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Mei, Fan

Publications and source records attributed to Mei, Fan.

At least 37 records · Page 2

Tethered balloon system and High-Resolution Mass Spectrometry Reveal Increased Organonitrates Aloft Compared to the Ground Level

Atmospheric particles play critical roles in climate. However, significant knowledge gaps remain regarding the vertically resolved organic molecular-level composition of atmospheric particles due to aloft sampling challenges. To address this, we use a tethered balloon system at the Southern Great Plains Observatory and high-resolution mass spectrometry to, respectively, collect and characterize organic molecular formulas (MF) in the ground level and aloft (up to 750 m) samples. We show that organic MF uniquely detected aloft were dominated by organonitrates (139 MF; 54% of all uniquely detected aloft MF). Organonitrates that were uniquely detected aloft featured elevated O/C ratios (0.73 ± 0.23) compared to aloft organonitrates that were commonly observed at the ground level (0.63 ± 0.22). Unique aloft organic molecular composition was positively associated with increased cloud coverage, increased aloft relative humidity (~40% increase compared to ground level), and decreased vertical wind variance. Furthermore, 29% of extremely low volatility organic compounds in the aloft sample were truly unique to the aloft sample compared to the ground level, emphasizing potential oligomer formation at higher altitudes. Overall, this study highlights the importance of considering vertically resolved organic molecular composition (particularly for organonitrates) and hypothesizes that aqueous phase transformations and vertical wind variance may be key variables affecting the molecular composition of aloft organic aerosol.

54 ENVIRONMENTAL SCIENCES↗

ARM Aerial Facility (AAF) Merged Value-Added Product Report for Historical G-1 Field Campaigns

For 30 years, the U.S. Department of Energy (DOE) Office of Science supported an instrumented Grumman Gulfstream-1 (G-1) aircraft for atmospheric field campaigns. Data from the final decade of G-1 operations were archived by the Atmospheric Radiation Measurement (ARM) user facility Data Center (ADC) and made publicly available at no cost to all registered users. To ensure a consistent data format and to improve the accessibility of the ARM airborne data, an integrated data set was recently developed covering the final six years of G-1 operations (2013 to 2018). The integrated data set includes data collected from 236 flights (766.4 hours). Four of the seven field campaigns were based in the U.S. One campaign collected data from the wildfires in the U.S. Pacific Northwest and agricultural burns in the lower Mississippi River valley as part of the Biomass Burning Observation Project (BBOP) in 2013. In 2015, the ARM Cloud Aerosol Precipitation Experiment provided data on atmospheric rivers and associated aerosol-cloud interactions that produce heavy precipitation on the U.S. west coast during the early spring. Research data from Airborne Carbon Measurements-V (ACME-V), collected during the summer of 2015, gave scientists insight into trends and variability of trace gases in the atmosphere over the North Slope of Alaska to improve arctic climate models. In the early summer and autumn of 2016, the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign provided an extensive data set geared toward coupled processes that affect the life cycle of shallow clouds through the interaction among aerosol, cloud, land surface, and ecosystems. In 2014 (March and October), the airborne sampling moved outside of the U.S. to the city of Manaus in central Amazonia, Brazil, where residential and industrial emissions were extensively characterized by flights of the G-1. The GoAmazon2014/15 aircraft campaign data are being integrated with aquatic and terrestrial ecosystem measurements to quantify anthropogenic perturbations to a usually pristine tropical environment. Another international airborne mission was carried out in the Eastern North Atlantic region. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign saw the G-1 aircraft fly from Terceira Island in the Azores during the summer of 2017 and the winter of 2018. The campaign studied both seasons to measure key aerosol and cloud processes under various meteorological and cloud conditions with different aerosol sources. Then the G-1 deployed to the Sierras de Córdoba range in central Argentina from October to November 2018 for the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign to study orographic convective cloud interactions with their surrounding environment. These comprehensive datastreams provide much-needed insight into spatiotemporal variability of thermodynamic quantities, aerosol and cloud states, and properties for addressing essential science questions in Earth system process studies.

54 ENVIRONMENTAL SCIENCES↗

Bridging New Observational Capabilities and Process-Level Simulation: Insights into Aerosol Roles in the Earth System

The spatial distribution of ambient aerosol particles significantly impacts aerosol–radiation–cloud interactions, which contribute to the largest uncertainty in global anthropogenic radiative forcing estimations. However, the atmospheric boundary layer and lower free troposphere have not been adequately sampled in terms of spatiotemporal resolution, hindering a comprehensive characterization of various atmospheric processes and impeding our understanding of the Earth system. To address this research data gap, we have leveraged the development of uncrewed aerial systems (UAS) and advanced measurement techniques to obtain mesoscale spatial data on aerosol microphysical and optical properties around the U.S. Southern Great Plains (SGP) atmospheric observatory. Our study also benefits from state-of-the-art laboratory facilities that include three-dimensional molecular imaging techniques enabled by secondary ion mass spectrometry and nanogram-level chemical composition analysis via micronebulization aerosol mass spectrometry. Through our study, we have developed a framework for observation–modeling integration, enabling an examination of how various assumptions about the organic–inorganic components mixing state, inferred from chemical analysis, affect clouds and radiation in observation-constrained model simulations. By integrating observational constraints (derived from offline chemical analysis of the aerosol surface using collected samples) with in situ UAS observations, we have identified a prominent role of organic-enriched nanometer layers located at the surface of aerosol particles in determining profiles of aerosol optical and hygroscopic properties over the SGP observatory. Furthermore, we have improved the agreement between predicted clouds and ground-based cloud lidar measurements. This UAS–model–laboratory integration exemplifies how these new advanced capabilities can significantly enhance our understanding of aerosol–radiation–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

ARM Aerial Facility (AAF) Merged Value-Added Product Report for Historical G-1 Field Campaigns

For 30 years, the U.S. Department of Energy (DOE) Office of Science supported an instrumented Grumman Gulfstream-1 (G-1) aircraft for atmospheric field campaigns. Data from the final decade of G-1 operations were archived by the Atmospheric Radiation Measurement (ARM) user facility Data Center (ADC) and made publicly available at no cost to all registered users. To ensure a consistent data format and to improve the accessibility of the ARM airborne data, an integrated data set was recently developed covering the final six years of G-1 operations (2013 to 2018). The integrated data set includes data collected from 236 flights (766.4 hours). Four of the seven field campaigns were based in the U.S. One campaign collected data from the wildfires in the U.S. Pacific Northwest and agricultural burns in the lower Mississippi River valley as part of the Biomass Burning Observation Project (BBOP) in 2013. In 2015, the ARM Cloud Aerosol Precipitation Experiment provided data on atmospheric rivers and associated aerosol-cloud interactions that produce heavy precipitation on the U.S. west coast during the early spring. Research data from Airborne Carbon Measurements-V (ACME-V), collected during the summer of 2015, gave scientists insight into trends and variability of trace gases in the atmosphere over the North Slope of Alaska to improve arctic climate models. In the early summer and autumn of 2016, the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign provided an extensive data set geared toward coupled processes that affect the life cycle of shallow clouds through the interaction among aerosol, cloud, land surface, and ecosystems. In 2014 (March and October), the airborne sampling moved outside of the U.S. to the city of Manaus in central Amazonia, Brazil, where residential and industrial emissions were extensively characterized by flights of the G-1. The GoAmazon2014/15 aircraft campaign data are being integrated with aquatic and terrestrial ecosystem measurements to quantify anthropogenic perturbations to a usually pristine tropical environment. Another international airborne mission was carried out in the Eastern North Atlantic region. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign saw the G-1 aircraft fly from Terceira Island in the Azores during the summer of 2017 and the winter of 2018. The campaign studied both seasons to measure key aerosol and cloud processes under various meteorological and cloud conditions with different aerosol sources. Then the G-1 deployed to the Sierras de Córdoba range in central Argentina from October to November 2018 for the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign to study orographic convective cloud interactions with their surrounding environment. These comprehensive datastreams provide much-needed insight into spatiotemporal variability of thermodynamic quantities, aerosol and cloud states, and properties for addressing essential science questions in Earth system process studies.

54 ENVIRONMENTAL SCIENCES↗

Mapping the performance of a versatile water-based condensation particle counter (vWCPC) with numerical simulation and experimental study

Accurate airborne aerosol instrumentation is required to determine the spatial distribution of ambient aerosol particles, particularly when dealing with the complex vertical profiles and horizontal variations of atmospheric aerosols. A versatile water-based condensation particle counter (vWCPC) has been developed to provide aerosol concentration measurements under various environments with the advantage of reducing the health and safety concerns associated with using butanol or other chemicals as the working fluid. However, the airborne deployment of vWCPCs is relatively limited due to the lack of characterization of vWCPC performance at reduced pressures. Given the complex combinations of operating parameters in vWCPCs, modeling studies have advantages in mapping vWCPC performance. In this work, we thoroughly investigated the performance of a laminar-flow vWCPC using COMSOL Multiphysics® simulation coupled with MATLAB™. We compared it against a modified vWCPC (vWCPC model 3789, TSI, Shoreview, MN, USA). Our simulation determined the performance of particle activation and droplet growth in the vWCPC growth tube, including the supersaturation, $D$ p,kel,0 (smallest size of particle that can be activated), $D$ p,kel,50 (particle size activated with 50 % efficiency) profile, and final growth particle size D d under wide operating temperatures, inlet pressures $P$ (30–101 kPa), and growth tube geometry (diameter $D$ and initiator length $L$ ini ). The effect of inlet pressure and conditioner temperature on vWCPC 3789 performance was also examined and compared with laboratory experiments. The COMSOL simulation result showed that increasing the temperature difference (Δ$T$) between conditioner temperature $T$ con and initiator $T$ ini will reduce $D$ p,kel,0 and the cut-off size $D$ p,kel,50 of the vWCPC. In addition, lowering the temperature midpoint ($T$ mid = $\frac{T_{con}+T_{ini}}{2}$ increases the supersaturation and slightly decreases the $D$ p,kel . The droplet size at the end of the growth tube is not significantly dependent on raising or lowering the temperature midpoint but significantly decreases at reduced inlet pressure, which indirectly alters the vWCPC empirical cut-off size. Our study shows that the current simulated growth tube geometry ($D$=6.3 mm and $L$ ini =30 mm) is an optimized choice for current vWCPC flow and temperature settings. The current simulation can more realistically represent the $D$ p,kel for 7 nm vWCPC and also achieved good agreement with the 2 nm setting. Using the new simulation approach, we provide an optimized operation setting for the 7 nm setting. This study will guide further vWCPC performance optimization for applications requiring precise particle detection and atmospheric aerosol monitoring.

47 OTHER INSTRUMENTATION↗

High-Resolution Image Products Acquired from Mid-Sized Uncrewed Aerial Systems for Land–Atmosphere Studies

We assess the viability of deploying commercially available multispectral and thermal imagers designed for integration on small uncrewed aerial systems (sUASs, <25 kg) on a mid-size Group-3-classification UAS (weight: 25–600 kg, maximum altitude: 5486 m MSL, maximum speed: 128 m/s) for the purpose of collecting a higher spatial resolution dataset that can be used for evaluating the surface energy budget and effects of surface heterogeneity on atmospheric processes than those datasets traditionally collected by instrumentation deployed on satellites and eddy covariance towers. A MicaSense Altum multispectral imager was deployed on two very similar mid-sized UASs operated by the Atmospheric Radiation Measurement (ARM) Aviation Facility. This paper evaluates the effects of flight on imaging systems mounted on UASs flying at higher altitudes and faster speeds for extended durations. We assess optimal calibration methods, acquisition rates, and flight plans for maximizing land surface area measurements. We developed, in-house, an automated workflow to correct the raw image frames and produce final data products, which we assess against known spectral ground targets and independent sources. We intend this manuscript to be used as a reference for collecting similar datasets in the future and for the datasets described within this manuscript to be used as launching points for future research.

47 OTHER INSTRUMENTATION↗

Evaluation of Four Ground-based Retrievals of Cloud Droplet Number Concentration in Marine Stratocumulus with Aircraft In Situ Measurements

Cloud droplet number concentration (N d ) is crucial for understanding aerosol-cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based N d retrievals based on comprehensive datasets from the Atmospheric Radiation Measurements (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The N d retrieval methods use ARM ENA observatory ground-based remote sensing observations from a Micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP Value-added Product (VAP), all of which also retrieve cloud effective radius (r e ). The retrievals are compared against aircraft measurements from the Fast-Cloud Droplet Probe (FCDP) and the Cloud and Aerosol Spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the N d and cloud r e retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to four years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that N d (r e ) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify N d retrieval uncertainties and identify reliable N d retrieval scenarios. Of the retrieval methods, we recommend using the using the Micropulse lidar-based method given its good agreement with in situ measurements, it has less sensitivity to issues arising from precipitation and low cloud LWP/optical depth, and it has broad applicability by functioning for both day and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗

Observational study of relationships between entrainment rate, homogeneity of mixing, and cloud droplet relative dispersion

The entrainment–mixing process is key to the cloud’s dynamical and microphysical processes. However, to the best of our knowledge, no study has quantitatively linked entrainment rate and homogeneity of mixing. Additionally, their combined effects on cloud droplet relative dispersion and physical mechanisms are even more unclear. This study analyzed the aircraft measurements of cumulus clouds collected in the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems field campaign to identify these relationships. The relationship between the entrainment rate and homogeneous mixing degree was found to be moderately positive, and the underlying mechanisms related to mixing and evaporation time scales and environmental relative humidity were explored. The relationship between relative dispersion and entrainment rate changes from positive to negative with increasing entrainment rate, depending on the dominance of evaporation of large or small droplets. The relative dispersion first increases and then decreases with increasing homogeneous mixing degree, validating the results of previous model simulations. Further, the results shed new light on understanding the interactions between cloud microphysics and cloud dynamics through turbulent entrainment and mixing processes.

54 ENVIRONMENTAL SCIENCES↗

Performance of optical sensors for cloud measurements deployed by the ARM Aerial Facility during ACE-ENA

During the Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA), a variety of in situ optical sensors using shadow imaging, scattering and holography were deployed by the Atmospheric Radiation Measurement (ARM) Aerial Facility to determine cloud properties. Taking advantage of the wide, overlapping range of instrumentation, we compare in situ cloud data from several different measurement methods for droplets up to 100 µm. Further, data processing was tailored to the encountered conditions, leading to good agreement. Improvements include noise reduction for holography and better out-of-focus correction for shadow imaging. Comparison between direct liquid water content measurements and optical sensors showed better agreement at higher droplet number concentrations (>120/cm 3 ).

47 OTHER INSTRUMENTATION↗

Molecular Imaging Reveals Two Distinct Mixing States of PM 2.5 Particles Sampled in a Typical Beijing Winter Pollution Case

Mixing states of aerosol particles are crucial for understanding the role of aerosols in influencing air quality and climate. However, a fundamental understanding of the complex mixing states is still lacking because most traditional analysis techniques only reveal bulk chemical and physical properties with limited surface and 3-D information. In this research, 3-D molecular imaging enabled by ToF-SIMS was used to elucidate the mixing states of PM 2.5 samples obtained from a typical Beijing winter haze event. In light pollution cases, a thin organic layer covers separated inorganic particles, while in serious pollution cases, ion exchange and an organic-inorganic mixing surface on large-area particles were observed. Finally, the new results provide key 3-D molecular information of mixing states, which is highly desirable for reducing uncertainty and bias in representing aerosol-cloud interactions in current Earth System Models, and improving the understanding of aerosols on air quality and human health.

3-D molecular imaging↗

Vertical Gradient of Size-Resolved Aerosol Compositions over the Arctic Reveals Cloud Processed Aerosol in-Cloud and above Cloud

Arctic aerosols play a significant role in the aerosol-radiation and aerosol-cloud interactions, but ground-based measurements are insufficient to explain the interaction of aerosols and clouds in a vertically stratified Arctic atmosphere. This study shows the vertical variability of aerosol particle composition via tethered balloon system at Oliktok Point, Alaska, in August 2019, at different cloud layers for two case studies (background aerosol condition and polluted condition). Multi-modal micro-spectroscopy analysis of samples during the background case reveals a broadening of chemically specific size distribution above cloud top with a high abundance of sulfate and core-shell morphology, suggesting possible cloud processing of aerosols. The pollution case also indicates a broadening of size distribution at the upper cloud layer with the dominance of carbonaceous aerosol, which suggests the potential of carbonaceous aerosols for Arctic cloud formation. Here this study provides insights into the vertical profile of Arctic aerosols on cloud formation.

54 ENVIRONMENTAL SCIENCES↗