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Partition between supercooled liquid droplets and ice crystals in mixed-phase clouds based on airborne in situ observations

Abstract. The onset of ice nucleation in mixed-phase clouds determines the lifetime and microphysical properties of ice clouds. In this work, we develop a novel method that differentiates between various phases of mixed-phase clouds, such as clouds dominated by pure liquid or pure ice segments, compared with those having ice crystals surrounded by supercooled liquid water droplets or vice versa. Using this method, we examine the relationship between the macrophysical and microphysical properties of Southern Ocean mixed-phase clouds at −40 to 0 °C (e.g. stratiform and cumuliform clouds) based on the in situ aircraft-based observations during the US National Science Foundation Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) flight campaign. The results show that the exchange between supercooled liquid water and ice crystals from a macrophysical perspective, represented by the increasing spatial ratio of regions containing ice crystals relative to the total in-cloud region (defined as ice spatial ratio), is positively correlated with the phase exchange from a microphysical perspective, represented by the increasing ice water content (IWC), decreasing liquid water content (LWC), increasing ice mass fraction, and increasing ice particle number fraction (IPNF). The mass exchange between liquid and ice becomes more significant during phase 3 when pure ice cloud regions (ICRs) start to appear. Occurrence frequencies of cloud thermodynamic phases show a significant phase change from liquid to ice at a similar temperature (i.e. −17.5 °C) among three types of definitions of mixed-phase clouds based on ice spatial ratio, ice mass fraction, or IPNF. Aerosol indirect effects are quantified for different phases using number concentrations of aerosols greater than 100 or 500 nm (N>100 and N>500, respectively). N>500 shows stronger positive correlations with ice spatial ratios compared with N>100. This result indicates that larger aerosols potentially contain ice-nucleating particles (INPs), which facilitate the formation of ice crystals in mixed-phase clouds. The impact of N>500 is also more significant in phase 2 when ice crystals just start to appear in the mixed phase compared with phase 3 when pure ICRs have formed, possibly due to the competing aerosol indirect effects on primary and secondary ice production in phase 3. The thermodynamic and dynamic conditions are quantified for each phase. The results show stronger in-cloud turbulence and higher updraughts in phases 2 and 3 when liquid and ice coexist compared with pure liquid or ice (phases 1 and 4, respectively). The highest updraughts and turbulence are seen in phase 3 when supercooled liquid droplets are surrounded by ice crystals. These results indicate both updraughts and turbulence support the maintenance of supercooled liquid water amongst ice crystals. Overall, these results illustrate the varying effects of aerosols, thermodynamics, and dynamics through various stages of mixed-phase cloud evolution based on this new method that categorizes cloud phases.

54 ENVIRONMENTAL SCIENCES↗

Shortwave Array Spectroradiometer-Hemispheric (SAS-He): design and evaluation

A novel ground-based radiometer, referred to as the Shortwave Array Spectroradiometer-Hemispheric (SAS-He), is introduced. This radiometer uses the shadow-band technique to report total irradiance and its direct and diffuse components frequently (every 30 s) with continuous spectral coverage (350–1700 nm) and moderate spectral (~2.5 nm ultraviolet–visible and ~6 nm shortwave-infrared) resolution. The SAS-He's performance is evaluated using integrated datasets collected over coastal regions during three field campaigns supported by the US Department of Energy's Atmospheric Radiation Measurement (ARM) program, namely the (1) Two-Column Aerosol Project (TCAP; Cape Cod, Massachusetts), (2) Tracking Aerosol Convection Interactions Experiment (TRACER; in and around Houston, Texas), and (3) Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE; La Jolla, California). We compare (i) aerosol optical depth (AOD) and total optical depth (TOD) derived from the direct irradiance, as well as (ii) the diffuse irradiance and direct-to-diffuse ratio (DDR) calculated from two components of the total irradiance. As part of the evaluation, both AOD and TOD derived from the SAS-He direct irradiance are compared to those provided by a collocated Cimel sunphotometer (CSPHOT) at five (380, 440, 500, 675, 870 nm) and two (1020, 1640 nm) wavelengths, respectively. Additionally, the SAS-He diffuse irradiance and DDR are contrasted with their counterparts offered by a collocated multifilter rotating shadowband radiometer (MFRSR) at six (415, 500, 615, 675, 870, 1625 nm) wavelengths. Overall, reasonable agreement is demonstrated between the compared products despite the challenging observational conditions associated with varying aerosol loadings and diverse types of aerosols and clouds. For example, the AOD- and TOD-related values of root mean square error remain within 0.021 at 380, 440, 500, 675, 870, 1020, and 1640 nm wavelengths during the three field campaigns.

47 OTHER INSTRUMENTATION↗

Hunga Tonga–Hunga Ha′apai Volcano Impact Model Observation Comparison (HTHH-MOC) project: experiment protocol and model descriptions

The 2022 Hunga volcanic eruption injected a significant amount of water vapor and a moderate amount of sulfur dioxide into the stratosphere, causing observable responses in the climate system. We have developed a model–observation comparison project to investigate the evolution of volcanic water and aerosols and their impacts on atmospheric dynamics, chemistry, and climate, using several state-of-the-art chemistry climate models. The project goals are (1) to evaluate the current chemistry–climate models to quantify their performance in comparison to observations and (2) to understand atmospheric responses in the Earth system after this exceptional event and investigate the potential impacts in the projected future. To achieve these goals, we designed specific experiments for direct comparisons to observations, for example from balloons and the Microwave Limb Sounder satellite instrument. Experiment 1 consists of two sets of free-running ensemble experiments from 2022 to 2031: one with fixed sea-surface temperatures and sea ice and one with coupled ocean. These experiments will help to understand the long-term evolution of water vapor and aerosols; quantify HTHH effects on stratospheric and mesospheric temperatures, dynamics, and transport; understand the impact of dynamic changes on ozone chemistry; quantify the net radiative forcings; and evaluate any surface climate impact. Experiment 2 is a nudged-run experiment from 2022 to 2023 using observed meteorology. To allow participation of more climate models with varying complexities of aerosol simulation, we include two sets of simulations in Experiment 2: Experiment 2a is designed for models with internally generated aerosol, while Experiment 2b is designed for models using prescribed aerosol surface area density. This experiment will help to analyze H 2 O and aerosol evolution, quantify the net radiative forcings, understand the impacts on mid-latitude and polar O 3 chemistry, and allow close comparisons with observations.

Zhu, Yunqian [Univ. of Colorado, Boulder, CO (Unit↗

dlppi2 (b1)

The Doppler lidar (DL) is an active remote-sensing instrument that provides range- and time-resolved measurements of the line-of-sight component of air velocity (i.e., radial velocity) and attenuated aerosol backscatter. The DL operates in the near-infrared and is sensitive to backscatter from atmospheric aerosol, which are assumed to be ideal tracers of atmospheric wind fields. The DL works by transmitting short pulses of infrared laser light into the atmosphere. Atmospheric aerosols scatter a small fraction of that light energy back to the transceiver, where it is collected and recorded as a time-resolved signal. From the delay between the outgoing pulse and the backscattered signal, the instrument infers the distance to the scattering volume. Coherent detection is used to measure the Doppler frequency shift of the backscatter signal. This is accomplished by mixing the backscatter signal with a reference laser beam (i.e., local oscillator) of known frequency. The onboard signal processor then determines the Doppler frequency shift from the spectrum of the mixed signal. The Doppler frequency shift and thus the radial air velocity is determined from the peak of the Doppler spectrum. The attenuated backscatter is determined from the energy content of the Doppler spectra. The DL provides accurate measurements of radial velocity in regions of the atmosphere where aerosol concentrations are high enough to ensure good signal-to-noise ratio. Thus, valid data are usually limited to the atmospheric boundary layer where aerosol is ubiquitous. Valid measurements can also be obtained in elevated aerosol layers or in optically thin clouds above the boundary layer. Most of the ARM DLs have full upper-hemispheric scanning capability, enabling 3D mapping of turbulent flows in the atmospheric boundary layer. With the scanner pointed vertically, the DL provides height- and time-resolved measurements of vertical velocity.

54 ENVIRONMENTAL SCIENCES↗

CPC data from TAMU TRACER campaign in the Houston, TX region from July to September 2022

During TRACER, the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V) was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Onboard the ROAM-V, aerosol samples are drawn through a shared isokinetic inlet at a flow rate ranging from 3.5 to 7.0 LPM. A portion of this flow is directed through a cyclone impactor (Brechtel, Inc. Model SCC 0.732) and 0.3 LPM is directed to the CPC. To correct the data for particle losses, we used a two-step method. First, the measured SMPS size distributions were used to calculate total particle loss through the inlet for every SMPS scan at a single deployment location. Second, the CPC data was corrected for particle losses using the average of the total losses per scan. This calculation was done separately for each deployment location due to changes in the measured size distributions between locations. Particle loss from diffusion (based on Kesten, 1991 and Gormley, 1949), inertial impaction in 90-degree bends (based on Aerosol Measurement, 2011 and Crane, 1977), and cyclone impactor efficiency (based on Dirgo, 1985) were included in the loss calculation. When the SMPS was not sampling at a location (in the case of an instrument malfunction or operator error), the reported CPC data was corrected with an average of the total losses for the entire campaign at the specified deployment location (e.g., if we needed to correct Galveston data, then the average of all calculated losses at Galveston was taken). These flatline corrections were used for all data on 22/07/13, 22/07/20, 22/07/22, and the data from Galveston on 22/08/09. An additional flatline correction of 14% was applied to all CPC data based on laboratory calibration prior to and after the campaign. In laboratory calibrations, we identified that for the same sample of air the field CPC (GRIMM Model 5.403 CPC) undercounted the total concentration of particles by 14% compared to the ground truth laboratory CPC (TSI Model 3750). This data was collected for ARM Field Campaign AFC07055 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Kesten et. al. Calibration of a TSI Model 3025 Ultrafine Condensation Particle Counter. Aerosol Science and Technology, 15:2, 107-111, 1991. Gormley et. al. Diffusion from a Stream Flowing through a Cylindrical Tube. Proceedings of the Royal Irish Academy, Vol 52, 163-169, 1948. Aerosol Measurement: Principles, Techniques, and Applications, Third Edition. John Wiley & Sons, Inc, 2011. Crane et. al. Inertial Deposition of Particles in a Bent Pipe. Journal of Aerosol Science, Vol 8, 161-170, 1977. Dirgo et. al. Cyclone Collection Efficiency: Comparison of Experimental Results with Theoretical Predictions. Aerosol Science and Technology, 4:4, 401-415, 1985.

54 ENVIRONMENTAL SCIENCES↗

Ice nucleation measurements from DRUM impactors during TRACER campaign in the Houston TX region from July to September 2022

During TRACER, three Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM) were used to collect aerosols for ice nucleation measurements in the Brooks laboratory at Texas A&M University. The three instruments were located at AMF1 in La Porte, Ancillary site in Guy (ANC), and onboard the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V). ROAM-V was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and one of the Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Each DRUM sampler was operated at a flow rate of 23 LPM. Each DRUM has four stages where the aerodynamic diameter size cuts are as follows: stage 1 larger than 3 μm, stage 2 from 3 to 1.2 μm, stage 3 from 1.2 to 0.34 μm, and stage 4 from 0.34 to 0.15 μm. Pretreated aluminum foil was used as a substrate on all stages. At AMF1 and ANC sites, the DRUMs were operated on the shared aerosol inlet, with generous support of the DOE ARM site staff. These instruments rotated 24 mm per day and only contained aluminum foil substrates. Substrates were changed weekly and transported to Texas A&M for storage in -80C freezer until analysis. The DRUM onboard ROAM-V was operated at a faster rotation rate of 150 mm per day to clearly separate the multiple deployment locations for ROAM-V. For the ROAM-V DRUM, substrates were changed every deployment and transported to Texas A&M for storage in -80C freezer until analysis. At Texas A&M, ice nucleation experiments were conducted to measure the ice nucleation temperature of the ambient aerosol samples collected from the three DRUMs using our previously established procedures (Alsante et al., 2023; Fornea et al., 2009; Matthews et al., 2023). For ice nucleation, only samples collected on stage 3 were analyzed, given that these are the most relevant size (1.2 to 0.34 μm diameter) for potential ice nucleating particles. For the AMF1 and ANC sites, we cut and analyzed 2 mm (2-hour) samples. We analyzed the time periods of the AMF1 site instrument when the ROAM-V was deployed. A 72-hour period from July 11th at 23:49 through July 15th at 1:49 was analyzed from the ANC site instrument. For the ROAM-V instrument, we separated the daily samples by site location. Between 1- and 6-hour independent samples were analyzed at each location. We also cut the ROAM-V samples in half to allow for compositional analysis of the aerosol on the other half of the substrate. All viable samples from the ROAM-V were analyzed. Analysis was done using a custom-built ice nucleation apparatus, recently updated to include an array of 16 individual samples (Matthews et al., 2023). On our experimental setup, we used 100 μL of Ultra-High-Performance Liquid Chromatography (UHPLC) water (Sigma Aldrich, >99.9% purity) to wash off the aerosol from the DRUM substrate. Then, we micropipetted 2 μL droplet samples into each of the 16 wells of the array, using hydrophobically coated microscope slides. Experiments would cycle 28 times from 10 C to -40C over a 20-hour period. During analysis of the TRACER samples, nine experiments were conducted with UHPLC water process blanks that followed an identical preparation procedure. The average freezing temperature and standard deviation for these process blanks is -27.7±2.4 C. This data was collected for ARM Field Campaign AFC07023 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Alsante, A. N., Thornton, D. C., & Brooks, S. D. (2023). Ice nucleation catalyzed by the photosynthesis enzyme RuBisCO and other abundant biomolecules. Communications Earth & Environment, 4(1), 51. Fornea, A. P., Brooks, S. D., Dooley, J. B., & Saha, A. (2009). Heterogeneous freezing of ice on atmospheric aerosols containing ash, soot, and soil. Journal of Geophysical Research: Atmospheres, 114(D13). DOI:10.1029/2009JD011958 Matthews, B. H., Alsante, A. N., & Brooks, S. D. (2023). Pollen Emissions of Subpollen Particles and Ice Nucleating Particles. ACS Earth and Space Chemistry.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: NO/NOx Analyzer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: NO2/NO/NOx Monitor (2B-Technology) Header: - NO2_2B[ppb]: Concentration of nitrogen dioxide (NO2) measured at the time of the sampling, expressed in parts per billion. - NO_2B[ppb]: Concentration of nitric oxide (NO) measured at the time of the sampling, expressed in parts per billion. - NOx_2B[ppb]: Total concentration of nitrogen oxides (NOx, which includes NO and NO2) measured at the time of the sampling, expressed in parts per billion.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Scanning Mobility Particle Sizer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Scanning Mobility Particle Sizer (TSI), DMA Classifier Model 3082 + CPC Detector Model 3752. Data Notes: The SMPS dataset is limited due to necessary instrument maintenance and subsequent extensive downtime. Data is only available from October 21 to November 8, 2023. Post November 22, 2023, the NanoScan instrument provided coverage for the latter half of the campaign. To ensure consistency, the data was resampled into uniform size bins ranging from 15 nm to 667 nm. This adjustment was required due to changes in size bins and the maximum diameter that occurred after maintenance and repairs. Multiple Charge Correction applied, Nanoparticle Agglomerate Mobility Analysis not applied, and Diffusion Correction applied. Header: - List [15 nm to 667 nm] middle of the size bin in nanometers: Data reports the concentration particles in this size bin per cubic centimeter, dN/dLog(dp). - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Nano-Scanning Mobility Particle Sizer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: NanoScan SMPS Nanoparticle Sizer 3910 (TSI). Data Notes: The NanoScan replaced our SMPS, on November 22nd 2023 and ran until the end of the campaign. Header: - List [11 nm to 365 nm] middle of the size bin in nanometers: Data reports the concentration particles in this size bin per cubic centimeter, dN/dLog(dp). - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Proton Transfer Reaction Mass Spectrometer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: IONICON High-Resolution PTR-TOF-MS - Trace VOC Analyzer. Concentrations were calculated based on theoretical reaction rates of each species with H3O+. Details of the calculation are found in the PTR-MS Ionicon Manual. Data Notes: It is a high-resolution PTR-TOF-MS we have sub-selected relevant species. Contact us if you want additional data products from this instrument. Header: - CalculatedAcetonitrile[ppbv]: The concentration of acetonitrile expressed in parts per billion by volume (ppbv). - CalculatedAcetaldehyde[ppbv]: The concentration of acetaldehyde expressed in parts per billion by volume (ppbv). - CalculatedAcetone[ppbv]: The concentration of acetone expressed in parts per billion by volume (ppbv). - CalculatedAceticAcid[ppbv]: The concentration of acetic acid expressed in parts per billion by volume (ppbv). - CalculatedIsoprene[ppbv]: The concentration of isoprene expressed in parts per billion by volume (ppbv). - CalculatedMVK[ppbv]: The concentration of methyl vinyl ketone (MVK) and methacrolein (MACR) expressed in parts per billion by volume (ppbv). - CalculatedMEK[ppbv]: The concentration of methyl ethyl ketone (MEK) expressed in parts per billion by volume (ppbv). - CalculatedBenzene[ppbv]: The concentration of benzene expressed in parts per billion by volume (ppbv). - CalculatedToluene[ppbv]: The concentration of toluene expressed in parts per billion by volume (ppbv).

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Aerodynamic Part Sizer

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Aerodynamic particle sizer (TSI) Files data_10min_APS.csv Header: - List [0.54 to 19.81] middle of the size bin in microns: Data reports the concentration particles in this size bin per cubic centimeter, dN/dLog(dp). - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Cloud Condensation Nuclei Counter

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Cloud Condensation Nuclei Counter, single column (Droplet Measurements Technology) Files: data_10sec_CCNc.csv, data_10min_CCNc.csv Header: - SuperSaturation[unitless]: The level of supersaturation, expressed as a unitless percentage, at which cloud condensation nuclei (CCN) activity is measured. - NumberConcentration[/cm3]: Number concentration of particles acting as CCN at the baseline supersaturation level, measured in particles per cubic centimeter. - NumberConcentration_SS2[/cm3]: Number concentration of particles acting as CCN at a supersaturation level of 0.2%, measured in particles per cubic centimeter. - NumberConcentration_SS4[/cm3]: Number concentration of particles acting as CCN at a supersaturation level of 0.4%, measured in particles per cubic centimeter. - QualityControl_Flag[bool]: A boolean flag indicating whether the data point passed quality control checks. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement.

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Gas Monitors

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: G2401 Gas Concentration Analyzer (Picarro) Data Notes: The Picarro G2401 gas concentration analyzer provides simultaneous, precise measurement of carbon monoxide (CO), carbon dioxide (CO2), methane (CH4) at parts-per-billion (ppb), and water (H2O) vapor at parts per-million (ppm) sensitivity with negligible drift for atmospheric science, air quality, and emissions quantification. Header: - CO[ppm]: Concentration of carbon monoxide (CO) measured at the time of sampling, expressed in parts per million (ppm). - CO2[ppm]: Concentration of carbon dioxide (CO2) measured at the time of sampling, expressed in parts per million (ppm). - CH4[ppm]: Concentration of methane (CH4) measured at the time of sampling, expressed in parts per million (ppm). - H2O[%]: Water vapor content in the air at the time of the measurement, expressed as a percentage

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: Ground based counterflow virtual impactor

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Ground based counter flow virtual impactor (Brechtel Inc) Data Notes: A factor of 6.7 needs to be applied to all cloud droplet residual concentration to correct the enhancement of the concentration because all the residual samples collected at 100 lpm were delivered into the 15 lpm of CVI sample flow. [https://amt.copernicus.org/articles/5/1259/2012/amt-5-1259-2012.html] Header: - Visibility[m]: The atmospheric visibility at the time of measurement, expressed in meters. - QualityControl_Flag[bool]: A boolean flag indicating whether the measurement passed quality control checks. - Temperature[C]: The ambient temperature at the time of the measurement, expressed in degrees Celsius. - CVI_Flag[bool]: A boolean flag indicating whether the Counterflow Virtual Impactor (CVI) was active (true) or inactive (false) during the measurement. - RelativeHumidity[%]: The relative humidity at the time of the measurement, expressed as a percentage

54 ENVIRONMENTAL SCIENCES↗

EPCAPE-PT-LANL Measurements: PM Modulair 1

Coastal cities offer a unique environment for studying aerosol-cloud interactions and the effects of urban emissions on cloud properties. As part of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE), the Partitioning Thrust by Los Alamos National Laboratory (EPCAPE-PT-LANL) was conducted. Our campaign focused on measuring the optical and chemical properties of aerosols and their interactions within marine stratocumulus clouds in La Jolla, California. EPCAPE-PT-LANL enhances the primary goals of EPCAPE through innovative observations of vapor-phase transitions between aerosols and cloud droplets, the impact of black carbon on aerosol-cloud dynamics, and the effects of cloud processing on aerosol optical properties. Instrument: Quant-AQ MODULAIR. Mounted external to the instrument container, near the GCVI inlet. The MODULAIR™ air quality monitor uses the same patent-pending PM sensor found in the MODULAIR™-PM and adds four gas-phase measurements (CO, NO, NO2, and O3) to provide an all-in-one solution. Files data_10sec_Quant_Gas.csv, data_10min_Quant_Gas.csv Header: - CO[ppb]: Concentration of carbon monoxide (CO) measured at the time of sampling, expressed in parts per billion (ppb) - NO[ppb]: Concentration of nitric oxide (NO) measured at the time of sampling, expressed in parts per billion (ppb). - O3[ppb]: Concentration of ozone (O3) measured at the time of sampling, expressed in parts per billion (ppb). - Temperature[C]: The ambient temperature at the time of the measurement, expressed in degrees Celsius. - RelativeHumidity[%]: The relative humidity at the time of the measurement, expressed as a percentage. Files data_10sec_Quant_PM.csv, data_10min_Quant_PM.csv Header: - PM1[ug/m3]: Concentration of particulate matter with a diameter of 1 micron or less, measured in micrograms per cubic meter (µg/m³). - PM2-5[ug/m3]: Concentration of particulate matter with a diameter of 2.5 microns or less measured in micrograms per cubic meter (µg/m³). - PM10[ug/m3]: Concentration of particulate matter with a diameter of 10 microns or less, measured in micrograms per cubic meter (µg/m³). - Temperature[C]: The ambient temperature at the time of the measurement, expressed in degrees Celsius. - RelativeHumidity[%]: The relative humidity at the time of the measurement, expressed as a percentage.

54 ENVIRONMENTAL SCIENCES↗

Dust-planetary boundary layer interactions amplified by entrainment and advections

Mineral dust contributes to more than half of the global aerosol loading. However, the radiative impacts of dust aerosols on planetary boundary layer (PBL) structure have not been explored sufficiently. During a typical dust storm event over Tarim Basin, dust aerosols exhibit a well-mixed distribution during the daytime in spite of a shallow layer of dust particles accumulated at higher altitudes. By contrast, nocturnal dust plumes are located near the surface due to stable stratification. We demonstrate that these differentiated vertical distributions determine the spatial heterogeneity of dust loading, radiative fluxes and PBL height variations. Dust aerosols cause daytime PBL suppression and nighttime PBL promotion through modulating surface and atmospheric radiative budgets. Specifically, dust-induced cooling effect within PBL directly inhibits the daytime PBL development. PBL suppression effect is then amplified by entrainment processes resulting in excessively low PBL height, especially for dust particles below but near the PBL top. Dust plumes weaken updrafts from PBL and downdrafts of the free atmosphere, which further reduce the entrainment mixing through attenuating horizontal and vertical advection, and eventually amplify PBL suppression. At night, near-surface dust aerosols stimulate a warm and unstable lower atmosphere, generate warm advection heating and promote the PBL development. Our study highlights the importance of specifying entrainment parameters and nighttime advection activities in quantifying the dust-PBL interactions.

54 ENVIRONMENTAL SCIENCES↗

Cloud Condensation Nuclei Closure Study Using Airborne Measurements Over the Southern Great Plains

Abstract Airborne measurements of non‐refractory bulk aerosol chemical composition, aerosol size distributions, and cloud condensation nuclei (CCN) were conducted onboard a research aircraft during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems field campaign in the spring and summer of 2016. A CCN closure study for the entire campaign period was performed where measured CCN concentrations at 0.24% and 0.46% supersaturation were compared with the predicted CCN concentrations calculated using κ ‐Köhler theory, three different assumptions of aerosol mixing state, and various assumptions about hygroscopicity, density, and the insoluble fraction of organic particles. We found that the Closure Ratio (CR), calculated as the ratio of predicted to measured CCN concentrations, was equal to one under two different aerosol mixing state assumptions: (a) all particles are composed of 100% organic particles, and (b) particles are externally mixed and composed of pure sulfates, nitrates, and organic particles assuming hygroscopicity values for organic particles ( ) between 0.04 and 0.17. The use of internal mixing state assumption often led to overprediction of CCN concentrations but the agreement within ±20% with the measured CCN concentrations was observed under certain closure permutations. A similar agreement, that is, within ±20%, was also observed using permuted parameters concerning density (1 and 1.5 g cm −3 ) and an insoluble fraction (0% and 20%) of organic particles. These findings may provide constraints on to predict CCN concentrations at a remote continental Southern Great Plains site.

54 ENVIRONMENTAL SCIENCES↗

Size-resolved Eddy-Covariance Particle Flux Measurement during the TRACER Campaign (Final Report)

The main goal of the TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign was to study aerosol–cloud interactions during deep convection over the Houston area. This project deployed a suite of instrumentation with the aim to (1) quantify turbulent vertical particle fluxes during at DOE-ARM sites, including TRACER, (2) assess hygroscopic growth factors and hygroscopicity parameters of the material driving modal aerosol growth during new particle formation and growth events, (3) derive turbulent aerosol mass fluxes using co-located Doppler LIDAR measurements, and (4) create quality-controlled PI data products to support future research utilizing data collected during the TRACER campaign. This report summarized the main findings from the deployments at two DOE-ARM sites. Briefly, we found that new particle formation may occur aloft, in a residual layer, near the top of the boundary layer. Small grown particles appear later due to downward mixing with daytime turbulence. The species that are responsible for aerosol modal growth had hygroscopicity parameters varying between 0.05 and 0.34. These values systematically depended on the wind sector, suggesting that the chemical composition of the precursors differed. This work demonstrated that lidar retrievals of the elastic backscatter and Doppler velocity can be used to obtain surface number emissions of particles with a diameter greater than 0.53 µm. During TRACER, emission particle number fluxes peaked near ∼ 100 cm−2 s−1. Multiple quality-controlled PI data products that will support future TRACER related science were generated and made publically available.

54 ENVIRONMENTAL SCIENCES↗