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At least 19 records

Theory of In-Cloud Activation of Aerosols and Microphysical Quasi-Equilibrium in a Deep Updraft

The microphysical quasi-equilibrium in an ascending adiabatic parcel is elucidated by an analytical theory in 0D with drastic simplifications. The theory predicts how in-cloud activation is most likely to be triggered by the onset of precipitation during sufficient ascent, with the ascent only needing to approach almost twice the cloud-base updraft speed aloft. The precipitation and cloud condensate mass fields are coupled in a closed system in a simplified version of the model. The initial state of no precipitation is unstable with respect to a perturbation. In the 2D phase space of both mass fields, there is a neutral line. Unstable growth of precipitation mass drives the system to cross the line into a regime of stability. An attractor is then approached consisting of precipitation mass balanced by accretion of cloud mass and fallout. The cloud-particle number concentration also approaches a stable equilibrium governed by the balance between in-cloud activation aloft from the inexorably increasing supersaturation during vertical acceleration and accretion of cloud droplets by precipitation. Dimensionless numbers characterizing the microphysical equilibria and their stability are derived mathematically, including a condensation–precipitation efficiency and an in-cloud activation efficiency. The theory explains common observations of the orders of magnitude of liquid water content in convective and stratiform clouds. Finally, sensitivity tests of the numerically integrated theoretical equations are documented with respect to variations in cloud condensation nucleus (CCN) aerosols and updraft speed. In conclusion, it is shown that this theory of in-cloud activation, with an increasing supersaturation during ascent, applies to both ice-only and liquid-only cloud.

54 ENVIRONMENTAL SCIENCES↗

Cloud Condensation Nuclei Particle Counter (CCN) Instrument Handbook

The Cloud Condensation Nuclei Counter—CCN (Figure 1) is a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility instrument for measuring the concentration of aerosol particles that can act as cloud condensation nuclei [1, 2]. The CCN draws the sample aerosol through a column with thermodynamically unstable supersaturated water vapor that can condense onto aerosol particles. Particles that are activated, i.e., grown larger in this process, are counted (and sized) by an Optical Particle Counter (OPC). Thus, activated ambient aerosol particle number concentration as a function of supersaturation is measured. Models CCN-100 and CCN-200 differ only in the number of humidifier columns and related subsystems: CCN-100 has one column and CCN-200 has two columns along with dual flow systems and electronics.

54 ENVIRONMENTAL SCIENCES↗

Ice Nucleating Particles (INP) Raw Data

The ice nucleation spectrometer (INS) is an offline analytical measurement system used to process filter samples for freezing temperature spectra of immersion-mode ice-nucleating particle (INP) number concentrations. It is almost identical to the Colorado State University (CSU) ice spectrometer design. Filter samples are collected at ARM facilities routinely and during intensive operational periods, and on the ARM tethered balloon system operated by Sandia National Laboratories, then processed on the INS at CSU. This filter log contains the detailed metadata at all ARM sites where INP filter sample collection has occurred or is currently ongoing. Metadata include start and end times, vacuum line pressures and temperatures, and flow rates; total accumulated flow through each filter; and notes on collection issues or weather conditions. Users can also keep up to date with the status of filter and data processing, even before data are available on ARM's Data Discovery. Users can contact INP mentors Jessie Creamean or Thomas Hill with any questions.

54 ENVIRONMENTAL SCIENCES↗

Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 1: Observational data analysis

This study employed multiple techniques to investigate the contribution of grown new particles to the number concentration of cloud condensation nuclei (CCN) at various supersaturation (SS) levels at a rural mountain site in the North China Plain from 29 June to 14 July 2019. On 8 new particle formation (NPF) days, the total particle number concentrations (N cn ) were 8.4 ± 6.1×10 3 cm -3 , which was substantially higher compared to 4.7 ± 2.6×10 3 cm -3 on non-NPF days. However, the CCN concentration (Nccn) at 0.2 % SS and 0.4 % SS on the NPF days was significantly lower than those observed on non-NPF days (p<0.05). This was due to the lower cloud activation efficiency of preexisting particles resulting from organic vapor condensation and smaller number concentrations of preexisting particles on NPF days. A case-by-case examination showed that the grown new particles only yielded a detectable contribution to N ccn at 0.4 % SS and 1.0 % SS during the NPF event on 1 July 2019, accounting for 12 % ± 11 % and 23 % ± 12 % of N ccn , respectively. The increased N ccn during two other NPF events and at 0.2 % SS on 1 July 2019 were detectable but determined mainly by varying preexisting particles rather than grown new particles. In addition, the hygroscopicity parameter values, concentrations of inorganic and organic particulate components, and surface chemical composition of different sized particles were analyzed in terms of chemical drivers to grow new particles. The results showed that the grown new particles via organic vapor condensation generally had no detectable contribution to N ccn but incidentally did. However, this conclusion was drawn from a small size of observational data, leaving more observations, particularly long-term observations and the growth of preexisting particles to the CCN required size, needed for further investigation.

54 ENVIRONMENTAL SCIENCES↗

Fog particle concentrations

ngVIPS metadata and caveats: Column 1: Time, seconds after midnight UTC of beginning of time period. (60 sec values) Column 2: Relative concentration. Notes: Concentration values are observed values and assume ~4.0 m/s wind speed. (#/cm^3) Caveats: Observed particles with a very few exceptions were on the order of a few pixels (less than 10 microns). The size differential was insufficient to determine a particle size distribution. As the temperatures were relatively warm (and it can be 10C warmer inside the instrument) it is anticipated that some solid ice particles could have melted and some smaller liquid drops could have evaporated. A cyclic nature to the high resolution data was observed and determined to be caused by a focus issue. Each 60 second period included ~25 images. Particles are collected on a glass disk, but the disk isn't perfectly centered causing small particles to be slightly out of focus during part of the rotation. For that reason, we chose to report the average of the five highest values in a time period rather the average of all values. Higher resolution can be made available upon request, but a conversation with the PI would be important to fully understand the planned usage and if the higher resolution data were to be useful for the task. Please contact instrument PI, Carl Schmitt (naturalsystemsresearch@gmail.com) with any questions about these data.

54 ENVIRONMENTAL SCIENCES↗

The missing base molecules in atmospheric acid–base nucleation

Abstract Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the atmosphere. However, the acid–base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain the measured high formation rate of new particles. Here we present strong evidence for the existence of base molecules such as amines in the smallest atmospheric sulfuric acid clusters prior to their detection by mass spectrometers. We demonstrate that forming (H2SO4)1(amine)1 is the rate-limiting step in atmospheric H2SO4-amine nucleation and the uptake of (H2SO4)1(amine)1 is a major pathway for the initial growth of H2SO4 clusters. The proposed mechanism is very consistent with measured new particle formation in urban Beijing, in which dimethylamine is the key base for H2SO4 nucleation while other bases such as ammonia may contribute to the growth of larger clusters. Our findings further underline the fact that strong amines, even at low concentrations and when undetected in the smallest clusters, can be crucial to particle formation in the planetary boundary layer.

54 ENVIRONMENTAL SCIENCES↗

Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions

This is the final technical report for DOE DE-SC0021034 award entitled “Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions”. The overarching objective of this project was to gain a predictive understanding of the processes that lead from aerosols to ice-nucleating particles (INPs) to ice crystal number concentrations (ICNCs) in stratiform mixed-phase clouds where supercooled water droplets and ice crystals coexist, and to inform climate model parameterizations. During this four-year project we addressed the three main research goals of this objective: 1) Study the aerosol-INP link; 2) Develop an aerosol-cloud column model (AC-1D); and 3) Study the INP-ICNC link. Those activities significantly advanced our predictive understanding of how to represent INPs in could models and its implications on ice crystal number concentrations. The results have been published in five peer-reviewed publications with three more in review and preparation. It allowed for collaboration resulting in additional fourteen peer-reviewed publications that are concerned with the objective of this research project. This research has been communicated to the scientific community at national and international meetings and conferences by numerous talks, seminars, and posters including fifteen invited presentations. This project allowed training of four graduate students and one postdoctoral research associate resulting in one M.S. thesis and advancement to Ph.D. candidacy.

54 ENVIRONMENTAL SCIENCES↗

Measurements of aerosol microphysical and chemical properties in the central Arctic atmosphere during MOSAiC

The Arctic environment is transforming rapidly due to climate change. Aerosols’ abundance and physicochemical characteristics play a crucial, yet uncertain, role in these changes due to their influence on the surface energy budget through direct interaction with solar radiation and indirectly via cloud formation. Importantly, Arctic aerosol properties are also changing in response to climate change. Despite their importance, year-round measurements of their characteristics are sparse in the Arctic and often confined to lower latitudes at Arctic land-based stations and/or short high-latitude summertime campaigns. Here, we present unique aerosol microphysics and chemical composition datasets collected during the year-long Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, in the central Arctic. These datasets, which include aerosol particle number concentrations, size distributions, cloud condensation nuclei concentrations, fluorescent aerosol concentrations and properties, and aerosol bulk chemical composition (black carbon, sulfate, nitrate, ammonium, chloride, and organics) will serve to improve our understanding of high-Arctic aerosol processes, with relevance towards improved modelling of the future Arctic (and global) climate.

54 ENVIRONMENTAL SCIENCES↗

Relationships between Immersion Freezing and Crystal Habit for Arctic Mixed-Phase Clouds—A Numerical Study

Abstract The number concentration of ice particles in Arctic mixed-phase clouds is a major controlling factor of cloud lifetime. The relationships between ice nucleation mode and ice crystal habit development are not yet constrained by observations. This study uses a habit-predicting microphysical scheme within a 3D large-eddy simulation model to evaluate the relationship between immersion freezing and ice habit in a simulated Arctic mixed-phase cloud case. Three immersion freezing parameterizations are considered: a volume-dependent freezing scheme (VF), a parameterization limited to activated droplets (C-AC), and a parameterization limited to coarse aerosol particles (C-CM). Both C-AC and C-CM are based on classical nucleation theory. The freezing rate with VF is found to be greater in downdraft regions than in updraft regions due to the downdraft having a higher number concentration of large droplets. The C-AC cases show active freezing of small droplets near cloud top, whereas in the C-CM cases, mainly the 8–32- μ m-sized droplets freeze in updraft regions near the cloud base. Because the initial crystal size is assumed to affect the axis ratio of hexagonal plates, the VF cases produce crystals with larger axis ratios, resulting in smaller mode radii than the C-AC cases. In all cases, irregular polycrystals dominate near cloud top and a band-like structure develops within the cloud, which qualitatively agrees with previous observations. In the VF and C-CM cases, unactivated large droplets arising from coarse-mode aerosol particles contributed significantly to the freezing rate, producing an important influence on crystal habit.

54 ENVIRONMENTAL SCIENCES↗

New insights into ice multiplication using remote-sensing observations of slightly supercooled mixed-phase clouds in the Arctic

Significance During secondary ice events, ice particle number concentrations in mixed-phase clouds can increase by orders of magnitude with profound implications for the cloud evolution. However, characterization of secondary ice events in the natural environment has been a challenge for the community for decades. We show the long-term frequency of secondary ice events in Arctic supercooled clouds for temperatures warmer than − 10 ○ C, made possible by applying a remote-sensing technique to 6 y of data. Secondary ice events are found to occur preferentially in the presence of drizzle droplets, compared with the better-known rime-splintering process, causing up to a 1,000-fold enhancement in ice number concentration. These results provide critical insights for model parameterizations and future laboratory experiments.

54 ENVIRONMENTAL SCIENCES↗

Impacts of secondary ice production on Arctic mixed-phase clouds based on ARM observations and CAM6 single-column model simulations

For decades, measured ice crystal number concentrations have been found to be orders of magnitude higher than measured ice-nucleating particle number concentrations in moderately cold clouds. This observed discrepancy reveals the existence of secondary ice production (SIP) in addition to the primary ice nucleation. However, the importance of SIP relative to primary ice nucleation remains highly unclear. Furthermore, most weather and climate models do not represent SIP processes well, leading to large biases in simulated cloud properties. This study demonstrates a first attempt to represent different SIP mechanisms (frozen raindrop shattering, ice–ice collisional breakup, and rime splintering) in a global climate model (GCM). The model is run in the single column mode to facilitate comparisons with the Department of Energy (DOE)'s Atmospheric Radiation Measurement (ARM) Mixed-Phase Arctic Cloud Experiment (M-PACE) observations. We show the important role of SIP in four types of clouds during M-PACE (i.e., multilayer, single-layer stratus, transition, and frontal clouds), with the maximum enhancement in ice crystal number concentrations up to 4 orders of magnitude in moderately supercooled clouds. We reveal that SIP is the dominant source of ice crystals near the cloud base for the long-lived Arctic single-layer mixed-phase clouds. The model with SIP improves the occurrence and phase partitioning of the mixed-phase clouds, reverses the vertical distribution pattern of ice number concentrations, and provides a better agreement with observations. The findings of this study highlight the importance of considering SIP in GCMs.

54 ENVIRONMENTAL SCIENCES↗

African smoke particles act as cloud condensation nuclei in the wintertime tropical North Atlantic boundary layer over Barbados

Abstract. The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygroscopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds–Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions of dust and smoke particles increased, whereas the average κ slightly decreased (κ=0.46±0.10) from marine background conditions (κ=0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The NASA ACTIVATE Mission

The NASA Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE) conducted 162 joint flights with two aircraft over the northwest Atlantic to study aerosol–cloud interactions (ACIs), which represent the largest uncertainty in estimating total anthropogenic radiative forcing. The combination of a high-flying King Air and low-flying HU-25 Falcon, equipped with remote sensing and in situ instruments, characterized trace gases, aerosol particles, clouds, and meteorological variables with data collected nearly simultaneously below, within, and above marine boundary layer (MBL) clouds. Flights spanning warm and cold seasons across 3 years (2020–22) provided a broad range of conditions associated with aerosol particles, cloud properties (including particle size and phase), and meteorology, ideally suited for robust ACI calculations and assessing how well models simulate a wide range of MBL clouds from stratiform to cumulus. ACTIVATE data suggest that drivers of cloud droplet number concentration N d , including aerosol particles and MBL dynamics, vary between winter and summer months with a stronger potential to convert aerosol particles into cloud droplets in winter. Models of varying complexity not only highlight some skills in simulating winter and summer cloud types but also identify challenges that still need to be addressed such as treatment of turbulence, wet scavenging, and mesoscale organization. Remote sensing advances range from new retrieval methods for N d , cloud phase classification, vertically resolved aerosol and cloud condensation nuclei number concentration, and ocean surface wind speed. This work describes these scientific and technological advances along with efforts in outreach and open data science.

aerosol indirect effect↗

Comparison of aircraft measurements during GoAmazon2014/5 and ACRIDICON-CHUVA

The indirect effect of atmospheric aerosol particles on the Earth's radiation balance remains one of the most uncertain components affecting climate change throughout the industrial period. The large uncertainty is partly due to the incomplete understanding of aerosol–cloud interactions. One objective of the GoAmazon2014/5 and the ACRIDICON (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems)-CHUVA (Cloud Processes of the Main Precipitation Systems in Brazil) projects was to understand the influence of emissions from the tropical megacity of Manaus (Brazil) on the surrounding atmospheric environment of the rainforest and to investigate its role in the life cycle of convective clouds. During one of the intensive observation periods (IOPs) in the dry season from 1 September to 10 October 2014, comprehensive measurements of trace gases and aerosol properties were carried out at several ground sites. In a coordinated way, the advanced suites of sophisticated in situ instruments were deployed aboard both the US Department of Energy Gulfstream-1 (G1) aircraft and the German High Altitude and Long-Range Research Aircraft (HALO) during three coordinated flights on 9 and 21 September and 1 October. Here, we report on the comparison of measurements collected by the two aircraft during these three flights. Such comparisons are challenging but essential for assessing the data quality from the individual platforms and quantifying their uncertainty sources. Similar instruments mounted on the G1 and HALO collected vertical profile measurements of aerosol particle number concentrations and size distribution, cloud condensation nuclei concentrations, ozone and carbon monoxide mixing ratios, cloud droplet size distributions, and downward solar irradiance. We find that the above measurements from the two aircraft agreed within the measurement uncertainties. The relative fraction of the aerosol chemical composition measured by instruments on HALO agreed with the corresponding G1 data, although the total mass loadings only have a good agreement at high altitudes. Furthermore, possible causes of the discrepancies between measurements on the G1 and HALO are examined in this paper. Based on these results, criteria for meaningful aircraft measurement comparisons are discussed.

47 OTHER INSTRUMENTATION↗

Maximum Supersaturation in the Marine Boundary Layer Clouds Over the North Atlantic

Abstract The maximum supersaturation ( S x ) in clouds is a key parameter affecting the cloud's microphysical and radiative properties. We investigate the S x of the marine boundary layer clouds by combining airborne and surface observations in the Eastern North Atlantic. The cloud droplet number concentration ( N c ) in the least diluted cloud cores agrees well with the number concentration of particles larger than the Hoppel Minimum (HM) ( N >HM ) below clouds, indicating that the HM represents the average size threshold above which particles are activated to form cloud droplets. The S x values derived from surface observations vary from 0.10% to 0.50% from June 2017 to June 2018, with a clear seasonal variation exhibiting higher values during winter. Most of the S x variance (∼60%) can be explained by the cloud condensation nuclei (CCN) concentration and updraft velocity ( w ), with the CCN concentration playing a more important role than w in explaining the variation of S x . The influence of CCN concentration on S x leads to a buffered response of N c to aerosol perturbations. The response of N c to low aerosol concentration during winter is further buffered by the high w . The global Community Earth System Model (CESM) simulated S x values in the Azores have a positive bias compared to measured S x , likely due to overestimated w and underestimated CCN concentration. The CESM simulated S x exhibits higher values further north over the North Atlantic Ocean, which is attributed to stronger w . The suppression of S x by aerosol is also evident in regions with high CCN concentrations.

54 ENVIRONMENTAL SCIENCES↗

Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause

Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

54 ENVIRONMENTAL SCIENCES↗