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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Criegee Intermediates Compete Well with OH as a Cleaning Agent for Atmospheric Amides

Elucidating the chemical kinetics of stabilized Criegee intermediates (sCIs) in the atmosphere is critically important for climate modeling. Here, we report a class of very rapid bimolecular reactions of two sCIs, namely, CH 2 OO and syn-CH 3 CHOO, with amides. We used electronic structure calculations and kinetics calculations to elucidate a universal mechanism by which the oxygen atom of the carbonyl group in an amide is added to the carbon atom of the COO group in the sCI with simultaneous transfer of the amide hydrogen to the terminal oxygen atom of the carbonyl oxide of the sCI. The barriers for the mechanism are submerged below reactants by ∼9 kcal/mol, which means that the tight transition state is not the rate-determining step, and the rate constants are determined by loose free energy bottlenecks between the reactants and the precursor complexes. We calculate the rate constants due to these loose and barrierless transition states by variable-reaction-coordinate variational transition-state theory. We find that bimolecular reactions of sCIs with amides are very rapid, with rate constants 1 to 5 × 10 –10 cm 3 molecule –1 s –1 , which is a factor of 2 faster than the rate constants of carboxylic acids with sCIs and 10 2 faster than the rate constants of OH reactions with amides. This has the consequence that, under a wide range of conditions, sCIs are the major sink for atmospheric amides, in contrast to the usual assumption that OH radicals are the dominant sinks.

Amides↗
DOE OSTI2020

Impact of Changes to the Atmospheric Soluble Iron Deposition Flux on Ocean Biogeochemical Cycles in the Anthropocene

Abstract Iron can be a growth‐limiting nutrient for phytoplankton, modifying rates of net primary production, nitrogen fixation, and carbon export ‐ highlighting the importance of new iron inputs from the atmosphere. The bioavailable iron fraction depends on the emission source and the dissolution during transport. The impacts of anthropogenic combustion and land use change on emissions from industrial, domestic, shipping, desert, and wildfire sources suggest that Northern Hemisphere soluble iron deposition has likely been enhanced between 2% and 68% over the Industrial Era. If policy and climate follow the intermediate Representative Concentration Pathway 4.5 trajectory, then results suggest that Southern Ocean (>30°S) soluble iron deposition would be enhanced between 63% and 95% by 2100. Marine net primary productivity and carbon export within the open ocean are most sensitive to changes in soluble iron deposition in the Southern Hemisphere; this is predominantly driven by fire rather than dust iron sources. Changes in iron deposition cause large perturbations to the marine nitrogen cycle, up to 70% increase in denitrification and 15% increase in nitrogen fixation, but only modestly impacts the carbon cycle and atmospheric CO 2 concentrations (1–3 ppm). Regionally, primary productivity increases due to increased iron deposition are often compensated by offsetting decreases downstream corresponding to equivalent changes in the rate of phytoplankton macronutrient uptake, particularly in the equatorial Pacific. These effects are weaker in the Southern Ocean, suggesting that changes in iron deposition in this region dominates the global carbon cycle and climate response.

Hamilton, Douglas S.↗
DOE OSTI2019

Antarctic Sea Ice Expansion, Driven by Internal Variability, in the Presence of Increasing Atmospheric CO2

A number of physically-based hypotheses have been proposed to explain the surprising expansion of Antarctic sea ice area (SIA) over the satellite era (1979 to 2015). Here, we use a fully-coupled state-of-the-art global climate model to show that internal variability alone can produce such multidecadal periods of Antarctic SIA expansion even as atmospheric CO2 increases at observed rates and the planet warms. When our model is started from a relatively warm Southern Ocean state, Antarctic SIA sometimes (in one of three ensemble members) expands over multidecadal time scales at a rate comparable to that over the satellite era. SIA expansion occurs concurrently with rising atmospheric CO2 and warming global surface temperatures, and SIA trends by region and sector resemble those over the satellite era. Our results suggest that internal variability, particularly on long time scales over the Southern Ocean, may suffice to explain Antarctic SIA expansion over the satellite era.

Singh, Hansi AK↗
DOE OSTI2020

Relative Contributions of Atmospheric, Oceanic, and Coupled Processes to North Pacific and North Atlantic Variability

Patterns of sea surface temperature (SST) variability over the northern oceans arise from a combination of atmospheric, oceanic, and coupled processes. In this work, we use a novel methodology and a suite of observations to quantify the processes contributing to the dominant patterns of interannual SST variability over these regions. We decompose the upper ocean heat content tendency associated with such dominant patterns into contributions from different heat fluxes: (a) atmospherically driven, (b) surface feedbacks, and (c) oceanic. We find that in the subtropics, cloud radiative flux, turbulent heat flux, and residual oceanic processes each contributes substantially to North Pacific SST variability, whereas turbulent heat flux primarily induces North Atlantic SST variability. Cloud radiative fluxes therefore provide a major source of interannual SST variability in the North Pacific but not in the North Atlantic. In midlatitudes, SST fluctuations over the northern oceans are driven by the combination of turbulent and oceanic heat fluxes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Connection Between Mass Flux Transport and Eddy Diffusivity in Convective Atmospheric Boundary Layers

Turbulence parameterizations for convective boundary layer in coarse-scale atmospheric models usually consider a combination of the eddy-diffusive transport and a non-local transport, typically in the form of a mass flux term, such as the widely adopted eddy-diffusivity mass-flux (EDMF) approach. These two types of turbulent transport are generally considered to be independent of each other. Using results from large-eddy simulations, here, we show that a Taylor series expansion of the updraft and downdraft mass-flux transport can be used to approximate the eddy-diffusivity transport in the atmospheric surface layer and the lower part of the mixed layer, connecting both eddy-diffusivity and mass-flux transport theories in convective conditions, which also quantifies departure from the Monin-Obukhov similarity (MOS) in the surface layer. This study provides a theoretical support for a unified EDMF parameterization applied to both the surface layer and mixed layer and highlights important correction required for surface models relying on MOS

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

An Overview of Atmospheric Features Over the Western North Atlantic Ocean and North American East Coast - Part 1: Analysis of Aerosols, Gases, and Wet Deposition Chemistry

The Western North Atlantic Ocean (WNAO) and adjoining East Coast of North America are of great importance for atmospheric research and have been extensively studied for several decades. This broad region exhibits complex meteorological features, diverse cloud types, and a wide range of conditions associated with gas and particulate species that originate from many sources regionally and from other continents. As Part 1 of a 2-part paper series, this work provides a characterization of quantities associated with atmospheric chemistry, including gases, aerosols, and wet deposition, based on satellite observations, ground-based data, model simulations, and reanalysis products. Key results include spatial and seasonal differences in composition along the North American East Coast and over the WNAO associated with varying sources of smoke and dust and meteorological drivers such as temperature, moisture, and precipitation. Spatial and seasonal variations of tropospheric carbon monoxide and ozone highlight different pathways towards accumulation of these species in the troposphere. Spatial distributions of speciated aerosol optical depth and vertical profiles of aerosol mass mixing ratios show a clear seasonal cycle highlighting the influence of both natural and anthropogenic sources in addition to the impact of intercontinental transport on their vertical profiles. Analysis of long-term climate model simulations of aerosol species and satellite observations of carbon monoxide confirm that there has been a significant decline in recent decades among anthropogenic constituents owing to regulatory activities. The results can inform current and future lines of research for the region.

Corral, Andrea↗
DOE OSTI2020

An Evaluation of the Large‐Scale Atmospheric Circulation and Its Variability in CESM2 and Other CMIP Models

Abstract The Community Earth System Model 2 (CESM2) is the latest Earth System Model developed by the National Center for Atmospheric Research in collaboration with the university community and is significantly advanced in most components compared to its predecessor (CESM1). Here, CESM2's representation of the large‐scale atmospheric circulation and its variability is assessed. Further context is providedthrough comparison to the CESM1 large ensemble and other models from the Coupled Model Intercomparison Project (CMIP5 and CMIP6). This includes an assessment of the representation of jet streams and storm tracks, stationary waves, the global divergent circulation, the annular modes, the North Atlantic Oscillation, and blocking. Compared to CESM1, CESM2 is substantially improved in the representation of the storm tracks, Northern Hemisphere (NH) stationary waves, NH winter blocking and the global divergent circulation. It ranks within the top 10% of CMIP class models in many of these features. Some features of the Southern Hemisphere (SH) circulation have degraded, such as the SH jet strength, stationary waves, and blocking, although the SH jet stream is placed at approximately the correct location. This analysis also highlights systematic deficiencies in these features across the new CMIP6 archive, such as the continued tendency for the SH jet stream to be placed too far equatorward, the North Atlantic westerlies to be too strong over Europe, the storm tracks as measured by low‐level meridional wind variance to be too weak and a lack of blocking in the North Atlantic sector.

Simpson, Isla R.↗
DOE OSTI2020

Enlarged Nonclosure of Surface Energy Balance With Increasing Atmospheric Instabilities Linked to Changes in Coherent Structures

The nonclosure of surface energy balance remains an outstanding problem in eddy covariance (EC) measurements of land-surface fluxes of heat, water vapor, and CO 2 . Our data collected from an EC tower over a semiarid sagebrush ecosystem indicate that under unstable atmospheric conditions, the nonclosure becomes increased with increasing instability, consistent with many other studies. It is demonstrated that the increased nonclosure is not caused by the inadequate sampling of large-scale turbulent motions using a 30-min averaging interval, though the scales of turbulent motions dominating sensible and latent heat fluxes become enlarged with increasing instability. Quadrant analysis is then used to reveal that the flux contributions from ejections remain nearly constant with increasing instability, whereas the flux contributions from sweeps are reduced and their time fractions increase. Our results imply that the increased nonclosure of surface energy balance is associated with changes in turbulent structures including their dominant time scales and flux contributions of ejections and sweeps as the atmospheric instability increases, which require further studies using vertically distributed observations and/or large eddy simulations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m −2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m −2 . Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m −2 . Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m −2 .

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Cloud Process Coupling and Time Integration in the E3SM Atmosphere Model

Abstract In this study, we find significant sensitivity to the choice of time step for the Energy Exascale Earth System Model's atmospheric component, leading to large decreases in the magnitude of cloud forcing when the time step is reduced to 10 s. Reducing the time step size for the microphysics increases precipitation, leading to a drying of the atmosphere and an increase in surface evaporation. This effect is amplified when the microphysics is substepped together with other cloud physics processes. Coupling the model's dynamics and physics more frequently reduces cloud fraction at lower altitudes, while producing more cloud liquid at higher altitudes. Reducing the deep convection time step also reduces low cloud mass and cloud fraction. Together, these results suggest that cloud physics in a global circulation model can depend strongly on time step and, in particular, on the frequency with which cloud‐related processes are coupled with each other and with the model dynamics.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Tropical Cirrus in Global Storm-Resolving Models. Part II: Cirrus Life Cycle and Top-of-Atmosphere Radiative Fluxes

Cirrus clouds of various thicknesses and radiative characteristics extend over much of the tropics, especially around deep convection. They are difficult to observe due to their high altitude and sometimes small optical depths. They are also difficult to simulate in conventional global climate models, which have coarse grid spacings and simplified parameterizations of deep convection and cirrus formation. We investigate the representation of tropical cirrus in global storm-resolving models (GSRMs), which have higher spatial resolution and explicit convection and could more accurately represent cirrus cloud processes. This study uses GSRMs from the DYnamics of the Atmospheric general circulation Modeled On Non-hydrostatic Domains (DYAMOND) project. The aggregate life cycle of tropical cirrus is analyzed using joint albedo and outgoing longwave radiation (OLR) histograms to assess the fidelity of models in capturing the observed cirrus cloud populations over representative tropical ocean and land regions. The proportions of optically-thick deep convection, anvils, and cirrus vary across models and are portrayed in the vertical distribution of cloud cover and top-of-atmosphere radiative fluxes. Model differences in cirrus populations, likely driven by subgrid processes such as ice microphysics, dominate over regional differences between convectively-active tropical land and ocean locations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Strong Local Evaporative Cooling Over Land Due to Atmospheric Aerosols

Abstract Aerosols can enhance terrestrial productivity through increased absorption of solar radiation by the shaded portion of the plant canopy—the diffuse radiation fertilization effect. Although this process can, in principle, alter surface evaporation due to the coupling between plant water loss and carbon uptake, with the potential to change the surface temperature, aerosol‐climate interactions have been traditionally viewed in light of the radiative effects within the atmosphere. Here, we develop a modeling framework that combines global atmosphere and land model simulations with a conceptual diagnostic tool to investigate these interactions from a surface energy budget perspective. Aerosols increase the terrestrial evaporative fraction, or the portion of net incoming energy consumed by evaporation, by over 4% globally and as much as ∼40% regionally. The main mechanism for this is the increase in energy allocation from sensible to latent heat due to global dimming (reduction in global shortwave radiation) and slightly augmented by diffuse radiation fertilization. In regions with moderately dense vegetation (leaf area index >2), the local surface cooling response to aerosols is dominated by this evaporative pathway, not the reduction in incident radiation. Diffuse radiation fertilization alone has a stronger impact on gross primary productivity (+2.18 Pg C y −1 or +1.8%) than on land evaporation (+0.18 W m −2 or +0.48%) and surface temperature (−0.01 K). Our results suggest that it is important for land surface models to distinguish between quantity (change in total magnitude) and quality (change in diffuse fraction) of radiative forcing for properly simulating surface climate.

Chakraborty, TC↗
DOE OSTI2021

Investigating the Causes and Impacts of Convective Aggregation in a High Resolution Atmospheric GCM

Abstract A ∼50 km resolution atmospheric general circulation model (GCM) is used to investigate the impact of radiative interactions on spatial organization of convection, the model's mean state, and extreme precipitation events in the presence of realistic boundary conditions. Mechanism‐denial experiments are performed in which synoptic‐scale feedbacks between radiation and dynamics are suppressed by overwriting the model‐generated atmospheric radiative cooling rates with its monthly varying climatological values. When synoptic‐scale radiative interactions are disabled, the annual mean circulation and precipitation remain almost unchanged, however tropical convection becomes less aggregated, with an increase in cloud fraction and relative humidity in the free troposphere but a decrease in both variables in the boundary layer. Changes in cloud fraction and relative humidity in the boundary layer exhibit more sensitivity to the presence of radiative interactions than variations in the degree of aggregation. The less aggregated state is associated with a decrease in the frequency of extreme precipitation events, coincident with a decrease in the dynamical contribution to the magnitude of extreme precipitation. At regional scales, the spatial contrast in radiative cooling between dry and moist regions diminishes when radiative interactions are suppressed, reducing the upgradient transport of energy, degree of aggregation, and frequency of extreme precipitation events. However, the mean width of the tropical rain belt remains almost unaffected when radiative interactions are disabled. These results offer insights into how radiation‐circulation coupling affects the spatial organization of convection, distributions of clouds and humidity, and weather extremes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Evaluating Uncertainty and Modes of Variability for Antarctic Atmospheric Rivers

Abstract Antarctic atmospheric rivers (ARs) are driven by their synoptic environments and lead to profound and varying impacts along the coastlines and over the continent. The definition and detection of ARs over Antarctica accounts for large uncertainty in AR metrics, and consequently, impacts quantification. We find that Antarctic‐specific detection tools consistently capture the AR footprint inland over ice sheets, whereas most global detection tools do not. Large‐scale synoptic environments and associated ARs, however, are broadly consistent across detection tools. Using data from the Atmospheric River Tracking Method Intercomparison Project and global reanalyses, we quantify the uncertainty in Antarctic AR metrics and evaluate large‐scale environments in the context of decadal and interannual modes of variability. The Antarctic western hemisphere has stronger connections to both decadal and interannual modes of variability compared to East Antarctica, and the Indian Ocean Dipole’s influence on Antarctic ARs is stronger while in phase with El Nino Southern Oscillation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Contrasting Climatic Trends of Atmospheric River Occurrences Over East Asia

Atmospheric rivers (ARs) are increasingly recognized as a major driver of hydrological cycles, and are projected to increase around the world under a changing climate. However, the long-term trends of ARs over East Asia (EA) remains less elucidated. Here we fill the gap by developing a longest-ever archive of EA ARs, and examine its role in determining spatiotemporal precipitation variability over EA. We find contrasting changes in AR occurrences, with more frequent ARs in low latitudes but less in high latitudes during the period 1950-2020. The “dipole” pattern of decadal changes in AR occurrences is dictated by atmospheric dynamics (i.e., winds) in the north but thermodynamics (i.e., moisture) in the south. The reduced AR occurrences explain 49% of decreased annual precipitation in northern China, while more AR-related precipitation is observed in southern China. Furthermore, our results provide new insights into regional hydroclimate over EA by connecting it with large-scale weather systems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Surface‐Atmosphere Decoupling Prolongs Cloud Lifetime Under Warm Advection Due To Reduced Entrainment Drying

Abstract An initially well‐mixed stratocumulus deck can remain overcast for several tens of hours under warm‐advection conditions, although moisture supply is cut off from the ocean due to surface‐atmosphere decoupling (stabilization of the surface‐atmosphere interface). In this study, a set of idealized large‐eddy simulations were performed to investigate the physical mechanism of how warm‐air advection impacts the evolution of a pre‐existing stratocumulus deck. To mimic warm‐air advection, we decrease the sea surface temperature linearly over time in a doubly periodic domain. Given the same initial conditions, the stratocumulus deck is more persistent when experiencing warm‐air advection than cold‐air advection. This persistence is caused by reduced cloud‐top entrainment drying due to decoupling, a process more influential than the decoupling‐induced cutoff of moisture supply. This mechanism is more notable when the free troposphere becomes more humid. The relevance of the mechanism to previous observations of less low‐level cloudiness under warm‐advection conditions is discussed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Investigating the Diurnal Radiative, Turbulent, and Biophysical Processes in the Amazonian Canopy‐Atmosphere Interface by Combining LES Simulations and Observations

Abstract We investigate the atmospheric diurnal variability inside and above the Amazonian rainforest for a representative day during the dry season. To this end, we combine high‐resolution large‐eddy simulations that are constrained and evaluated against a comprehensive observation set, including CO 2 concentrations, gathered during GoAmazon2014/15. We design systematic numerical experiments to quantify whether a multilayer approach in solving the explicit canopy improves our canopy‐atmosphere representation. We particularly focus on the relationship between photosynthesis and plant transpiration, and their distribution at leaf and canopy scales. We found the variability of photosynthesis drivers like vapor pressure deficit and leaf temperature to be about 3 times larger for sunlit leaves compared to shaded leaves. This leads to a large spread on leaf stomatal conductance values with minimum and maximum values varying more than 100%. Regarding the turbulent structure, we find wind‐driven stripe‐like shapes at the canopy top and structures resembling convective cells at the canopy. Wind‐related variables provide the best spatiotemporal agreement between model and observations. The potential temperature and heat flux profiles agree with an observed decoupling near the canopy top interface, although with less variability and cold biases of up to 3 K. The increasing complexity on the biophysical processes leads to the largest disagreements for evaporation, CO 2 plant assimilation and soil efflux. The model is able to capture the correct dependences and trends with the magnitudes still differing. We finally discuss the need to revise leaf and soil models and to complete the observations at leaf and canopy levels.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

The Role of Atmospheric Rivers on Groundwater: Lessons Learned From an Extreme Wet Year

Abstract In the coastal regions of the western United States, atmospheric rivers (ARs) are associated with the largest precipitation generating storms and contribute up to half of annual precipitation, but the impact of ARs on the integrated hydrologic cycle, specifically on groundwater storage and hydrodynamics, is largely unknown. To better explore the hydrologic behavior of AR versus non‐AR event precipitation, we present a novel combination of two water tracking methods (one in the atmosphere and one in the subsurface) to explicitly track the full lifecycle of water parcels generated by ARs. Simulations of northern California's Cosumnes River watershed during the record wet 2017 water year are performed via the coupling of a high‐resolution regional climate model and a land surface‐groundwater model accounting for lateral groundwater flow. Despite ARs contributing more precipitation than non‐AR storms, we find less AR water is preferentially stored in aquifers by year end. Fractionally, ARs result in 300% less snow derived groundwater‐recharged compared to non‐AR precipitation. Rain‐on‐snow (RoS) plays an important role in AR‐driven discharge, where over 50% of total discharge from ARs snow is from RoS events. Finally, despite record‐breaking annual precipitation, simulated groundwater depletion occurs by year end due to estimates of groundwater pumping activities. The results from these simulations serve as a partial analogue of future hydrologic conditions where ARs are expected to intensify and provide a greater fraction of annual precipitation due to climate change.

54 ENVIRONMENTAL SCIENCES↗