Use In Atmospheric Models Research Articles

Effect of secondary ice production processes on the simulation of ice pellets using the Predicted Particle Properties microphysics scheme

Abstract. Ice pellets can form when supercooled raindrops collide with small ice particles that can be generated through secondary ice production processes. The use of atmospheric models that neglect these collisions can lead to an overestimation of freezing rain. The objective of this study is therefore to understand the impacts of collisional freezing and secondary ice production on simulations of ice pellets and freezing rain. We studied the properties of precipitation simulated with the Predicted Particle Properties (P3) microphysics scheme for two distinct secondary ice production processes. Improvements to the representation of ice pellets and ice crystals in P3 were analyzed by simulating an ice pellet storm that occurred over eastern Canada in January 2020. Those simulations showed that adding secondary ice production processes increased the accumulation of ice pellets but led to unrealistic size distributions of precipitation particles. Realistic size distributions of ice pellets were obtained by modifying the collection of raindrops by small ice particles and the merging criteria of ice categories in P3.

Cloudiness Parameterization for Use in Atmospheric Models: A Review and New Perspectives

In atmospheric models, the representation of cloudiness is a direct linkage between the moisture amount and associated radiative forcing. This paper begins by providing a review of the parameterization of cloudiness that has been used for numerical weather predictions and climate studies. The inherent uncertainties in representing a partial fraction of clouds for radiation feedback and in evaluating it against the corresponding observations are focused. It is also stated that the major hydrometeor categories of water substances such as cloud ice and water that are responsible for cloud cover are readily available in modern weather and climate models. Inconsistencies in cloud cover and hydrometeors, even in the case of the prognostic method, are discussed. The compensating effect of cloudiness for radiative feedback is found to imply that the condensed water amount itself is more influential on the radiative forcing, rather than the accuracy of the cloudiness. Based on the above perspectives, an alternative diagnostic parameterization method is proposed, utilizing a monotonic relation between the cloud water amounts and cloudiness that are obtained from aircraft and satellite observations. The basic premise of this approach lies in the accuracy of the water substance in the models, indicating that future efforts need to be given to improvements in physical processes concerning hydrometeor properties for the accurate representation of cloud radiative feedback.

Characterising the vertical structure of buildings in cities for use in atmospheric models

Urban schemes for numerical weather prediction (NWP) often assume an infinite street canyon with constant height and width, impacting turbulent and radiative fluxes. We develop parameterisations for urban morphology profiles, with five complexity levels, using data from six cities at 2 km × 2 km resolution. Comparisons of parameterised building plan area to these ‘true’ data show that 90% of building fraction profiles have bias errors (BE) at any height of <0.03. An effective building diameter (D) is used to characterise the proportionality between building plan area and building normalised perimeter length. The six-city mean D is 21 m. Relations for D have normalised BE (nBE) < 16%, increasing to 26% when total wall area is assumed to be unknown. Impacts from using these new morphology relations are tested with SPARTACUS-Urban radiative transfer simulations. The effective shortwave albedo has a nBE 2–10% (cf. ‘true’). Within-canyon absorption have larger nBEs, suggesting the bulk albedo hides within-canopy errors. Overall, nBE increase as less morphology data are provided, notably when omitting total wall area. We conclude that urban vertical variability using the proposed relations are acceptable for NWP, requiring only: surface building plan area, mean building height, and effective building diameter.

Unimolecular Kinetics of Stabilized CH3CHOO Criegee Intermediates: syn-CH3CHOO Decomposition and anti-CH3CHOO Isomerization.

The kinetics of the unimolecular decomposition of the stabilized Criegee intermediate syn-CH3CHOO has been investigated at temperatures between 297 and 331 K and pressures between 12 and 300 Torr using laser flash photolysis of CH3CHI2/O2/N2 gas mixtures coupled with time-resolved broadband UV absorption spectroscopy. Fits to experimental results using the Master Equation Solver for Multi-Energy well Reactions (MESMER) indicate that the barrier height to decomposition is 67.2 ± 1.3 kJ mol–1 and that there is a strong tunneling component to the decomposition reaction under atmospheric conditions. At 298 K and 760 Torr, MESMER simulations indicate a rate coefficient of 150–81+176 s–1 when tunneling effects are included but only 5–2+3 s–1 when tunneling is not considered in the model. MESMER simulations were also performed for the unimolecular isomerization of the stabilized Criegee intermediate anti-CH3CHOO to methyldioxirane, indicating a rate coefficient of 54–21+34 s–1 at 298 K and 760 Torr, which is not impacted by tunneling effects. Expressions to describe the unimolecular kinetics of syn- and anti-CH3CHOO are provided for use in atmospheric models, and atmospheric implications are discussed.

Process-Level Modeling Can Simultaneously Explain Secondary Organic Aerosol Evolution in Chambers and Flow Reactors

Secondary organic aerosol (SOA) data gathered in environmental chambers (ECs) have been used extensively to develop parameters to represent SOA formation and evolution. The EC-based parameters are usually constrained to less than one day of photochemical aging but extrapolated to predict SOA aging over much longer timescales in atmospheric models. Recently, SOA has been increasingly studied in oxidation flow reactors (OFRs) over aging timescales of one to multiple days. However, these OFR data have been rarely used to validate or update the EC-based parameters. The simultaneous use of EC and OFR data is challenging because the processes relevant to SOA formation and evolution proceed over very different timescales, and both reactor types exhibit distinct experimental artifacts. In this work, we show that a kinetic SOA chemistry and microphysics model that accounts for various processes, including wall losses, aerosol phase state, heterogeneous oxidation, oligomerization, and new particle formation, can simultaneously explain SOA evolution in EC and OFR experiments, using a single consistent set of SOA parameters. With α-pinene as an example, we first developed parameters by fitting the model output to the measured SOA mass concentration and oxygen-to-carbon (O:C) ratio from an EC experiment (<1 day of aging). We then used these parameters to simulate SOA formation in OFR experiments and found that the model overestimated SOA formation (by a factor of 3-16) over photochemical ages ranging from 0.4 to 13 days, when excluding the abovementioned processes. By comprehensively accounting for these processes, the model was able to explain the observed evolution in SOA mass, composition (i.e., O:C), and size distribution in the OFR experiments. This work suggests that EC and OFR SOA data can be modeled consistently, and a synergistic use of EC and OFR data can aid in developing more refined SOA parameters for use in atmospheric models.

The Mega-MUSCLES Spectral Energy Distribution of TRAPPIST-1

Abstract We present a 5 Å–100 μm spectral energy distribution (SED) of the ultracool dwarf star TRAPPIST-1, obtained as part of the Mega-MUSCLES Treasury Survey. The SED combines ultraviolet and blue-optical spectroscopy obtained with the Hubble Space Telescope, X-ray spectroscopy obtained with XMM-Newton, and models of the stellar photosphere, chromosphere, transition region, and corona. A new differential emission measure model of the unobserved extreme-ultraviolet spectrum is provided, improving on the Lyα–EUV relations often used to estimate the 100–911 Å flux from low-mass stars. We describe the observations and models used, as well as the recipe for combining them into an SED. We also provide a semiempirical, noise-free model of the stellar ultraviolet spectrum based on our observations for use in atmospheric modeling of the TRAPPIST-1 planets.

Use of Atmospheric Models to Survey Wind Potential, a Case Study for Alegria I Wind Park, Guamare/Rn

The current Brazilian energy matrix is configured in hydrothermal generation capable of serving the entire territory, however, the extensive availability of renewable sources denotes a high advantage for exploration due to the reduced emission of greenhouse gases. The numerical modeling involved in the wind survey consolidates the efficiency of computational tools in exploring areas with potential for installing wind turbines. Thus, the validation of the WRF mesoscale model occurred through data from the meteorological station of INMET in the city of Natal/RN, owing to the similarity regarding the relief of Guamare/RN, in which the Alegria I wind farm is located. The meteorological variables used were: wind speed and direction, and statistical parameters: mean, standard deviation, correlation coefficient, Root Mean Square Error (RMSE) and Bias. The WAsP allowed the estimation of the annual energy production of 150.771MWh from the Alegria I wind farm, as well as the evaluation of belt losses caused by turbulence due to the high number of wind turbines.

Adaptation of the Predicted Particles Properties (P3) Microphysics Scheme for Large-Scale Numerical Weather Prediction

AbstractA parameterization for the subgrid-scale cloud and precipitation fractions has been incorporated into the Predicted Particle Properties (P3) microphysics scheme for use in atmospheric models with relatively coarse horizontal resolution. The modified scheme was tested in a simple 1D kinematic model and in the Canadian Global Environmental Multiscale (GEM) model using an operational global NWP configuration with a 25-km grid spacing. A series of 5-day forecast simulations was run using P3 and the much simpler operational Sundqvist condensation scheme as a benchmark for comparison. The effects of using P3 in a global GEM configuration, with and without the modifications, were explored through statistical metrics of common forecast fields against upper-air and surface observations. Diagnostics of state variable tendencies from various physics parameterizations were examined to identify possible sources of errors resulting from the use of the modified scheme. Sensitivity tests were performed on the coupling between the deep convection parameterization scheme and the microphysics, specifically regarding assumptions in the physical properties of detrained ice. It was found that even without recalibration of the suite of moist physical parameterizations, substituting the Sundqvist condensation scheme with the modified P3 microphysics resulted in some significant improvements to the temperature and geopotential height bias throughout the troposphere and out to day 5, but with degradation to error standard deviation toward the end of the integrations, as well as an increase in the positive bias of precipitation quantities. The modified P3 scheme was thus shown to hold promise for potential use in coarse-resolution NWP systems.

Errors and uncertainties in a gridded carbon dioxide emissions inventory

Emission inventories (EIs) are the fundamental tool to monitor compliance with greenhouse gas (GHG) emissions and emission reduction commitments. Inventory accounting guidelines provide the best practices to help EI compilers across different countries and regions make comparable, national emission estimates regardless of differences in data availability. However, there are a variety of sources of error and uncertainty that originate beyond what the inventory guidelines can define. Spatially explicit EIs, which are a key product for atmospheric modeling applications, are often developed for research purposes and there are no specific guidelines to achieve spatial emission estimates. The errors and uncertainties associated with the spatial estimates are unique to the approaches employed and are often difficult to assess. This study compares the global, high-resolution (1 km), fossil fuel, carbon dioxide (CO2), gridded EI Open-source Data Inventory for Anthropogenic CO2 (ODIAC) with the multi-resolution, spatially explicit bottom-up EI geoinformation technologies, spatio-temporal approaches, and full carbon account for improving the accuracy of GHG inventories (GESAPU) over the domain of Poland. By taking full advantage of the data granularity that bottom-up EI offers, this study characterized the potential biases in spatial disaggregation by emission sector (point and non-point emissions) across different scales (national, subnational/regional, and urban policy-relevant scales) and identified the root causes. While two EIs are in agreement in total and sectoral emissions (2.2% for the total emissions), the emission spatial patterns showed large differences (10~100% relative differences at 1 km) especially at the urban-rural transitioning areas (90–100%). We however found that the agreement of emissions over urban areas is surprisingly good compared with the estimates previously reported for US cities. This paper also discusses the use of spatially explicit EIs for climate mitigation applications beyond the common use in atmospheric modeling. We conclude with a discussion of current and future challenges of EIs in support of successful implementation of GHG emission monitoring and mitigation activity under the Paris Climate Agreement from the United Nations Framework Convention on Climate Change (UNFCCC) 21st Conference of the Parties (COP21). We highlight the importance of capacity building for EI development and coordinated research efforts of EI, atmospheric observations, and modeling to overcome the challenges.

Developing and bounding ice particle mass- and area-dimension expressions for use in atmospheric models and remote sensing

Abstract. Ice particle mass- and projected area-dimension (m-D and A-D) power laws are commonly used in the treatment of ice cloud microphysical and optical properties and the remote sensing of ice cloud properties. Although there has long been evidence that a single m-D or A-D power law is often not valid over all ice particle sizes, few studies have addressed this fact. This study develops self-consistent m-D and A-D expressions that are not power laws but can easily be reduced to power laws for the ice particle size (maximum dimension or D) range of interest, and they are valid over a much larger D range than power laws. This was done by combining ground measurements of individual ice particle m and D formed at temperature T &lt; −20 °C during a cloud seeding field campaign with 2-D stereo (2D-S) and cloud particle imager (CPI) probe measurements of D and A, and estimates of m, in synoptic and anvil ice clouds at similar temperatures. The resulting m-D and A-D expressions are functions of temperature and cloud type (synoptic vs. anvil), and are in good agreement with m-D power laws developed from recent field studies considering the same temperature range (−60 °C &lt; T &lt; −20 °C).

Glyoxal and Methylglyoxal Setschenow Salting Constants in Sulfate, Nitrate, and Chloride Solutions: Measurements and Gibbs Energies.

Knowledge about Setschenow salting constants, KS, the exponential dependence of Henry's Law coefficients on salt concentration, is of particular importance to predict secondary organic aerosol (SOA) formation from soluble species in atmospheric waters with high salt concentrations, such as aerosols. We have measured KS of glyoxal and methylglyoxal for the atmospherically relevant salts (NH4)2SO4, NH4NO3, NaNO3, and NaCl and find that glyoxal consistently "salts-in" (KS of -0.16, -0.06, -0.065, -0.1 molality(-1), respectively) while methylglyoxal "salts-out" (KS of +0.16, +0.075, +0.02, +0.06 molality(-1)). We show that KS values for different salts are additive and present an equation for use in atmospheric models. Additionally, we have performed a series of quantum chemical calculations to determine the interactions between glyoxal/methylglyoxal monohydrate with Cl(-), NO3(-), SO4(2-), Na(+), and NH4(+) and find Gibbs free energies of water displacement of -10.9, -22.0, -22.9, 2.09, and 1.2 kJ/mol for glyoxal monohydrate and -3.1, -10.3, -7.91, 6.11, and 1.6 kJ/mol for methylglyoxal monohydrate with uncertainties of 8 kJ/mol. The quantum chemical calculations support that SO4(2-), NO3(-), and Cl(-) modify partitioning, while cations do not. Other factors such as ion charge or partitioning volume effects likely need to be considered to fully explain salting effects.

Generalizing Cloud Overlap Treatment to Include the Effect of Wind Shear

Abstract Six months of CloudSat and CALIPSO observations have been divided into over 8 million cloud scenes and collocated with ECMWF wind analyses to identify an empirical relationship between cloud overlap and wind shear for use in atmospheric models. For vertically continuous cloudy layers, cloud decorrelates from maximum toward random overlap as the layer separation distance increases, and the authors demonstrate a systematic impact of wind shear on the resulting decorrelation length scale. As expected, cloud decorrelates over smaller distances as wind shear increases. A simple, empirical linear fit parameterization is suggested that is straightforward to add to existing radiation schemes, although it is shown that the parameters are quite sensitive to the processing details of the cloud mask data and also to the fitting method used. The wind shear–overlap dependency is implemented in the radiation scheme of the ECMWF Integrated Forecast System. It has a similar-magnitude impact on the radiative budget as that of switching from a fixed decorrelation length scale to the latitude-dependent length scale presently used in the operational model, altering the zonal-mean, top-of-atmosphere, equator-to-midlatitude gradient of shortwave radiation by approximately 2 W m−2.

An intercomparison study between RAMS and CRES-Flow-NS models and evaluation with wind tunnel experimental data: Toward improving atmospheric modeling for wind resource assessment

The use of atmospheric models for wind resource assessment in complex terrain is limited by their coarse resolution. Using non-hydrostatic mesoscale models such as RAMS, fine resolution grids and a proper turbulent closure scheme such as the k–ε, it is theoretically possible to describe orographic shear-induced turbulence at microscale level with certain accuracy. In such cases, microscale CFD models modified to represent the interaction of the atmospheric boundary layer with the local orography are proven to show accurate results in idealized cases such as neutral stratification. On the other hand, their limitation in representing real atmospheric interaction between large scale structures and thermal stratification with the flow pattern can introduce significant errors in evaluating wind energy potential. In this work, proper modifications of the RAMS model were performed to simulate 2D wind flow over an isolated hill at high resolution configuration. The results have been compared with the CFD model CRES-Flow-NS and with wind tunnel experimental data. It is found that RAMS is able to reproduce basic flow features with comparable accuracy as the CFD model. This work is part of a major effort to make RAMS a reliable tool for atmospheric flow simulations of various complexity.

CBrF3 (Halon-1301): UV absorption spectrum between 210 and 320K, atmospheric lifetime, and ozone depletion potential

• CBrF 3 (Halon-1301) UV absorption spectrum measurement. • Evaluation of the absorption spectrum temperature dependence. • Reduced uncertainty in the model calculated Halon-1301 atmospheric lifetime and ozone depletion potential. CBrF 3 (Halon-1301) is a man-made ozone depleting substance that is a major source of bromine in the Earth’s stratosphere. Halon-1301 is predominantly removed from the atmosphere by UV photolysis in the stratosphere at wavelengths between 200 and 225 nm. The existing level of uncertainty in the Halon-1301 UV absorption spectrum temperature-dependence directly impacts the ability to model stratospheric ozone chemistry and climate change. In this work, the UV absorption spectrum of Halon-1301 between 195 and 235 nm was measured over the temperature range 210–320 K. An empirical parameterization of the spectrum and its temperature dependence is presented. The present results are critically compared with results from previous studies and the current recommendation for use in atmospheric models. A global annually averaged lifetime for Halon-1301 of 74.6 (73.7–75.5) years was calculated using a 2-D atmospheric model and the present results. The range of lifetimes given in parenthesis represents the possible values due solely to the 2 σ uncertainty in the Halon-1301 UV spectrum obtained in this work. In addition, the CBrF 3 ozone depletion potential was calculated using the 2-D model to be 18.6 (±0.1) using the UV spectrum and 2 σ uncertainty from this work.

Atmospheric chemistry of enols: a theoretical study of the vinyl alcohol + OH + O(2) reaction mechanism.

Enols are emerging as trace atmospheric components that may play a significant role in the formation of organic acids in the atmosphere. We have investigated the hydroxyl radical ((•)OH) initiated oxidation chemistry of the simplest enol, vinyl alcohol (ethenol, CH2═CHOH), using quantum chemical calculations and energy-grained master equation simulations. A lifetime of around 4 h was determined for vinyl alcohol in the presence of tropospheric levels of (•)OH. The reaction proceeds by (•)OH addition at both the α (66%) and β (33%) carbons of the π-system, yielding the C-centered radicals (•)CH2CH(OH)2, and HOCH2C(•)HOH, respectively. Subsequent trapping by O2 leads to the respective peroxyl radicals. About 90% of the chemically activated population of the major peroxyl radical adduct (•)O2CH2CH(OH)2 is predicted to undergo fragmentation to produce formic acid and formaldehyde, with regeneration of (•)OH. The minor peroxyl radical HOCH2C(OO(•))HOH is even less stable and undergoes almost exclusive HO2(•) elimination to form glycolaldehyde (HOCH2CHO). Formation of the latter has not been proposed before in the oxidation of vinyl alcohol. A kinetic mechanism for use in atmospheric modeling is provided, featuring phenomenological rate coefficients for formation of the three main product channels ((•)O2CH2CH(OH)2 [8%]; HC(O)OH + HCHO + (•)OH [56%]; HOCH2CHO + HO2(•) [37%]). Our study supports previous findings that vinyl alcohol should be rapidly removed from the atmosphere by reaction with (•)OH and O2 with glycolaldehyde being identified as a previously unconsidered product. Most importantly, it is shown that direct chemically activated reactions can lead to (•)OH and HO2(•) (HOx) recycling.

Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol

Secondary organic aerosol (SOA) constitutes a major fraction of submicrometer atmospheric particulate matter. Quantitative simulation of SOA within air-quality and climate models--and its resulting impacts--depends on the translation of SOA formation observed in laboratory chambers into robust parameterizations. Worldwide data have been accumulating indicating that model predictions of SOA are substantially lower than ambient observations. Although possible explanations for this mismatch have been advanced, none has addressed the laboratory chamber data themselves. Losses of particles to the walls of chambers are routinely accounted for, but there has been little evaluation of the effects on SOA formation of losses of semivolatile vapors to chamber walls. Here, we experimentally demonstrate that such vapor losses can lead to substantially underestimated SOA formation, by factors as much as 4. Accounting for such losses has the clear potential to bring model predictions and observations of organic aerosol levels into much closer agreement.

The very short-lived ozone depleting substance CHBr&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; (bromoform): revised UV absorption spectrum, atmospheric lifetime and ozone depletion potential

Abstract. CHBr3 (bromoform) is a short-lived atmospheric trace compound that is primarily of natural origin and is a source of reactive bromine in both the troposphere and stratosphere. Estimating the overall atmospheric impact of CHBr3 and its transport to the stratosphere requires a thorough understanding of its atmospheric loss processes, which are primarily UV photolysis and reaction with the OH radical. In this study, UV absorption cross sections, σ (λ ,T), for CHBr3 were measured at wavelengths between 300 and 345 nm at temperatures between 260 and 330 K using cavity ring-down spectroscopy. The present results are compared with currently recommended values for use in atmospheric models, and the discrepancies are discussed. A parameterization of the CHBr3 UV spectrum for use in atmospheric models is developed, and illustrative photolysis rate calculations are presented to highlight the impact of the revised σ (λ, T) values on its calculated local lifetimes. For example, the photolysis rate in the tropical region obtained with the present spectral data is 10–15% lower (longer lifetime) than obtained using currently recommended cross section values. Seasonally dependent ozone depletion potentials (ODPs) for CHBr3 emitted in the Indian sub-continent were calculated to be 0.10, 0.34, 0.72, and 0.23 (winter, spring, summer, fall) using the semi-empirical relationship of Brioude et al. (2010).

On the use of exponential time integration methods in atmospheric models

Exponential integration methods offer a highly accurate approach to the time integration of large systems of differential equations. In recent years, they have attracted increased attention in a number of diverse fields due to advances in their computational efficiency. This has been as a result of the use of Krylov subspace methods for the approximation of the matrix exponentials which typically arise. In this work, we investigate the potential of exponential integration methods for use in atmospheric models. Two schemes are implemented in a shallow water model and tested against reference explicit and semi-implicit methods. In a number of experiments with standard test cases, the exponential methods are found to yield very accurate solutions with time-steps far longer than even the semi-implicit method allows. The relative efficiency of the exponential integrators, which depends mainly on the choice of the specific algorithm used for the calculation of the matrix exponent, is also discussed. The future work aimed at further improvements of the proposed methodology is outlined.

1,2-Dichlorohexafluoro-cyclobutane (1,2-c-C4F6Cl2, R-316c) a Potent Ozone Depleting Substance and Greenhouse Gas: Atmospheric Loss Processes, Lifetimes, and Ozone Depletion and Global Warming Potentials for the (E) and (Z) Stereoisomers

The atmospheric processing of (E)- and (Z)-1,2-dichlorohexafluoro-cyclobutane (1,2-c-C4F6Cl2, R-316c) was examined in this work as the ozone depleting (ODP) and global warming (GWP) potentials of this proposed replacement compound are presently unknown. The predominant atmospheric loss processes and infrared absorption spectra of the R-316c isomers were measured to provide a basis to evaluate their atmospheric lifetimes and, thus, ODPs and GWPs. UV absorption spectra were measured between 184.95 to 230 nm at temperatures between 214 and 296 K and a parametrization for use in atmospheric modeling is presented. The Cl atom quantum yield in the 193 nm photolysis of R-316c was measured to be 1.90 ± 0.27. Hexafluorocyclobutene (c-C4F6) was determined to be a photolysis co-product with molar yields of 0.7 and 1.0 (±10%) for (E)- and (Z)-R-316c, respectively. The 296 K total rate coefficient for the O((1)D) + R-316c reaction, i.e., O((1)D) loss, was measured to be (1.56 ± 0.11) × 10(-10) cm(3) molecule(-1) s(-1) and the reactive rate coefficient, i.e., R-316c loss, was measured to be (1.36 ± 0.20) × 10(-10) cm(3) molecule(-1) s(-1) corresponding to a ~88% reactive yield. Rate coefficient upper-limits for the OH and O3 reaction with R-316c were determined to be <2.3 × 10(-17) and <2.0 × 10(-22) cm(3) molecule(-1) s(-1), respectively, at 296 K. The quoted uncertainty limits are 2σ and include estimated systematic errors. Local and global annually averaged lifetimes for the (E)- and (Z)-R-316c isomers were calculated using a 2-D atmospheric model to be 74.6 ± 3 and 114.1 ± 10 years, respectively, where the estimated uncertainties are due solely to the uncertainty in the UV absorption spectra. Stratospheric photolysis is the predominant atmospheric loss process for both isomers with the O((1)D) reaction making a minor, ~2% for the (E) isomer and 7% for the (Z) isomer, contribution to the total atmospheric loss. Ozone depletion potentials for (E)- and (Z)-R-316c were calculated using the 2-D model to be 0.46 and 0.54, respectively. Infrared absorption spectra for (E)- and (Z)-R-316c were measured at 296 K and used to estimate their radiative efficiencies (REs) and GWPs; 100-year time-horizon GWPs of 4160 and 5400 were obtained for (E)- and (Z)-R-316c, respectively. Both isomers of R-316c are shown in this work to be long-lived ozone depleting substances and potent greenhouse gases.

CFCl3 (CFC‐11): UV absorption spectrum temperature dependence measurements and the impact on its atmospheric lifetime and uncertainty

AbstractCFCl3 (CFC‐11) is both an atmospheric ozone‐depleting and potent greenhouse gas that is removed primarily via stratospheric UV photolysis. Uncertainty in the temperature dependence of its UV absorption spectrum is a significant contributing factor to the overall uncertainty in its global lifetime and, thus, model calculations of stratospheric ozone recovery and climate change. In this work, the CFC‐11 UV absorption spectrum was measured over a range of wavelength (184.95–230 nm) and temperature (216–296 K). We report a spectrum temperature dependence that is less than that currently recommended for use in atmospheric models. The impact on its atmospheric lifetime was quantified using a 2‐D model and the spectrum parameterization developed in this work. The calculated global annually averaged lifetime was 58.1 ± 0.7 years (2σ uncertainty due solely to the spectrum uncertainty). The lifetime is slightly reduced and the uncertainty significantly reduced from that obtained using current UV spectrum recommendations.