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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 OSTI2025

Physics or Knob‐Tuning? Tropical Anvil Peak Is Captured by GCMs

Tropical anvil clouds peak near 200 hPa and significantly impact Earth's climate, yet its physical realism in coarse‐resolution General Circulation Models (GCMs) remains debated. We examine anvil cloud formation by performing simulations with a GCM with a hierarchy of cloud fraction schemes ranging from a complex prognostic Tiedtke scheme to a simple binary scheme. All schemes consistently reproduce the anvil peak. The robust anvil peak arises because extremely cold temperatures at the upper troposphere facilitate frequent saturation events, producing clouds that disproportionately influence mean cloud fraction. Sensitivity experiments with enhanced evaporation of cloud condensate unexpectedly show increased anvil coverage, highlighting how slight evaporative moistening reinforces local saturation in cold upper‐tropospheric conditions. These results demonstrate that the tropical anvil cloud peak emerges from fundamental thermodynamic constraints, rather than specific cloud fraction parameterization choices.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Collective excitations of a bound-in-the-continuum condensate

Spectra of low-lying elementary excitations are critical to characterize properties of bosonic quantum fluids. Usually these spectra are difficult to observe, due to low occupation of non-condensate states compared to the ground state. Recently, low-threshold Bose-Einstein condensation was realised in a symmetry-protected bound state in the continuum, at a saddle point, thanks to coupling of this electromagnetic resonance to semiconductor excitons. While it has opened the door to long-living polariton condensates, their intrinsic collective properties are still unexplored. Here we unveil the peculiar features of the Bogoliubov spectrum of excitations in this system. Thanks to the dark nature of the bound-in-the-continuum state, collective excitations lying directly above the condensate become observable in enhanced detail. We reveal interesting aspects, such as energy-flat parts of the dispersion characterized by two parallel stripes in photoluminescence pattern, pronounced linearization at non-zero momenta in one of the directions, and a strongly anisotropic velocity of sound.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Porous condensers can double the efficiency of membrane distillation

Among membrane distillation (MD) configurations, air gap MD (AGMD) has superior energy efficiency at high salinity. However, flooding of the gap prevents optimal thin gap depths as water removal is a challenge. To address these challenges, this work provides the first analysis of efficiency enhancement via porous wicking conductive condensers in MD. To do so, we examined performance with experiments and comprehensive thermo-fluid numerical models; we find that the porous wick condenser significantly improves thermal efficiency, gain output ratio (GOR), and flux. MD experiments show that the porous copper foam improves the thermal efficiency of air gap membrane distillation up to 40 % and water flux up to 144 %. Numerical modeling shows the porous copper foam improves the GOR of membrane distillation in high salinity by 98.7 %, outperforming air gap MD, permeate gap MD, and conductive gap MD. Furthermore, the optimized thickness and permeability of porous condensers significantly help eliminate the risk of flooding in AGMD.

42 ENGINEERING↗

DOE OSTI2023

Polariton Condensation in Gap-Confined States of Photonic Crystal Waveguides

Here, the development of patterned multiquantum well heterostructures in GaAs/AlGaAs waveguides has recently made it possible to achieve exciton-polariton condensation in a topologically protected bound state in the continuum (BIC). Polariton condensation was shown to occur above a saddle point of the two-dimensional polariton dispersion in a one-dimensional photonic crystal waveguide. A rigorous analysis of the condensation phenomenon in these systems, as well as the role of the BIC, is still missing. In the present Letter, we theoretically and experimentally fill this gap by showing that polariton confinement resulting from the negative effective mass and the photonic energy gap in the dispersion play a key role in enhancing the relaxation toward the condensed state. In fact, our results show that low-threshold polariton condensation is achieved within the effective trap created by the exciting laser spot, regardless of whether the resulting confined mode is long-lived (polariton BIC) or short-lived (lossy mode). In both cases, the spatial quantization of the polariton condensate and the threshold differences associated to the corresponding state lifetime are measured and characterized. For a given negative mass, a slightly lower condensation threshold from the polariton BIC mode is found and associated to its reduced radiative losses, as compared to the lossy one.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Two-fluid model of rf current condensation in magnetic islands

The stabilization of tearing modes with rf waves is subject to a nonlinear effect, termed rf current condensation, that has the potential to greatly enhance and localize current driven within magnetic islands. Here we extend previous investigations of this effect with a two fluid model that captures the balance of diffusive and thermal equilibration processes within the island. We show that the effective power and resulting strength of the condensation effect can be greatly enhanced by avoiding collisional heat loss to the ions. The relative impact of collisions on the overall power balance within the island depends on the ratio of the characteristic diffusion timescale and the electron–ion equilibration time, rather than the latter alone. Although relative heat loss to ions increases with island size, the heating efficiency does as well. In particular, we show that the latter safely dominates for large deposition profiles, as is typically the case for lower hybrid current drive. This supports the possibility of passive stabilization of neoclassical tearing modes without the precise aiming of the rf waves required for electron cyclotron current drive stabilization.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Evaluating Scaling Effects of Steam Condensation Physics-based Model for Small Modular Reactor

This study focused on assessing condensation heat transfer (CHT) models for enhancing the passive safety of small modular reactors (SMRs). It also encompassed a review of the theoretical and semi-theoretical CHT models and correlations. Condensation models such as the degradation factor, heat and mass transfer analogy (HMTA), and boundary layer models are used to study advanced nuclear reactor PCCS. The previous CHT models were developed for small tube geometries, which differ from the containment of SMR. This study examined the scaled relations of a physics-based CHT model for analyzing laminar and turbulent film condensation downward flow conditions inside scaled tube geometries.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2023

Presentation: Evaluating scaling effects of steam condensation physics-based model for small modular reactors safety

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2021

Semi-Automated Creation of Density Functional Tight Binding Models through Leveraging Chebyshev Polynomial-Based Force Fields

Density functional tight binding (DFTB) is an attractive method for accelerated quantum simulations of condensed matter due to its enhanced computational efficiency over standard density functional theory (DFT) approaches. However, DFTB models can be challenging to determine for individual systems of interest, especially for metallic and interfacial systems where different bonding arrangements can lead to significant changes in electronic states. In this regard, we have created a rapid-screening approach for determining systematically improvable DFTB interaction potentials that can yield transferable models for a variety of conditions. Our method leverages a recent reactive molecular dynamics force field where many-body interactions are represented by linear combinations of Chebyshev polynomials. This allows for the efficient creation of multi-center representations with relative ease, requiring only a small investment in initial DFT calculations. Here, we have focused our workflow on TiH 2 as a model system and show that a relatively small training set based on unit-cell-sized calculations yields a model accurate for both bulk and surface properties. Our approach is easy to implement and can yield reliable DFTB models over a broad range of thermodynamic conditions, where physical and chemical properties can be difficult to interrogate directly and there is historically a significant reliance on theoretical approaches for interpretation and validation of experimental results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

The Impacts of Rotational Mixing on the Precipitation Simulated by a Convection Permitting Model

With increased availability of computational resources, regional and global scale convection-permitting model (CPM, Δx ~ 1–10 km) simulations are becoming more common. CPMs have improved accuracy in their representation of deep convection and mesoscale convective systems (MCSs) compared to coarser resolution models. However, CPMs still exhibit convective cloud and precipitation biases relative to observations, notably a lesser frequency of light precipitation rates and greater frequency of heavy precipitation rates. In this work we hypothesize that these CPM biases are related to under-resolved mixing between convective updrafts and their surrounding environment. To test this hypothesis, we introduce a parameterization to the Weather Research and Forecasting model (WRF) that adds a small angular rotation of the grid-scale flow about the axis perpendicular to the plane of convective drafts. This rotated flow is then allowed to alter advection of moisture and hydrometeors. The effects of such mixing on precipitation characteristics are evaluated in month-long 4-km grid spacing simulations over the Amazon. The enhanced mixing transports moisture and condensate from convective cores to other areas including downdrafts. This increases the frequency of low-precipitable water and light precipitation. It also decreases the frequency of intense precipitation from isolated deep convection and MCSs, increases cloud top temperatures, reduces radar echo-top heights, and increases overall precipitation by altering the relationship of precipitation with precipitable water, in better agreement with observations. The results suggest when optimized using multiple observations, such an approach may provide a path toward more accurate representation of convection and precipitation statistics in convection-permitting simulations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Thermal chains and entrainment in cumulus updrafts, Part 2: Analysis of idealized simulations

Research has suggested that the structure of deep convection often consists of a series of rising thermals, or “thermal chain”, which contrasts with existing conceptual models that are used to construct cumulus parameterizations. In this work, simplified theoretical expressions for updraft properties obtained in Part 1 of this study are used to develop a hypothesis explaining why this structure occurs. In this hypothesis, cumulus updraft structure is strongly influenced by organized entrainment below the updraft’s vertical velocity maximum. In a dry environment, this enhanced entrainment can locally reduce condensation rates and increase evaporation, thus eroding buoyancy. For moderate-to-large initial cloud radius R, this breaks up the updraft into a succession of discrete pulses of rising motion (i.e., a thermal chain). For small R, this leads to the structure of a single, isolated rising thermal. In contrast, moist environments are hypothesized to favor plume-like updrafts for moderate-to-large R. In a series of axisymmetric numerical cloud simulations, R and environmental relative humidity (RH) are systematically varied to test this hypothesis. Vertical profiles of fractional entrainment rate, passive tracer concentration, buoyancy, and vertical velocity from these runs agree well with vertical profiles calculated from the theoretical expressions in Part 1. Analysis of the simulations supports the hypothesized dependency of updraft structure on R and RH, that is, whether it consists of an isolated thermal, a thermal chain, or a plume, and the role of organized entrainment in driving this dependency. Additional 3-dimensional (3-D) turbulent cloud simulations are analyzed, and the behavior of these 3-D runs is qualitatively consistent with the theoretical expressions and axisymmetric simulations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Estimation of secondary organic aerosol viscosity from explicit modeling of gas-phase oxidation of isoprene and α -pinene

Abstract. Secondary organic aerosols (SOA) are major components of atmospheric fine particulate matter, affecting climate and air quality. Mounting evidence exists that SOA can adopt glassy and viscous semisolid states, impacting formation and partitioning of SOA. In this study, we apply the GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere) model to conduct explicit chemical modeling of isoprene photooxidation and α-pinene ozonolysis and their subsequent SOA formation. The detailed gas-phase chemical schemes from GECKO-A are implemented into a box model and coupled to our recently developed glass transition temperature parameterizations, allowing us to predict SOA viscosity. The effects of chemical composition, relative humidity, mass loadings and mass accommodation on particle viscosity are investigated in comparison with measurements of SOA viscosity. The simulated viscosity of isoprene SOA agrees well with viscosity measurements as a function of relative humidity, while the model underestimates viscosity of α-pinene SOA by a few orders of magnitude. This difference may be due to missing processes in the model, including autoxidation and particle-phase reactions, leading to the formation of high-molar-mass compounds that would increase particle viscosity. Additional simulations imply that kinetic limitations of bulk diffusion and reduction in mass accommodation coefficient may play a role in enhancing particle viscosity by suppressing condensation of semi-volatile compounds. The developed model is a useful tool for analysis and investigation of the interplay among gas-phase reactions, particle chemical composition and SOA phase state.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Aerosol Hygroscopic Growth, Mixing State, and Cloud Condensation Nuclei Activity during TRACER (Field Campaign Report)

Convective clouds play a critical role in the Earth’s climate system. Recent research has shown that a realistic representation of convective processes is critical to constraining climate sensitivity in global climate models. Theoretical and modeling studies showed that aerosols could have strong dynamic feedback to convection in warm and humid environments through enhancing ice-related processes and condensational growth. A few observation-based studies also suggested the influence of aerosols on convective cloud and precipitation properties. However, robust observational quantification of an aerosol effect on convective clouds isolated from other factors remains elusive. Understanding the impact of aerosol on convective clouds requires knowledge of the cloud condensation nuclei (CCN) spectrum, which represents the number of particles that uptake water and form cloud droplets as a function of supersaturation. The water uptake by aerosol is also of critical importance for the direct interaction of aerosol with radiation (i.e., aerosol direct effect) due to light scattering and absorption by aerosol. While both droplet activation under supersaturated conditions (i.e., relative humidity RH > 100%) and the hygroscopic growth under sub-saturated conditions (i.e., RH < 100%) are strongly influenced by particle hygroscopicity, the thermodynamic regimes and measurement methods are quite different. Aerosol particles, especially organic particles, can exhibit higher hygroscopicity for droplet activation than that for hygroscopic growth. In the subsaturated regime, the hygroscopicity of organic particles can also vary strongly with RH. However, global climate models usually treat organic species in aerosols with a constant hygroscopicity, potentially introducing substantial uncertainties in the quantification of aerosol radiative effects.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Effect of inversion asymmetry on the superconducting and exciton condensates of bilayer graphene

Inversion asymmetry in bilayer graphene can be tuned by the displacement field. As a result, the band dispersion in biased bilayer graphene acquires flatband regions near the Dirac points along with a nontrivial band geometry. We analyze the effect of inversion asymmetry on the critical temperature and superfluid stiffness of the superconducting state of AB-stacked graphene bilayer and the exciton condensate in double layers formed by two AB-stacked graphene bilayers. We find that the geometric superfluid stiffness in bilayer graphene superconductors is negligible due to the small superconducting gap. Furthermore, since the geometric superfluid stiffness is maximized for a constant order parameter, it can be neglected in biased bilayer graphene superconductors with any pairing symmetry. In contrast, the displacement field enhances the geometric superfluid stiffness in exciton condensates. It is most prominent at low densities and high displacement fields. Here, a consequence of the geometric superfluid stiffness is a modest enhancement of the Berezinskii-Kosterlitz-Thouless transition temperature in bilayer graphene’s exciton condensate.

BKT transition↗

DOE OSTI2021

Incorporation and Assembly of a Light-Emitting Enzymatic Reaction into Model Protein Condensates

Eukaryotic cells partition enzymes and other cellular components into distinct subcellular compartments to generate specialized biochemical niches. A subclass of these compartments form in the absence of lipid membranes, via liquid-liquid phase separation of proteins to form biomolecular condensates or “membraneless organelles” such as nucleoli, stress granules, and P-bodies. Because of their ability to form compartments from simple starting materials, membraneless organelles are an attractive target for engineering new functionalities in both living cells and protocells. In this work, we demonstrate incorporation of novel enzymatic activity in protein coacervates with a light-generating enzyme, NanoLuc, to produce bioluminescence. Using condensates comprised of the disordered RGG domain of C. elegans LAF-1, we show functionalization of condensates with enzymatic activity in vitro and that localization to protein coacervates enhances the assembly and activity of split enzymes. To build condensates that function as light emitting reactors, we designed a NanoLuc enzyme flanked by RGG domains. Furthermore, the resulting condensates concentrated NanoLuc by 10-fold over bulk solution and display significantly increased net reaction rates. We further show that condensate viscosity impacts light emission due to diffusion-limited behavior. By splitting NanoLuc enzyme into its constituent components, we demonstrate that NanoLuc activity can be reconstituted via co-condensation. Further, we demonstrate control of the spatial localization of enzyme within condensates by targettng NanoLuc to the surface of in vitro condensates. Collectively, this work demonstrates that membraneless organelles can be endowed with localized enzymatic activity, and that this activity can be spatially and temporally controlled via enzyme reconstitution and design of protein surfactants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Cloud response to co-condensation of water and organic vapors over the boreal forest

Abstract. Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance the number of aerosol particles that activate to form cloud droplets. The boreal forest is an important source of biogenic organic vapors, but the role of these vapors in co-condensation has not been systematically investigated. In this work, the environmental conditions under which strong co-condensation-driven cloud droplet number enhancements would be expected over the boreal biome are identified. Recent measurement technology, specifically the Filter Inlet for Gases and AEROsols (FIGAERO) coupled to an iodide-adduct chemical ionization mass spectrometer (I-CIMS), is utilized to construct volatility distributions of the boreal atmospheric organics. Then, a suite of CPM simulations initialized with a comprehensive set of concurrent aerosol observations collected in the boreal forest of Finland during spring 2014 is performed. The degree to which co-condensation impacts droplet formation in the model is shown to be dependent on the initialization of temperature, relative humidity, updraft velocity, aerosol size distribution, organic vapor concentration, and the volatility distribution. The predicted median enhancements in cloud droplet number concentration (CDNC) due to accounting for the co-condensation of water and organics fall on average between 16 % and 22 %. This corresponds to activating particles 10–16 nm smaller in dry diameter that would otherwise remain as interstitial aerosol. The highest CDNC enhancements (ΔCDNC) are predicted in the presence of a nascent ultrafine aerosol mode with a geometric mean diameter of ∼ 40 nm and no clear Hoppel minimum, indicative of pristine environments with a source of ultrafine particles (e.g., via new particle formation processes). Such aerosol size distributions are observed 30 %–40 % of the time in the studied boreal forest environment in spring and fall when new particle formation frequency is the highest. To evaluate the frequencies with which such distributions are experienced by an Earth system model over the whole boreal biome, 5 years of UK Earth System Model (UKESM1) simulations are further used. The frequencies are substantially lower than those observed at the boreal forest measurement site (< 6 % of the time), and the positive values, peaking in spring, are modeled only over Fennoscandia and the western parts of Siberia. Overall, the similarities in the size distributions between observed and modeled (UKESM1) are limited, which would limit the ability of this model, or any model with a similar aerosol representation, to project the climate relevance of co-condensation over the boreal forest. For the critical aerosol size distribution regime, ΔCDNC is shown to be sensitive to the concentrations of semi-volatile and some intermediate-volatility organic compounds (SVOCs and IVOCs), especially when the overall particle surface area is low. The magnitudes of ΔCDNC remain less affected by the more volatile vapors such as formic acid and extremely low- and low-volatility organic compounds (ELVOCs and LVOCs). The reasons for this are that most volatile organic vapors condense inefficiently due to their high volatility below the cloud base, and the concentrations of LVOCs and ELVOCs are too low to gain significant concentrations of soluble mass to reduce the critical supersaturations enough for droplet activation to occur. A reduction in the critical supersaturation caused by organic condensation emerges as the main driver of the modeled ΔCDNC. The results highlight the potential significance of co-condensation in pristine boreal environments close to sources of fresh ultrafine particles. For accurate predictions of co-condensation effects on CDNC, also in larger-scale models, an accurate representation of the aerosol size distribution is critical. Further studies targeted at finding observational evidence and constraints for co-condensation in the field are encouraged.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Multistage Surface-Heated Vacuum Membrane Distillation Process Enables High Water Recovery and Excellent Heat Utilization: A Modeling Study

Surface-heated membrane distillation (MD) enhances the energy efficiency of desalination by mitigating temperature polarization (TP). However, systematic investigations of larger scale, multistage, surface-heated MD system with high water recovery and heat recycling are limited. Here, we explore the design and performance of a multistage surface-heated vacuum MD (SHVMD) with heat recovery through a comprehensive finite difference model. In this process, the latent heat of condensation is recovered through an internal heat exchanger (HX) using the retentate from one stage as the condensing fluid for the next stage and an external HX using the feed as the condensing fluid. Model results show that surface heating enhances the performance compared to conventional vacuum MD (VMD). Specifically, in a six-stage SHVMD process, 54.44% water recovery and a gained output ratio (GOR) of 3.28 are achieved with a surface heat density of 2000 W m –2 , whereas a similar six-stage VMD process only reaches 18.19% water recovery and a GOR of 2.15. Mass and energy balances suggest that by mitigating TP, surface heating increases the latent heat trapped in vapor. The internal and external HXs capture and reuse the additional heat, which enhances the GOR values. We show for SHVMD that the hybrid internal/external heat recovery design can have GOR value 1.44 times higher than that of systems with only internal or external heat recovery. Furthermore, by only increasing six stages to eight stages, a GOR value as high as 4.35 is achieved. The results further show that surface heating can reduce the energy consumption of MD for brine concentration. As a result, the multistage SHVMD technology exhibits a promising potential for the management of brine from industrial plants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Characteristics and effects of aerosols during blowing snow events in the central Arctic

Sea salt aerosol (SSaer) significantly impacts aerosol-radiation and aerosol-cloud interactions, and sublimated blowing snow is hypothesized to be an important SSaer source in polar regions. Understanding blowing snow and other wind-sourced aerosols’ climate relevant properties is needed, especially during winter when Arctic amplification is greatest. However, most of our understanding of blowing snow SSaer comes from modeling studies, and direct observations are sparse. Additionally, SSaer can originate from multiple sources, making it difficult to disentangle emission processes. Here, we present comprehensive observations of wind-sourced aerosol during blowing snow events from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition in the central Arctic. High wind speed strongly enhances total aerosol number, submicron sodium chloride mass, cloud condensation nuclei concentrations, and scattering coefficients. Generally, the relative response of aerosol properties to wind speed enhancement is strongest in fall when Arctic aerosol concentrations are lowest. Blowing snow events showed similar aerosol and environmental properties across events, apart from occasions with high snow age (>6 days since last snowfall). Coarse-mode number concentrations (>1 μm) are better explained by variability in wind speed averaged over 12-h air mass back trajectories arriving at the MOSAiC site compared to local, instantaneous wind speed, suggesting the importance of regional transport and consideration of air mass history for wind-driven aerosol production. These MOSAiC observations provide new insights into wind-driven aerosol in the central Arctic and may help validate modeling studies and improve model parameterizations particularly for aerosol direct and indirect radiative forcing.

54 ENVIRONMENTAL SCIENCES↗