all cirrus. While most of the H-H cirrus were of in situ origin, the cirrus formed at mid-latitudes and measured at high latitudes (M-H) were mainly of liquid origin. A pristine Arctic background atmosphere with scarce availability of ice nuclei and the extended growth of few nucleated ice crystals may explain the observed RHi and size distributions. The M-H cirrus are a mixture of the properties of M-M and H-H cirrus (preserving some of the initial properties acquired at mid-latitudes and transforming under Arctic atmospheric conditions). Our analyses indicate that part of the cirrus found at high latitudes are actually formed at mid-latitudes, and therefore affected by mid-latitude air masses, which have a greater anthropogenic influence. [ABSTRACT FROM AUTHOR]