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At least 271 records · Page 15

Benchmark calculations of radiative forcing by greenhouse gases

Changes in concentrations of greenhouse gases lead to changes in radiative fluxes throughout the atmosphere. The value of this change, the instantaneous radiative forcing, varies across climate models, due partly to differences in the distribution of clouds, humidity, and temperature across models, and partly due to errors introduced by approximate treatments of radiative transfer. This paper describes an experiment within the Radiative Forcing Model Intercomparision Project that uses benchmark calculations made with line–by–line models to identify parameterization error in the representation of absorption and emission by greenhouse gases. Clear–sky instantaneous forcing by greenhouse gases is computed using a set of 100 profiles, selected from a re–analysis of present–day conditions, that represent the global annual mean forcing from pre–industrial times to the present–day with sampling errors of less than 0.01 W m –2 . Six contributing line–by–line models agree in their estimate of this forcing to within 0.025 W m –2 while even recently–developed parameterizations have typical errors four or more times larger, suggesting both that the samples reveal true differences among line–by–line models and that parameterization error will be readily identifiable. Agreement among line–by–line models is better in the longwave than in the shortwave where differing treatments of the water vapor vapor continuum affect estimates of forcing by carbon dioxide and methane. The impacts of clouds on instantaneous radiative forcing are estimated from climate model simulations. Here, the adjustment due to stratospheric temperature change by assuming fixed dynamical heating. Adjustments are large only for ozone and for carbon dioxide, for which stratospheric cooling introduces modest non–linearity.

54 ENVIRONMENTAL SCIENCES↗

High-Latitude Stratospheric Aerosol Geoengineering Can Be More Effective if Injection Is Limited to Spring

Stratospheric aerosol geoengineering focused on the Arctic could substantially reduce local and worldwide impacts of anthropogenic global warming. Because the Arctic receives little sunlight during the winter, stratospheric aerosols present in the winter at high latitudes have little impact on the climate, whereas stratospheric aerosols present during the summer achieve larger changes in radiative forcing. Injecting SO 2 in the spring leads to peak aerosol optical depth (AOD) in the summer. We demonstrate that spring injection produces approximately twice as much summer AOD as year-round injection and restores approximately twice as much September sea ice, resulting in less increase in stratospheric sulfur burden, stratospheric heating, and stratospheric ozone depletion per unit of sea ice restored. Furthermore, we also find that differences in AOD between different seasonal injection strategies are small compared to the difference between annual and spring injection.

58 GEOSCIENCES↗

Dry Deposition Methods Based on Turbulence Kinetic Energy: 1. Evaluation of Various Resistances and Sensitivity Studies Using a Single‐Point Model

Different functions are used to account for turbulence strength in the atmospheric boundary layer for different stability regimes. These functions are one of the sources for differences among different atmospheric models' predictions and associated biases. Also, turbulence strength is underrepresented in some of the resistance formulations. Here, to address these issues with dry deposition, firstly we take advantage of three‐dimensional (3‐D) turbulence information in estimating resistances by proposing and validating a 3‐D turbulence velocity scale that is relevant for different stability regimes of boundary layer. Secondly, we hypothesize and validate that friction velocity measured by 3‐D sonic anemometer can be effectively replaced by the new turbulence velocity scale multiplied by the von Karman constant. Finally, we (a) present a set of resistance formulations for ozone (O 3 ) based on the 3‐D turbulence velocity scale; (b) intercompare estimations of such resistances with those obtained using existing formulations; and, (c) evaluate simulated O 3 fluxes using a single‐point dry deposition model against long‐term observations of O 3 fluxes at the Harvard Forest (MA) site. Results indicate that the new resistance formulations work very well in simulating surface latent heat and O 3 fluxes when compared to respective existing formulations and measurements at a decadal time scale. Findings from this research may help to improve the capability of dry deposition schemes for better estimation of dry deposition fluxes and create opportunities for the development of a community dry deposition model for use in regional/global air quality models.

54 ENVIRONMENTAL SCIENCES↗

Variability of Water Vapor in the Tropical Middle Atmosphere Observed From Satellites and Interpreted Using SD-WACCM Simulations

Water vapor in the middle atmosphere plays an essential role in global warming, ozone depletion, and the formation of polar stratospheric and mesospheric clouds. We show that tropical middle atmospheric water vapor simulated with the specified-dynamics version of the Whole Atmosphere Community Climate Model (SD-WACCM) is consistent with changes observed in a merged satellite data set, which encompasses the period 1993–2020. Consistent with previous work, we find no significant trend in the stratosphere in either the observations or the simulation; in the mesosphere, we find a long-term trend of 0.1 ppmv per decade, but only in the observations. We also analyze an SD-WACCM simulation for the longer period 1980–2019 to quantify the contribution of various factors to the decadal variation of middle atmospheric water vapor. Over 1980–1995, the simulated water vapor in the upper stratosphere and mesosphere, averaged zonally and over ±30° latitude, increases by 0.30 ppmv per decade due to increasing methane emissions. After 1995, a significant abrupt decrease of water vapor of 0.37 ppmv per decade and then a gradual increase of 0.33 ppmv per decade result from changes in stratospheric cold point temperature. The cold-point temperature is strongly influenced by the strength of the Brewer-Dobson circulation. The acceleration of the Brewer-Dobson circulation before about 2003 leads to a cooler tropical tropopause and a decrease of water vapor, and the deceleration thereafter leads to corresponding warming of the tropopause and an increase in water vapor.

54 ENVIRONMENTAL SCIENCES↗

Sensitivity of deep convection and cross-tropopause water transport to microphysical parameterizations in WRF

Deep convective storms can overshoot the tropopause, thus altering the composition of the stratosphere by vertically transporting tropospheric air. The transport of water vapor and ice particles into a sub-saturated environment can hydrate the stratosphere, with implications for radiative forcing and ozone chemistry. Cloud-resolved models, if employed at high spatial resolutions, are used to probe process-level questions about cross-tropopause deep convective hydration and its controls. There is considerable diversity in model representations of processes associated with water transport and transformation, and the choice of a microphysics scheme affects model skill in simulating deep convective events. This motivates our evaluation of state-of-the-art, as well as widely used standard schemes, in a high spatial- and temporal-resolution framework. Six bulk microphysics schemes were employed in a WRF-LES setup, initialized with a sounding profile representative of a tropopause-overshooting storm. Here, we used an idealized framework to isolate the effect of microphysics on the dominant processes that control the reach of deep convection and stratospheric hydration. All schemes produced the highest reaching updrafts 8-12 hours into the simulation but the strength and persistence of updrafts varied across the schemes; maximum storm heights ranged 9.1-12.6 km across the schemes. Varying microphysics produced large differences in the vertical extent and horizontal aggregation of convection, and an order of magnitude spread in above-tropopause water vapor concentrations.

54 ENVIRONMENTAL SCIENCES↗

Pyrocumulonimbus Events Over British Columbia in 2017: An Ensemble Model Study of Parameter Sensitivities and Climate Impacts of Wildfire Smoke in the Stratosphere

Abstract The Pyrocumulonimbus (pyroCb) events over British Columbia in 2017 were observed in the lower stratosphere for about 8–10 months after the smoke injections. Several previous studies used global climate models to investigate the physical parameters for the 2017 pyroCb events, but the conclusions show strong model dependency. In this study, we use the Energy Exascale Earth System Model (E3SM) and complete an ensemble of runs exploring three injection parameters: smoke aerosol mass, the percentage of black carbon within the smoke aerosols, and plume injection height. Additionally, we consider the heterogeneous reaction of ozone and primary organic matter. According to the satellite daily observed aerosol optical depth (AOD), we find that the best ensemble member is the simulation with 0.4 Tg of smoke, 3% of which is black carbon, a 13.5 km smoke injection height, and a 10 −5 probability factor of the heterogeneous reaction. Besides AOD, we examine the ensemble score based on the metrics used in previous studies: the metrics of the extinction coefficient at 18 km altitude and the maximum plume height. The conclusion of the best estimate of the injection parameters for 2017 pyroCb events shows strong not only model but also evaluation metric dependency. We use the Random Forest machine learning technique to quantify the relative importance of each parameter in accurately simulating the 2017 pyroCb events and find that the injection height is the most critical feature, no matter which metric is used to score the ensemble members.

54 ENVIRONMENTAL SCIENCES↗

The Modeled Seasonal Cycles of Surface N 2 O Fluxes and Atmospheric N 2 O

Nitrous oxide (N 2 O) is a greenhouse gas and stratospheric ozone-depleting substance with large and growing anthropogenic emissions. Previous studies identified the influx of N 2 O-depleted air from the stratosphere to partly cause the seasonality in tropospheric N 2 O (aN 2 O), but other contributions remain unclear. Here, we combine surface fluxes from eight land and four ocean models from phase 2 of the Nitrogen/N 2 O Model Intercomparison Project with tropospheric transport modeling to simulate aN 2 O at eight remote air sampling sites for modern and pre-industrial periods. Models show general agreement on the seasonal phasing of zonal-average N 2 O fluxes for most sites, but seasonal peak-to-peak amplitudes differ several-fold across models. The modeled seasonal amplitude of surface aN 2 O ranges from 0.25 to 0.80 ppb (interquartile ranges 21%–52% of median) for land, 0.14–0.25 ppb (17%–68%) for ocean, and 0.28–0.77 ppb (23%–52%) for combined flux contributions. The observed seasonal amplitude ranges from 0.34 to 1.08 ppb for these sites. The stratospheric contributions to aN 2 O, inferred by the difference between the surface-troposphere model and observations, show 16%–126% larger amplitudes and minima delayed by ~1 month compared to Northern Hemisphere site observations. Land fluxes and their seasonal amplitude have increased since the pre-industrial era and are projected to grow further under anthropogenic activities. Our results demonstrate the increasing importance of land fluxes for aN 2 O seasonality. Considering the large model spread, in situ aN 2 O observations and atmospheric transport-chemistry models will provide opportunities for constraining terrestrial and oceanic biosphere models, critical for projecting carbon-nitrogen cycles under ongoing global warming.

54 ENVIRONMENTAL SCIENCES↗

Wind‐Associated Melt Trends and Contrasts Between the Greenland and Antarctic Ice Sheets

Föhn and katabatic winds (downslope winds) can increase ice sheet surface melt, run-off, and ice-shelf vulnerability to hydrofracture and are poorly constrained on the Greenland and Antarctic ice sheets (GIS and AIS). We use regional climate model simulations of the GIS and AIS to quantify and intercompare trends in downslope winds and associated melt since 1960. Results reveal surface melt associated with downslope wind is significant on both the GIS and AIS representing 27.5 ± 4.5% and 19.7 ± 3.8% of total surface melt respectively. Wind-associated melt has decreased 31.8 ± 5.3% on the AIS while total melt decreased 15.4 ± 2.4% due to decreased föhn-induced melt on the Antarctic Peninsula and increasing stratospheric ozone. Wind-associated melt has increased 10.3 ± 2.5% on the GIS, combining with a more positive North Atlantic Oscillation and warmer surface to increase total melt 34 ± 5.8%.

58 GEOSCIENCES↗

Substorm Driven Chorus Waves: Decay Timescales and Implications for Pulsating Aurora

Abstract Energetic electron precipitation (EEP) associated with pulsating aurora can transfer greater than 30 keV electrons from the outer radiation belt region into the upper atmosphere and can deplete atmospheric ozone via collisions that produce NOx and HOx molecules. Our knowledge of exactly how EEP occurs is incomplete. Previous studies have shown that pitch angle scattering between electrons and lower‐band chorus waves can cause pulsating aurora associated with EEP and that substorms play an important role. In this work, we quantify the timescale of chorus wave decay following substorms and compare that to previously determined timescales. We find that the chorus decay e‐folding time varies based on magnetic local time (MLT), magnetic latitude, and wave frequency. The shortest timescales occur for lower‐band chorus in the 21 to 9 MLT region and compares, within uncertainty, to the energetic pulsating aurora timescale of Troyer et al. (2022, https://doi.org/10.3389/fspas.2022.1032552 ) for energetic pulsating aurora. We are able to further support this connection by modeling our findings in a quasi‐linear diffusion simulation. These results provide observations of how chorus waves behave after substorms and add additional statistical evidence linking energetic pulsating aurora to substorm driven lower‐band chorus waves.

Troyer, Riley N.↗

The GFDL Variable-Resolution Global Chemistry-Climate Model for Research at the Nexus of US Climate and Air Quality Extremes

We present a variable-resolution global chemistry-climate model (AM4VR) developed at NOAA's Geophysical Fluid Dynamics Laboratory (GFDL) for research at the nexus of US climate and air quality extremes. AM4VR has a horizontal resolution of 13 km over the US, allowing it to resolve urban-to-rural chemical regimes, mesoscale convective systems, and land-surface heterogeneity. With the resolution gradually reducing to 100 km over the Indian Ocean, we achieve multi-decadal simulations driven by observed sea surface temperatures at 50% of the computational cost for a 25-km uniform-resolution grid. In contrast with GFDL's AM4.1 contributing to the sixth Coupled Model Intercomparison Project at 100 km resolution, AM4VR features much improved US climate mean patterns and variability. In particular, AM4VR shows improved representation of: precipitation seasonal-to-diurnal cycles and extremes, notably reducing the central US dry-and-warm bias; western US snowpack and summer drought, with implications for wildfires; and the North American monsoon, affecting dust storms. AM4VR exhibits excellent representation of winter precipitation, summer drought, and air pollution meteorology in California with complex terrain, enabling skillful prediction of both extreme summer ozone pollution and winter haze events in the Central Valley. AM4VR also provides vast improvements in the process-level representations of biogenic volatile organic compound emissions, interactive dust emissions from land, and removal of air pollutants by terrestrial ecosystems. We highlight the value of increased model resolution in representing climate–air quality interactions through land-biosphere feedbacks. AM4VR offers a novel opportunity to study global dimensions to US air quality, especially the role of Earth system feedbacks in a changing climate.

54 ENVIRONMENTAL SCIENCES↗

Long‐Term Impacts of Global Solid Biofuel Emissions on Ambient Air Quality and Human Health for 2000–2019

Globally, solid biofuels (SB) have been widely used for household cooking and energy production for decades due to electricity shortages and socio-economic barriers to adopting renewable energy alternatives. This has detrimental effects on air quality, human health, and climate through trace gas and aerosol emissions. Despite numerous studies, the long-term consequences of SB emissions remain poorly understood. Here, we use the Community Earth System Model and the Community Emissions Data System emission inventory to investigate the SB emission impacts on air quality and human health for 2000–2019. Global SB emission increased the ambient PM 2.5 (particulate matter with aerodynamic diameters ≤2.5 μm) and ozone (O 3 ) concentrations up to 23.61 μg/m 3 and 13.69 ppbv, with significant effects found in India, China, and the Rest of Asia (ROA). Our study estimates total annual premature deaths (APDs) associated with global SB-attributable PM 2.5 and O 3 exposure as 1.11 million [95% confidence interval (95% CI): 1.00–1.22 million] in 2000 up to 1.43 million (95% CI: 1.30–1.56 million) in 2019. China's SB emissions and associated APDs have reduced substantially, whereas India and ROA had a major leap in both estimates in 2019 compared to 2000. China's progress in cutting residential SB emissions accounts for its improvements. Our study urges the reduction of SB usage and emissions to potentially improve overall air quality and human health conditions, especially in highly populated, low- and middle-income countries, where the poor air quality and associated health burden attributable to SB emissions are estimated to be higher.

O 3↗

A Single Compartment Relaxed Eddy Accumulation Method

The relaxed eddy accumulation (REA) method is a widely-known technique that measures turbulent fluxes of scalar quantities. The REA technique has been used to measure turbulent fluxes of various compounds, such as methane, ethene, propene, butene, isoprene, nitrous oxides, ozone, and others. The REA method requires the accumulation of scalar concentrations in two separate compartments that conditionally sample updrafts and downdraft events. It is demonstrated here that the assumptions behind the conventional or two-compartment REA approach allow for one-compartment sampling, therefore called a one compartment or 1-C-REA approach, thereby expanding its operational utility. The one-compartment sampling method is tested across various land cover types and atmospheric stability conditions, and it is found that the one-compartment REA can provide results comparable to those determined from conventional two-compartment REA. This finding enables rapid expansion and practical utility of REA in studies of surface-atmosphere exchanges, interactions, and feedbacks.

Banerjee, T.↗

Anthropogenic extremely low volatility organics (ELVOCs) Govern the Growth of Molecular Clusters over the Southern Great Plains during the Springtime

New particle formation (NPF) and growth govern cloud condensation nuclei (CCN) concentrations in many regions. The mechanisms governing the nucleation of molecular clusters vary substantially in different regions of the atmosphere. Additionally, the growth of these clusters from ~2 to 20 nm sizes is often governed by the availability of extremely low volatility organic vapours (ELVOCs). While the pathways to ELVOC formation from the oxidation of biogenic monoterpenes with ozone is better understood, the chemical and mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are not well understood. We integrate measurements and three-dimensional regional model simulations with the Weather Research and Forecasting Model coupled to chemistry (WRF-Chem) to understand the processes governing new particle formation and growth and secondary organic aerosol (SOA) formation during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) field campaign at the Southern Great Plains (SGP) observatory in Oklahoma, and contrast it with a site within the Bankhead National Forest (BNF), Alabama in Southeast USA, where 5-year long measurements will begin in 2024. Simulations show that nucleation rates are at least an order of magnitude higher at SGP compared to BNF during the springtime days (April 28 and May 14, 2016), largely due to lower H2SO4 concentrations at BNF, which are needed for nucleation. In addition, the larger CS at BNF (compared to SGP) increase the loss of molecular clusters by coagulation to pre-existing particles. Among the 8 different nucleation mechanisms in WRF-Chem, we find that the amine+H2SO4 nucleation mechanism dominates at the SGP site, while the pure organic ion induced nucleation mechanism dominates over BNF. Through various WRF-Chem sensitivity simulations, we find that anthropogenic ELVOCs are critical for explaining the growth of newly formed particles and the resulting number size distribution observed near the surface at the SGP site during the daytime. In addition, we show that treating organic particles as semisolid, with strong diffusion-limited uptake of organic vapours, brings model predictions into closer agreement with the observed evolution of particle size distribution. Simulations also predict that anthropogenic SOA, formed by the oxidation of aromatic volatile organic compounds (VOCs), is the dominant organic aerosol component at SGP, while biogenic SOA dominates particle composition at the BNF site in Southeast USA on these days.

Shrivastava, ManishKumar B.↗

Implementation of Sub‐Grid Scale Temperature Perturbations Induced by Non‐Orographic Gravity Waves in WACCM6

Abstract Atmospheric gravity waves can play a significant role on atmospheric chemistry through temperature fluctuations. A recent modeling study introduced a method to implement subgrid‐scale orographic gravity‐wave‐induced temperature perturbations in the Whole Atmosphere Community Climate Model (WACCM). The model with a wave‐induced temperature parameterization was able to reproduce for example, the influence of mountain wave events on atmospheric chemistry, as highlighted in previous literature. Here we extend the subgrid‐scale wave‐induced temperature parameterization to also include non‐orographic gravity waves arising from frontal activity and convection. We explore the impact of these waves on middle atmosphere chemistry, particularly focusing on reactions that are strongly sensitive to temperature. The non‐orographic gravity waves increase the variability of chemical reaction rates, especially in the lower mesosphere. As an example, we show that this, in turn, leads to increases in the daytime ozone variability. To demonstrate another impact, we briefly investigate the role of non‐orographic gravity waves in cirrus cloud formation in this model. Consistent with findings from the previous study focusing on orographic gravity waves, non‐orographic waves also enhance homogeneous nucleation and increase cirrus clouds. The updated method used enables the global chemistry‐climate model to account for both orographic and non‐orographic gravity‐wave‐induced subgrid‐scale dynamical perturbations in a consistent manner.

Yook, Simchan [Department of Earth Atmospheric and↗

Deep Convection‐Driven Downward Transport of Trace Gases and Aerosols From the Free Troposphere to the Boundary Layer

Deep convective clouds regulate Earth's energy and moisture budgets, yet their impact on the atmospheric boundary layer (BL) composition remains underexplored. Using long-term observations from three mid-latitude sites, we show that deep convection (DC) consistently enhances nighttime surface ozone and is often accompanied by modest increases in ultrafine particle concentrations. Within the BL, the condensational growth of these transported ultrafine particles may contribute up to 60% of total cloud condensation nuclei (CCN). Mass flux calculations suggest that short-lived convective cores (∼30 min) account for ∼2% of total vertical air mass transport relative to steady entrainment, increasing to ∼13% when the trailing stratiform regions are included. These results show that DC provides an episodic but efficient pathway linking the free troposphere and BL, influencing oxidant budgets, CCN variability, and climate forcing. Accurately representing this process in climate models may help reduce uncertainties in climate projections, under both preindustrial and present-day conditions.

54 ENVIRONMENTAL SCIENCES↗

Disappearance of Superconductivity Due to Vanishing Coupling in the Overdoped Bi 2 Sr 2 CaCu 2 O 8+δ

In cuprate superconductors, superconductivity is accompanied by a ‘plethora of orders’, and phenomena that complicate our understanding of superconductivity in these materials. Prominent in the underdoped regime, these orders weaken or vanish with overdoping. Here, we approach the superconducting phase from the more conventional overdoped side. We present angle-resolve photoemission spectroscopy studies of Bi 2 Sr 2 CaCu 2 O 8+δ , cleaved and annealed in ozone to increase the doping all the way to the non-superconducting phase. In this work, we show that the mass renormalizationin the antinodal region of the Fermi surface, associated with the structure in the quasiparticle self-energy, that possibly reflects the pairing, weakens with doping and completely disappears precisely where superconductivity disappears the evidence that in the overdoped regime, superconductivity is determined by the coupling strength. A doping dependence and an abrupt disappearance above the transition temperature eliminate phononic mechanism of the observed renormalization and identify the onset of spin-fluctuations as its likely origin.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Pressure-stabilized divalent ozonide CaO 3 and its impact on Earth's oxygen cycles

High pressure can drastically alter chemical bonding and produce exotic compounds that defy conventional wisdom. Especially significant are compounds pertaining to oxygen cycles inside Earth, which hold key to understanding major geological events that impact the environment essential to life on Earth. Here we report the discovery of pressure-stabilized divalent ozonide CaO3 crystal that exhibits intriguing bonding and oxidation states with profound geological implications. Our computational study identifies a crystalline phase of CaO 3 by reaction of CaO and O 2 at high pressure and high temperature conditions; ensuing experiments synthesize this rare compound under compression in a diamond anvil cell with laser heating. High-pressure x-ray diffraction data show that CaO 3 crystal forms at 35 GPa and persists down to 20 GPa on decompression. Analysis of charge states reveals a formal oxidation state of -2 for ozone anions in CaO 3 . These findings unravel the ozonide chemistry at high pressure and offer insights for elucidating prominent seismic anomalies and oxygen cycles in Earth’s interior. We further predict multiple reactions producing CaO 3 by geologically abundant mineral precursors at various depths in Earth’s mantle.

58 GEOSCIENCES↗

Economy-wide evaluation of CO 2 and air quality impacts of electrification in the United States

Adopting electric end-use technologies instead of fossil-fueled alternatives, known as electrification, is an important economy-wide decarbonization strategy that also reduces criteria pollutant emissions and improves air quality. In this study, we evaluate CO 2 and air quality co-benefits of electrification scenarios by linking a detailed energy systems model and a full-form photochemical air quality model in the United States. We find that electrification can substantially lower CO 2 and improve air quality and that decarbonization policy can amplify these trends, which yield immediate and localized benefits. In particular, transport electrification can improve ozone and fine particulate matter (PM 2.5 ), though the magnitude of changes varies regionally. However, growing activity from non-energy-related PM 2.5 sources—such as fugitive dust and agricultural emissions—can offset electrification benefits, suggesting that additional measures beyond CO 2 policy and electrification are needed to meet air quality goals. We illustrate how commonly used marginal emissions approaches systematically underestimate reductions from electrification.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗