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At least 19 records

Quantifying sensitivities of ice crystal number and sources of ice crystal number variability in CAM 5.1 using the adjoint of a physically based cirrus formation parameterization

Abstract We present the adjoint of a cirrus formation parameterization that computes the sensitivity of ice crystal number concentration to updraft velocity, aerosol, and ice deposition coefficient. The adjoint is driven by simulations from the National Center for Atmospheric Research Community Atmosphere Model version 5.1 CAM 5.1 to understand the sensitivity of formed ice crystal number concentration to 13 variables and quantify which contribute to its variability. Sensitivities of formed ice crystal number concentration to updraft velocity, sulfate number, and is sufficient but sulfate number concentration is low, indicating a sulfate‐limited regime. Outside of the tropics, competition between homogeneous and heterogeneous nucleation may shift annually averaged sensitivities to higher magnitudes, when infrequent strong updrafts shift crystal production away from purely heterogeneous nucleation. Outside the tropics, updraft velocity is responsible for approximately 52.70% of the ice crystal number variability. In the tropics, sulfate number concentration and updraft jointly control variability in formed crystal number concentration. Insoluble aerosol species play a secondary, but still important, role in influencing the variability in crystal concentrations, with coarse‐mode dust being the largest contributor at nearly 50% in certain regions. On a global scale, more than 95% of the temporal variability in crystal number concentration can be described by temperature, updraft velocity, sulfate number, and coarse‐mode dust number concentration.

Sheyko, B. A.↗

A Theory for the Balance between Warm Rain and Ice Crystal Processes of Precipitation in Mixed-Phase Clouds

Abstract Mixed-phase clouds contain both supercooled cloud liquid and ice crystals. In principle, precipitation may be initiated either by the liquid phase or by the ice phase. Ice crystals may grow by vapor diffusion to become snow (“ice crystal process”), forming “cold” precipitation. Equally, cloud droplets, when large enough, coalesce to form “warm” precipitation by the “warm rain process.” Warm rain could be supercooled and freeze as “warm” graupel. In the present paper, a new simplified theoretical analysis is provided to examine the microphysical system consisting of three species of hydrometeor, namely, cloud liquid, “cold ice” (crystals, snow), and “warm rain” (frozen or supercooled). This is obtained by nondimensionalizing and simplifying the evolution equations for the mass of each species. Analytical formulas are given for equilibria. Feedback analysis shows that the sign of the feedback is linked to the abundance of precipitation, with a neutral surface in the 3D phase space. The system’s precipitation amount explodes while in the initial unstable regime, crossing the neutral surface and approaching the equilibrium point that is a stable attractor. Positive and negative feedbacks are elucidated. In a standard case, the cold ice mass is about 1000 times larger than the warm rain mass. To illustrate the physical behavior of the theory, sensitivity tests are performed with respect to environmental conditions (e.g., aerosol, updraft speed) and microphysical parameters (e.g., riming and sedimentation rates for cold ice). Cold ice prevails, especially in fast ascent, due to its low bulk density, favoring slow sedimentation and a wide cross-sectional area for riming. Significance Statement The theory elucidates how the ice phase can prevail in the precipitation from any mixed-phase clouds with supercooled cloud liquid and crystals. The ice phase radically suppresses cloud liquid by riming when active and “wins” the competition against coalescence. This prevalence of ice is shown to arise from the low bulk density of snow. The cloud is viewed as a system of negative and positive feedbacks that prevail in realms of stability and instability in a 3D phase space.

Meteorology & Atmospheric Sciences↗

Effects of pre-existing ice crystals on cirrus clouds and comparison between different ice nucleation parameterizations with the Community Atmosphere Model (CAM5)

In order to improve the treatment of ice nucleation in a more realistic manner in the Community Atmosphere Model version 5.3 (CAM5.3), the effects of pre-existing ice crystals on ice nucleation in cirrus clouds are considered. In addition, by considering the in-cloud variability in ice saturation ratio, homogeneous nucleation takes place spatially only in a portion of the cirrus cloud rather than in the whole area of the cirrus cloud. Compared to observations, the ice number concentrations and the probability distributions of ice number concentration are both improved with the updated treatment. The pre-existing ice crystals significantly reduce ice number concentrations in cirrus clouds, especially at mid- to high latitudes in the upper troposphere (by a factor of ~10). Furthermore, the contribution of heterogeneous ice nucleation to cirrus ice crystal number increases considerably. Besides the default ice nucleation parameterization of Liu and Penner (2005, hereafter LP) in CAM5.3, two other ice nucleation parameterizations of Barahona and Nenes (2009, hereafter BN) and Kärcher et al. (2006, hereafter KL) are implemented in CAM5.3 for the comparison. In-cloud ice crystal number concentration, percentage contribution from heterogeneous ice nucleation to total ice crystal number, and pre-existing ice effects simulated by the three ice nucleation parameterizations have similar patterns in the simulations with present-day aerosol emissions. However, the change (present-day minus pre-industrial times) in global annual mean column ice number concentration from the KL parameterization (3.24 × 10 6 m -2 ) is less than that from the LP (8.46 × 10 6 m -2 ) and BN (5.62 × 10 6 m -2 ) parameterizations. As a result, the experiment using the KL parameterization predicts a much smaller anthropogenic aerosol long-wave indirect forcing (0.24 W m -2 ) than that using the LP (0.46 W m −2 ) and BN (0.39 W m -2 ) parameterizations.

54 ENVIRONMENTAL SCIENCES↗

Understanding cirrus ice crystal number variability for different heterogeneous ice nucleation spectra

Abstract. Along with minimizing parameter uncertainty, understanding the cause of temporal and spatial variability of the nucleated ice crystal number, N i , is key to improving the representation of cirrus clouds in climate models. To this end, sensitivities of N i to input variables like aerosol number and diameter provide valuable information about nucleation regime and efficiency for a given model formulation. Here we use the adjoint model of the adjoint of a cirrus formation parameterization (Barahona and Nenes, 2009b) to understand N i variability for various ice-nucleating particle (INP) spectra. Inputs are generated with the Community Atmosphere Model version 5, and simulations are done with a theoretically derived spectrum, an empirical lab-based spectrum and two field-based empirical spectra that differ in the nucleation threshold for black carbon particles and in the active site density for dust. The magnitude and sign of N i sensitivity to insoluble aerosol number can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, which reveals a disparity in aerosol surface properties. N i sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters; this low temperature sensitivity regime has been experimentally reported before but never deconstructed as done here.

54 ENVIRONMENTAL SCIENCES↗

A Machine Learning Framework for Predicting Microphysical Properties of Ice Crystals From Cloud Particle Imagery

The microphysical properties of ice crystals are important because they significantly alter the radiative properties and spatiotemporal distributions of clouds, which in turn strongly affect Earth's climate. However, it is challenging to measure key properties of ice crystals, such as mass or morphological features. Here, we present a proof-of-concept framework for predicting three-dimensional (3D) microphysical properties of ice crystals from in situ two-dimensional (2D) imagery. First, we computationally generated synthetic ice crystals using 3D modeling software along with geometric parameters estimated from the 2021 Ice Cryo-Encapsulation Balloon (ICEBall) field campaign. Then, we used synthetic crystals to train machine learning (ML) models to predict effective density ($ρ_e$), effective surface area ($A_e$), and number of bullets ($N_b$) from synthetic rosette imagery. On unseen synthetic images, our ML models accurately predicted ice crystal properties. ResNet-18 performed best, achieving $R^2$ values of 0.99 and 0.98 for $ρ_e$ and $A_e$, respectively, and MAE of 0.10 for mathematical equation in single view tasks. Stereo view ResNet-18 further reduced RMSE by 40% for $ρ_e$ and $A_e$ and reduced MAE by 0.08 for $N_b$. This work provides a novel ML-driven framework for estimating ice microphysical properties from in situ imagery, which will allow for downstream constraints on microphysical parameterizations, such as the mass-size relationship.

Ko, J. [Columbia Univ., New York, NY (United State↗

Partition between supercooled liquid droplets and ice crystals in mixed-phase clouds based on airborne in situ observations

Abstract. The onset of ice nucleation in mixed-phase clouds determines the lifetime and microphysical properties of ice clouds. In this work, we develop a novel method that differentiates between various phases of mixed-phase clouds, such as clouds dominated by pure liquid or pure ice segments, compared with those having ice crystals surrounded by supercooled liquid water droplets or vice versa. Using this method, we examine the relationship between the macrophysical and microphysical properties of Southern Ocean mixed-phase clouds at −40 to 0 °C (e.g. stratiform and cumuliform clouds) based on the in situ aircraft-based observations during the US National Science Foundation Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) flight campaign. The results show that the exchange between supercooled liquid water and ice crystals from a macrophysical perspective, represented by the increasing spatial ratio of regions containing ice crystals relative to the total in-cloud region (defined as ice spatial ratio), is positively correlated with the phase exchange from a microphysical perspective, represented by the increasing ice water content (IWC), decreasing liquid water content (LWC), increasing ice mass fraction, and increasing ice particle number fraction (IPNF). The mass exchange between liquid and ice becomes more significant during phase 3 when pure ice cloud regions (ICRs) start to appear. Occurrence frequencies of cloud thermodynamic phases show a significant phase change from liquid to ice at a similar temperature (i.e. −17.5 °C) among three types of definitions of mixed-phase clouds based on ice spatial ratio, ice mass fraction, or IPNF. Aerosol indirect effects are quantified for different phases using number concentrations of aerosols greater than 100 or 500 nm (N>100 and N>500, respectively). N>500 shows stronger positive correlations with ice spatial ratios compared with N>100. This result indicates that larger aerosols potentially contain ice-nucleating particles (INPs), which facilitate the formation of ice crystals in mixed-phase clouds. The impact of N>500 is also more significant in phase 2 when ice crystals just start to appear in the mixed phase compared with phase 3 when pure ICRs have formed, possibly due to the competing aerosol indirect effects on primary and secondary ice production in phase 3. The thermodynamic and dynamic conditions are quantified for each phase. The results show stronger in-cloud turbulence and higher updraughts in phases 2 and 3 when liquid and ice coexist compared with pure liquid or ice (phases 1 and 4, respectively). The highest updraughts and turbulence are seen in phase 3 when supercooled liquid droplets are surrounded by ice crystals. These results indicate both updraughts and turbulence support the maintenance of supercooled liquid water amongst ice crystals. Overall, these results illustrate the varying effects of aerosols, thermodynamics, and dynamics through various stages of mixed-phase cloud evolution based on this new method that categorizes cloud phases.

54 ENVIRONMENTAL SCIENCES↗

Development and characterization of an ice-selecting pumped counterflow virtual impactor (IS-PCVI) to study ice crystal residuals

Separation of particles that play a role in cloud activation and ice nucleation from interstitial aerosols has become necessary to further understand aerosol-cloud interactions. The pumped counterflow virtual impactor (PCVI), which uses a vacuum pump to accelerate the particles and increase their momentum, provides an accessible option for dynamic and inertial separation of cloud elements. However, the use of a traditional PCVI to extract large cloud hydrometeors is difficult mainly due to its small cut-size diameters (< 5 µm). Here, for the first time we describe a development of an ice-selecting PCVI (IS-PCVI) to separate ice in controlled mixed-phase cloud system based on the particle inertia with the cut-off diameter ≥ 10 µm. We also present its laboratory application demonstrating the use of the impactor under a wide range of temperature and humidity conditions. The computational fluid dynamics simulations were initially carried out to guide the design of the IS-PCVI. After fabrication, a series of validation laboratory experiments were performed coupled with the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) expansion cloud simulation chamber. In the AIDA chamber, test aerosol particles were exposed to the ice supersaturation conditions (i.e., RH ice > 100 %), where a mixture of droplets and ice crystals was formed during the expansion experiment. In parallel, the flow conditions of the IS-PCVI were actively controlled, such that it separated ice crystals from a mixture of ice crystals and cloud droplets, which were of diameter ≥ 10 µm. These large ice crystals were passed through the heated evaporation section to remove the water content. Afterwards, the residuals were characterized with a suite of online and offline instruments downstream of the IS-PCVI. These results were used to assess the optimized operating parameters of the device in terms of (1) the critical cut-size diameter, (2) the transmission efficiency and (3) the counterflow-to-input flow ratio. Particle losses were characterized by comparing the residual number concentration to the rejected interstitial particle number concentration. Overall results suggest that the IS-PCVI enables inertial separation of particles with a volume-equivalent particle size in the range of ~&thinsp;10–30 µm in diameter with small inadvertent intrusion (~ &thinsp;5 %) of unwanted particles.

54 ENVIRONMENTAL SCIENCES↗

Prognostic simulations of mixed-phase clouds with model AC-1D v1.0: the impact of aerosol types and freezing parameterizations on ice crystal budgets

Mixed-phase clouds at high latitudes contribute to the uncertainty in predicting cloud feedbacks and climate sensitivity, mainly due to the complexity of microphysical processes that influence the partitioning between the supercooled liquid and ice phases, and hence, cloud radiative effects on regional scales. Particularly in Arctic mixed-phase clouds, the activation of ice-nucleating particles (INPs) from various aerosol populations remains a leading source of uncertainty. We developed an aerosol-cloud one-dimensional (AC-1D) model, which provides a novel framework to prognostically treat INP and ice crystal budgets while explicitly accounting for polydisperse and multicomponent aerosol that activate INPs following different freezing parameterizations. The AC-1D model is informed by large-eddy simulations to probe the impact of INP representation on predicted ice crystal number concentrations (N i ) and ice crystal budgets in mixed-phase Arctic stratus. We apply three immersion freezing (IMF) parameterizations, two time-independent (singular) and one time-dependent (classical nucleation theory), to predict the evolution of the INP reservoir and resulting ice crystal budget from polydisperse mineral dust, organic (humic-like substances), and sea spray aerosol particle size distributions. Our analysis focuses on how variations in aerosol number concentration and cloud system parameters such as cloud cooling rate, cloud-top entrainment rate, and ice crystal fall speed influence the INP reservoir and ice crystal budgets. Furthermore, this study investigates the competitive ice nucleation dynamics in mixed aerosol environments and provides a process-level quantification of the INP budget terms, which directly controls ice crystal budgets. For all studied case scenarios, the aerosol types and associated particle size distributions significantly impact INP and N i , and the choice between a time-dependent and a singular freezing description yields orders-of-magnitude differences in the predicted INP and N i over the 10 h simulation time, reflecting typical cloud lifetimes. Our results show that the influence of cloud cooling, INP entrainment, and sedimentation varies significantly depending on the chosen freezing parameterization. These findings underscore the critical need for robust IMF parameterizations and precise cloud system observations to enhance the accuracy of models in predicting mixed-phase cloud structure and evolution.

Arctic clouds↗

An experimental and numerical study of the light scattering properties of ice crystals with black carbon inclusions

Here, we investigate the optical properties of ice crystals nucleated on atmospheric black carbon (BC). The parameters examined in this study are the shape of the ice crystal, the volume fraction of the BC inclusion, and its location inside the crystal. We report on new spectrometer measurements of forward scattering and backward polarization from ice crystals nucleated on BC particles and grown under laboratory-controlled conditions. Data from the Cloud and Aerosol Spectrometer with Polarization (CASPOL) are used for direct comparison with single-particle calculations of the scattering phase matrix. Geometrical optics and discrete dipole approximation techniques are jointly used to provide the best compromise of flexibility and accuracy over a broad range of size parameters. Together with the interpretation of the trends revealed by the CASPOL measurements, the numerical results confirm previous reports on absorption cross-section magnification in the visible light range. Even taking into account effects of crystal shape and inclusion position, the ratio between absorption cross-section of the compound particle and the absorption cross-section of the BC inclusion alone (the absorption magnification) has a lower bound of 1.5; this value increases to 1.7 if the inclusion is centered with respect to the crystal. The simple model of BC-ice particle presented here also offers new insights on the effect of the relative position of the BC inclusion with respect to the crystal's outer surfaces, the shape of the crystal, and its size.

54 ENVIRONMENTAL SCIENCES↗

Implementation of a comprehensive ice crystal formation parameterization for cirrus and mixed-phase clouds in the EMAC model (based on MESSy 2.53)

A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations (ICNCs). The parameterization of Barahona and Nenes (2009, hereafter BN09) allows for the treatment of ice nucleation taking into account the competition for water vapour between homogeneous and heterogeneous nucleation in cirrus clouds. Furthermore, the influence of chemically heterogeneous, polydisperse aerosols is considered by applying one of the multiple ice nucleating particle parameterizations which are included in BN09 to compute the heterogeneously formed ice crystals. BN09 has been modified in order to consider the pre-existing ice crystal effect and implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC parameterizations, BN09 produces fewer ice crystals in the upper troposphere but higher ICNCs in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. Overall, ICNCs agree well with the observations, especially in cold cirrus clouds (at temperatures below 205 K), although they are underestimated between 200 and 220 K. As BN09 takes into account processes which were previously neglected by the standard version of the model, it is recommended for future EMAC simulations.

58 GEOSCIENCES↗

Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions

This is the final technical report for DOE DE-SC0021034 award entitled “Application of aerosol-ice nucleating particle closure to establish the leading parameters governing ice crystal number concentration under commonly observed mixed-phase cloud conditions”. The overarching objective of this project was to gain a predictive understanding of the processes that lead from aerosols to ice-nucleating particles (INPs) to ice crystal number concentrations (ICNCs) in stratiform mixed-phase clouds where supercooled water droplets and ice crystals coexist, and to inform climate model parameterizations. During this four-year project we addressed the three main research goals of this objective: 1) Study the aerosol-INP link; 2) Develop an aerosol-cloud column model (AC-1D); and 3) Study the INP-ICNC link. Those activities significantly advanced our predictive understanding of how to represent INPs in could models and its implications on ice crystal number concentrations. The results have been published in five peer-reviewed publications with three more in review and preparation. It allowed for collaboration resulting in additional fourteen peer-reviewed publications that are concerned with the objective of this research project. This research has been communicated to the scientific community at national and international meetings and conferences by numerous talks, seminars, and posters including fifteen invited presentations. This project allowed training of four graduate students and one postdoctoral research associate resulting in one M.S. thesis and advancement to Ph.D. candidacy.

54 ENVIRONMENTAL SCIENCES↗

Dimensions and aspect ratios of natural ice crystals

During the 2006 Tropical Warm Pool International Cloud Experiment (TWP-ICE) in the tropics, the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) in the Arctic, and the 2010 Small PARTicles In CirrUS (SPARTICUS) campaign at mid-latitudes, high-resolution images of ice crystals were recorded by a Cloud Particle Imager at temperatures ( T ) between -87 and 0 °C. The projected maximum dimension ( D '), length ( L '), and width ( W ') of pristine columns, plates, and component bullets of bullet rosettes were measured using newly developed software, the Ice Crystal Ruler. The number of bullets in each bullet rosette was also measured. Column crystals were further distinguished as either horizontally oriented columns or columns with other orientations to eliminate any orientation effect on the measured dimensions. The dimensions and aspect ratios (AR, the dimension of the major axis divided by the dimension of the minor axis) of crystals were determined as functions of temperature, geophysical location, and type of cirrus. Dimensions of crystals generally increased with temperature. Columns and bullets had larger dimensions (i.e., W ') of the minor axis (i.e., a axis) for a given dimension (i.e., D ' or L ') of the major axis (i.e., c axis), and thus smaller AR, as T increased, whereas this trend did not occur for plate crystals. The average number of branches in bullet rosettes was 5.50 ± 1.35 during three campaigns and 6.32 ± 1.34 (5.46 ± 1.34; 4.95 ± 1.01) during TWP-ICE (SPARTICUS; ISDAC). The AR of bullets increased with the number of branches in bullet rosettes. Most dimensions of crystals and ARs of columnar crystals measured during SPARTICUS were larger than those measured during TWP-ICE and ISDAC at &minus;67 < T < -35 °C and at &minus;40 < T < &minus;15 °C, respectively. The relative occurrence of varying pristine habits depended strongly on cirrus type (i.e., anvil or non-anvil clouds), with plates especially occurring more frequently in anvils. The L – W relationships of columns derived using current data exhibited a strong dependence on temperature; similar relationships determined in previous studies were within the range of the current data.

54 ENVIRONMENTAL SCIENCES↗

Impact of aerosols on ice crystal size

The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (R ei ), which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on R ei under different meteorological conditions using 9-yearsatellite observations. We find that the responses of R ei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the “Twomey effect” for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of R ei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of R ei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol–cloud radiative forcing produced by ice clouds.

54 ENVIRONMENTAL SCIENCES↗

A Study of the Optical Properties of Ice Crystals with Black Carbon Inclusions

The report focuses on the modification of the optical properties of ice crystals due to atmospheric black carbon (BC) contamination: the objective is to advance the predictive capabilities of climate models through an improved understanding of the radiative properties of compound particles. The shape of the ice crystal (as commonly found in cirrus clouds and contrails), the volume fraction of the BC inclusion, and its location inside the crystal are the three factors examined in this study. In the multiscale description of this problem, where a small absorbing inclusion modifies the optical properties of a much larger non-absorbing particle, state-of-the-art discretization techniques are combined to provide the best compromise of flexibility and accuracy over a broad range of sizes.

54 ENVIRONMENTAL SCIENCES↗

Effect of Orientation of Ice Crystals in Cirrus on Direct and Scattered Solar Radiation Fluxes

The problem of solar radiation transfer by cirrus containing horizontally oriented ice crystals urgent today is considered. The results of a complex radiation experiment are described in which solar radiation fluxes at the Earth’s surface are measured and high-level clouds are vertically sensed by a polarization lidar. The lidar allows the full backscattering phase matrix (BSPM) to be determined. The degree of orientation of ice crystals in cirrus is estimated from the form of the BSPM elements and their interrelations. It is shown experimentally for the first time that the degree of orientation of crystalline particles in cirrus has a significant effect on the direct and scattered solar radiation fluxes arriving at the Earth’s surface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Modeling of Aircraft Measurements of Ice Crystal Concentration in the Arctic and a Parameterization for Mixed-Phase Cloud

Abstract In this study, two parameterizations of ice nucleation rate on dust particles are used in a parcel model to simulate aircraft measurements of ice crystal number concentration Ni in the Arctic. The parcel model has detailed microphysics for droplet and ice nucleation, growth, and evaporation with prescribed vertical air velocities. Three dynamic regimes are considered, including large-scale ascent, cloud-top generating cells, and their combination. With observed meteorological conditions and aerosol concentrations, the parcel model predicts the number concentrations of size-resolved ice crystals, which may be compared to aircraft measurements. Model results show rapid changes with height/time in relative humidity, Ni, and thermodynamic phase partitioning, which is not resolved in current climate and weather forecasting models. Parameterizations for ice number and nucleation rate in mixed-phase stratus clouds are thus developed based on the parcel model results to represent the time-integrated effect of some microphysical processes in large-scale models.

54 ENVIRONMENTAL SCIENCES↗