Temporal and vertical distributions of the occurrence of the cirrus clouds over the coastal station in the Indian monsoon region

Knowledge of the spatiotemporal coverage of the cirrus clouds is vital in quantifying the radiation budget of the earth-atmosphere system. In this paper, we present the diurnal and vertical distributions of the occurrence of the cirrus clouds during different seasons as well as its interannual variation over Kattankulathur (12.82° N, 80.04° E), east coast of the Bay of Bengal. The long-term (2016–2018) continuous observations of micropulse lidar (MPL) demonstrate the laminar and descending cirrus clouds that occur either as single or multiple layers. The single-layer cirrus occurrence shows a diurnal pattern with frequent occurrence in the late evening (~30–40 %) while multiple-layer cirrus clouds occurrence and early morning (~10–20 %), respectively. For the diurnal pattern in single layer cirrus cloud occurrences, convective processes dominate during the pre-monsoon, southwest (SW), and northeast (NE) monsoon seasons, while the freeze-drying process is favourable during the winter season. However, both convective and freeze-drying processes are dominant in the diurnal pattern of the multiple-layer cirrus occurrences. The occurrence is maximum (~40 %) during the SW and NE monsoon seasons and minimum (~25 %) during the winter. The vertical distributions indicate that the maximum occurrence is confined within the tropical tropopause layer (TTL) during all the seasons. The cirrus cloud rarely occurs above the tropopause; however, it frequently occurs below the TTL during all the seasons. The vertical extent of the occurrence has broader altitude coverage (~8–17 km) during December–March and June–September while narrower during April–May (~10–17 km) and October–November (~9–15 km). The cirrus clouds occurrence also exhibits interannual variations with higher occurrence during 2016 compared to 2017 and 2018 in association with El Nino Southern Oscillation (ENSO).

Changes in cirrus cloud properties and occurrence over Europe during the COVID-19-caused air traffic reduction

By inducing linear contrails and contrail cirrus, air traffic has a main impact on the ice cloud coverage and occurrence. During the COVID-19 pandemic, civil air traffic over Europe was significantly reduced, in March and April 2020, to about 80 % compared to the year before. This unique situation allows us to study the effect of air traffic on cirrus clouds. This work investigates, based on satellite lidar measurements, if and how cirrus cloud properties and occurrence changed over Europe in the course of COVID-19. Cirrus cloud properties are analyzed for different years between 2014 and 2019, which showed similar meteorological conditions for the month of April as in 2020. The meteorological conditions for March, however, were warmer and drier in 2020 than the previous years. The average thickness of cirrus clouds was reduced to 1.18 km in March 2020 compared to a value of 1.40 km under normal conditions, which is stronger than expected from the aviation reduction due to the less favorable meteorology for ice cloud formation. While the April results in 2020 were only slightly reduced, with an average thickness of 70 m thinner than the composite mean of the previous 6 years. Comparing the different years shows that the cirrus cloud occurrence was reduced by about 17 %–30 %, with smaller cloud thicknesses found in 2020 for both months. In addition, the cirrus clouds measured in 2020 possess smaller values of the particle linear depolarization ratio (PLDR) than the previous years at a high significance level for both months, especially at colder temperatures (T<-50 ∘C). The same analyses are extended to the observations over the USA and China. Besides the regional discrimination of cirrus clouds, we reach the final conclusion that cirrus clouds show significant changes in PLDR in both March and April over Europe, no changes in both months over China, and significant changes only in April over the USA.

Above-aircraft cirrus cloud and aerosol optical depth from hyperspectral irradiances measured by a total-diffuse radiometer

This study develops the use of spectral total and diffuse irradiance measurements, made from a prototype hyperspectral total-diffuse Sunshine Pyranometer (SPN-S), to retrieve layer fine-mode aerosol (τaer) and total optical depths from airborne platforms. Additionally, we use spectral analysis in an attempt to partition the total optical depth it into its τaer and cirrus cloud optical depth (τcld) components in the absence of coarse-mode aerosols. Two retrieval methods are developed: one leveraging information in the diffuse irradiance, and the other using spectral characteristics of the transmitted direct beam, with each approach best suited for specific cloud and aerosol conditions. SPN-S has advantages over traditional sun-photometer systems including no moving parts and a low cost. However, a significant drawback of the instrument is that it is unable to measure the direct beam irradiance as accurately as sun-photometers. To compensate for the greater measurement uncertainty of the radiometric irradiances these retrieval techniques employ ratioed inputs or spectral information to reduce output uncertainty. This analysis uses irradiance measurements from SPN-S and the Solar Spectral Flux Radiometer (SSFR) aboard the National Aeronautics and Space Administration’s (NASA) P-3 aircraft during the 2018 deployment of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign and the 2019 Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) mission to quantify above-aircraft cirrus τcld and derive vertical profiles of layer τaer. Validation of the τaer retrieval is accomplished by comparison with collocated measurements of direct solar irradiance made by the Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) and in situ measurements of aerosol optical depth. For the aggregated 2018 ORACLES results, regression between the SPN-S based method and sun-photometer τaer values yield a slope of 0.96 with an R2 of 0.96, while the root-mean-square error (RMSE) is 3.0 × 10−2. When comparing the retrieved τaer to profiles of integrated in situ measurements of optical extinction, the slope, R2, and RMSE values for ORACLES are 0.90, 0.96, 3.4 × 10−2, and for CAMP2Ex are 0.94, 0.97, 3.4 × 10−2 respectively. This paper is a demonstration of methods for deriving cloud and aerosol optical properties in environments where both atmospheric constituents may be present. With improvements to the low-cost SPN-S radiometer instrument, it may be possible to extend these methods to a broader set of sampling applications, such as ground-based settings.

High homogeneous freezing onsets of sulfuric acid aerosol at cirrus temperatures

Homogeneous freezing of aqueous solution aerosol particles is an important process for cloud ice formation in the upper troposphere. There the air temperature is low, the ice supersaturation can be high and the concentration of ice-nucleating particles is too low to initiate and dominate cirrus cloud formation by heterogeneous ice nucleation processes. The most common description to quantify homogeneous freezing processes is based on the water activity criterion (WAC) as proposed by Koop et al. (2000). The WAC describes the homogeneous nucleation rate coefficients only as a function of the water activity, which makes this approach well applicable in numerical models. In this study, we investigate the homogeneous freezing behavior of aqueous sulfuric acid aerosol particles by means of a comprehensive collection of laboratory-based homogeneous freezing experiments conducted at the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber, which were conducted as part of 17 measurement campaigns since 2007. The most recent experiments were conducted during October 2020 with special emphasis on temperatures below 200 K. Aqueous sulfuric acid aerosol particles of high purity were generated by particle nucleation in a gas flow composed of clean synthetic air and sulfuric acid vapor, which was added to the AIDA chamber. The resulting chamber aerosol had number concentrations from 30 cm−3 up to several thousand per cubic centimeter with particle diameters ranging from about 30 nm to 1.1 µm. Homogeneous freezing of the aerosol particles was measured at simulated cirrus formation conditions in a wide range of temperatures between 185 and 230 K with a steady increase of relative humidity during each experiment. At temperatures between about 205 K and about 230 K, the AIDA results agree well with the WAC-based predictions of homogeneous freezing onsets. At lower temperatures, however, the AIDA results show an increasing deviation from the WAC-based predictions towards higher freezing onsets. For temperatures between 185 and 205 K, the WAC-based ice saturation ratios for homogeneous freezing onsets increase from about 1.6 to 1.7, whereas the AIDA measurements show an increase from about 1.7 to 2.0 in the same temperature range. Based on the experimental results of our direct measurements, we suggest a new fit line to formulate the onset conditions of homogeneous freezing of sulfuric acid aerosol particles as an isoline for nucleation rate coefficients between 5×108 and 1013 cm−3 s−1. The potential significant impacts of the higher homogeneous freezing thresholds, as directly observed in the AIDA experiments under simulated cirrus formation conditions, on the model prediction of cirrus cloud occurrence and related cloud radiative effects are discussed.

Ice nucleation activities of soot particles internally mixed with sulphuric acid at cirrus cloud conditions

Soot particles are important candidates for ice nucleating particles (INPs) in cirrus cloud formation which is known to exert a warming effect on climate. Bare soot particles, generally hydrophobic and fractal, mainly exist near emission sources. Coated or internally mixed soot particles are more abundant in the atmosphere and have a higher probability to impact cloud formation and climate. However, the ice nucleation ability of coated soot particles is not as well understood as that of freshly produced soot particles. In this study, two samples, a propane (C3H8) flame soot and a commercial carbon black were coated with varying wt % of sulphuric acid (H2SO4). The ratio of coating material mass to the mass of bare soot particle was controlled and progressively increased from less than 5 wt % to over 100 wt %. Both bare and coated soot particle ice nucleation activities were investigated with a continuous flow diffusion chamber operated at mixed-phase and cirrus cloud conditions. The mobility size and mass distribution of size selected soot particles with/without H2SO4 coating were measured by a scanning mobility particle sizer (SMPS) and a centrifugal particle mass analyser (CPMA) running in parallel. The mixing state and morphology of soot particles were characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). In addition, the evidence for the presence of H2SO4 on coated soot particle surface is shown by Energy Dispersive X-ray spectroscopy (EDX). Our study demonstrates that H2SO4 coatings suppress the ice nucleation activity of soot particles to varying degrees depending on the coating thickness, but in a non-linear fashion. Thin coatings causing pore filling in the soot-aggregate inhibits pore condensation and freezing (PCF). Thick coatings promote particle ice activation via droplet homogeneous freezing. Overall, our findings reveal that H2SO4 coatings will suppress soot particle ice nucleation abilities in the cirrus cloud regime, having implications for the fate of soot particles with respect to cloud formation in the upper troposphere.

Cirrus cloud thinning using a more physically-based ice microphysics scheme in the ECHAM-HAM GCM

Cirrus cloud thinning (CCT) is a relatively new radiation management proposal to counteract anthropogenic climate warming by targeting Earth’s terrestrial radiation balance. The efficacy of this method was presented in several general circulation model (GCM) studies that showed widely varied radiative responses, originating in part from the differences in the representation of cirrus ice microphysics between the different GCMs. The recent implementation of a new, more physically based ice microphysics scheme (Predicted Particle Properties, P3) that abandons ice hydrometeor size class separation into the ECHAM-HAM GCM, coupled to a new approach for calculating cloud fractions that increases the relative humidity (RH) thresholds for cirrus cloud formation, motivated a reassessment of CCT efficacy. In this study, we first compared CCT sensitivity between the new cloud fraction approach and the original ECHAM-HAM cloud fraction approach. With the P3 scheme and the higher RH thresholds for cirrus cloud formation, we find a significant cooling response of −0.36 Wm−2 only for our simulation with a seeding particle concentration of 1 L−1, due mostly to rapid cloud adjustments. The most notable response is the reduction of the maximum global-mean net top-of-atmosphere (TOA) radiative anomalies from overseeding by more than 50 %, from 9.0 Wm−2 with the original cloud fraction approach, down to 4.3 Wm−2 using the new cloud fraction RH thresholds by avoiding artificial ice-cloud expansion upon ice nucleation. We attribute the large positive TOA anomalies to seeding particles overtaking both homogeneous nucleation and heterogeneous nucleation on mineral dust particles within cirrus clouds to produce more numerous and smaller ice crystals. This effect is amplified by longer ice residence times in clouds due to the more realistic, slower removal of ice via sedimentation in the P3 scheme. In an effort to avoid this overtaking effect of seeding particles, we increased the default critical ice saturation ratio (Si,seed) for ice nucleation on seeding particles from the default value of 1.05 to 1.35 in a second sensitivity test. With the higher Si,seed we eliminate overseeding and are able to produce cooling responses over a broader range of seeding particle concentrations, with the largest cooling of −0.32 Wm−2 for a seeding particle concentration of 10 L−1, which suggests that Si,seed is a key factor to consider for future CCT studies. However, the global-mean TOA anomalies contain high uncertainty. In response, we examined the TOA responses regionally and found that specific regions only show a small potential for targeted CCT, which is partially enhanced by using the larger Si,seed. Finally, in a seasonal analysis of TOA responses to CCT, we find that our results do not support the previous finding that high-latitude wintertime seeding is a feasible strategy to enhance CCT efficacy, as seeding in our model enhances the already positive cirrus longwave cloud radiative effect. Instead, our results show that summertime cooling occurs due to adjustments of lower-lying mixed-phase and liquid clouds. Therefore, we conclude that CCT is unlikely to act as a feasible climate intervention strategy on a global scale, and should be investigated further with higher-resolution studies in potential target regions and with studies dedicated to assessing potentially realistic seeding particle materials.

Contrail formation within cirrus: high-resolution simulations using ICON-LEM

Contrail formation within natural cirrus introduces large perturbations in cirrus ice crystal number concentrations leading to modifications in cirrus microphysical and optical properties. The number of contrail ice crystals formed in an aircraft plume depends on the atmospheric state and aircraft and fuel properties. Our aim is to study the impact of pre-existing cirrus on the contrail formation processes. We analyze contrail ice nucleation within cirrus and the survival of contrail ice crystals within the vortex phase and their change due to the presence of cirrus ice crystals within the high-resolution ICON-LEM at a horizontal resolution of 625 m over Germany. We have selected two different synoptic situations sampling a large range of cirrus cloud properties from very thick cirrus connected with a frontal system to very thin cirrus within a high-pressure system. We find that contrail formation within cirrus often leads to increases in cirrus ice crystal numbers by a few orders of magnitude. Pre-existing cirrus has an impact on contrail ice crystal number concentrations only if the cirrus is optically thick. In thick cirrus, contrail ice nucleation rates and ice crystal survival rates within the vortex phase are both increased. The sublimation of the cirrus ice crystals sucked into and subsequently sublimated within the aircraft’s engine leads to an increase in the contrail formation threshold by up to 0.7 K which causes an increase in the number of nucleated contrail ice crystals. This increase can be large at lower flight levels where ambient temperatures are close to the contrail formation threshold temperature and when the ice water content of the pre-existing cirrus cloud is large. During the contrail’s vortex phase the aircraft plume is trapped within the descending vortices in which the decrease in plume relative humidity leads to the sublimation of contrail ice crystals. This contrail ice crystal loss can be modified by the cirrus ice crystals that are mixed into the plume before the start of the vortex phase. In particular, high ice crystal number concentrations and large ice water content of the pre-existing cirrus cloud or low contrail ice crystal numbers are associated with significant increases in the contrail ice crystal survival rates.

High Homogeneous Freezing Onsets of Sulfuric Acid Aerosol at Cirrus Temperatures

Homogeneous freezing of aqueous solution aerosol particles is an important process for cloud ice formation in theupper troposphere. There the air temperature is low, the ice supersaturation can be high, and the concentration of ice-nucleating particles is too low to initiate and dominate cirrus cloud formation by heterogeneous ice nucleation processes. The most common description to quantify homogeneous freezing processes is based on the water activity criterion (WAC) as proposed by Koop et al. (2000). The WAC describes the homogeneous nucleation rate coefficients only as a function of the water activity, temperature and size of the aqueous aerosol particles, which makes this approach well applicable in numerical models. In this study, we investigate the homogeneous freezing behaviour of aqueous sulfuric acid aerosol particles by means of a comprehensive collection of laboratory homogeneous freezing experiments conducted at the AIDA (Aerosol Interaction and Dynamicsin the Atmosphere) cloud simulation chamber, which were conducted as part of 17 measurement campaigns since 2007. The most recent experiments were conducted during October 2020 with special emphasis on temperatures below 200 K. Aqueous sulfuric acid aerosol particles were generated at high purity by particle nucleation in a gas flow composed of clean synthetic air and sulfuric acid vapor, which was added to the AIDA chamber. The resulting chamber aerosol had number concentrations from 30 cm−3 up to several 1000 cm−3 with particle diameters ranging from about 30 nm to 1.1 μm. Homogeneous freezing of the aerosol particles was measured at simulated cirrus formation conditions in a wide range of temperatures between 185 K and 230 K with a steady increase of relative humidity during each experiment. At temperatures between about 205 K and about 230 K, the AIDA results agree well with the WAC-based predictions of homogeneous freezing onsets. At lower temperatures, however, the AIDA results show an increasing deviation from the WAC-based predictions towards higher freezing onsets. For temperatures between 185 K and 205 K, the WAC-based ice saturation ratios for homogeneous freezing onsets increase from about 1.6 to 1.7, whereas the AIDA measurements show an increase from about 1.7 to 2.0 in the same temperature range. Based on our experimental results, we suggest a new fit line as a parameterization for the onset conditions of homogeneous freezing of sulfuric acid aerosol particles. As a next step, we propose the new parameterization to be implemented in atmospheric models as an improved version of the WAC-based parameterization from Koop et al. (2000). The new homogeneous freezing thresholds may have significant impacts on the prediction of cirrus cloud occurrence and related cloud radiative effects.