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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
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DOE OSTI2024

Thermal Stability of Au Rhombic Dodecahedral Nanocrystals Can Be Greatly Enhanced by Coating Their Surface with an Ultrathin Shell of Pt

Rhombic dodecahedral nanocrystals have been considered particularly difficult to synthesize because they are enclosed by {110}, a low-index facet with the greatest surface energy. Recently, we demonstrated the use of seed-mediated growth for the facile and robust synthesis of Au rhombic dodecahedral nanocrystals (AuRD). While the unique shape and surface structure of AuRD are desirable for potential applications in plasmonics and catalysis, respectively, their high surface energy makes them highly susceptible to thermal degradation. Here we demonstrate that it is feasible to greatly improve the thermal stability with some sacrifice to the plasmonic properties of the original AuRD by coating their surface with an ultrathin shell made of Pt. Our in situ electron microscopy analysis indicates that the ultrathin Pt coating can increase the thermal stability from 60 up to 450 °C, a trend that is also supported by the results from a computational study.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Molecular Characterization of Organosulfate-Dominated Aerosols over Agricultural Fields from the Southern Great Plains by High-Resolution Mass Spectrometry

The molecular composition of organic aerosols, especially for day/nighttime variations of organosulfates above agricultural fields, is not well understood despite profound impacts on regional climate, crop production, air quality, and human health. Here, nanospray desorption electrospray ionization with high-resolution mass spectrometry (nano-DESI-HRMS) is used to interrogate the molecular composition of organic aerosols collected at the Southern Great Plains, located in an agricultural region of Oklahoma. Identified molecular formulae featured carbon, hydrogen, oxygen (CHO), nitrogen (CHNO), and/or sulfur (CHOS, CHNOS), with higher organosulfate proportions during daytime (41%) compared to nighttime (30%). In this work, nighttime aerosols featured increases in CHO, CHNO, and extremely low volatility organic carbon (ELVOC) species. However, due to high relative humidity, the nighttime aerosols phase state was found to be more liquid-like than daytime aerosols using parametrized glass transition temperatures. Aerosol molecular composition from an anthropogenically influenced plume (southerly winds) showed significant increases in CHOS and ELVOC species. By comparison with chamber studies, CHOS species are suspected to be of mixed biogenic and anthropogenic origin, whereas CHNOS species (not identified in the southerly winds) are suggested to predominately be of biogenic origin. Overall, this study provides key insight into organosulfates above agricultural fields, demonstrating dependence upon day/night cycles and episodic anthropogenic emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Observational Evidence of State‐Dependent Positive and Negative Land Surface Feedback on Afternoon Deep Convection Over the Southern Great Plains

Abstract The detection of soil moisture‐precipitation feedback is complicated by the dependence of feedback sign on atmospheric state and cloud types. We evaluated responses of convective clouds to changes in surface evaporative fraction (EF) from satellite and ground‐based measurements over the Southern Great Plains in summer months. Strong responses to EF were inferred only after accounting for tropospheric states supporting systematically positive or negative responses. State dependence (inferred from controlled model experiments) explains the weak response found in previous studies. The probability of transitions from shallow to deep cumulus, and subsequent precipitation onset, increases by 58% over drier surfaces in weakly stratified environments having deeper boundary layers. Boundary layer dynamics play a more important role than low‐level relative humidity in these environments. Wetter surfaces yield increased deep convection in moist and thermally stratified environments. The distinct pathways of convective initiation over dry and wet land surfaces can play important roles in drought onset and termination.

Qiu, Shaoyue↗
DOE OSTI2020

Fine-Scale Variability of Observed and Simulated Surface Albedo Over the Southern Great Plains

Surface albedo can be highly variable in both space and time. The Department of Energy’s Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field study provides a unique opportunity to characterize the variability over the Southern Great Plains of the United States using integrated tower, aircraft, and satellite observations of the surface albedo and Normalized Difference Vegetation Index (NDVI). The primary advantage of the aircraft and satellite observations is the ability to examine the spatial distribution of surface albedo and NDVI over a large area, while the tower measurements have the ability to examine both diurnal and day-to-day variability at a single location. In general, consistency was found between both the broadband (BB) albedo and NDVI measured from the surface, air and space. There was a small increase from 0.186 to 0.194 in the aircraft BB surface albedo between May and September (about 4% change), while the MODIS black-sky BB surface albedo increased from 0.151 to 0.166 over the same period (about 10% change) while the standard deviations in the aircraft and MODIS BB albedo were similar. The largest seasonal differences in both the aircraft BB albedo and NDVI were found for areas with winter wheat or forest, while areas with pasture or grasses showed a smaller seasonal diversity. The Weather Research and Forecasting (WRF) model was used to simulate the BB surface albedo. In comparison with the aircraft and satellite observations, the WRF-simulated BB surface albedo had no seasonal change and a much narrower distribution.

Berg, Larry K.↗
DOE OSTI2020

Modeling Spatial Heterogeneity in Surface Turbulent Heat Flux in the U.S. Southern Great Plains

Advances in numerical modeling of cloud dynamics are driving a need for improved land model prediction at convective storm scales. Here, satellite and ground-based vegetation remote sensing data were combined with land model experiments to more accurately characterize land surface spatial heterogeneity in the Community Land Model (CLM4.0). The new subgrid classification of plant functional types (PFT) and leaf area index (LAI) enables consistent comparison between models and ground-based flux measurements in the U.S. southern Great Plains. Errors in vegetation data sets (inferred from comparison between 250 m satellite and ground-based LAI), while large, had less impact on the simulated characteristics of spatial heterogeneity compared to errors in model representation of surface energy partitioning (between latent and sensible heat flux) and its relationship to LAI. Predicted spatial heterogeneity in surface energy partitioning was enhanced after replacing soil and stomatal resistance parameters with a new set that better predicts the observed relationship to LAI. These modifications increase the number of smaller (mesoscale) dry land patches having higher sensible heat flux. The parameter experiments suggest that vegetation state and processes (transpiration) act to broaden the size spectrum of surface heat flux heterogeneity, which can influence clouds and convective initiation. Moreover, improvements in vegetation input data and model parameters had partially compensating effects on surface flux heterogeneity, indicating the importance of evaluating input data and parameterizations together to improve prediction at higher spatial resolutions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Future changes in the Great Plains Low-Level Jet governed by seasonally dependent pattern changes in the North Atlantic Subtropical High

The southerly Great Plains low-level jet (GPLLJ) plays an important role in the Central US hydroclimate, but our understanding of its response to global warming remains elusive. Here we show that the GPLLJ will intensify and intrude deeper under warming in both spring and autumn but change marginally in summer. This response is governed by seasonally dependent pattern changes of the North-Atlantic subtropical high (NASH). In spring and autumn, with a substantial poleward shift in the North America westerly jet, the NASH expands poleward notably. The anomalous surface high poleward of the NASH enhances the southerly GPLLJ to its west. In summer, however, the poleward westerly-jet shift is weak and changes in the NASH manifest a westward extension, which only marginally affects the GPLLJ. Among models, the NASH expansion and GPLLJ enhancement are correlated with the poleward jet shift, highlighting its critical role in regulating the future NASH and GPLLJ changes.

58 GEOSCIENCES↗
DOE OSTI2021

Impact of Lateral Flow on Surface Water and Energy Budgets over the Southern Great Plains – A Modeling Study

As we see the horizontal grid spacing decrease, treatment of hydrologic processes in land surface models, such as the lateral flow of surface and subsurface flow, need to be explicitly represented. Unlike previous studies that mainly focused on the mountainous regions, in this study the offline WRF-Hydro model is employed to study the impact of lateral flow on soil moisture and energy fluxes over the relatively flat southern Great Plains (SGP). The vast amount of measurements over the SGP provide an unique opportunity to assess the model behavior. In addition, newly developed land surface properties and input forcing are ingested into the model, in an attempt to reduce uncertainties associated with the initial and boundary forcing and help to identify model deficiencies. Our results show that the more realistic inputs (parameters, soil types, forcing) lead to larger underestimation of latent heat flux and dry bias, indicating the existence of model structural uncertainty (embedded errors) in WRF-Hydro that need to be characterized to inform future model development efforts. Including lateral flow processes partly mitigates the model deficiencies in representing hydrologic processes and alleviates the dry bias. In particular, both surface and subsurface lateral flow increase soil moisture mainly over the lower elevations, except that subsurface flow also affects soil moisture over steeper terrains. Additional simulations are performed to assess the effect of routing resolution on model results. When LSM resolution is high, noticeable differences in soil moisture are produced between different routing resolutions especially over steep terrain. Whereas when LSM resolution is coarse, differences between routing resolutions become negligible, especially over flat terrain.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Simulating the Effects of Surface Energy Partitioning on Convective Organization: Case Study and Observations in the US Southern Great Plains

Realistic cloud-resolving simulations were performed to study the effects of surface energy partitioning (surface sensible and latent heat fluxes) on the organization of isolated convection into larger mesoscale convective systems (MCSs) near the US Southern Great Plains. The role of cold pools in mediating surface-convection interactions was explored. Better organized MCSs tended to occur in the experiments with perturbed wetter soil (and more active vegetation), regardless of the effects of soil moisture on the diurnal timing of convective triggering. Wetter soil led to shallower boundary layers and more convective available potential energy than drier soil. The roles of cold pools on convection are lifecycle-stage dependent: A dry surface allows more numerous colliding cold pools, thereby aiding in convective triggering by reducing entrainment in the early stages, and providing gust-front uplift in later stages. However, horizontal propagation of the cold-pool density current can outrun the convective system, creating a slantwise updraft and thus weakening the gust front uplift in later stages. This effect calls into question previous cold pool parameterizations, in which the gust front uplift is mainly proportional to the negative buoyancy of cold air. Finally, both the model and observation show an enhancement of surface latent heat flux during the passage of a gust front at night, suggesting that a positive feedback between the surface and convection helps MCSs to persist into the nighttime.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

How Does Land Cover and Its Heterogeneity Length Scales Affect the Formation of Summertime Shallow Cumulus Clouds in Observations From the US Southern Great Plains?

This study investigates the effects of heterogeneous land covers on shallow cumulus (ShCu) clouds at the US Southern Great Plains using high-resolution satellite and land cover data. During late summer, ShCu occurs over cities the most frequently and over open waters the least frequently, and more often over forest than over grassland. The preferential occurrence of ShCu over forest relative to grassland is consistent with surface measurements showing larger heat fluxes over forests. This preferential occurrence also varies with the length scales of land patches with the largest cloud occurrence difference shifting from smaller length scales (<9 km) during midday to larger scales (>9 km) in the early afternoon. Consistent with theory, these signals are more pronounced under low wind conditions. The preferential length scale shift with time suggests the existence of secondary circulations that strengthen and promote convergence over larger spatial scales as the differential land surface heating intensifies.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Estimation of Possible Primary Biological Particle Emissions and Rupture Events at the Southern Great Plains ARM Site

We use 10 years of data from the Department of Energy (DoE) Atmospheric Radiation Measurements (ARM) United States Southern Great Plains (SGP) site with nearby regional pollen and fungal spore measurements to indirectly estimate the seasonal influence of these two primary biological aerosol particles (PBAP). We estimate possible primary emissions of larger PBAP and PBAP rupture events, which form submicron organic aerosol during precipitation or high relative humidity. High pollen counts at two urban stations near SGP occur during late winter/early spring (day of year (DOY) 50–120) and late summer (DOY 240–310). Around 4–19 days per year show possible pollen events (PPE) when near-surface lidar observations of daily linear particle depolarization ratio >0.1 are coincident with high organic aerosol fraction. For PPE days with rainfall, aerosol size distribution observations show enhanced submicron particle concentrations consistent with pollen rupture events. For fungal spores, high fungal spore counts occur during late spring/early summer (DOY 110–195) and late summer/autumn (DOY 220–340). Based on size distribution observations, up to 7% of days have possible fungal spore rupture events (PFE) with higher aerosol number count specifically over the range expected for fungal spore fragment mobility diameter (20–50 nm). These short-lived PFE correlate with rainfall or occur after prolonged exposure to rainfall (e.g., >10 h). While the SGP site lacks direct measurements of bioaerosol and large particle sizes, this analysis suggests that PBAP primary emissions and rupture events could occur about 32 days per year, representing an important component of the aerosol budget during seasonal emissions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Aerosol Activation in Radiation Fog at the Atmospheric Radiation Program Southern Great Plains Site

Environmental supersaturation is a key parameter in the formation of fog and clouds, yet it cannot be measured directly and must be inferred. Calculating the ambient supersaturation in fog requires knowledge of the aerosol hygroscopicity as well as particle size distribution, and relatively few values have been reported in the literature. Here we use κ-Köhler theory to derive aerosol activation properties based on particle hygroscopicity and dry particle size distributions, and then estimate the effective peak supersaturation during eight cases of radiative fog at the Southern Great Plains site in rural north-central Oklahoma, USA. The mean hygroscopicity parameter κ of particles likely to act as cloud condensation nuclei varied from 0.14 to 0.43. Ambient effective peak supersaturation during the fog episodes was between 0.01%–0.07%, with most values below 0.04%. Furthermore, the minimum 50% dry activation diameter generally ranged between 300–400 nm with little activation of particles with diameters below 300 nm.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Trends in Downwelling Longwave Radiance Over the Southern Great Plains

Downwelling longwave radiation is an important part of the surface energy budget. Spectral trends in the downwelling longwave radiance (DLR) provide insight into the radiative drivers of climate change. In this research, we process and analyze a 23-year DLR record measured by the Atmospheric Emitted Radiance Interferometer (AERI) at the U.S. Department of Energy Atmospheric Radiation Program Southern Great Plains (SGP) site. Two AERIs were deployed at SGP with an overlapping observation period of about 10 years, which allows us to examine the consistency and accuracy of the measurements and to account for discrepancies between them due to errors associated with the instruments themselves. We then analyzed the all-sky radiance trends in DLR, which are associated with the surface warming trend at SGP during this same period and also the complex changes in meteorological conditions. For instance, the observed radiance in the CO2 absorption band follows closely the near-surface air temperature variations. The significant positive radiance trends in weak absorption channels, such as in the wings of the CO 2 band and in the weak absorption channels in the H 2 O vibration-rotational band, show earlier detectability of climate change. The magnitude of the radiance trend uncertainty in the DLR record mainly results from internal climate variability rather than from measurement error, which highlights the importance of continuing the DLR spectral measurements to unambiguously detect and attribute climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Long‐Term Observations of Turbulence Vertical Velocity Spectra in a Convective Mixed Layer: Dependence on Land‐Surface Forcing in the U.S. Southern Great Plains

Doppler lidar vertical velocity retrievals were analyzed for the scale and structure of mixed-layer turbulence over a 7-year period, on fair-weather warm season days (442 cases) in the U.S. Southern Great Plains. Based on the hypothesized influence of land-surface forcing and updraft size on convective boundary layer clouds, a spectral analysis was performed to quantify effects of surface forcing (surface buoyancy flux, friction velocity, and evaporative fraction) on turbulence scale. Significant (order-of-magnitude) variations in spectral density were found in the energy-production subrange and mesoscale regimes. Integral scale decreased with increasing buoyancy flux (and Monin-Obukhov stability parameter), while spectral density in the energy-production subrange increased, implying a transition to buoyancy-driven cellular structures with narrower updrafts. The influence of stability parameter was limited to the neutral to convective transition, and could not explain the wide variation in spectral density in the mesoscale regime. However, high friction velocity (u* > 0.5 m s –1 ) was associated with larger integral scale (updraft width), and a greater portion of spectral density in the mesoscale regime. Lidar profiles and radar reflectivity for individual cases revealed evidence of roll and wave-like structures contributing to mesoscale variability on high friction velocity days, suggesting shear instabilities on days with wetter land surface conditions and smaller buoyancy flux. The role of friction velocity emphasizes the multivariate nature of surface influences on turbulence, and implies that variance-based turbulence closures may not be adequate for capturing effects of surface forcing on updraft size.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cloud Condensation Nuclei Closure Study Using Airborne Measurements Over the Southern Great Plains

Abstract Airborne measurements of non‐refractory bulk aerosol chemical composition, aerosol size distributions, and cloud condensation nuclei (CCN) were conducted onboard a research aircraft during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems field campaign in the spring and summer of 2016. A CCN closure study for the entire campaign period was performed where measured CCN concentrations at 0.24% and 0.46% supersaturation were compared with the predicted CCN concentrations calculated using κ ‐Köhler theory, three different assumptions of aerosol mixing state, and various assumptions about hygroscopicity, density, and the insoluble fraction of organic particles. We found that the Closure Ratio (CR), calculated as the ratio of predicted to measured CCN concentrations, was equal to one under two different aerosol mixing state assumptions: (a) all particles are composed of 100% organic particles, and (b) particles are externally mixed and composed of pure sulfates, nitrates, and organic particles assuming hygroscopicity values for organic particles ( ) between 0.04 and 0.17. The use of internal mixing state assumption often led to overprediction of CCN concentrations but the agreement within ±20% with the measured CCN concentrations was observed under certain closure permutations. A similar agreement, that is, within ±20%, was also observed using permuted parameters concerning density (1 and 1.5 g cm −3 ) and an insoluble fraction (0% and 20%) of organic particles. These findings may provide constraints on to predict CCN concentrations at a remote continental Southern Great Plains site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Observation and Reanalysis Derived Relationships Between Cloud and Land Surface Fluxes Across Cumulus and Stratiform Coupling Over the Southern Great Plains

Abstract Understanding interactions between low clouds and land surface fluxes is critical to comprehending Earth's energy balance, yet their relationships remain elusive, with discrepancies between observations and modeling. Leveraging long‐term field observations over the Southern Great Plains, this investigation revealed that cloud‐land interactions are closely connected to cloud‐land coupling regimes. Observational evidence supports a dual‐mode interaction: coupled stratiform clouds predominate in low sensible heat scenarios, while coupled cumulus clouds dominate in high sensible heat scenarios. Reanalysis data sets, MERRA‐2 and ERA‐5, obscure this dichotomy owing to a shortfall in representing boundary layer clouds, especially in capturing the initiation of coupled cumulus in high sensible heat scenarios. ERA‐5 demonstrates a relatively closer alignment with observational data, particularly in capturing relationships between cloud frequency and latent heat, markedly outperforming MERRA‐2. Our study underscores the necessity of distinguishing different cloud coupling regimes, essential to the understanding of their interactions for advancing land‐atmosphere interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Summer Convective Precipitation Changes Over the Great Lakes Region Under a Warming Scenario

To understand future summer precipitation changes over the Great Lakes Region (GLR), we performed an ensemble of regional climate simulations through the Pseudo-Global Warming (PGW) approach. We found that different types of convective precipitation respond differently to the PGW signal. Isolated deep convection (IDC), usually concentrated in the southern domain, shows an increase in precipitation to the north of the GLR. Mesoscale convective systems (MCSs), usually concentrated upwind of the GLR, shift to the downwind region with increased precipitation. Thermodynamic variables such as convective available potential energy (CAPE) and convective inhibition energy (CIN) are found to increase across almost the entire studied domain, creating a potential environment more favorable for stronger convection systems and less favorable for weaker ones. Meanwhile, changes in the lifting condensation level (LCL) and level of free convection (LFC) show a strong correlation with variations in convective precipitation, highlighting the significance of these thermodynamic factors in controlling precipitation over the domain. Our results indicate that the decrease in LCL and LCF in areas with increased convective precipitation is mainly due to increased atmospheric moisture. In response to the prescribed warming perturbation, MCSs occur more frequently downwind, while localized IDCs exhibit more intense rain rates, longer durations, and larger rainfall area.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Investigating Aerosol Hygroscopicity in the Subcloud Transition Zone and at the Surface in the Southern Great Plains

Aerosols beneath a cloud base, a subcloud transition zone (SCTZ), are key to understand both the aerosol-cloud interaction and aerosol-radiation interactions. Lidars have been the primary means of observing aerosols in the SCTZ by virtue of enhanced light scattered by aerosol particles. The enhanced light maybe caused by several factors: the aerosol swelling effect due to hygroscopicity under high relative humidity, cloud 3-dimensional (3D) effect, aerosol nucleation into cloud droplets, etc. While each factor and process has been known, their relative contributions are much poorly quantified. This study explores the hygroscopicity and optical properties of aerosols in the SCTZ and at ground level in the Southern Great Plains (SGP) region. Utilizing comprehensive observational data from the U.S. Department of Energy's Atmospheric Radiation Measurement at the Oklahoma SGP site, including ground-based aerosol measurements and Raman lidar profiles from April 2021 to April 2022, this study extensively analyzes the influence of aerosol hygroscopic growth and cloud fragments on aerosol optical properties. Distinct seasonal variations in aerosol hygroscopic characteristics are revealed. At the ground level, aerosols in autumn and winter exhibit stronger hygroscopicity due to a higher proportion of inorganic content than summer. In the SCTZ, aerosols during summer show enhanced backscatter due to strong cloud fragmentation effects, with numerous cloud fragments elevating hygroscopicity beyond that observed in autumn and winter. These insights are crucial for understanding the interactions between aerosols at the surface and cloud layers, evaluating cloud condensation nuclei beneath clouds, and their implications for atmospheric radiation and climate modeling.

Hu, Rong [Beijing Normal University, Beijing (Chin↗
DOE OSTI2025

Assessment of Extinction‐, Satellite‐, and Model‐Based Vertical Cloud Condensation Nuclei (CCN) Retrieval Methods Using Airborne CCN Measurements Over the Southern Great Plains

Abstract Accurate estimates of the vertical profile of cloud condensation nuclei (CCN) concentration are crucial to better quantify aerosol‐cloud interactions. We assessed the correlation between the vertical CCN concentrations obtained from extinction‐, satellite‐, and model‐based retrieval methods and airborne CCN concentrations collected at 0.24% supersaturation within the 3, 9, 27, and 81 km regions centered over the U.S. Department of Energy's Atmospheric Radiation Measurement User Facility Southern Great Plains (SGP) site during the spring and summer of 2016. The extinction profiles at a wavelength 355 nm were provided by the ground‐based Raman lidar. Our analysis showed moderate correlation between dry‐corrected extinction and airborne CCN data. We found the retrieved number concentration of CCN (RNCCN) method showed regression best‐fit slopes close to unity and consistent prediction errors for the majority of the data. The Lenhardt et al. (2023, https://doi.org/10.5194/amt‐16‐2037‐2023 ) method showed similar conclusions but only during spring, whereas the Mamouri and Ansmann (2016, https://doi.org/10.5194/acp‐16‐5905‐2016 ) method showed poor correlation. The Shinozuka et al. (2015, https://doi.org/10.5194/acp‐15‐7585‐2015 ) satellite‐based method exhibited reasonable agreement during summer but poor correlation during periods where both high (∼1,400 #/cm 3 ) and low (∼50 #/cm 3 ) airborne CCN concentrations were observed. The Copernicus Atmosphere Monitoring Service reanalysis modeled 3‐D CCN data set showed a moderate to weak positive correlation but performed poorly at high airborne CCN concentrations. Our analysis suggests the extinction‐based RNCCN method performed better than other methods across most observation periods under the diverse meteorological conditions observed at the SGP site.

54 ENVIRONMENTAL SCIENCES↗