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DOE OSTI2021

Drop Size Distribution Variability in Central Argentina during RELAMPAGO-CACTI

The Remote sensing of Electrification, Lightning, And Meso-scale/micro-scale Processes with Adaptive Ground Observations (RELAMPAGO) and the Cloud, Aerosol, and Complex Terrain Interactions Experiment Proposal (CACTI) field campaigns provided an unprecedented thirteen-disdrometer dataset in Central Argentina during the Intensive (IOP, 15 November to 15 December 2018) and Extended (EOP, 15 October 2018 to 30 April 2019) Observational Periods. The drop size distribution (DSD) parameters and their variability were analyzed across the region of interest, which was divided into three subregions characterized by the differing proximity to the Sierras de Córdoba (SDC), in order to assess the impact of complex terrain on the DSD parameters. A rigorous quality control of the data was first performed. The frequency distributions of DSD-derived parameters were analyzed, including the normalized intercept parameter (logN w ), the mean volume diameter (D 0 ), the mean mass diameter (D m ), the shape parameter (μ), the liquid water content (LWC), and the rain rate (R). The region closest to the SDC presented higher values of logN w , lower D 0 , and higher μ, while the opposite occurred in the farthest region, i.e., the concentration of small drops decreased while the concentration of bigger drops increased with the distance to the east of the SDC. Furthermore, the region closest to the SDC showed a bimodal distribution of D 0 : the lower values of D 0 were associated with higher values of logN w and were found more frequently during the afternoon, while the higher D 0 were associated with lower logN w and occurred more frequently during the night. The data were analyzed in comparison to the statistical analysis of Dolan et al. 2018 and sorted according to the classification proposed in the cited study. The logN w -D 0 and LWC-D 0 two-dimensional distributions allowed further discussion around the applicability of other mid-latitude and global precipitation classification schemes (startiform/convection) in the region of interest. Finally, three precipitation case studies were analyzed with supporting polarimetric radar data in order to relate the DSD characteristics to the precipitation type and the microphysical processes involved in each case.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Phase Doppler Interferometry for Efficient Cloud Drop Size Distribution, Number Density, and LWC Measurements

Threats to aviation safety as a result of super-cooled large drops (SLD) has been addressed by the FAA rules change (14 CFR Part 25) with the additional icing certification requirement. SLD clouds often consist of bi-modal drop size spectra leading to significant problems in simulating and characterizing these conditions in situ and in icing wind tunnels. Legacy instrumentation for measuring drop size distributions and liquid water content are challenged under these conditions. The large size range measurement problem is addressed with the development of the Phase Doppler Interferometer, Flight Probe Dual-Range (PDI FPDR). The method is described in this report along with the measurement capabilities including the dynamic measurement range and overall working size range. The PDI instrument bases drop size measurements on the light wavelength as the measurement length scale. The light wavelength is a much more robust scale, especially as compared to the light scattering intensity. Additionally, methods for accurately characterizing the sample volume in situ based on measured drop velocity and transit time are reviewed, given the importance of this parameter for merging results and measuring LWC. Droplet coincidence in the sample volume can be problematic so this condition is treated with an innovative signal parsing approach. Measurement examples acquired in the NASA IRT are provided. Measurements of LWC showed good agreement with the Artium Particle Imaging (PI) instrument but diverged from the tunnel calibration results for larger MVD values.

42 ENGINEERING↗

DOE OSTI2020

Impacts of long-range transport of aerosols on marine-boundary-layer clouds in the eastern North Atlantic

Vertical profiles of aerosols are inadequately observed and poorly represented in climate models, contributing to the current large uncertainty associated with aerosol–cloud interactions. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) aircraft field campaign near the Azores islands provided ample observations of vertical distributions of aerosol and cloud properties. Here we utilize the in situ aircraft measurements from the ACE-ENA and ground-based remote-sensing data along with an aerosol-aware Weather Research and Forecast (WRF) model to characterize the aerosols due to long-range transport over a remote region and to assess their possible influence on marine-boundary-layer (MBL) clouds. The vertical profiles of aerosol and cloud properties measured via aircraft during the ACE-ENA campaign provide detailed information revealing the physical contact between transported aerosols and MBL clouds. The European Centre for Medium-Range Weather Forecasts Copernicus Atmosphere Monitoring Service (ECMWF-CAMS) aerosol reanalysis data can reproduce the key features of aerosol vertical profiles in the remote region. The cloud-resolving WRF sensitivity experiments with distinctive aerosol profiles suggest that the transported aerosols and MBL cloud interactions (ACIs) require not only aerosol plumes to get close to the marine-boundary-layer top but also large cloud top height variations. Based on those criteria, the observations show that the occurrence of ACIs involving the transport of aerosol over the eastern North Atlantic (ENA) is about 62 % in summer. For the case with noticeable long-range-transport aerosol effects on MBL clouds, the susceptibilities of droplet effective radius and liquid water content are -0.11 and +0.14, respectively. When varying by a similar magnitude, aerosols originating from the boundary layer exert larger microphysical influence on MBL clouds than those entrained from the free troposphere.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Comprehensive quantification of height dependence of entrainment mixing between stratiform cloud top and environment

Different entrainment-mixing processes of turbulence are crucial to processes related to clouds; however, only a few qualitative studies have been concentrated on the vertical distributions of entrainment-mixing mechanisms with low vertical resolutions. To quantitatively study vertical profiles of entrainment-mixing mechanisms with a high resolution, the stratiform clouds observed in the Physics of Stratocumulus Top (POST) project are examined. The unique sawtooth flight pattern allows for an examination of the vertical distributions of entrainment-mixing mechanisms with a 5 m vertical resolution. Relative standard deviation of volume mean radius divided by relative standard deviation of liquid water content is introduced to be a new estimation of microphysical homogeneous mixing degree, to overcome difficulties of determining the adiabatic microphysical properties required in existing measures. The vertical profile of this new measure indicates that entrainment-mixing mechanisms become more homogeneous with decreasing altitudes and are consistent with the dynamical measures of Damköhler number and transition scale number. Further analysis shows that the vertical variation of entrainment-mixing mechanisms with decreasing altitudes is due to the increases of turbulent dissipation rate in cloud and relative humidity in droplet-free air and the decrease of size of droplet-free air. The results offer insights into the theoretical understanding and parameterizations of vertical variation of entrainment-mixing mechanisms.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Impacts of long-range-transported mineral dust on summertime convective cloud and precipitation: a case study over the Taiwan region

As one of the most abundant atmospheric aerosols and effective ice nuclei, mineral dust affects clouds and precipitation in the Earth system. Here numerical experiments are carried out to investigate the impacts of dust aerosols on summertime convective clouds and precipitation over the mountainous region of Taiwan by acting as ice-nucleating particles. We run the Weather Research and Forecasting model (WRF) with the Morrison two-moment and spectral-bin microphysics (SBM) schemes at 3 km resolution, using dust number concentrations from a global chemical transport model (GEOS-Chem-APM). The case study indicates that the long-range-transported mineral dust, with relatively low number concentrations, can notably affect the properties of convective clouds (ice and liquid water contents, cloud top height, and cloud coverage) and precipitation (spatial pattern and intensity). The effects of dust are evident during strong convective periods, with significantly increased ice water contents in the mixed-phase regime via the enhanced heterogeneous freezing. With both the Morrison and SBM schemes, we see the invigoration effects of dust aerosols on the convective intensity through enhanced condensation and deposition latent heating. The low-altitude dust particles are uplifted to the freezing level by updrafts, which, in turn, enhance the convective cloud development through immersion freezing and convective invigoration. Compared to the Morrison scheme, the SBM scheme predicts more realistic precipitation and different invigoration effects of dust. The differences are partially attributed to the saturation adjustment approach utilized in the bulk scheme, which leads to a stronger enhancement of condensation at midlatitudes to low altitudes and a weaker deposition increase at the upper level.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

The importance of Aitken mode aerosol particles for cloud sustenance in the summertime high Arctic – a simulation study supported by observational data

The potential importance of Aitken mode particles (diameters ~ 25–80 nm) for stratiform mixed-phase clouds in the summertime high Arctic (>80° N) has been investigated using two large-eddy simulation models. We find that, in both models, Aitken mode particles significantly affect the simulated microphysical and radiative properties of the cloud and can help sustain the cloud when accumulation mode concentrations are low (< 10–20 cm –3 ), even when the particles have low hygroscopicity (hygroscopicity parameter – κ=0.1). However, the influence of the Aitken mode decreases if the overall liquid water content of the cloud is low, either due to a higher ice fraction or due to low radiative cooling rates. An analysis of the simulated supersaturation (ss) statistics shows that the ss frequently reaches 0.5 % and sometimes even exceeds 1 %, which confirms that Aitken mode particles can be activated. The modelling results are in qualitative agreement with observations of the Hoppel minimum obtained from four different expeditions in the high Arctic. Our findings highlight the importance of better understanding Aitken mode particle formation, chemical properties and emissions, particularly in clean environments such as the high Arctic.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Quantifying vertical wind shear effects in shallow cumulus clouds over Amazonia

Abstract. This study analyses and quantifies the effects of vertical wind shear (VWS) on the properties of shallow cumulus cloud fields over Central Amazonia. We perform idealised simulations with high resolution (50 m horizontally and 20 m vertically) using the Dutch Atmospheric Large-Eddy Simulation (DALES) model, changing the initial conditions and large-scale forcing of VWS. The resulting cloud field is analysed by applying a cloud tracking algorithm to generate Lagrangian datasets of the life cycle of individual clouds as well as their time-varying core and margin dimensions. The reference run has no wind speed or directional shear and represents a typical day in the local dry season. Numerical experiments with moderate and high wind speed shear are simulated by adding linear increases in the wind speed of 1.2 and 2.4 m s−1 km−1, respectively. Three additional runs are made by adding 90∘ of wind rotation between the surface and the top of the domain (5 km) on top of the three wind speed shear conditions. We find that clouds developing in a sheared environment have horizontal equivalent diameter increased by up to 100 m on average, but the cloud depth is reduced. Our quantification shows that VWS tends to increase the size of the cloud cores but reduces their relative area, volume, and mass fractions compared to the overall cloud dimensions. The addition of 2.4 m s−1 km−1 of VWS decreases the relative core area by about 0.03 (about 10 % of the overall average) and its volume and mass ratios by about 0.05 (10 %–25 % in relative terms). Relevant for the cloud transport properties is that the updraught speed and the liquid water content are lower within the cores, and consequently so is the upward mass flux. All quantifications of mean cloud properties point to the inhibition of convective strength by VWS, therefore hampering the shallow-to-deep transition. However, open questions still remain given that the individually deepest clouds were simulated under high environmental shear, even though they occur in small numbers. This could indicate other indirect effects of VWS that have opposite effects on cloud development if found to be significant in the future.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

The influence of multiple groups of biological ice nucleating particles on microphysical properties of mixed-phase clouds observed during MC3E

Abstract. A new empirical parameterization (EP) for multiple groups of primary biological aerosol particles (PBAPs) is implemented in the aerosol–cloud model (AC) to investigate their roles as ice nucleating particles (INPs). The EP describes the heterogeneous ice nucleation by (1) fungal spores, (2) bacteria, (3) pollen, (4) detritus of plants, animals, and viruses, and (5) algae. Each group includes fragments from the originally emitted particles. A high-resolution simulation of a midlatitude mesoscale squall line by AC is validated against airborne and ground observations. Sensitivity tests are carried out by varying the initial vertical profiles of the loadings of individual PBAP groups. The resulting changes in warm and ice cloud microphysical parameters are investigated. The changes in warm microphysical parameters, including liquid water content and cloud droplet number concentration, are minimal (<10 %). Overall, PBAPs have little effect on the ice number concentration (<6 %) in the convective region. In the stratiform region, increasing the initial PBAP loadings by a factor of 1000 resulted in less than 40 % change in ice number concentrations. The total ice concentration is mostly controlled by various mechanisms of secondary ice production (SIP). However, when SIP is intentionally shut down in sensitivity tests, increasing the PBAP loading by a factor of 100 has an effect of less than 3 % on the ice phase. Further sensitivity tests revealed that PBAPs have little effect on surface precipitation and on the shortwave and longwave flux (<4 %) for a 100-fold perturbation in PBAPs.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Assessing the cloud radiative bias at Macquarie Island in the ACCESS-AM2 model

Abstract. As a long-standing problem in climate models, large positive shortwave radiation biases exist at the surface over the Southern Ocean, impacting the accurate simulation of sea surface temperature, atmospheric circulation, and precipitation. Underestimations of low-level cloud fraction and liquid water content are suggested to predominantly contribute to these radiation biases. Most model evaluations for radiation focus on summer and rely on satellite products, which have their own limitations. In this work, we use surface-based observations at Macquarie Island to provide the first long-term, seasonal evaluation of both downwelling surface shortwave and longwave radiation in the Australian Community Climate and Earth System Simulator Atmosphere-only Model version 2 (ACCESS-AM2) over the Southern Ocean. The capacity of the Clouds and the Earth’s Radiant Energy System (CERES) product to simulate radiation is also investigated. We utilize the novel lidar simulator, the Automatic Lidar and Ceilometer Framework (ALCF), and all-sky cloud camera observations of cloud fraction to investigate how radiation biases are influenced by cloud properties. Overall, we find an overestimation of +9.5±33.5 W m−2 for downwelling surface shortwave radiation fluxes and an underestimation of -2.3±13.5 W m−2 for downwelling surface longwave radiation in ACCESS-AM2 in all-sky conditions, with more pronounced shortwave biases of +25.0±48.0 W m−2 occurring in summer. CERES presents an overestimation of +8.0±18.0 W m−2 for the shortwave and an underestimation of -12.1±12.2 W m−2 for the longwave in all-sky conditions. For the cloud radiative effect (CRE) biases, there is an overestimation of +4.8±28.0 W m−2 in ACCESS-AM2 and an underestimation of -7.9±20.9 W m−2 in CERES. An overestimation of downwelling surface shortwave radiation is associated with an underestimated cloud fraction and low-level cloud occurrence. We suggest that modeled cloud phase is also having an impact on the radiation biases. Our results show that the ACCESS-AM2 model and CERES product require further development to reduce these radiation biases not just in shortwave and in all-sky conditions, but also in longwave and in clear-sky conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

High sensitivity of simulated fog properties to parameterized aerosol activation in case studies from ParisFog

Aerosols influence fog properties such as visibility and lifetime by affecting fog droplet number concentrations (N d ). Numerical weather prediction (NWP) models often represent aerosol–fog interactions using highly simplified approaches. Incorporating prognostic size-resolved aerosol microphysics from climate models could allow them to simulate N d and aerosol–fog interactions without incurring excessive computational expense. However, microphysics code designed for coarse spatial resolution may struggle with sub-kilometer-scale grid spacings. Here, we test the ability of the UK Met Office Unified Model to simulate aerosol and fog properties during case studies from the ParisFog field campaign in 2011. We examine the sensitivity of fog properties to variations in N d caused by modifications to simulated aerosol activation. Our model, with a 500 m horizontal resolution and interactive aerosol and cloud microphysics, significantly underpredicts N d , although it only slightly underestimates the cloud condensation nuclei concentration. With an updated version of the Abdul-Razzak and Ghan (2000) activation scheme, we produce N d that are more consistent with those predicted by a cloud parcel model under fog-like conditions. We activate droplets only by adiabatic cooling. We incorporate more realistic hygroscopicities for sulfate and organic aerosols and explore the sensitivity of simulated N d to unresolved updrafts. We find that both N d and simulated fog liquid water content are very sensitive to the updated activation scheme but remain less affected by the update to hygroscopicities. Our improvements offer insights into the physical processes regulating N d in stable conditions, potentially laying foundations for improved operational fog forecasts that incorporate interactive aerosol simulations or aerosol climatologies.

Ghosh, Pratapaditya [Carnegie Mellon University, P↗

DOE OSTI2022

Rain on snow (ROS) understudied in sea ice remote sensing: a multi-sensor analysis of ROS during MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate)

Abstract. Arctic rain on snow (ROS) deposits liquid water onto existing snowpacks. Upon refreezing, this can form icy crusts at the surface or within the snowpack. By altering radar backscatter and microwave emissivity, ROS over sea ice can influence the accuracy of sea ice variables retrieved from satellite radar altimetry, scatterometers, and passive microwave radiometers. During the Arctic Ocean MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, there was an unprecedented opportunity to observe a ROS event using in situ active and passive microwave instruments similar to those deployed on satellite platforms. During liquid water accumulation in the snowpack from rain and increased melt, there was a 4-fold decrease in radar energy returned at Ku- and Ka-bands. After the snowpack refroze and ice layers formed, this decrease was followed by a 6-fold increase in returned energy. Besides altering the radar backscatter, analysis of the returned waveforms shows the waveform shape changed in response to rain and refreezing. Microwave emissivity at 19 and 89 GHz increased with increasing liquid water content and decreased as the snowpack refroze, yet subsequent ice layers altered the polarization difference. Corresponding analysis of the CryoSat-2 waveform shape and backscatter as well as AMSR2 brightness temperatures further shows that the rain and refreeze were significant enough to impact satellite returns. Our analysis provides the first detailed in situ analysis of the impacts of ROS and subsequent refreezing on both active and passive microwave observations, providing important baseline knowledge for detecting ROS over sea ice and assessing their impacts on satellite-derived sea ice variables.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

ARM Aerial Facility (AAF) - Unmanned Aircraft Systems, Cloud Droplet Probe

The Cloud Droplet Probe (CDP) is designed to measure cloud droplet size distribution from 2 µm to 50 µm. The CDP and an appropriate data system can also calculate various other parameters including particle concentrations, effective diameter (ED), Median Volume Diameter (MVD), and Liquid Water Content (LWC).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

60v1varanaecmwf (c1)

60v1varanaecmwf

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

60v0varanaecmwf (c1)

60v0varanaecmwf

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

ARM Aerial Facility (AAF) - Unmanned Aircraft Systems, Cloud Droplet Probe with QC and lat/lon/alt

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Profiles of Radiative Fluxes at ENA

Profiles of radiative fluxes observed at the Atmospheric Radiation Measurement (ARM)’s Eastern North Atlantic (ENA) observatory along with the ancillary measurements are reported. The below-cloud drizzle properties were derived by combining the data from the ceilometer and Ka-band ARM Zenith Radar (KAZR) following the technique explained by Ghate et al. (2021 JAMC). The cloud and drizzle water path values were derived from the brightness temperatures reported by the microwave radiometer following the technique of Cadeddu et al. (2020 AMT). The cloud water path was then scaled to the KAZR-reported radar reflectivity to calculate profiles of liquid water content (LWC). Following the analysis from Ghate et al. (2023 JGR), cloud droplet effective radius was calculated using the number concentration value of 100 cm-3. The cloud properties, along with the thermodynamic properties, served as an input to the Rapid Radiative Transfer Model (RRTM) to yield profiles of radiative fluxes at a 1-minute temporal and 50-m vertical resolution. The fluxes were then averaged to hourly temporal resolution for analysis. In Mitra et al. (2025 JClim), the calculated profiles were compared against those derived from the satellite measurements (SYN1deg). Flux profiles from the SYN1deg and the thermodynamic and cloud properties used for deriving them are also reported here. Both all-sky and clear-sky radiative flux profiles were calculated. Due to the large data volume, the surface and top-of-atmosphere (TOA) radiative fluxes for the six-year period, and the hourly profiles of the radiative fluxes for January 2018, are submitted here. Full profiles of radiative fluxes calculated from the thermodynamic and cloud properties measured at the ENA site at 1-minute temporal and 50-m vertical resolution for a six-year period are available from the authors. Six files here correspond to the following data: 1_ENARAD_CERES_with_cld_amount_timeseries.nc: Time-series of hourly values of RRTM-simulated values of upwelling and downwelling fluxes at the surface and TOA, observed boundary-layer cloud fractions, and upwelling and downwelling fluxes from the SYN1deg from July 2015 to January 2022. 2_CERES_2018_at_CERES_levels.nc: SYN1deg radiative fluxes at six levels for the year 2018. 3_ENARad_2018_at_CERES_levels.nc: RRTM calculated fluxes at the SYN1deg vertical levels for the year 2018. 4_ENARad_rrtminputs_hourly_201801.nc: Thermodynamic and cloud properties used as an input to the RRTM for January 2018. 5_CERES_inputs_hourly_201801.nc: Thermodynamic and cloud properties utilized by SYN1deg algorithm for January 2018. 6_ENARAD_hourly_201801.nc: Full profiles of hourly averaged radiative fluxes from the RRTM simulations for January 2018.

Atmosphere↗

DOE OSTI2022

Estimating Drizzle Parameters by Aircraft Sampling

In-cloud supersaturation is calculated from aircraft derived measurements of the in-cloud vertical gradient of liquid water content, vertical velocity, the pt and 3 rd cloud droplet radius moments and a parameter related to the heat and mass transport during condensation and evaporation of cloud droplets. The aircraft data where taken during the VOCALS 2008 study in marine stratocumulus clouds off the coast of Chile. Approximately 16000 discrete samples, 2.5 meter in length, were used in the present analysis of in-cloud supersaturation and its variability, both of which are indicative of turbulent processes within the cloud and their significant impact on drizzle formation. Two additional drizzle parameters, the eddy persistence time and the variance of fluctuations in in-cloud droplet growth rate were also estimated from this data set. These results will help to constrain parameterizations of underlying turbulent microphysical processes of clouds and thereby advance the future development of warm cloud and precipitation models for climate simulation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Fast and Non-Destructive Determination of Water Content in Ionic Liquids at Varying Temperatures by Raman Spectroscopy and Multivariate Regression Analysis

Imidazolium acetate ionic liquids (ILs) have been utilized as promising solvents in many applications that involve varying water content and temperature. These experimental variables affect the anion-cation intermolecular interactions, which in turn influence the performance of the ILs in these applications. Here, this paper shows Raman spectroscopy can be used as an operando method to measure water content in IL solvents when simultaneous temperature changes may occur. The Raman spectra of 1-alkyl-3-methylimidazolium acetate ILs (alkyl chain length n = 2, 4, 6, 8) with varying water content (from 0.028 to 0.899 water mole fraction) and temperature (from 78.1 K to 423.1 K) were measured. Increasing the water content or decreasing the temperature of the tested ILs weakens the anion-cation intermolecular interactions. The water content of these ILs can be quantified even in conditions when the temperature is changing using Raman spectroscopy combined with multivariate regression analysis, including principal component regression (PCR), partial-least-squares regression (PLSR), and artificial neural networks (ANNs). The ANN model combined with partial-least-squares (PLS) achieves the highest prediction accuracy of water content in ILs at varying temperatures (RMSECV = 0.017, R 2 CV = 99.1%, RMSEP = 0.019, R 2 P = 98.8%, RPD = 8.93). Raman spectroscopy provides a potential fast non-destructive operando method to monitor the water content of ILs even in applications when the temperature may be simultaneously altered; this information can lead to the optimized use of these ILs in many applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗