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At least 91 records · Page 5

State of the Carbon Cycle - Consequences of Rising Atmospheric CO2

The rise of atmospheric CO2, largely attributable to human activity through fossil fuel emissions and land-use change, has been dampened by carbon uptake by the ocean and terrestrial biosphere. We outline the consequences of this carbon uptake as direct and indirect effects on terrestrial and oceanic systems and processes for different regions of North America and the globe. We assess the capacity of these systems to continue to act as carbon sinks. Rising CO2 has decreased seawater pH; this process of ocean acidification has impacted some marine species and altered fundamental ecosystem processes with further effects likely. In terrestrial ecosystems, increased atmospheric CO2 causes enhanced photosynthesis, net primary production, and increased water-use efficiency. Rising CO2 may change vegetation composition and carbon storage, and widespread increases in water use efficiency likely influence terrestrial hydrology and biogeochemical cycling. Consequences for human populations include changes to ecosystem services including cultural activities surrounding land use, agricultural or harvesting practices. Commercial fish stocks have been impacted and crop production yields have been changed as a result of rising CO2. Ocean and terrestrial effects are contingent on, and feedback to, global climate change. Warming and modified precipitation regimes impact a variety of ecosystem processes, and the combination of climate change and rising CO2 contributes considerable uncertainty to forecasting carbon sink capacity in the ocean and on land. Disturbance regime (fire and insects) are modified with increased temperatures. Fire frequency and intensity increase, and insect lifecycles are disrupted as temperatures move out of historical norms. Changes in disturbance patterns modulate the effects of rising CO2 depending on ecosystem type, disturbance frequency, and magnitude of events. We discuss management strategies designed to limit the rise of atmospheric CO2 and reduce uncertainty in forecasts of decadal and centennial feedbacks of rising atmospheric CO2 on carbon storage.

Carbon Cycle↗

Variational and phase response analysis for limit cycles with hard boundaries, with applications to neuromechanical control problems

Motor systems show an overall robustness, but because they are highly nonlinear, understanding how they achieve robustness is difficult. In many rhythmic systems, robustness against perturbations involves response of both the shape and the timing of the trajectory. This makes the study of robustness even more challenging. To understand how a motor system produces robust behaviors in a variable environment, we consider a neuromechanical model of motor patterns in the feeding apparatus of the marine mollusk Aplysia californica (Shaw et al. in J Comput Neurosci 38(1):25–51, 2015; Lyttle et al. in Biol Cybern 111(1):25–47, 2017). We established in (Wang et al. in SIAM J Appl Dyn Syst 20(2):701–744, 2021. https://doi.org/10.1137/20M1344974) the tools for studying combined shape and timing responses of limit cycle systems under sustained perturbations and here apply them to study robustness of the neuromechanical model against increased mechanical load during swallowing. Interestingly, we discover that nonlinear biomechanical properties confer resilience by immediately increasing resistance to applied loads. In contrast, the effect of changed sensory feedback signal is significantly delayed by the firing rates’ hard boundary properties. Our analysis suggests that sensory feedback contributes to robustness in swallowing primarily by shifting the timing of neural activation involved in the power stroke of the motor cycle (retraction). This effect enables the system to generate stronger retractor muscle forces to compensate for the increased load, and hence achieve strong robustness. The approaches that we are applying to understanding a neuromechanical model in Aplysia, and the results that we have obtained, are likely to provide insights into the function of other motor systems that encounter changing mechanical loads and hard boundaries, both due to mechanical and neuronal firing properties.

59 BASIC BIOLOGICAL SCIENCES↗

Satellite Observations of the Tropical Terrestrial Carbon Balance and Interactions With the Water Cycle During the 21st Century

A constellation of satellites are now in orbit providing information about terrestrial carbon and water storage and fluxes. These combined observations show that the tropical biosphere has changed significantly in the last two decades from the combined effects of climate variability and land use. Large areas of forest have been cleared in both wet and dry forests, increasing the source of carbon to the atmosphere. Concomitantly, tropical fire emissions have declined, at least until 2016, from changes in land-use practices and rainfall, increasing the net carbon sink. Measurements of carbon stocks and fluxes from disturbance and recovery and of vegetation photosynthesis show significant regional variability of net biosphere exchange (NBE) and gross primary productivity (GPP) across the tropics and are tied to seasonal and interannual changes in water fluxes and storage. Comparison of satellite based estimates of evapotranspiration (ET), photosynthesis, and the deuterium content of water vapor with patterns of total water storage and rainfall demonstrate the presence of vegetation-atmosphere interactions and feedback mechanisms across tropical forests. However, these observations of stocks, fluxes and inferred interactions between them do not point unambiguously to either positive or negative feedbacks in carbon and water exchanges. These ambiguities highlight the need for assimilation of these new measurements with Earth System models for a consistent assessment of process interactions, along with focused field campaigns that integrate ground, aircraft and satellite measurements, to quantify the controlling carbon and water processes and their feedback mechanisms.

58 GEOSCIENCES↗

Temperature-dependence of oxidation and carburization of Grade 91 steel in CO 2 containing impurities

Future CO 2 based power systems require steels resistant to corrosion in high-temperature CO 2 -rich environments. Candidate 9Cr ferritic-martensitic steels degrade by surface oxidation and substrate carburization, both of which can be strongly affected by impurities in the CO 2 . In this study we examined Grade 91 steel exposed to 95%CO 2 -4%H 2 O-1%O 2 with/without 0.1% SO 2 at 1 atm and 550, 600, 650° C for up to 3000 h to establish the temperature-dependence of these processes. SO 2 showed little effect on oxidation at 550-600° C but reduced carburization, while the combination of SO 2 and faster alloy diffusion at 650° C resulted in significant reduction in both oxidation and carburization.

36 MATERIALS SCIENCE↗

Thruster Injector Faceplate Testing in Support of the Aerojet Rocket-Based Combined Cycle (RBCC) Concept

To satisfy RBCC rocket thruster requirements of high performance and a minimum amount of free hydrogen at plume boundary, a new impinging injector element using gaseous hydrogen and gaseous oxygen as the propellants has been designed. Analysis has shown that this injector design has potential to provide a high specific impulse (Isp) while minimizing the amount of free hydrogen that is available to be burned with incoming secondary flow. Past studies and test programs have shown that gas/gas-impinging elements typically result in high injector face temperatures due to combustion occurring close to the face. Since this design is new, there is no hot fire experience with this element. Objectives of this test program were to gain experience and hot fire test data on this new rocket thruster element design and injector faceplate pattern. Twenty-two hot fire tests were run with maximum mixture ratio (MR) and chamber pressure (Pc) obtained at 7.25 and 1,822 psia, respectively. Post-test scanning microscope (SEM) images show only slight faceplate erosion during testing. This injector element design performed well and can be operated at design conditions: (1) Pc of 2,000 psia and MR of 7.0 and (2) Pc of 1,000 psia and MR of 5.0.

Fazah, M. M.↗

Integration of Pumped Heat Energy Storage with Fossil-Fired Power Plant (Final Report)

The project team of Southwest Research Institute ® (SwRI ® ), Malta Inc. (Malta), and Luminant Generation Company LLC (Luminant) completed a feasibility study for the integration of a 100-MW, 10-hour (1000-MWh) Malta Pumped Heat Energy Storage (MPHES) system with multiple full-sized fossil-fired electricity generation units (EGU) in Luminant portfolio. MPHES is a long-duration, molten-salt-energy storage technology that uses turbomachinery and heat exchangers to transfer energy to a thermal storage media when charging, and removes the heat in a similar fashion when discharging. With high round trip efficiency (60-65%) and long lifespan (30+ years), MPHES provides economic benefits to the fossil-asset owners that can be scaled to integrate with assets across their portfolio. This technology uses hardware components, workforce personnel, and skillsets similar to those used by fossil EGUs, allowing for synergy when co-locating the two technologies. Luminant has approximately 39,000 megawatts of generation across 12 states, operating in six of the seven competitive markets in the U.S. and powered by a diverse portfolio of natural gas, nuclear, coal, and solar facilities. The DeCordova plant in Granbury, Texas, a simple cycle natural gas peaker power plant, was used as the fossil-fired asset in this project. The local market in Granbury, Texas has many influences, including several nearby power plants, a Luminant-owned nuclear plant (Comanche Peak), and substantial wind energy, which causes both negative pricing at night and high market volatility. Reducing false starts of the DeCordova plant and better responding to market volatility would be an economic advantage. Luminant is currently integrating battery storage plant on site to begin addressing these challenges. Integrating long-duration storage, like MPHES, would expand this capability beyond one hour of storage and have the potential to greatly reduce the total number of gas turbine starts. The MPHES charging requirement could help offset the overnight operating costs of Comanche Peak, which cannot load follow, and the nearby Luminant-owned Wise County combined cycle plant that cycles too often. Following the assessment of Luminant’s ERCOT-based portfolio for integration compatibility with Malta’s PHES system and the project tasks of conceptual study, technoeconomic analysis, technology gap assessment, and commercialization plan, the project team effort has resulted in several key outcomes: (1) Identification of market trends in a high-wind penetration market outside a major metropolitan area; (2) Creation of a dispatching model for the MPHES system and the pairing of Li-ion battery with a gas turbine in a real time market; (3) Revenue and cost estimations for operating MPHES alongside a gas peaker plant with real dispatching considerations and comparison with variations in the Malta implementation, including doubling the storage capacity and using two discharge drivetrains; (4) Potential carbon emission reductions possible by replacing gas turbine operation with Malta PHES operation; and (5) Summary of literature-based future market predictions for Texas.

20 FOSSIL-FUELED POWER PLANTS↗

Techno-Economic Analysis of a Cryogenic Flux Capacitor for Grid Storage

Abstract The Cryogenic Flux Capacitor (CFC) is a cold, dense fluid storage core with integrated design features that afford the designer flexibility and provide new possibilities for the storage and discharge of energy. The stored energy, in this case, is represented by hydrogen physically bonded within the nanoscale pores within the aerogel composite blanket material, and the process of bonding or debonding is governed by principles of physical adsorption (physisorption) and thermodynamics. The large surface area afforded by the nanoporous aerogel (∼1,000 m2/g) allows for storage densities close to, or in some cases exceeding, that of normal boiling point liquids. Its performance easily exceeds what can be achieved via ambient temperature, high-pressure gas storage for an equivalent volume. CFC storage is predicted to be easily scalable, is constructed from readily available commercial materials, lends itself to a range of pressure applications, and is geometry insensitive. The high energy density of CFC-stored hydrogen allows long durations of storage, such as daily to monthly cycling, which corresponds to approximately 10 to 100 hours of duration, respectively. The techno-economic analysis examines different types of hydrogen storage for commercial viability. The assessment includes the use of hydrogen blended with natural gas in a combined cycle gas turbine. The study provides results for a range of blends from 100% natural gas to 100% hydrogen. The required fuel usages are estimated for the intended application in a grid scenario that features large amounts of renewable penetration, 10 hours, and as a baseload, 100 hours. The study presents preliminary estimates of the capital cost of storage and operating cost of storage. In addition, the cost of firing natural gas and capturing the carbon dioxide (CO2) in a carbon capture and sequestration (CCS) system is assessed. Based on the study, it is shown that CFC can competitively meet performance and cost needs for grid-based energy storage.

08 HYDROGEN↗

Scaling carbon fluxes from eddy covariance sites to globe: synthesis and evaluation of the FLUXCOM approach

FLUXNET comprises globally distributed eddy-covariance-based estimates of carbon fluxes between the biosphere and the atmosphere. Since eddy covariance flux towers have a relatively small footprint and are distributed unevenly across the world, upscaling the observations is necessary to obtain global-scale estimates of biosphere–atmosphere exchange. Based on cross-consistency checks with atmospheric inversions, sun-induced fluorescence (SIF) and dynamic global vegetation models (DGVMs), here we provide a systematic assessment of the latest upscaling efforts for gross primary production (GPP) and net ecosystem exchange (NEE) of the FLUXCOM initiative, where different machine learning methods, forcing data sets and sets of predictor variables were employed. Spatial patterns of mean GPP are consistent across FLUXCOM and DGVM ensembles (R 2 >0.94 at 1° spatial resolution) while the majority of DGVMs show, for 70 % of the land surface, values outside the FLUXCOM range. Global mean GPP magnitudes for 2008–2010 from FLUXCOM members vary within 106 and 130 PgC yr -1 with the largest uncertainty in the tropics. Seasonal variations in independent SIF estimates agree better with FLUXCOM GPP (mean global pixel-wise R 2 ~0.75) than with GPP from DGVMs (mean global pixel-wise R 2 ~0.6). Seasonal variations in FLUXCOM NEE show good consistency with atmospheric inversion-based net land carbon fluxes, particularly for temperate and boreal regions (R 2 >0.92). Interannual variability of global NEE in FLUXCOM is underestimated compared to inversions and DGVMs. The FLUXCOM version which also uses meteorological inputs shows a strong co-variation in interannual patterns with inversions (R 2 =0.87 for 2001–2010). Mean regional NEE from FLUXCOM shows larger uptake than inversion and DGVM-based estimates, particularly in the tropics with discrepancies of up to several hundred grammes of carbon per square metre per year. These discrepancies can only partly be reconciled by carbon loss pathways that are implicit in inversions but not captured by the flux tower measurements such as carbon emissions from fires and water bodies. We hypothesize that a combination of systematic biases in the underlying eddy covariance data, in particular in tall tropical forests, and a lack of site history effects on NEE in FLUXCOM are likely responsible for the too strong tropical carbon sink estimated by FLUXCOM. Furthermore, as FLUXCOM does not account for CO 2 fertilization effects, carbon flux trends are not realistic. Overall, current FLUXCOM estimates of mean annual and seasonal cycles of GPP as well as seasonal NEE variations provide useful constraints of global carbon cycling, while interannual variability patterns from FLUXCOM are valuable but require cautious interpretation. Exploring the diversity of Earth observation data and of machine learning concepts along with improved quality and quantity of flux tower measurements will facilitate further improvements of the FLUXCOM approach overall.

54 ENVIRONMENTAL SCIENCES↗

Development of an Integrated Nozzle for a Symmetric, RBCC Launch Vehicle Configuration

The development of rocket based combined cycle (RBCC) engines is highly dependent upon integrating several different modes of operation into a single system. One of the key components to develop acceptable performance levels through each mode of operation is the nozzle. It must be highly integrated to serve the expansion processes of both rocket and air-breathing modes without undue weight, drag, or complexity. The NASA GTX configuration requires a fixed geometry, altitude-compensating nozzle configuration. The initial configuration, used mainly to estimate weight and cooling requirements was a 1 So half-angle cone, which cuts a concave surface from a point within the flowpath to the vehicle trailing edge. Results of 3-D CFD calculations on this geometry are presented. To address the critical issues associated with integrated, fixed geometry, multimode nozzle development, the GTX team has initiated a series of tasks to evolve the nozzle design, and validate performance levels. An overview of these tasks is given. The first element is a design activity to develop tools for integration of efficient expansion surfaces With the existing flowpath and vehicle aft-body, and to develop a second-generation nozzle design. A preliminary result using a "streamline-tracing" technique is presented. As the nozzle design evolves, a combination of 3-D CFD analysis and experimental evaluation will be used to validate the design procedure and determine the installed performance for propulsion cycle modeling. The initial experimental effort will consist of cold-flow experiments designed to validate the general trends of the streamline-tracing methodology and anchor the CFD analysis. Experiments will also be conducted to simulate nozzle performance during each mode of operation. As the design matures, hot-fire tests will be conducted to refine performance estimates and anchor more sophisticated reacting-flow analysis.

Smith, Timothy D.↗

Method for spinning up a three-axis controlled spacecraft

A three-axis controlled spacecraft (1), typically a satellite, is spun up about its roll axis (20) prior to firing a motor (2), i.e., a perigee kick motor, to achieve the requisite degree of angular momentum stiffness. Thrusters (21) for imparting rotation about the roll axis (20) are activated in open-loop fashion, typically at less than full duty cycle. Cross-axis torques induced by this rotational motion are compensated for by means of closed control loops for each of the pitch and yaw axes (30, 40, respectively). Each closed control loop combines a prebias torque (72) with torques (75, 74) representative of position and rate feedback information, respectively. A deadband (52) within each closed control loop can be widened during the spinup, to conserve fuel. Position feedback information (75) in each of the control loops is disabled upon saturation of the gyroscope associated with the roll axis (20).

Vorlicek, Preston L.↗

CECE: Expanding the Envelope of Deep Throttling Technology in Liquid Oxygen/Liquid Hydrogen Rocket Engines for NASA Exploration Missions

As one of the first technology development programs awarded by NASA under the Vision for Space Exploration, the Pratt & Whitney Rocketdyne (PWR) Deep Throttling, Common Extensible Cryogenic Engine (CECE) program was selected by NASA in November 2004 to begin technology development and demonstration toward a deep throttling, cryogenic engine supporting ongoing trade studies for NASA s Lunar Lander descent stage. The CECE program leverages the maturity and previous investment of a flight-proven hydrogen/oxygen expander cycle engine, the PWR RL10, to develop and demonstrate an unprecedented combination of reliability, safety, durability, throttlability, and restart capabilities in high-energy, cryogenic, in-space propulsion. The testbed selected for the deep throttling demonstration phases of this program was a minimally modified RL10 engine, allowing for maximum current production engine commonality and extensibility with minimum program cost. Four series of demonstrator engine tests have been successfully completed between April 2006 and April 2010, accumulating 7,436 seconds of hot fire time over 47 separate tests. While the first two test series explored low power combustion (chug) and system instabilities, the third test series investigated and was ultimately successful in demonstrating several mitigating technologies for these instabilities and achieved a stable throttling ratio of 13:1. The fourth test series significantly expanded the engine s operability envelope by successfully demonstrating a closed-loop control system and extensive transient modeling to enable lower power engine starting, faster throttle ramp rates, and mission-specific ignition testing. The final hot fire test demonstrated a chug-free, minimum power level of 5.9%, corresponding to an overall 17.6:1 throttling ratio achieved. In total, these tests have provided an early technology demonstration of an enabling cryogenic propulsion concept with invaluable system-level technology data acquisition toward design and development risk mitigation for future lander descent main engines.

Giuliano, Victor J.↗

Atmospheric processing and aerosol aging responsible for observed increase in absorptivity of long-range-transported smoke over the southeast Atlantic

Biomass burning aerosol (BBA) from agricultural fires in southern Africa contributes about one-third of the global carbonaceous aerosol load. These particles have strong radiative effects in the southeast Atlantic (SEA), which depend in part on the radiative contrast between the aerosol layer in the free troposphere (FT) and the underlying cloud layer. However, there is large disagreement in model estimates of aerosol-driven climate forcing due to uncertainties in the vertical distribution, optical properties, and life cycle of these particles. This study applies a novel method combining remote sensing observations with regional model outputs to investigate the aging of the BBA and its impact on the optical properties during transatlantic transport from emission sources in Africa to the SEA. Results show distinct variations in extinction Ångström exponent (EAE) and single-scattering albedo (SSA) as aerosols age. Near the source, fresh aerosols are characterized by low mean SSA (0.84) and high EAE (1.85), indicating smaller, highly absorbing particles. By isolating marine contributions from the total column during BBA transport across the SEA, our analysis reveals an initial decrease in BBA absorptivity, with mean FT SSA of 0.87 after 6–7 d, followed by increased absorptivity with mean FT SSA of 0.84 after 10 d, suggesting enhanced absorption due to chemical aging. These findings indicate that BBA becomes more absorbing during extended transport across the SEA, with implications for reducing model uncertainties. Our remote-sensing-based results agree well with previous in situ studies and offer new insights into aerosol–radiation interactions and the energy balance over the SEA.

54 ENVIRONMENTAL SCIENCES↗

Channel Selection for the Advanced Baseline Imager (ABI)

The GOES-R (Geostationary Operational Environmental Satellite-R) Imager will be the fourth generation imaging radiometer flown in 40 years that observes the western hemisphere from geosynchronous orbit. The Imager is an international resource for information about unpredictable short-term mesoscale phenomena such as severe storms, precipitation, clouds and fog, fires and volcanoes. As such, it must provide: (1) continuity of service, (2) valuable new capabilities, and (3) synergy with the companion fleet of imaging radiometers. This combination of requirements lead to a suite of channels evolved from the generations of LEO (low Earth orbit) and GEO- (geosynchronous Earth orbit) and -sounders. To maximize the science and applications payoff from its unique viewpoint, the next generation GOES Imager should concentrate upon regional measurements of the chaotic atmospheric phenomena involving water and the diurnal cycle -- energy potential, moisture transport, phase changes, precipitation, and cloud climatology.

Chesters, Dennis↗

A History of Welding on the Space Shuttle Main Engine (1975 to 2010)

The Space Shuttle Main Engine (SSME) is a high performance, throttleable, liquid hydrogen fueled rocket engine. High thrust and specific impulse (Isp) are achieved through a staged combustion engine cycle, combined with high combustion pressure (approx.3000psi) generated by the two-stage pump and combustion process. The SSME is continuously throttleable from 67% to 109% of design thrust level. The design criteria for this engine maximize performance and weight, resulting in a 7,800 pound rocket engine that produces over a half million pounds of thrust in vacuum with a specific impulse of 452/sec. It is the most reliable rocket engine in the world, accumulating over one million seconds of hot-fire time and achieving 100% flight success in the Space Shuttle program. A rocket engine with the unique combination of high reliability, performance, and reusability comes at the expense of manufacturing simplicity. Several innovative design features and fabrication techniques are unique to this engine. This is as true for welding as any other manufacturing process. For many of the weld joints it seemed mean cheating physics and metallurgy to meet the requirements. This paper will present a history of the welding used to produce the world s highest performance throttleable rocket engine.

Zimmerman, Frank R.↗

Forecasting Global Fire Emissions on Subseasonal to Seasonal (S2S) Time Scales

Fire emissions of gases and aerosols alter atmospheric composition and have substantial impacts on climate, ecosystem function, and human health. Warming climate and human expansion in fire‐prone landscapes exacerbate fire impacts and call for more effective management tools. Here we developed a global fire forecasting system that predicts monthly emissions using past fire data and climate variables for lead times of 1 to 6 months. Using monthly fire emissions from the Global Fire Emissions Database (GFED) as the prediction target, we fit a statistical time series model, the Autoregressive Integrated Moving Average model with eXogenous variables (ARIMAX), in over 1,300 different fire regions. Optimized parameters were then used to forecast future emissions. The forecast system took into account information about region‐specific seasonality, long‐term trends, recent fire observations, and climate drivers representing both large‐scale climate variability and local fire weather. We cross‐validated the forecast skill of the system with different combinations of predictors and forecast lead times. The reference model, which combined endogenous and exogenous predictors with a 1 month forecast lead time, explained 52% of the variability in the global fire emissions anomaly, considerably exceeding the performance of a reference model that assumed persistent emissions during the forecast period. The system also successfully resolved detailed spatial patterns of fire emissions anomalies in regions with significant fire activity. This study bridges the gap between the efforts of near‐real‐time fire forecasts and seasonal fire outlooks and represents a step toward establishing an operational global fire, smoke, and carbon cycle forecasting system.

vapor pressure↗

A Simple Model for Rotating Detonation Rocket Engine Sizing and Performance Estimates

A Rotating Detonation Rocket Engine (RDRE) model is described which characterizes the device as an essentially infinite number of circumferentially arranged, sequentially firing pulse detonation engine (PDE) tubes. The PDE tubes are in turn treated as lumped-parameter chambers, each of which executes a dynamic (i.e. time dependent) Atkinson cycle with an allowance for a finite Mach number during the refill portion of the cycle. The formulation results in several free parameters which are used to essentially tune the model such that it closely matches higher fidelity computational fluid dynamic RDRE simulations in terms of performance, flow rates, etc. The simplicity of the model allows for straightforward combination with component models (e.g. turbopumps, cooling jackets, etc.) as well as implementation within larger vehicle simulations. Such capability allows for realistic mission analyses and benefits studies which will help to determine the best application for the RDRE concept.

detonation↗

A Simple Model for Rotating Detonation Rocket Engine Sizing and Performance Estimates

A Rotating Detonation Rocket Engine (RDRE) model is described which characterizes the device as an essentially infinite number of circumferentially arranged, sequentially firing pulse detonation engine (PDE) tubes. The PDE tubes are in turn treated as lumped-parameter chambers, each of which executes a dynamic (i.e. time dependent) Atkinson cycle with an allowance for a finite Mach number during the refill portion of the cycle. The formulation results in several free parameters which are used to essentially tune the model such that it closely matches higher fidelity computational fluid dynamic RDRE simulations in terms of performance, flow rates, etc. The simplicity of the model allows for straightforward combination with component models (e.g. turbopumps, cooling jackets, etc.) as well as implementation within larger vehicle simulations. Such capability allows for realistic mission analyses and benefits studies which will help to determine the best application for the RDRE concept.

detonation↗

Diel cycle impacts on the chemical and light absorption properties of organic carbon aerosol from wildfires in the western United States

Abstract. Organic aerosol (OA) emissions from biomass burning have been the subject of intense research in recent years, involving a combination of field campaigns and laboratory studies. These efforts have aimed at improving our limited understanding of the diverse processes and pathways involved in the atmospheric processing and evolution of OA properties, culminating in their accurate parameterizations in climate and chemical transport models. To bring closure between laboratory and field studies, wildfire plumes in the western United States were sampled and characterized for their chemical and optical properties during the ground-based segment of the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign. Using a custom-developed multiwavelength integrated photoacoustic-nephelometer spectrometer in conjunction with a suite of instruments, including an oxidation flow reactor equipped to generate hydroxyl (OH⚫) or nitrate (NO3⚫) radicals to mimic daytime or nighttime oxidative aging processes, we investigated the effects of multiple equivalent hours of OH⚫ or NO3⚫ exposure on the chemical composition and mass absorption cross-sections (MAC(λ)) at 488 and 561 nm of OA emitted from wildfires in Arizona and Oregon. We found that OH⚫ exposure induced a slight initial increase in absorption corresponding to short timescales; however, at longer timescales, the wavelength-dependent MAC(λ) decreased by a factor of 0.72 ± 0.08, consistent with previous laboratory studies and reports of photobleaching. On the other hand, NO3⚫ exposure increased MAC(λ) by a factor of up to 1.69 ± 0.38. We also noted some sensitivity of aerosol aging to different fire conditions between Arizona and Oregon. The MAC(λ) enhancement following NO3⚫ exposure was found to correlate with an enhancement in CHO1N and CHOgt1N ion families measured by an Aerodyne aerosol mass spectrometer.

54 ENVIRONMENTAL SCIENCES↗