Engineering topics

Wang, Jian (ORCID:0000000228154170)

Publications and source records attributed to Wang, Jian (ORCID:0000000228154170).

16 records

DOE OSTI2023

Examining the vertical heterogeneity of aerosols over the Southern Great Plains

Abstract. Atmospheric aerosols affect the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical structure, lifetime, and coverage of clouds (indirect effects). Both aerosol direct and indirect effects are affected by the vertical distribution of aerosols in the atmosphere, which is further influenced by a range of processes, such as aerosol dynamics, long-range transport, and entrainment. However, many observations of these processes are based on ground measurements, limiting our ability to understand the vertical distribution of aerosols and simulate their impact on clouds and climate. In this work, we examined the vertical heterogeneity of aerosols over the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) using data collected from the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign. The vertical profiles of meteorological and aerosol physiochemical properties up to 2500 m above are examined based on the 38 flights conducted during the HI-SCALE campaign. The aerosol properties over the SGP show strong vertical heterogeneity and seasonal variabilities. The aerosol concentrations at the surface are the highest due to strong emissions at ground level. In general, the mode diameter of aerosols during summer (∼ 100 nm) is larger than that during spring (∼ 30 nm), a result of enhanced condensational growth due to enriched volatile organic compounds in summer. The concentration of aerosols below 30 nm in the boundary layer (BL) (e.g., below 1000 m) during spring is higher than that during summer, a result of the stronger new particle formation (NPF) events due to the reduced condensation sink in spring. In the BL, the size of the aerosols gradually increases with altitude due to condensational growth and cloud processing. However, the chemical composition of the aerosols remained similar, with organics and sulfates representing 59.8 ± 2.2 % and 22.7 ± 2.1 %, respectively, of the total mass in the BL. Through the vertical profiles of aerosol properties, we observed NPF events in the upper BL during 7 out of 38 research flights, where the newly formed particles continue to grow as they are mixed down to the surface. There is also an indication that deep convection brings aerosols from the free troposphere (FT) to the surface, where they grow to contribute to the cloud condensation nuclei (CCN). Overall, the vertical heterogeneity of aerosols over the SGP is influenced by aerosol dynamics (new particle formation, growth, and cloud processing) and transport processes (mixing in the BL, long-range transport, entrainment, and convective downward transport). Case studies showing the influence of these factors are discussed.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Arctic warming by abundant fine sea salt aerosols from blowing snow

Abstract The Arctic warms nearly four times faster than the global average, and aerosols play an increasingly important role in Arctic climate change. In the Arctic, sea salt is a major aerosol component in terms of mass concentration during winter and spring. However, the mechanisms of sea salt aerosol production remain unclear. Sea salt aerosols are typically thought to be relatively large in size but low in number concentration, implying that their influence on cloud condensation nuclei population and cloud properties is generally minor. Here we present observational evidence of abundant sea salt aerosol production from blowing snow in the central Arctic. Blowing snow was observed more than 20% of the time from November to April. The sublimation of blowing snow generates high concentrations of fine-mode sea salt aerosol (diameter below 300 nm), enhancing cloud condensation nuclei concentrations up to tenfold above background levels. Using a global chemical transport model, we estimate that from November to April north of 70° N, sea salt aerosol produced from blowing snow accounts for about 27.6% of the total particle number, and the sea salt aerosol increases the longwave emissivity of clouds, leading to a calculated surface warming of +2.30 W m −2 under cloudy sky conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

Abstract. Atmospheric ice nucleation impacts the hydrological cycle and climate by modifying the radiative properties of clouds. To improve our predictive understanding of ice formation, ambient ice-nucleating particles (INPs) need to be collected and characterized. Measurements of INPs at lower latitudes in a remote marine region are scarce. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign, in the region of the Azores islands, provided the opportunity to collect particles in the marine boundary layer (MBL) and free troposphere (FT) by aircraft during the campaign's summer and winter intensive operation period. The particle population in samples collected was examined by scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy. The identified INPs were analyzed by scanning electron microscopy with energy-dispersive X-ray analysis. We observed differences in the particle population characteristics in terms of particle diversity, mixing state, and organic volume fraction between seasons, mostly due to dry intrusion events during winter, as well as between the sampling locations of the MBL and FT. These differences are also reflected in the temperature and humidity conditions under which water uptake, immersion freezing (IMF), and deposition ice nucleation (DIN) proceed. Identified INPs reflect typical particle types within the particle population on the samples and include sea salt, sea salt with sulfates, and mineral dust, all associated with organic matter, as well as carbonaceous particles. IMF and DIN kinetics are analyzed with respect to heterogeneous ice nucleation rate coefficients, Jhet, and ice nucleation active site density, ns, as a function of the water criterion Δaw. DIN is also analyzed in terms of contact angles following classical nucleation theory. Derived MBL IMF kinetics agree with previous ACE-ENA ground-site INP measurements. FT particle samples show greater ice nucleation propensity compared to MBL particle samples. This study emphasizes that the types of INPs can vary seasonally and with altitude depending on sampling location, thereby showing different ice nucleation propensities, which is crucial information when representing mixed-phase cloud and cirrus cloud microphysics in models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Multi-campaign ship and aircraft observations of marine cloud condensation nuclei and droplet concentrations

In situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP 2 EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosol-cloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Using aircraft measurements to characterize subgrid-scale variability of aerosol properties near the Atmospheric Radiation Measurement Southern Great Plains site

Abstract. Complex distributions of aerosol properties evolve in space and time as a function of emissions, new particle formation, coagulation, condensational growth, chemical transformation, phase changes, turbulent mixing and transport, removal processes, and ambient meteorological conditions. The ability of chemical transport models to represent the multi-scale processes affecting the life cycle of aerosols depends on their spatial resolution since aerosol properties are assumed to be constant within a grid cell. Subgrid-scale-dependent processes that affect aerosol populations could have a significant impact on the formation of particles, their growth to cloud condensation nuclei (CCN) sizes, aerosol–cloud interactions, dry deposition and rainout and hence their burdens, lifetimes, and radiative forcing. To address this issue, we characterize subgrid-scale variability in terms of measured aerosol number, size, composition, hygroscopicity, and CCN concentrations made by repeated aircraft flight paths over the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystem (HI-SCALE) campaign. Subgrid variability is quantified in terms of both normalized frequency distributions and percentage difference percentiles using grid spacings of 3, 9, 27, and 81 km that represent those typically used by cloud-system-resolving models as well as the current and next-generation climate models. Even though the SGP site is a rural location, surprisingly large horizontal gradients in aerosol properties were frequently observed. For example, 90 % of the 3, 9, and 27 km cell mean organic matter concentrations differed from the 81 km cell around the SGP site by as much as ∼ 46 %, large spatial variability in aerosol number concentrations and size distributions were found during new particle formation events, and consequently 90 % of the 3, 9, and 27 km cell mean CCN number concentrations differed from the 81 km cell mean by as much as ∼ 38 %. The spatial variability varied seasonally for some aerosol properties, with some having larger spatial variability during the spring and others having larger variability during the late summer. While measurements at a single surface site cannot reflect the surrounding variability of aerosol properties at a given time, aircraft measurements that are averaged within an 81 km cell were found to be similar to many, but not all, aerosol properties measured at the ground SGP site. This analysis suggests that it is reasonable to directly compare most ground SGP site aerosol measurements with coarse global climate model predictions. In addition, the variability quantified by the aircraft can be used as an uncertainty range when comparing the surface point measurements with model predictions that use coarse grid spacings.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Automated identification of local contamination in remote atmospheric composition time series

Abstract. Atmospheric observations in remote locations offer a possibility of exploring trace gas and particle concentrations in pristine environments. However, data from remote areas are often contaminated by pollution from local sources. Detecting this contamination is thus a central and frequently encountered issue. Consequently, many different methods exist today to identify local contamination in atmospheric composition measurement time series, but no single method has been widely accepted. In this study, we present a new method to identify primary pollution in remote atmospheric datasets, e.g., from ship campaigns or stations with a low background signal compared to the contaminated signal. The pollution detection algorithm (PDA) identifies and flags periods of polluted data in five steps. The first and most important step identifies polluted periods based on the derivative (time derivative) of a concentration over time. If this derivative exceeds a given threshold, data are flagged as polluted. Further pollution identification steps are a simple concentration threshold filter, a neighboring points filter (optional), a median, and a sparse data filter (optional). The PDA only relies on the target dataset itself and is independent of ancillary datasets such as meteorological variables. All parameters of each step are adjustable so that the PDA can be “tuned” to be more or less stringent (e.g., flag more or fewer data points as contaminated). The PDA was developed and tested with a particle number concentration dataset collected during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition in the central Arctic. Using strict settings, we identified 62 % of the data as influenced by local contamination. Using a second independent particle number concentration dataset also collected during MOSAiC, we evaluated the performance of the PDA against the same dataset cleaned by visual inspection. The two methods agreed in 94 % of the cases. Additionally, the PDA was successfully applied to a trace gas dataset (CO2), also collected during MOSAiC, and to another particle number concentration dataset, collected at the high-altitude background station Jungfraujoch, Switzerland. Thus, the PDA proves to be a useful and flexible tool to identify periods affected by local contamination in atmospheric composition datasets without the need for ancillary measurements. It is best applied to data representing primary pollution. The user-friendly and open-access code enables reproducible application to a wide suite of different datasets. It is available at https://doi.org/10.5281/zenodo.5761101 (Beck et al., 2021).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Regularized inversion of aerosol hygroscopic growth factor probability density function: application to humidity-controlled fast integrated mobility spectrometer measurements

Abstract. Aerosol hygroscopic growth plays an important role in atmospheric particle chemistry and the effects of aerosol on radiation and hence climate. The hygroscopic growth is often characterized by a growth factor probability density function (GF-PDF), where the growth factor is defined as the ratio of the particle size at a specified relative humidity to its dry size. Parametric, least-squares methods are the most widely used algorithms for inverting the GF-PDF from measurements of the humidified tandem differential mobility analyzer (HTDMA) and have been recently applied to the GF-PDF inversion from measurements of the humidity-controlled fast integrated mobility spectrometer (HFIMS). However, these least-squares methods suffer from noise amplification due to the lack of regularization in solving the ill-posed problem, resulting in significant fluctuations in the retrieved GF-PDF and even occasional failures of convergence. In this study, we introduce nonparametric, regularized methods to invert the aerosol GF-PDF and apply them to HFIMS measurements. Based on the HFIMS kernel function, the forward convolution is transformed into a matrix-based form, which facilitates the application of the nonparametric inversion methods with regularizations, including Tikhonov regularization and Twomey's iterative regularization. Inversions of the GF-PDF using the nonparameteric methods with regularization are demonstrated using HFIMS measurements simulated from representative GF-PDFs of ambient aerosols. The characteristics of reconstructed GF-PDFs resulting from different inversion methods, including previously developed least-squares methods, are quantitatively compared. The result shows that Twomey's method generally outperforms other inversion methods. The capabilities of Twomey's method in reconstructing the pre-defined GF-PDFs and recovering the mode parameters are validated.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic

Abstract. Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K, including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Impact of dry intrusion events on the composition and mixing state of particles during the winter Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA)

Abstract. Long-range transport of continental emissions has a far-reaching influence over remote regions, resulting in substantial change in the size, morphology, and composition of the local aerosol population and cloud condensation nuclei (CCN) budget. Here, we investigate the physicochemical properties of atmospheric particles collected on board a research aircraft flown over the Azores during the winter 2018 Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) campaign. Particles were collected within the marine boundary layer (MBL) and free troposphere (FT) after long-range atmospheric transport episodes facilitated by dry intrusion (DI) events. Chemical and physical properties of individual particles were investigated using complementary capabilities of computer-controlled scanning electron microscopy and X-ray spectromicroscopy to probe particle external and internal mixing state characteristics. Furthermore, real-time measurements of aerosol size distribution, cloud condensation nuclei (CCN) concentration, and back-trajectory calculations were utilized to help bring into context the findings from offline spectromicroscopy analysis. While carbonaceous particles were found to be the dominant particle type in the region, changes in the percent contribution of organics across the particle population (i.e., external mixing) shifted from 68 % to 43 % in the MBL and from 92 % to 46 % in FT samples during DI events. This change in carbonaceous contribution is counterbalanced by the increase in inorganics from 32 % to 57 % in the MBL and 8 % to 55 % in FT. The quantification of the organic volume fraction (OVF) of individual particles derived from X-ray spectromicroscopy, which relates to the multi-component internal composition of individual particles, showed a factor of 2.06 ± 0.16 and 1.11 ± 0.04 increase in the MBL and FT, respectively, among DI samples. We show that supplying particle OVF into the κ-Köhler equation can be used as a good approximation of field-measured in situ CCN concentrations. We also report changes in the κ values in the MBL from κMBL, non-DI=0.48 to κMBL, DI=0.41, while changes in the FT result in κFT, non-DI=0.36 to κFT, DI=0.33, which is consistent with enhancements in OVF followed by the DI episodes. Our observations suggest that entrainment of particles from long-range continental sources alters the mixing state population and CCN properties of aerosol in the region. The work presented here provides field observation data that can inform atmospheric models that simulate sources and particle composition in the eastern North Atlantic.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP)

Abstract. Cloud condensation nuclei (CCN) spectrum and the CCN activated fraction of size-resolved aerosols (SR-CCN) were measured at a rural site on Long Island during the Department of Energy (DOE) aerosol life cycle intensive operational period (ALC-IOP) from 15 July to 15 August 2011. During the last week of the ALC-IOP, the dependence of the activated fraction on aerosol volatility was characterized by sampling downstream of a thermodenuder (TD) operated at temperatures up to 100 ∘C. Here we present aerosol properties, including aerosol total number concentration, CCN spectrum, and the CCN hygroscopicity, for air masses of representative origins during the ALC-IOP. The hygroscopicity of organic species in the aerosol is derived from CCN hygroscopicity and chemical composition. The dependence of organic hygroscopicity on the organic oxidation level (e.g., atomic O:C ratio) agrees well with theoretical predictions and results from previous laboratory and field studies. The derived κorg and O:C ratio first increase as TD temperature increases from 20 ∘C (i.e., ambient temperature) to 50 or 75 ∘C and then decrease as TD temperature further increases to 100 ∘C. The initial increases of O:C and κorg with TD temperature below 50 ∘C are likely due to evaporation of more volatile organics with relatively lower O:C and hygroscopicity such as primary organic aerosol. At the high TD temperatures, the decreases of O:C and κorg indicate that evaporated organics were more oxygenated and had lower molecular weights. These trends are different from previous laboratory experiments and field observations, which reported that organic O:C increased monotonically with increasing TD temperature, whereas κorg decreased with the TD temperature. One possible reason is that previous studies were either focused on laboratory-generated secondary organic aerosol (SOA) or based on field observations at locations more dominated by SOA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Rapid measurement of RH-dependent aerosol hygroscopic growth using a humidity-controlled fast integrated mobility spectrometer (HFIMS)

Abstract. The ability of aerosol particles to uptake water (hygroscopic growth) is an important determinant of aerosol optical properties and radiative effects. Aerosol hygroscopic growth is traditionally measured by humidified tandem differential mobility analyzers (HTDMA), in which size-selected dry particles are exposed to elevated relative humidity (RH), and the size distribution of humidified particles is subsequently measured using a scanning mobility particle sizer. As a scanning mobility particle sizer can measure only one particle size at a time, HTDMA measurements are time consuming, and ambient measurements are often limited to a single RH level. Pinterich et al. (2017b) showed that fast measurements of aerosol hygroscopic growth are possible using a humidity-controlled fast integrated mobility spectrometer (HFIMS). In HFIMS, the size distribution of humidified particles is rapidly captured by a water-based fast integrated mobility spectrometer (WFIMS), leading to a factor of ∼10 increase in measurement time resolution. In this study we present a prototype HFIMS that extends fast hygroscopic growth measurements to a wide range of atmospherically relevant RH values, allowing for more comprehensive characterizations of aerosol hygroscopic growth. A dual-channel humidifier consisting of two humidity conditioners in parallel is employed such that aerosol RH can be quickly stepped among different RH levels by sampling from alternating conditioners. The measurement sequence is also optimized to minimize the transition time between different particle sizes. The HFIMS is capable of measuring aerosol hygroscopic growth of six particle diameters under five RH levels ranging from 20 % to 85 % (30 separate measurements) every 25 min. The performance of this HFIMS is characterized and validated using laboratory-generated ammonium sulfate aerosol standards. Measurements of ambient aerosols are shown to demonstrate the capability of HFIMS to capture the rapid evolution of aerosol hygroscopic growth and its dependence on both size and RH.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Dilution impacts on smoke aging: evidence in Biomass Burning Observation Project (BBOP) data

Abstract. Biomass burning emits vapors and aerosols into the atmosphere that can rapidly evolve as smoke plumes travel downwind and dilute, affecting climate- and health-relevant properties of the smoke. To date, theory has been unable to explain observed variability in smoke evolution. Here, we use observational data from the Biomass Burning Observation Project (BBOP) field campaign and show that initial smoke organic aerosol mass concentrations can help predict changes in smoke aerosol aging markers, number concentration, and number mean diameter between 40–262 nm. Because initial field measurements of plumes are generally >10 min downwind, smaller plumes will have already undergone substantial dilution relative to larger plumes and have lower concentrations of smoke species at these observations closest to the fire. The extent to which dilution has occurred prior to the first observation is not a directly measurable quantity. We show that initial observed plume concentrations can serve as a rough indicator of the extent of dilution prior to the first measurement, which impacts photochemistry, aerosol evaporation, and coagulation. Cores of plumes have higher concentrations than edges. By segregating the observed plumes into cores and edges, we find evidence that particle aging, evaporation, and coagulation occurred before the first measurement. We further find that on the plume edges, the organic aerosol is more oxygenated, while a marker for primary biomass burning aerosol emissions has decreased in relative abundance compared to the plume cores. Finally, we attempt to decouple the roles of the initial concentrations and physical age since emission by performing multivariate linear regression of various aerosol properties (composition, size) on these two factors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Vertical dependence of horizontal variation of cloud microphysics: observations from the ACE-ENA field campaign and implications for warm-rain simulation in climate models

Abstract. In the current global climate models (GCMs), the nonlinearity effect of subgrid cloud variations on the parameterization of warm-rain process, e.g., the autoconversion rate, is often treated by multiplying the resolved-scale warm-rain process rates by a so-called enhancement factor (EF). In this study, we investigate the subgrid-scale horizontal variations and covariation of cloud water content (qc) and cloud droplet number concentration (Nc) in marine boundary layer (MBL) clouds based on the in situ measurements from a recent field campaign and study the implications for the autoconversion rate EF in GCMs. Based on a few carefully selected cases from the field campaign, we found that in contrast to the enhancing effect of qc and Nc variations that tends to make EF > 1, the strong positive correlation between qc and Nc results in a suppressing effect that tends to make EF < 1. This effect is especially strong at cloud top, where the qc and Nc correlation can be as high as 0.95. We also found that the physically complete EF that accounts for the covariation of qc and Nc is significantly smaller than its counterpart that accounts only for the subgrid variation of qc, especially at cloud top. Although this study is based on limited cases, it suggests that the subgrid variations of Nc and its correlation with qc both need to be considered for an accurate simulation of the autoconversion process in GCMs.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗