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At least 73 records · Page 4

Suppressing Atmospheric Degradation of Sulfide-Based Solid Electrolytes via Ultrathin Metal Oxide Layers

Sulfide-based solid-state electrolytes (SSEs) are promising materials with superior Li-ion conductivity; however, their poor atmospheric stability limits commercial manufacturing at scale. Here, we investigate the impact of ultrathin metal oxide layers deposited via atomic layer deposition (ALD) on the stability of Li 6 PS 5 Cl (LPSCl). Al 2 O 3 layers grown directly on LPSCl particles significantly stabilize the surface chemistry and Li-ion transport properties relative to uncoated material upon exposure to both an ambient atmosphere (22% relative humidity, RH) and humidified O 2 (100% RH). Detailed investigations indicate that coatings impede the surface and bulk degradation kinetics of exposed materials, even for coatings as thin as ∼1 Å. Furthermore, this suggests that stabilization is due to more than just a physical barrier. Shifts in valence band edge positions of coated LPSCl indicate that ALD coatings alter the surface electronic structure and resulting oxidation tendency of underlying LPSCl, suggesting new avenues to improving the environmental stability of sulfide SSEs.

Atmospheric chemistry↗

A New Method to Retrieve the Diurnal Variability of Planetary Boundary Layer Height from Lidar Under Different Thermodynamic Stability Conditions

The planetary boundary layer height (PBLH) is an important parameter for understanding the accumulation of pollutants and the dynamics of the lower atmosphere. Lidar has been used for tracking the evolution of PBLH by using aerosol backscatter as a tracer, assuming aerosol is generally well-mixed in the PBL; however, the validity of this assumption actually varies with atmospheric stability. This is demonstrated here for stable boundary layers (SBL), neutral boundary layers (NBL), and convective boundary layers (CBL) using an 8-year dataset of micropulse lidar (MPL) and radiosonde (RS) measurements at the ARM Southern Great Plains, and MPL at the GSFC site. Due to weak thermal convection and complex aerosol stratification, traditional gradient and wavelet methods can have difficulty capturing the diurnal PBLH variations in the morning and forenoon, as well as under stable conditions generally. A new method is developed that combines lidar-measured aerosol backscatter with a stability dependent model of PBLH temporal variation (DTDS). The latter helps “recalibrate” the PBLH in the presence of a residual aerosol layer that does not change in harmony with PBL diurnal variation. The hybrid method offers significantly improved PBLH detection, with better correlation and smaller biases, under most thermodynamic conditions, especially for SBL and CBL. Relying on the physical process of PBL diurnal development, different schemes are developed for growing, maintenance, and decaying periods. Comprehensive evaluation of this new method shows much better tracking of diurnal PBLH variation and significantly smaller biases under various pollution levels.

Tianning Su↗

Possible Influences of Air Pollution, Dust and Sandstorms on the Indian Monsoon

In Asian monsoon countries, such as China and India, human health and safety problems caused by air pollution are becoming increasingly serious, due to the increased loading of atmospheric pollutants from waste gas emissions and from rising energy demand associated with the rapid pace of industrialization and modernization. Meanwhile, uneven distribution of monsoon rain associated with flash floods or prolonged drought, has caused major loss of human life and damage to crops and.property with devastating societal impacts. Historically, air-pollution and monsoons research are treated as separate problems. However recent studies have suggested that the two problems may be intrinsically linked and need to be studied jointly. Fundamentally, aerosols can affect precipitation through radiative effects cif suspended particles in the atmosphere (direct effect) and/or by interfering and changing: the cloud and precipitation formation processes (indirect effect). Based on their optical properties, aerosols can be classified into two types.: those that absorb solar radiation, and those that do not. Both types of aerosols scatter sunlight and reduce the amount of solar radiation from reaching the Earth's surface, causing it to cool. The surface cooling increases atmospheric stability and reduces convection potential, Absorbing aerosols, however, in addition to cooling the surface, can heat the atmosphere. The heating of the atmosphere may reduce the amount of low clouds by increased evaporation in cloud drops. The heating, however, may induce rising motion, enhance low-level moisture, convergence and, hence, increases rainfall, The latent heating from enhanced rainfall may excite feedback processes in the large-scale circulation, further amplify.the initial response to aerosol heating and producing more rain. Additionally, aerosols can increase the concentration of cloud condensation nuclei (CCN), increase cloud amount and decrease coalescence and collision rates, leading to reduced precipitation. However, in the presence of increasing moist and warm air, the reduced coalescence/collision may lead to supercooled drops at higher altitudes where ice precipitation falls and melts. The latent heat release from freezing aloft and melting below implies greater upward heat transport in polluted clouds and invigorate deep convection. In this way, aerosols may lead to increased local convection. Hence, depending on the ambient large-scale conditions and dynamical feedback processes, aerosols' effect on precipitation can be positive, negative or mixed. In the Asian monsoon and adjacent regions, the aerosol forcing and responses of the water cycle are even more complex, Both direct and indirect effects may take place locally and simultaneously, interacting with each other. in addition to local effects, monsoon rainfall may be affected by aerosols transported from other regions and intensified through large-scale circulation and moisture feedback. Thus, dust transported by the large-scale circulation from the adjacent deserts to northern India may affect rainfall over the Bay of Bengal; sulphate and black carbon front industrial pollution in central, southern China and northern India may affect the rainfall regime over the Korean peninsula and Japan; organic and black carbon front biomass burning from Indo-China may modulate the pre-monsoon rainfall regime over southern China and coastal regions, contributing to variability in differential heating and cooling of the atmosphere and to the land-sea thermal contrast. During the pre-monsoon season and monsoon breaks, it has been suggested that radiative forcing by absorbing aerosols have nearly the same order of magnitude as the forcing due to latent heating from convection and surface fluxes. The magnitude of the total aerosol radiative cooling due to sulphates and soot is of the order of 20-40 W/m2 over the Asian monsoon land region in the pre-monsoon season, compared to about 1-2 W/m2 for global warng. However, the combined forcing at the surface and in the atmosphere, including all species. if aerosols, and details of aerosol mixing, and impacts on the energy and water cycles in the monsoon land regions, are not well known.

Lau, William K. M.↗

Editorial: Resolving atmospheric flow in complex environments: recent experiments in terrain and forest canopies

The characterization of atmospheric flows in complex environments, which may include steep terrain slopes and heterogeneous vegetation and/or forest cover, is a long-standing challenge in boundary-layer meteorology. Atmospheric observations are complicated by the presence of transient, terrain-induced flow features, forest-canopy-atmosphere interactions, and atmospheric stability effects, not to mention the logistical hurdles involved with instrument deployment, data analysis, and quality control. Furthermore, challenges in atmospheric modeling arise due to numerical errors associated with complex terrain flows, as well as reliance on simplified parameterizations for unresolved processes such as turbulent mixing and land-surface or forest-canopy-atmosphere interactions. These modeling challenges are exacerbated in the so-called “gray zone,” wherein features of interest have length scales that are similar to the model grid spacing, or when the principal flow layer is smaller than the grid spacing (e.g., slope flows).

54 ENVIRONMENTAL SCIENCES↗

Aerosols consistently suppress the convective boundary layer development

Aerosols with different vertical distribution and various optical properties induce diverse heating rates and thereby affecting convective boundary layer (CBL) development. Our results showed consistent CBL-suppression of aerosols during daytime with numerical experiments, in which aerosols were specified at different heights with synthesized single scattering albedo from 64 studies and asymmetry factor from 20 studies globally. Absorbing aerosols concentrated below but close to the CBL top had the strongest suppression effect on CBL development relative to that concentrated near surface or above CBL. Aerosol cooling effect by attenuating incident solar radiation and surface heat flux exceeded its warming effect by reheating the atmosphere layer with absorbed shortwave radiation, and eventually declined net heating rate, which inhibited CBL development, lowered mixed-layer potential temperature and stabilized atmospheric stratification. Stove effect of absorbing aerosols (CBL enhancement) under a zero background aerosol extinction coefficient is negligible for dominant dome effect (CBL suppression) which consistently suppresses CBL development regardless of aerosol vertical height and background aerosol extinction coefficient. Our study also highlighted the importance of specifying background aerosol extinction coefficient in numerical experiments for accurate assessment of aerosol radiative forcing and CBL-aerosol interactions.

54 ENVIRONMENTAL SCIENCES↗

Probing Interfacial Reaction Pathways in Atomic Layer Deposition on Sulfide Superionic Conductors

Sulfide superionic conductors (e.g., argyrodite Li 6 PS 5 Cl, LPSCl) are extremely promising for all solid-state batteries, but poor atmospheric stability and high interfacial reactivity limit widespread adoption. Coating LPSCl powders with ultrathin coatings using atomic layer deposition (ALD) mitigates these problems, protecting against atmospheric degradation and reducing reactivity with Li metal, yielding more stable cycling. Despite significant promise, the ALD mechanism is unknown, hampering the development of new coating chemistries. In this study, we elucidate the mechanism for Al 2 O 3 ALD on LPSCl using trimethyl aluminum (TMA) and H 2 O by combining in situ Fourier transform infrared spectroscopy, ex situ solid-state magic angle spinning nuclear magnetic resonance, UV Raman spectroscopy, X-ray photoelectron spectroscopy, and density functional theory calculations. We determine that ALD Al 2 O 3 nucleates promptly via TMA reaction with native —OH, —SH, and PS 3 -OH groups to form transient C–Al–O(S) species that are rapidly hydrolyzed during the subsequent H 2 O exposure. This reversible transformation maintains surface nucleophilicity and prevents sulfide decomposition. The resulting layer-by-layer growth leads to highly conformal Al 2 O 3 coatings on LPSCl that are readily scalable to ≥ 50 g quantities using a rotating drum fixture. This detailed understanding of ALD surface reactions provides critical insights guiding the selection of future ALD chemistries with improved performance.

atomic layer deposition↗

Relating Satellite-Based Contrail Detection to NWA Output

Contrail-induced cloud cover has been shown to be a significant factor in regional climate change over the United States of America. As air traffic increases, the potential for globally significant impacts also rises. To better understand and predict these potential climatic effects, it is necessary to develop models that can accurately represent contrail properties based on ambient atmospheric variables including temperature, relative humidity and winds. Several high-resolution numerical weather analyses (NWA) including the 20-km Rapid Update Cycle (RUC) and the University of Oklahoma Center for Analysis and Prediction of Storms Advanced Regional Prediction System (ARPS) can provide the temperature, humidity and wind information necessary to diagnose contrail formation. One outstanding problem that must be addressed to achieve a realistic simulation of contrails is the large uncertainties in upper tropospheric relative humidity (UTH) in numerical weather analyses. Current numerical weather analyses tend to underestimate UTH due to large dry biases in the balloon soundings used to construct the analyses. To evaluate each of the models, we match several months of contrail properties derived from satellite and surface observations to the NWA-derived humidity, vertical velocity, wind shear and atmospheric stability. The relationships between several contrail properties (including optical depth and areal contrail coverage) and the NWA-derived statistics will be analyzed to determine under which atmospheric conditions widespread contrail outbreaks are favored.

Duda, David P.↗

New methods to improve the vertical extrapolation of near-surface offshore wind speeds

Accurate characterization of the offshore wind resource has been hindered by a sparsity of wind speed observations that span offshore wind turbine rotor-swept heights. Although public availability of floating lidar data is increasing, most offshore wind speed observations continue to come from buoy-based and satellite-based near-surface measurements. The aim of this study is to develop and validate novel vertical extrapolation methods that can accurately estimate wind speed time series across rotor-swept heights using these near-surface measurements. We contrast the conventional logarithmic profile against three novel approaches: a logarithmic profile with a long-term stability correction, a single-column model, and a machine-learning model. These models are developed and validated using 1 year of observations from two floating lidars deployed in US Atlantic offshore wind energy areas. We find that the machine-learning model significantly outperforms all other models across all stability regimes, seasons, and times of day. Machine-learning model performance is considerably improved by including the air–sea temperature difference, which provides some accounting for offshore atmospheric stability. Finally, we find no degradation in machine-learning model performance when tested 83 km from its training location, suggesting promising future applications in extrapolating 10 m wind speeds from spatially resolved satellite-based wind atlases.

17 WIND ENERGY↗

Observations on gas exchange and element recycle within a gas-closed algal-mouse system

Life support systems based on bioregeneration rely on the control and manipulation of organisms. Algae are potentially useful for a variety of Closed Ecological Life Support System (CELSS) functions including the revitalization of atmospheres, production of food and for nitrogen fixation. The results of experiments conducted with a gas-closed algal-mouse system designed to investigate gas exchange phenomena under varying algal environmental conditions, and the ability of algae to utilize oxidized mouse solid waste are reported. Inherent instabilities exist between the uptake and release of carbon dioxide (CO2) and oxygen (O2) by the mouse and algae in a gas-closed system. Variations in light intensity and cell density alter the photosynthetic rate of the algae and enable short-term steady-state concentrations of atmospheric CO2 and O2. Different nitrogen sources (urea and nitrate) result in different algal assimilatory quotients (AQ). Combinations of photosynthetic rate and AQ ratio manipulations were examined for their potential in stabilizing atmospheric gas concentrations in the gas-closed algal-mouse system.

Smernoff, D. T.↗

Towards quantifying mesoscale flows in the troposphere using Raman lidar and Sondes

Water vapor plays an important role in the energetics of the boundary layer processes which in turn play a key role in regulating regional and global climate. It plays a primary role in Earth's hydrological cycle, in radiation balance as a direct absorber of infrared radiation, and in atmospheric circulation as a latent heat energy source, as well as in determining cloud development and atmospheric stability. Water vapor concentration, expressed as a mass mixing ratio (g kg(exp -l)), is conserved in all meteorological processes except condensation and evaporation. This property makes it an ideal choice for studying many of the atmosphere's dynamic features. Raman scattering measurements from lidar also allow retrieval of water vapor mixing ratio profiles at high temporal and vertical resolution. Raman lidars sense water vapor to altitudes not achievable with towers and surface systems, sample the atmosphere at much higher temporal resolution than radiosondes or satellites, and do not require strong vertical gradients or turbulent fluctuations in temperature that is required by acoustic sounders and radars. Analysis of highly-resolved water vapor profiles are used here to characterize two important mesoscale flows: thunderstorm outflows and a cold front passage. The data were obtained at the Atmospheric Radiation Measurement Site (CART) by the groundbased Department of Energy/Sandia National Laboratories lidar (CART Raman lidar or CARL) and Goddard Space Flight Center Scanning Raman Lidar (SRL). A detailed discussion of the SRL and CARL performance during the IOPs is given by others in this meeting.

Demoz, B.↗

Determining the power-law wind-profile exponent under near-neutral stability conditions at sea

On the basis of 30 samples from near-simultaneous overwater measurements by pairs of anemometers located at different heights in the Gulf of Mexico and off the Chesapeake Bay, Virginia, the mean and standard deviation for the exponent of the power-law wind profile over the ocean under near-neutral atmospheric stability conditions were determined to be 0.11 +/- 0.03. Because this mean value is obtained from both deep and shallow water environments, it is recommended for use at sea to adjust the wind speed measurements at different heights to the standard height of 10 m above the mean sea surface. An example to apply this P value to estimate the momentum flux or wind stress is provided.

Hsu, S. A.↗

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.↗

Arctic Cloud Response to a Perturbation in Sea Ice Concentration: The North Water Polynya

Surface and atmosphere energy exchanges play an important role in the Arctic climate system by influencing the lower atmospheric stability and humidity, sea ice melt and growth, and surface temperature. Sea ice significantly alters the character of these energy exchanges relative to ice-free ocean. The observed decline in Arctic sea ice since 1979 motivates questions related to the evolving role of surface-atmosphere coupling and potential feedbacks on the Arctic system. Due to the strong wintertime cloud warming effect, a critical question concerns the potential response of low clouds to Arctic sea ice decline. Previous approaches relied on interannual variability to investigate the cloud response to sea ice decline. However, the covariation between atmospheric conditions and sea ice makes it difficult to define an observational control when using interannual variability. To circumvent this difficulty, we exploit the recurring North Water polynya, an episodic opening in the northern Baffin Bay sea ice, as a natural laboratory to isolate the cloud response to a rapid, near-step perturbation in sea ice. Our results show that during the event, (a) low-cloud cover is 10%–33% larger over the polynya than nearby sea ice, (b) cloud liquid water content is up to 400% larger over the polynya than nearby sea ice, and (c) the surface cloud radiative effect is 18 W/sq. m larger over the polynya than nearby sea ice. Our results provide evidence that the low-cloud response during a polynya is a positive feedback lengthening the event.

Emily E. Monroe↗

Characterization of wind speed and directional shear at the AWAKEN field campaign site

The American wake experiment (AWAKEN) is taking place in northern Oklahoma, USA, close to the Atmospheric Radiation Measurement Southern Great Plains (ARM SGP) atmospheric observatory. The planning for the deployment of the instruments in this observational field campaign required an assessment of the wind characteristics of the site. This paper analyzes long-term data collected by instruments at the ARM SGP observatory to characterize the winds near the AWAKEN site. The analysis shows that this site experiences high wind shear and veer events with a large number of nocturnal low-level jets. A total of 7086 low-level jet wind profiles over 6 years are examined and found to be dominant from the south and southeast. Significant nocturnal wind veer is observed, which causes southerly wind near the surface to become westerly wind aloft. By identifying a strong relationship between atmospheric stability and wind shear, the wind shear at the site is predicted using the Monin–Obukhov similarity theory (MOST) and validated with the observational data collected by a scanning Doppler lidar. The results show that wind speed at a height of 91 m, a proxy hub height for wind turbines in this area, can be predicted from data collected at a height of 10 m with a bias of −0.35 and 0.65 m s−1 in unstable and stable atmospheric boundary layers, respectively. The bias of the predicted wind speed is mostly in the region of low wind speed, and wind speed above 5 m s−1 at a height of 91 m can be predicted with a bias of less than 0.2 m s−1, and the limitations of the MOST in predicting winds during the stably stratified boundary layer is well-observed.

17 WIND ENERGY↗

Quantifying the Aerosol Semi-Direct Effect in the NASA GEOS-5 AGCM

Aerosols such as black carbon, dust, and some organic carbon species both scatter and absorb incoming solar radiation. This direct aerosol radiative forcing (DARF) redistributes solar energy both by cooling the surface and warming the atmosphere. As a result, these aerosols affect atmospheric stability and cloud cover (the semi-direct effect, or SDE). Furthermore, in regions with persistent high loadings of absorbing aerosols (e.g. Asia), regional circulation patterns may be altered, potentially resulting in changes in precipitation patterns. Here we investigate aerosol-climate coupling using the NASA Goddard Earth Observing System model version 5 (GEOS-5) atmospheric general circulation model (AGCM), in which we have implemented an online version of the Goddard Chemistry, Aerosol, Radiation and Transport (GOCART) model. GOCART includes representations of the sources, sinks, and chemical transformation of externally mixed dust, sea salt, sulfate, and carbonaceous aerosols. We examine a series of free-running ensemble climate simulations of the present-day period (2000-2009) forced by observed sea surface temperatures to determine the impact of aerosols on the model climate. The SDE and response of each simulation is determined by differencing with respect to the control simulation (no aerosol forcing). In a free-running model, any estimate of the SDE includes changes in clouds due both to atmospheric heating from aerosols and changes in circulation. To try and quantify the SDE without these circulation changes we then examine the DARF and SDE in GEOS-5 with prescribed meteorological analyses introduced by the MERRA analysis. By doing so, we are able to examine changes in model clouds that occur on shorter scales (six hours). In the GEOS-5 data assimilation system (DAS), the analysis is defined as the best estimate of the atmospheric state at any given time, and it is determined by optimally combining a first-guess short-term GCM forecast with all available observations. The Incremental Analysis Update (IAU) is added to the model forecast tendencies to align them with the analysis every six hours, thus preventing longer timescale feedbacks due to the aerosol forcing. We calculate the SDE by comparing model runs with and without aerosols, and the difference in the IAU between these runs is a useful metric with which to evaluate the impact of the SDE on the model atmosphere and clouds. Decreasing the IAU indicates that the aerosol direct and semi-direct effects act to reduce the bias between the model and observations and vice versa.

Randles, Cynthia A.↗

Temperature profiling at the American WAKE ExperimeNt (AWAKEN): methodology and uncertainty quantification

We quantify the accuracy of the temperature profiling from ground-based spectral infrared radiance observations at the American WAKE ExperimeNt (AWAKEN). Results from pre-campaign tests and comparisons with in-situ ground-based and airborne sensors at AWAKEN indicate that temperature profiles agree satisfactorily with traditional instruments for wind energy applications. The bias is within a fraction of a degree and appears to be related to atmospheric stability. Root-mean-square differences from the reference instruments are always smaller than a degree and are often well described by the online uncertainty estimation product. Height-to-height and site-to-site temperature differences are in excellent agreement with in-situ observations, which justifies the use of temperature profilers to characterize static stability and spatial gradients of temperature.

17 WIND ENERGY↗

Predicting wind farm operations with machine learning and the P2D‐RANS model: A case study for an AWAKEN site

Abstract The power performance and the wind velocity field of an onshore wind farm are predicted with machine learning models and the pseudo‐2D RANS model, then assessed against SCADA data. The wind farm under investigation is one of the sites involved with the American WAKE experimeNt (AWAKEN). The performed simulations enable predictions of the power capture at the farm and turbine levels while providing insights into the effects on power capture associated with wake interactions that operating upstream turbines induce, as well as the variability caused by atmospheric stability. The machine learning models show improved accuracy compared to the pseudo‐2D RANS model in the predictions of turbine power capture and farm power capture with roughly half the normalized error. The machine learning models also entail lower computational costs upon training. Further, the machine learning models provide predictions of the wind turbulence intensity at the turbine level for different wind and atmospheric conditions with very good accuracy, which is difficult to achieve through RANS modeling. Additionally, farm‐to‐farm interactions are noted, with adverse impacts on power predictions from both models.

17 WIND ENERGY↗