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At least 109 records · Page 6

Single-shot ultrafast dynamics of nanosecond pulsed plasmas: Transition from ps–ns nonequilibrium to near-full ionization

The ultrafast multi-stage evolution of state-defining properties in atmospheric-pressure nanosecond pulsed plasmas is quantified using single-discharge, jitter-free, continuous streak-sweep spectroscopy of N 2 (C → B) molecular and N + /O + ionic species with a single-shot time resolution as short as ∼160 ps. An early period of extreme nonequilibrium is observed with vibrational temperatures [T V (C)] dropping from ∼8000 K at <200 ps after plasma breakdown to <4000 K within ∼1 ns, with near-ambient rotational temperatures [T R (C)] ∼ 300 K due to limited collisional energy transfer. This early-time T V (C) trend is representative of a direct and unquenched look into the high-energy tail of the electron energy distribution function; thus, it tracks real-time changes in the mean electron energy via the N2(C) emission signatures. This is followed by the rapid onset of N + /O + ionic emission after a distinct time delay of ∼14.9 ns due to multistep chemical kinetics. The ionic emission enables determination of electron densities (n e ) >2 × 10 19 cm −3 and electron temperatures (T e ) >36 000 K, indicating the transition to a nearly fully ionized regime. The ps–ns temporal dynamics are also compared between air and N 2 plasmas to assess the influence of collisional partners, as well as across the anode, cathode, and central gap regions to identify spatial variations in plasma behavior. Finally, this work demonstrates versatile continuously probing approach capable of spectro-temporal and spatially resolved single-shot measurements of key state variables in the ps–ns evolution of atmospheric-pressure nanosecond pulsed plasmas.

Electric discharges↗

Black hole spin in X-ray binaries: giving uncertainties an $\mathcal{f}$

The two established techniques for measuring black hole spin in X-ray binaries often yield conflicting results, which must be resolved before either method may be deemed robust. In practice, black hole spin measurements based on fitting the accretion disc continuum effectively do not marginalize over the colour-correction factor f col . This factor parametrizes spectral hardening of the disc continuum by the disc atmosphere, whose true properties are poorly constrained. We incorporate reasonable systematic uncertainties in f col into the eight (non-maximal) black hole spin measurements vetted by the disc continuum fitting community. In most cases, an f col uncertainty of ±0.2–0.3 dominates the black hole spin error budget. We go on to demonstrate that plausible departures in f col values from those adopted by the disc continuum fitting practitioners can bring the discrepant black hole spins into agreement with those from iron line modelling. Systematic uncertainties in f col , such as the effects of strong magnetization, should be better understood before dismissing their potentially dominant impact on the black hole spin error budget.

4U 1543–47↗

A tandem radiative/evaporative cooler for weather-insensitive and high-performance daytime passive cooling

Radiative cooling and evaporative cooling with low carbon footprint are regarded as promising passive cooling strategies. However, the intrinsic limits of continuous water supply with complex systems for evaporative cooling, and restricted cooling power as well as the strict requirement of weather conditions for radiative cooling, hinder the scale of their practical applications. Here, we propose a tandem passive cooler composed of bilayer polymer that enables dual-functional passive cooling of radiation and evaporation. Specifically, the high reflectivity to sunlight and mid-infrared emissivity of this polymer film allows excellent radiative cooling performance, and its good atmospheric water harvesting property of underlayer ensures self-supply of water and high evaporative cooling power. Consequently, this tandem passive cooler overcomes the fundamental difficulties of radiative cooling and evaporative cooling and shows the applicability under various conditions of weather/climate. It is expected that this design can expand the practical application domain of passive cooling.

54 ENVIRONMENTAL SCIENCES↗

High-Spectral Resolution Lidar (HSRL) Instrument Handbook

High-spectral-resolution lidar (HSRL) systems provide vertical profiles of optical depth, backscatter cross-section, depolarization, and backscatter phase function. All HSRL measurements are calibrated by reference to molecular scattering, which is measured at each point in the lidar profile. Like the Raman lidar (RL), but unlike simple backscatter lidars such as the micropulse lidar (MPL), this enables the HSRL to measure backscatter cross-sections and optical depths without prior assumptions about the scattering properties of the atmosphere. The depolarization observations allow robust discrimination between ice and water clouds. Rigorous error estimates can be computed for all measurements. A very narrow angular field of view reduces multiple scattering contributions. The small field of view, coupled with a narrow optical bandwidth, nearly eliminates noise due to scattered sunlight. The laser transmitter is a diode-pumped, frequency-doubled Nd:YAG laser. Narrow-band, single-frequency operation is provided by injection seeding with a single-frequency, cw-diode-pumped diode laser. The main laser cavity is maintained in resonance with the seed laser by adjusting the cavity length to minimize the time between the Q-switch trigger and the emission of the laser pulse. The emission wavelength is tuned via temperature control of the seed laser crystal and is locked to line #1109 of the iodine absorption spectra. Locking is accomplished by minimizing the transmission through a 2-cm-long iodine absorption cell. Use of a high-repetition-rate laser and expansion of the transmitted beam through a 400-mm telescope reduces the transmitted energy density to eye-safe levels. It is possible to look directly into the output beam without hazard. The receiver and transmitter use the same afocal telescope, simplifying the maintenance of stable alignment of the transmitter and receiver although the angular FOV is only 100 μrad. The small FOV and the 4-kHz repetition rate also limit the near-field signal strength, making it possible to record continuous profiles that start at an altitude of ~100 m and extend to 30 km using photon counting detectors. The small FOV also suppresses multiple scattering contributions.

54 ENVIRONMENTAL SCIENCES↗

Beryllium (Be) Handbook

Beryllium (Be), atomic number 4, is a silver gray metal of low density (1.85g/cm 3 ), moderately high melting point (1289°C), and quite good stability in the atmosphere. Favorable mechanical properties, particularly specific stiffness (elastic modulus/density), have resulted in a number of weight-critical structural applications. Other notable properties of beryllium include good dimensional stability, high specific heat and extremely high transparency to X-radiation. The nuclear properties of beryllium include a high neutron scattering cross section (6 barns for thermal neutrons) and a low neutron absorption cross section (0.009 barns for thermal neutrons) making it a good choice for a neutron reflector. The (n, 2n) reaction in beryllium also makes it suitable for a neutron multiplier.

36 MATERIALS SCIENCE↗

Collaborative Research: Understanding Nanoparticle-Plasma Interactions in Dusty Non-Thermal Plasmas by Nanoparticle Probes and Online Aerosol Characterization

Research Objectives The goal of this research project is to understand the nature of charge interactions between plasmas and aerosol particles. Specifically, the project has the following objectives: 1) Study the effect of solid nanoparticles on properties of an atmospheric pressure plasma. 2) Study the influence of plasma density on the final charge of nanoparticles. 3) Develop a theoretical understanding of charge decay and charge dynamics in the spatial afterglow in support of experimental observations of the final charge of nanoparticles exiting a plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Measurement report: A comparison of ground-level ice-nucleating-particle abundance and aerosol properties during autumn at contrasting marine and terrestrial locations

Abstract. Ice-nucleating particles (INPs) are an essential class of aerosols found worldwide that have far-reaching but poorly quantified climate feedback mechanisms through interaction with clouds and impacts on precipitation. These particles can have highly variable physicochemical properties in the atmosphere, and it is crucial to continuously monitor their long-term concentration relative to total ambient aerosol populations at a wide variety of sites to comprehensively understand aerosol–cloud interactions in the atmosphere. Hence, our study applied an in situ forced expansion cooling device to measure ambient INP concentrations and test its automated continuous measurements at atmospheric observatories, where complementary aerosol instruments are heavily equipped. Using collocated aerosol size, number, and composition measurements from these sites, we analyzed the correlation between sources and abundance of INPs in different environments. Toward this aim, we have measured ground-level INP concentrations at two contrasting sites, one in the Southern Great Plains (SGP) region of the United States with a substantial terrestrially influenced aerosol population and one in the Eastern North Atlantic Ocean (ENA) region with a primarily marine-influenced aerosol population. These measurements examined INPs mainly formed through immersion freezing and were performed at a ≤ 12 min resolution and with a wide range of heterogeneous freezing temperatures (Ts above −31 °C) for at least 45 d at each site. The associated INP data analysis was conducted in a consistent manner. We also explored the additional offline characterization of ambient aerosol particle samples from both locations in comparison to in situ data. From our ENA data, on average, INP abundance ranges from ≈ 1 to ≈ 20 L−1 (−30 °C ≤ T ≤ −20 °C) during October–November 2020. Backward air mass trajectories reveal a strong marine influence at ENA with 75.7 % of air masses originating over the Atlantic Ocean and 96.6 % of air masses traveling over open water, but analysis of particle chemistry suggests an additional INP source besides maritime aerosols (e.g., sea spray aerosols) at ENA. In contrast, 90.8 % of air masses at the SGP location originated from the North American continent, and 96.1 % of the time, these air masses traveled over land. As a result, organic-rich SGP aerosols from terrestrial sources exhibited notably high INP abundance from ≈ 1 to ≈ 100 L−1 (−30 °C ≤ T ≤ −15 °C) during October–November 2019. The probability density function of aerosol surface area-scaled immersion freezing efficiency (ice nucleation active surface site density; ns) was assessed for selected freezing temperatures. While the INP concentrations measured at SGP are higher than those of ENA, the ns(T) values of SGP (≈ 105 to ≈ 107 m−2 for −30 °C ≤ T ≤ −15 °C) are reciprocally lower than ENA for approximately 2 orders of magnitude (≈ 107 to ≈ 109 m−2 for −30 °C ≤ T ≤ −15 °C). The observed difference in ns(T) mainly stems from varied available aerosol surface areas, Saer, from two sites (Saer,SGP > Saer,ENA). INP parameterizations were developed as a function of examined freezing temperatures from SGP and ENA for our study periods.

54 ENVIRONMENTAL SCIENCES↗

Aerosol characteristics at the Southern Great Plains site during the HI-SCALE campaign

Abstract. Large uncertainties exist in global climate model predictions of radiative forcing due to insufficient understanding and simplified numerical representation of cloud formation and cloud–aerosol interactions. The Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign was conducted near the DOE's Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in north-central Oklahoma to provide a better understanding of land–atmosphere interactions, aerosol and cloud properties, and the influence of aerosol and land–atmosphere interactions on cloud formation. The HI-SCALE campaign consisted of two intensive observational periods (IOPs) (April–May and August–September, 2016), during which coincident measurements were conducted both on the G-1 aircraft platform and at the SGP ground site. In this study we focus on the observations at the SGP ground site. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed, characterizing chemistry of non-refractory aerosol and trace gases, respectively. Contributions from various aerosol sources, including biogenic and biomass burning emissions, were retrieved using factor analysis of the AMS data. In general, the organic aerosols at the SGP site was highly oxidized, with oxygenated organic aerosol (OOA) identified as the dominant factor for both the spring and summer IOP though more aged in spring. Cases of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) and biomass burning events were further investigated to understand additional sources of organic aerosol. Unlike other regions largely impacted by IEPOX chemistry, the IEPOX SOA at SGP was more highly oxygenated, likely due to the relatively weak local emissions of isoprene. Biogenic emissions appear to largely control the formation of organic aerosol (OA) during the HI-SCALE campaign. Potential HOM (highly oxygenated molecule) chemistry likely contributes to the highly oxygenated feature of aerosols at the SGP site, with impacts on new particle formation and global climate.

54 ENVIRONMENTAL SCIENCES↗

AI‐Driven Robot Enables Synthesis‐Property Relation Prediction for Metal Halide Perovskites in Humid Atmosphere

Materials Acceleration Platforms (MAPs) – also known as self-driving laboratories– present a new paradigm for materials science and promise an order of magnitude accelerated materials discovery compared to the traditional trial-and-error approach. Metal halide perovskites (MHPs) are an emerging class of materials for optoelectronic applications but are plagued by irreproducible optoelectronic quality, particularly for films fabricated in a humid atmosphere. Here, in this work, a machine learning (ML)-guided closed-loop platform is developed with a multimodal data fusion approach to predict synthesis–property relations for the optical quality of MHP thin films in relative humidities (RHs) ranging from 5–55%. The efficiency of this approach is confirmed by the fast-dropping learning rate to 2% after experimentally sampling less than 1% of the possible 5,000+ combinations. The prediction of synthesis–property relations is done by optical and imaging characterizations. In situ photoluminescence characterization revealed the origin of thin film quality variation at different RH. These insights provide an avenue for controlling the MHP crystallization by fine-tuning the synthesis parameters and RH for a given chemistry, thus lifting the need for stringent atmosphere control. The MAP enables an accelerated screening and understanding of the synthesis design space, facilitating rational synthesis recipe choice for a wide range of materials.

AI-driven robot↗

Atmospheric Radiation Measurement (ARM) airborne field campaign data products between 2013 and 2018

Airborne measurements are pivotal for providing detailed, spatiotemporally resolved information about atmospheric parameters and aerosol and cloud properties, thereby enhancing our understanding of dynamic atmospheric processes. For 30 years, the US Department of Energy (DOE) Office of Science supported an instrumented 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) Data Center 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 dataset was recently developed covering the final 6 years of G-1 operations (2013 to 2018, https://doi.org/10.5439/1999133; Mei and Gaustad, 2024). The integrated dataset includes data collected from 236 flights (766.4 h), which covered the Arctic, the US Southern Great Plains (SGP), the US West Coast, the eastern North Atlantic (ENA), the Amazon Basin in Brazil, and the Sierras de Córdoba range in Argentina. These comprehensive data streams provide much-needed insight into spatiotemporal variability in the thermodynamic quantities and aerosol and cloud properties for addressing essential science questions in Earth system process studies. This paper describes the DOE ARM merged G-1 datasets, including information on the acquisition, data collection challenges and future potentials, and quality control processes. It further illustrates the usage of this merged dataset to evaluate the Energy Exascale Earth System Model (E3SM) with the Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package.

54 ENVIRONMENTAL SCIENCES↗

Aerosols from anthropogenic and biogenic sources and their interactions – modeling aerosol formation, optical properties, and impacts over the central Amazon basin

The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous GoAmazon 2014–2015 studies showed that nitrogen oxide (NO x = NO + NO 2 ) and sulfur oxide (SO x ) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (g aer ), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The g aer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.

54 ENVIRONMENTAL SCIENCES↗

Doppler Lidar Measurements of Wind Variability and LLJ Properties in Central Oklahoma during the August 2017 Land–Atmosphere Feedback Experiment

Abstract Low-level jets (LLJs) are an important nocturnal source of wind energy in the U.S. Great Plains. An August 2017 lidar-based field-measurement campaign [the Land–Atmosphere Feedback Experiment (LAFE)] studied LLJs over the central SGP site in Oklahoma and found nearly equal occurrences of the usual southerly jets and postfrontal northeasterly jets—typically rare during this season—for an opportunity to compare the two types of LLJs during this month. Southerly winds were stronger than the northeasterlies by more than 4 m s −1 on average, reflecting a significantly higher frequency of winds stronger than 12 m s −1 . The analysis of this dataset has been expanded to other SGP Doppler-lidar sites to quantify the variability of winds and LLJ properties between sites of different land use. Geographic variations of winds over the study area were noted: on southerly wind nights, the winds blew stronger at the highest, westernmost sites by 2 m s −1 , whereas on the northeasterly flow nights, the easternmost sites had the strongest wind speeds. Lidar measurements at 5 sites during August 2017, contrasted to the 2016–21 summertime data, revealed unusual wind and LLJ conditions. Temporal hodographs using hourly averaged winds at multiple heights revealed unorganized behavior in the turbulent stable boundary layer (SBL) below the jet nose. Above the nose, some nights showed veering qualitatively similar to inertial oscillation (IO) behavior, but at amplitudes much smaller than expected for an IO, whereas other nights showed little veering. Vertical hodographs had a linear shape in the SBL, indicating little directional shear there, and veering above, resulting in a hook-shaped hodograph with height. Significance Statement Doppler-lidar measurements at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) were used to quantify the variability of winds and low-level jet (LLJ) properties between five sites of different land use and wind regimes across this area. Knowledge of wind and LLJ structure and dynamics is important for many applications, and strong southerly LLJ winds at night are an important resource for wind energy. The analysis of multiyear (2016–21) summertime LLJ parameters provided insight into the LLJ climatology in this part of the Great Plains.

Meteorology & Atmospheric Sciences↗

Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment

Abstract. The impacts of soot particles on climate and human health depend on the concentration of black carbon (BC) as well as the thickness and composition of the coating material, i.e., organic and inorganic compounds internally mixed with BC. In this study, the size-resolved chemical composition of BC-containing aerosol was measured using a high-resolution soot particle aerosol mass spectrometer (SP-AMS) during wintertime in Fresno, California, a location influenced by abundant combustion emissions and frequent fog events. Concurrently, particle optical properties were measured to investigate the BC absorption enhancement. Positive matrix factorization (PMF) analysis was performed on the SP-AMS mass spectral measurements to explore the sources of soot particles and the atmospheric processes affecting the properties of BC coatings. The analysis revealed that residential woodburning and traffic are the dominant sources of soot particles. Alongside primary soot particles originating from biomass burning (BBOABC) and vehicles (HOABC) two distinct types of processed BC-containing aerosol were identified: fog-related oxidized organic aerosol (FOOABC) and winter-background OOABC (WOOABC). Both types of OOABC showed evidence of having undergone aqueous processing, albeit with differences. The concentration of FOOABC was substantially elevated during fog events, indicating the formation of aqueous secondary organic aerosol (aqSOA) within fog droplets. On the other hand, WOOABC was present at a relatively consistent concentration throughout the winter and was likely related to the formation of secondary organic aerosol (SOA) in both the gas phase and aerosol liquid water. By comparing the chemical properties and temporal variations in FOOABC and WOOABC, we gain insights into the key aging processes of BC aerosol. It was found that aqueous-phase reactions facilitated by fog droplets had a significant impact on the thickness and chemical composition of BC coatings, thereby affecting the light absorption and hygroscopic properties of soot particles. These findings underscore the important role of chemical reactions occurring within clouds and fogs and influencing the climate forcing of BC aerosol in the atmosphere.

54 ENVIRONMENTAL SCIENCES↗

Graph characterization of higher-order structure in atmospheric chemical reaction mechanisms

Atmospheric chemical reactions play an important role in air quality and climate change. While the structure and dynamics of individual chemical reactions are fairly well understood, the emergent properties of the entire atmospheric chemical system, which can involve many different species that participate in many different reactions, are not well described. In this work, we leverage graph-theoretic techniques to characterize patterns of interaction (“motifs”) in three different representations of gas-phase atmospheric chemistry, termed “chemical mechanisms.” These widely used mechanisms, the master chemical mechanism, the GEOS-Chem mechanism, and the Super-Fast mechanism, vary dramatically in scale and application, but they all generally aim to simulate the abundance and variability of chemical species in the atmosphere. This motif analysis quantifies the fundamental patterns of interaction within the mechanisms, which are directly related to their construction. For example, the gas-phase chemistry in the very small Super-Fast mechanism is entirely composed of bimolecular reactions, and its motif distribution matches that of an individual bimolecular reaction well. The larger and more complex mechanisms show emergent motif distributions that differ strongly from any specific reaction type, consistent with their complexity. The proposed motif analysis demonstrates that while these mechanisms all have a similar design goal, their higher-order structure of interactions differs strongly and thus provides a novel set of tools for exploring differences across chemical mechanisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Insights of warm-cloud biases in Community Atmospheric Model 5 and 6 from the single-column modeling framework and Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) observations

There has been a growing concern that most climate models predict precipitation that is too frequent, likely due to lack of reliable subgrid variability and vertical variations in microphysical processes in low-level warm clouds. In this study, the warm-cloud physics parameterizations in the singe-column configurations of NCAR Community Atmospheric Model version 6 and 5 (SCAM6 and SCAM5, respectively) are evaluated using ground-based and airborne observations from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign near the Azores islands during 2017–2018. The 8-month single-column model (SCM) simulations show that both SCAM6 and SCAM5 can generally reproduce marine boundary layer cloud structure, major macrophysical properties, and their transition. The improvement in warm-cloud properties from the Community Atmospheric Model 5 and 6 (CAM5 to CAM6) physics can be found through comparison with the observations. Meanwhile, both physical schemes underestimate cloud liquid water content, cloud droplet size, and rain liquid water content but overestimate surface rainfall. Modeled cloud condensation nuclei (CCN) concentrations are comparable with aircraft-observed ones in the summer but are overestimated by a factor of 2 in winter, largely due to the biases in the long-range transport of anthropogenic aerosols like sulfate. We also test the newly recalibrated autoconversion and accretion parameterizations that account for vertical variations in droplet size. Compared to the observations, more significant improvement is found in SCAM5 than in SCAM6. This result is likely explained by the introduction of subgrid variations in cloud properties in CAM6 cloud microphysics, which further suppresses the scheme's sensitivity to individual warm-rain microphysical parameters. The predicted cloud susceptibilities to CCN perturbations in CAM6 are within a reasonable range, indicating significant progress since CAM5 which produces an aerosol indirect effect that is too strong. The present study emphasizes the importance of understanding biases in cloud physics parameterizations by combining SCM with in situ observations.

54 ENVIRONMENTAL SCIENCES↗

Spectral solar irradiance on inclined surfaces: A fast Monte Carlo approach

Estimating spectral plane-of-array (POA) solar irradiance on inclined surfaces is an important step in the design and performance evaluation of both photovoltaic and concentrated solar plants. This work introduces a fast, line-by-line spectral, Monte Carlo (MC) radiative transfer model approach to simulate anisotropic distributions of shortwave radiation through the atmosphere as photon bundles impinge on inclined surfaces. This fast Monte Carlo approach reproduces the angular distribution of solar irradiance without the undesirable effects of spatial discretization and thus computes detailed POA irradiance values on surfaces at any orientation and also when surfaces are subjected to the anisotropic ground and atmospheric scattering. Polarization effects are also easily incorporated into this approach that can be considered as direct numerical simulation of the physics involved. Here, we compare our Monte Carlo radiative transfer model with the most widely used empirical transposition model, Perez4, under various conditions. The results show that the Perez4 model reproduces the more detailed Monte Carlo simulations with less than 10% deviation under clear skies for all relevant surface tilt and azimuth angles. When optically thin clouds are present, observed deviations are larger, especially when the receiving surface is strongly tilted. Deviations are also observed for large azimuth angle differences between the receiving surface and the solar position. When optically thick clouds are present, the two models agree within 15% deviation for nearly all surface orientation and tilt angles. The overall deviations are smaller when compared with cases for optically thin clouds. The Perez4 model performs very well (6.0% deviation) in comparison with the detailed MC simulations for all cases, thus validating its widespread use for practical solar applications. When detailed atmospheric profiles and cloud optical properties are available, the proposed fast Monte Carlo radiative model reproduces accurate spectral and angular POA irradiance levels for various atmospheric and cloud cover conditions, surface orientations, and different surface and ground properties.

42 ENGINEERING↗

Optical properties and composition of viscous organic particles found in the Southern Great Plains

Abstract. Atmospheric high-viscosity organic particles (HVOPs) were observed in samples of ambient aerosols collected in April and May 2016 in the Southern Great Plains of the United States. These particles were apportioned as either airborne soil organic particles (ASOPs) or tar balls (TBs) from biomass burning based on spetro-microscopic imaging and assessments of meteorological records of smoke and precipitation data. Regardless of their apportionment, the number fractions of HVOPs were positively correlated (R2=0.85) with increased values of absorption Ångström exponent (AAE) measured in situ for ambient aerosol at the site. Extending this correlation to 100 % HVOPs yields an AAE of 2.6, similar to previous literature reports of the class of light-absorbing organic particles known as brown carbon (BrC). One out of the three samples investigated had a significant number of ASOPs, while the other two samples contained TBs. Although there are chemical similarities between ASOPs and TBs, they can be distinguished based on composition inferred from near-edge absorption X-ray fine structure (NEXAFS) spectroscopy. ASOPs were distinguished from TBs based on their average -COOH/C=C and -COOH/COH peak ratios, with ASOPs having lower ratios. NEXAFS spectra of filtered soil organic brine particles nebulized from field samples of standing water deposited after rain were consistent with ASOPs when laboratory particles were generated by bubble bursting at the air–organic brine interface. However, particles generated by nebulizing the bulk volume of soil organic brine had a particle composition different from ASOPs. These observations are consistent with the raindrop generation mechanism responsible for ASOP emissions in the area of study. In contrast, nebulized samples carry with them higher fractions of soil inorganics dissolved in the bulk volume of soil brine, which are not aerosolized by the raindrop mechanism. Our results support the bubble bursting mechanism of particle generation during rainfall resulting in the ejection of soil organics into the atmosphere. In addition, our results show that ASOPs may only be atmospherically relevant during times when suitable emission conditions are met.

54 ENVIRONMENTAL SCIENCES↗