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At least 73 records · Page 4

Secondary Organic Aerosol from OH Oxidation of Acyclic Terpenes Is More Viscous and Less Volatile than That of Their Cyclic Analogs

Biogenic volatile organic compounds (BVOCs), a dominant source of secondary organic aerosol (SOA) globally, exhibit emission rates and composition that are plant species-specific and vary with environmental stressors. A common outcome of plant stress is increased emissions of acyclic terpenes. The paucity of information about acyclic terpene SOA chemistry contributes to uncertainties in predictions of SOA global loadings and impacts on Earth’s radiative budget, particularly in a changing climate where acyclic terpene emissions could become more prominent. This study compared properties of SOA derived from OH oxidation of acyclic and cyclic monoterpenes (ß-ocimene, a-pinene) and sesquiterpenes (ß-farnesene, ß-caryophyllene). Single particle mass spectrometry was used for assessing shape, density, and evaporation kinetics of size-selected SOA particles, and nanospray desorption electrospray ionization high-resolution mass spectrometry (nano-DESI-HRMS) was used to measure molecular composition of SOA. Acyclic terpene SOA exhibited higher viscosity and lower volatility compared to cyclic terpene SOA, and had a greater volume fraction remaining (VFR) after ~24 hours of evaporation - approximately 1.3-1.6 times higher VFR than that of cyclic terpene SOA. Additionally, HRMS analysis revealed greater chemical diversity and higher fractions of extremely low volatility compounds (56-62% ELVOC/LVOC) in acyclic terpene SOA compared to cyclic counterparts (25-37% ELVOC/LVOC). Our findings highlight the potential importance of accounting for acyclic terpene aerosol chemistry under conditions of plant stress to improve predictions of SOA loadings and impacts.

SOA physical properties↗

Reducing uncertainty of high-latitude ecosystem models through identification of key parameters

Abstract Climate change is having significant impacts on Earth’s ecosystems and carbon budgets, and in the Arctic may drive a shift from an historic carbon sink to a source. Large uncertainties in terrestrial biosphere models (TBMs) used to forecast Arctic changes demonstrate the challenges of determining the timing and extent of this possible switch. This spread in model predictions can limit the ability of TBMs to guide management and policy decisions. One of the most influential sources of model uncertainty is model parameterization. Parameter uncertainty results in part from a mismatch between available data in databases and model needs. We identify that mismatch for three TBMs, DVM-DOS-TEM, SIPNET and ED2, and four databases with information on Arctic and boreal above- and belowground traits that may be applied to model parametrization. However, focusing solely on such data gaps can introduce biases towards simple models and ignores structural model uncertainty, another main source for model uncertainty. Therefore, we develop a causal loop diagram (CLD) of the Arctic and boreal ecosystem that includes unquantified, and thus unmodeled, processes. We map model parameters to processes in the CLD and assess parameter vulnerability via the internal network structure. One important substructure, feed forward loops (FFLs), describe processes that are linked both directly and indirectly. When the model parameters are data-informed, these indirect processes might be implicitly included in the model, but if not, they have the potential to introduce significant model uncertainty. We find that the parameters describing the impact of local temperature on microbial activity are associated with a particularly high number of FFLs but are not constrained well by existing data. By employing ecological models of varying complexity, databases, and network methods, we identify the key parameters responsible for limited model accuracy. They should be prioritized for future data sampling to reduce model uncertainty.

54 ENVIRONMENTAL SCIENCES↗

Impact of Alkali and Alkali‐Earth Cations on Ni‐Catalyzed Dimerization of Butene

Abstract The presence of alkali (Na + or Li + ) or alkali‐earth (Ca 2+ or Mg 2+ ) cations adjusting the acid‐base properties on amorphous silica‐alumina influences markedly the catalytic properties of supported Ni for 1‐butene dimerization. The low concentration of Brønsted acid sites on these catalysts reduces the double bond isomerization of butene and inhibits the formation of dimethylhexene as primary product. While the alkali and alkali‐earth cations act as weak Lewis acid sites, only Ni 2+ sites are catalytically active for dimerization of 1‐butene. n ‐Octene and methylheptene are formed selectively as primary products; dimethylhexene is a secondary product. The open environment of the Ni 2+ sites does not induce different reaction pathways compared to Ni 2+ in the pores of zeolites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cities Are Concentrators of Complex, MultiSectoral Interactions Within the Human-Earth System

Cities are concentrators of complex, multi-sectoral interactions. As keystones in the interconnected human-Earth system, cities have an outsized impact on the Earth system. We describe a multi-lens framework for organizing our understanding of the complexity of urban systems and scientific research on urban systems, which may be useful for natural system scientists exploring the ways their work can be made more actionable. We then describe four critical dimensions along which improvements are needed to advance the urban research that addresses urgent climate challenges: (a) solutions-oriented research, (b) equity-centered assessments which rely on fine-scale human and ecological data, (c) co-production of knowledge, and (d) better integration of human and natural systems occurring through theory, observation, and modeling.

54 ENVIRONMENTAL SCIENCES↗

Large-misalignment mechanism for the formation of compact axion structures: Signatures from the QCD axion to fuzzy dark matter

Axions are some of the best motivated particles beyond the Standard Model. We show how the attractive self-interactions of dark matter (DM) axions over a broad range of masses, from 10 –22 eV to 10 7 GeV, can lead to nongravitational growth of density fluctuations and the formation of bound objects. This structure formation enhancement is driven by parametric resonance when the initial field misalignment is large, and it affects axion density perturbations on length scales of order the Hubble horizon when the axion field starts oscillating, deep inside the radiation-dominated era. This effect can turn an otherwise nearly scale-invariant spectrum of adiabatic perturbations into one that has a spike at the aforementioned scales, producing objects ranging from dense DM halos to scalar-field configurations such as solitons and oscillons. We call this class of cosmological scenarios for axion DM production “the large-misalignment mechanism.” In this work, we explore observational consequences of this mechanism for axions with masses up to 10 eV. For axions heavier than 10 –5 eV, the compact axion halos are numerous enough to significantly impact Earth-bound direct detection experiments, yielding intermittent but coherent signals with repetition rates exceeding one per decade and crossing times less than a day. These episodic increases in the axion density and kinematic coherence suggest new approaches for axion DM searches, including for the QCD axion. Dense structures made up of axions from 10 –22 eV to 10 –5 eV are detectable through gravitational lensing searches, and their gravitational interactions can also perturb baryonic structures and alter star formation. At very high misalignment amplitudes, the axion field can undergo self-interaction-induced implosions long before matter-radiation equality, producing potentially-detectable low-frequency stochastic gravitational waves.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The lightness of water vapor helps to stabilize tropical climate

Moist air is lighter than dry air at the same temperature, pressure, and volume because the molecular weight of water is less than that of dry air. We call this the vapor buoyancy effect. Although this effect is well documented, its impact on Earth’s climate has been overlooked. Here, we show that the lightness of water vapor helps to stabilize tropical climate by increasing the outgoing longwave radiation (OLR). In the tropical atmosphere, buoyancy is horizontally uniform. Then, the vapor buoyancy in the moist regions must be balanced by warmer temperatures in the dry regions of the tropical atmosphere. These higher temperatures increase tropical OLR. This radiative effect increases with warming, leading to a negative climate feedback. At a near present-day surface temperature, vapor buoyancy is responsible for a radiative effect of 1 W/m 2 and a negative climate feedback of about 0.15 W/m 2 per kelvin.

54 ENVIRONMENTAL SCIENCES↗

Fast and sensitive measurements of sub-3 nm particles using Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM)

New particle formation (NPF) is the atmospheric process whereby gas molecules react and nucleate to form detectable particles. NPF has a strong impact on Earth's radiative balance as it produces roughly half of global cloud condensation nuclei. However, the time resolution and sensitivity of current instrumentation are inadequate in measuring the size distribution of sub-3 nm particles, the particles critical for understanding NPF. Here we present the Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM), a method to measure the concentrations of freshly nucleated particles. The CPC FARM consists of five CPCs operating in parallel, each configured to operate at different detectable particle sizes between 1–3 nm. This study explores two methods to calculate the size distribution from the differential measurements across the CPC channels. The performance of both inversion methods was tested against the size distribution measured by a pair of stepping particle mobility sizers (SMPSs) during an ambient air sampling study in Pittsburgh, PA. Observational results indicate that the CPC FARM is more accurate with higher time resolution and sensitivity in the sub-3 nm range compared to the SMPS.

Cheng, Darren [Carnegie Mellon Univ., Pittsburgh, ↗

NeuralMie (v1.0): an aerosol optics emulator

The direct interactions of atmospheric aerosols with radiation significantly impact the Earth's climate and weather and are important to represent accurately in simulations of the atmosphere. This work introduces two contributions to enable a more accurate representation of aerosol optics in atmosphere models: (1) NeuralMie, a neural network Mie scattering emulator that can directly compute the bulk optical properties of a diverse range of aerosol populations and is appropriate for use in atmosphere simulations where aerosol optical properties are parameterized, and (2) TAMie, a fast Python-based Mie scattering code based on the Toon and Ackerman (1981) Mie scattering algorithm that can represent both homogeneous and coated particles. TAMie achieves speed and accuracy comparable to established Fortran Mie codes and is used to produce training data for NeuralMie. NeuralMie is highly flexible and can be used for a wide range of particle types, wavelengths, and mixing assumptions. It can represent core-shell scattering and, by directly estimating bulk optical properties, is more efficient than existing Mie code and Mie code emulators while incurring negligible error compared to existing aerosol optics parameterization schemes (0.08 % mean absolute percentage error).

54 ENVIRONMENTAL SCIENCES↗

The OSIRIS-REx Sample Return Capsule re-entry: A coordinated seismo-acoustic observational campaign for the study of meteor phenomena

Objects entering Earth’s atmosphere at hypersonic velocities may generate powerful acoustic waves. Depending on atmospheric conditions and acoustic propagation paths, they may be captured using ground or balloon-borne microbarometers and microphones. Impacts into the Earth’s atmosphere by asteroids in a meter-size range are sporadic and unannounced, and thus, well-documented scientific observations of asteroids are rare and generally happen by chance. Arriving from interplanetary space at hypervelocity, spacecraft are considered analogues for low velocity meteoroids and asteroids impacting the Earth’s atmosphere, and as such provide unprecedented and unique opportunity to carry out planned observational campaigns and perform detailed studies of meteor phenomena. However, since the end of the Apollo era, only four instances of a hypersonic re-entry of an artificial body from interplanetary space with an incident speed of 11-12 km/s have been observed and studied. These were the Sample Return Capsules (SRCs) that brought physical samples of extraterrestrial material back to Earth (Genesis, Stardust, Hayabusa 1, Hayabusa 2). These re-entries were also detected by infrasound and/or seismic sensors. The next opportunity to observe an artificial meteor will be on 24 September 2023 with the re-entry of NASA’s OSIRIS-REx SRC that will bring samples of the carbonaceous near-Earth asteroid Bennu. The re-entry consists of several flight phases, including hypersonic and supersonic, providing a unique opportunity to observe these by infrasound and seismic sensors. We will discuss observational campaign efforts aimed to capture geophysical signals generated by the OSIRIS-REx SRC re-entry. This campaign utilizes an unparalleled number of instruments, both ground and airborne, strategically positioned in the immediate and extended region around the projected re-entry trajectory to maximize the scientific output.

47 - OTHER INSTRUMENTATION↗

Correction and calibration of atmospheric impact observations in GOES GLM data

The Earth's atmosphere is impacted daily by both meteoroids and artificial objects. Calibrated observations of the emitted light at sufficiently high sampling rates can enable or improve the estimation of impactor attributes such as size, cohesion, trajectory, and composition, but are difficult to obtain owing to the unpredictability, brevity, and high dynamic (brightness) range of impacts. Ground-based camera systems have successfully monitored small regions of the atmosphere at video frame rates and with limited radiometric capabilities, but most impacts occur over the 70% of the Earth's surface covered by water and are therefore missed by these networks. The Geostationary Lightning Mapper (GLM) instruments aboard Geostationary Operational Environmental Satellites 16 and 17 provide near-hemispherical coverage at 500 frames per second. These data have been shown to contain the signatures of many independently confirmed impacts, often from both viewing angles simultaneously, and constitute an observational resource that is currently unparalleled in the public domain. NASA's Asteroid Threat Assessment Project has implemented an automated impact detection pipeline that processes data from GLM daily. Given a detected impact, the GLM data contain a wealth of information for use in quantitative follow-up analyses. However, impact events differ from lightning in ways that violate key assumptions built into GLM's design. The result is that GLM's onboard processing introduces errors into pixel observations of impact events and the calibrated energies near the periphery of the detector may be substantially overestimated. We present methods for mitigating these and other issues to produce a data product more suitable for impact analyses than the existing GLM lightning product.

58 GEOSCIENCES↗

Scaling Global Warming Impacts on Ocean Ecosystems: Lessons From a Suite of Earth System Models

An important technique used by climate modelers to isolate the impacts of increasing greenhouse gasses on Earth System processes is to simulate the impact of an abrupt increase in carbon dioxide. The spatial pattern of change provides a “fingerprint” that is generally much larger than natural variability. Insofar as the response to radiative forcing is linear (the impact of quadrupling CO 2 is twice the impact of doubling CO 2 ) this fingerprint can then be used to estimate the impact of historical greenhouse gas forcing. However, the degree to which biogeochemical cycles respond linearly to radiative forcing has rarely been tested. In this paper, we evaluate which ocean biogeochemical fields are likely to respond linearly to changing radiative forcing, which ones do not, and where linearity breaks down. We also demonstrate that the representation of lateral mixing by mesoscale eddies, which varies significantly across climate models, plays an important role in modulating the breakdown of linearity. Globally integrated surface rates of biogeochemical cycling (primary productivity, particulate export) respond in a relatively linear fashion and are only moderately sensitive to mixing. By contrast, the habitability of the interior ocean (as determined by hypoxia and calcite supersaturation) behaves non-linearly and is very sensitive to mixing. This is because the deep ocean, as well as certain regions in the surface ocean, are very sensitive to the magnitude of deep wintertime convection. The cessation of convection under global warming is strongly modulated by the representation of eddy mixing.

54 ENVIRONMENTAL SCIENCES↗

Noble gas insights into early impact delivery and volcanic outgassing to Earth's atmosphere: A limited role for the continental crust

Earth's atmosphere, crust and mantle have evolved together through continuous geochemical exchange throughout Earth's history. Constraints on the transport of volatile elements and compounds between these reservoirs are crucial for understanding how Earth could have stayed habitable for extended periods of time. In this work, we present a new forward model of He, Ne and Ar in the mantle, crust and atmosphere. We explore concentrations of noble gases at the end of accretion, bulk silicate Earth K/U ratios, crustal growth scenarios, and upper mantle processing rates throughout Earth's history. We search for parameter combinations that simultaneously satisfy observational constraints on present-day mantle 4 He/ 3 He and 40 Ar/ 36 Ar (sensitive to mantle outgassing and continental crust growth, which depletes the mantle of U, Th and K), atmospheric 20 Ne/ 22 Ne (which tracks the mix of outgassed vs. delivered Ne in the atmosphere), and atmospheric 40 Ar/ 36 Ar in the past and today (sensitive to volatile delivery, mantle outgassing and crustal growth). Leveraging this intertwined set of noble gas abundances and isotopic compositions yields new constraints on initial noble gas abundances in the mantle and on the proportions of atmospheric volatiles originating from delivery by impact degassing, mantle outgassing, and degassing of the continental crust. We find that atmospheric Ar isotopic evolution is primarily sensitive to the mantle processing rate history; the atmospheric Ar isotopic record should therefore not be used to reconstruct continental crust growth, but instead provides valuable insights into mantle processing rates. Our model predicts a measurably low 20 Ne/ 22 Ne ratio of ~9.7 in Archean atmospheric samples. Most of atmospheric primordial 36 Ar was directly delivered by chondritic bodies and not transferred to the atmosphere during an intense early episode of mantle outgassing. Nitrogen delivered by impact degassing could account for the present-day atmospheric nitrogen inventory.

58 GEOSCIENCES↗

Optical Properties of Individual Tar Balls in the Free Troposphere

Tar balls are brown carbonaceous particles, highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are believed to have a significant impact on the Earth’s radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory “Ottavio Vittori” on Mt. Cimone, Italy (2165 meters above sea level) using multi-modal micro-spectroscopy. Our results show that tar balls contributed 50% of carbonaceous particles by number in the size range from 0.25 to 1.8 µm. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average refractive index of inhomogeneously and homogenously mixed tar balls (1.40 - 0.03i, and 1.36 - 0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model (SBDART) and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 Wm-2 (on a clear sky day) to 9.5 Wm-2 (when clouds are below the aerosol layer). In conclusion, understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.

54 ENVIRONMENTAL SCIENCES↗

Potential ecological impacts of climate intervention by reflecting sunlight to cool Earth

As the effects of anthropogenic climate change become more severe, several approaches for deliberate climate intervention to reduce or stabilize Earth’s surface temperature have been proposed. Solar radiation modification (SRM) is one potential approach to partially counteract anthropogenic warming by reflecting a small proportion of the incoming solar radiation to increase Earth’s albedo. While climate science research has focused on the predicted climate effects of SRM, almost no studies have investigated the impacts that SRM would have on ecological systems. The impacts and risks posed by SRM would vary by implementation scenario, anthropogenic climate effects, geographic region, and by ecosystem, community, population, and organism. Complex interactions among Earth’s climate system and living systems would further affect SRM impacts and risks. We focus here on stratospheric aerosol intervention (SAI), a well-studied and relatively feasible SRM scheme that is likely to have a large impact on Earth’s surface temperature. We outline current gaps in knowledge about both helpful and harmful predicted effects of SAI on ecological systems. Desired ecological outcomes might also inform development of future SAI implementation scenarios. In addition to filling these knowledge gaps, increased collaboration between ecologists and climate scientists would identify a common set of SAI research goals and improve the communication about potential SAI impacts and risks with the public. Without this collaboration, forecasts of SAI impacts will overlook potential effects on biodiversity and ecosystem services for humanity.

54 ENVIRONMENTAL SCIENCES↗

Interdisciplinary Workshop on the Impacts of Land Use and Land Management on Earth System Evolution, Biogeochemical Cycles, Extremes, and Inter-Sectoral Dynamics (Final Report)

The Aspen Global Change Institute (AGCI) convened a week-long interdisciplinary science workshop from September 15-20, 2019 entitled, “Impacts of Land Use and Land Management on Earth System Evolution, Biogeochemical Cycles, Extremes, and Inter-Sectoral Dynamics.” The purpose of the workshop was to advance research on the impacts of land use and land management on climate, carbon emissions, and extremes, as well as the impact of land-use change on important societal issues such as food, water, and energy security. The workshop was co-chaired by Kate Calvin (PNNL), George Hurtt (University of Maryland), and Dave Lawrence (National Center for Atmospheric Research). Co-funders of the workshop included NASA, NOAA, and travel support for European colleagues through CRESCENDO. This workshop brought together 31 professionals with expertise across biogeochemistry, climate impacts, mitigation, land use datasets, and societal impacts to coordinate on upcoming research and publications on the role of biogeochemical and biophysical properties of the Earth surface and their implications for climate, as conducted through the Land Use model Intercomparison Project (LUMIP), which is part of Phase 6 of the Coupled Model Intercomparison Project (CMIP6). A primary outcome of the meeting was the definition and planning of a series of LUMIP papers that will rely on the LUMIP and CMIP6 simulations. By the end of the meeting more than twenty papers and paper lead authors had been identified and scoped out. Around ten of these papers were submitted by the December 31, 2019 IPCC deadline.

54 ENVIRONMENTAL SCIENCES↗

Impact of organic acids on extraction of rare earth elements: Mechanisms and optimization

Organic acids are increasingly recognized as an environmentally friendly and efficient selective leaching agent of critical minerals. However, their impact on subsequent extraction processes remains unclear. This study investigates the extraction behavior of rare earth elements (REEs), representative of critical minerals, in the presence of various organic acids, including citric acid, maleic acid, malonic acid, DL-malic acid, L(+)-tartaric acid, and L-ascorbic acid. The results show that organic acids slightly reduce the extraction of REEs but greatly increase the extraction of aluminum (Al³⁺), making it harder to separate REEs from other elements. To avoid this, it is best to keep organic acid concentrations as low as possible in practical applications. However, by optimizing extraction conditions, these negative effects can be minimized. Specifically, adjusting the contact time between solutions allows for efficient REE extraction while limiting unwanted aluminum extraction. Among the acids tested, malonic acid and L(+)-tartaric acid were found to be the most effective for selectively extracting REEs. Mechanistically, organic acids are likely to form complexes with REEs and D2EHPA during extraction, except for Y (III), offering practical guidelines for optimizing REE recovery. Beyond extraction, this study also highlights a way to recover organic acids by precipitating REEs from stripping solutions using oxalic acid, which adds both environmental and economic benefits. Furthermore, these findings provide useful insights for optimizing REE recovery and offer a reference for extracting other critical minerals from solutions containing organic acids.

D2EHPA↗

Stellar wind impact on early atmospheres around unmagnetized Earth-like planets

ABSTRACT Stellar rotation at early ages plays a crucial role in the survival of primordial atmospheres around Earth-mass exoplanets. Earth-like planets orbiting fast-rotating stars may undergo complete photoevaporation within the first few hundred Myr driven by the enhanced stellar XUV [X-rays and extreme ultraviolet (EUV)] radiation, while planets orbiting slow-rotating stars are expected to experience difficulty in losing their primordial envelopes. Besides the action of stellar radiation, stellar winds induce additional erosion on these primordial atmospheres, altering their morphology, extent, and causing supplementary atmospheric losses. In this paper, we study the impact of activity-dependent stellar winds on primordial atmospheres to evaluate the extent to which the action of these winds can be significant in the whole planetary evolution at early evolutionary stages. We performed 3D magnetohydrodynamical (MHD) simulations of the interaction of photoevaporating atmospheres around unmagnetized Earth-mass planets in the time span between 50 and 500 Myr, analysing the joint evolution of stellar winds and atmospheres for both fast- and slow-rotating stars. Our results reveal substantial changes in the evolution of primordial atmospheres when influenced by fast-rotating stars, with a significant reduction in extent at early ages. In contrast, atmospheres embedded in the stellar winds from slow-rotating stars remain largely unaltered. The interaction of the magnetized stellar winds with the ionized upper atmospheres of these planets allows us to evaluate the formation and evolution of different MHD structures, such as double bow shocks and induced magnetospheres. This work will shed light on the first evolutionary stages of Earth-like exoplanets, which are of crucial relevance in terms of planet habitability.

Astronomy & Astrophysics↗