scholarly journals Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn

2009 ◽  
Vol 9 (1) ◽  
pp. 991-1049 ◽  
Author(s):  
P. Martinerie ◽  
E. Nourtier-Mazauric ◽  
J.-M. Barnola ◽  
W. T. Sturges ◽  
D. R. Worton ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Numerical Models ◽  
Atmospheric Model ◽  
Calculated Concentration ◽  
Low Concentrations ◽  
Radiative Model ◽  
Green Function Approach ◽  
Atmospheric Concentrations ◽  
Depth Concentration

Abstract. The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are insignificant. Our results indicate that the emissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6 are well constrained, whereas it is not the case for CFC-114 and CCl4. Significant emission-dependent changes in the lifetimes of halocarbons destroyed in the stratosphere were obtained. Those result from the time needed for their transport from the surface where they are emitted to the stratosphere where they are destroyed. Efforts should be made to update and reduce the large uncertainties on CFC lifetimes.

scholarly journals Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn

2009 ◽  
Vol 9 (12) ◽  
pp. 3911-3934 ◽  
Author(s):  
P. Martinerie ◽  
E. Nourtier-Mazauric ◽  
J.-M. Barnola ◽  
W. T. Sturges ◽  
D. R. Worton ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Numerical Models ◽  
Atmospheric Model ◽  
Calculated Concentration ◽  
Low Concentrations ◽  
Radiative Model ◽  
Green Function Approach ◽  
Atmospheric Concentrations ◽  
Depth Concentration

Abstract. The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are small. Our results indicate that the emissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6 are well constrained, whereas it is not the case for CFC-114 and CCl4. Significant emission-dependent changes in the lifetimes of halocarbons destroyed in the stratosphere were obtained. Those result from the time needed for their transport from the surface where they are emitted to the stratosphere where they are destroyed. Efforts should be made to update and reduce the large uncertainties on CFC lifetimes.

Planet Earth

2020 ◽  
pp. 1-38
Author(s):  
John Evans
Keyword(s):  
Molecular Structure ◽  
Global Warming ◽  
Energy Balance ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Fossil Fuels ◽  
Residence Times ◽  
Atmospheric Gases ◽  
Energy Demands ◽  
Atmospheric Concentrations

The pressure on planetary resources is substantially driven by increases in energy demands that have been mostly met by the combustion of fossil fuels. The basis of the warming in the troposphere is explained starting from the molecular structure of atmospheric components and their resulting rotational and vibrational spectra. From the absorptions in the infrared, the radiative efficiencies of atmospheric gases can be established. The residence times of gases in the atmosphere is explained on the basis of their atmospheric chemistry. Taking these factors together with atmospheric concentrations, the Global-Warming and -Temperature Potentials can be derived. The overall energy balance in the atmosphere is shown and the resulting net radiative forcing. The principle of the sustainability triangle is explained showing that reduction in radiative forcing may be achievable by a summation of contributions.

scholarly journals Evaluating the accuracy and uncertainty of atmospheric and wave model hindcasts during severe events using model ensembles

2021 ◽  
Author(s):  
Ali Abdolali ◽  
Andre van der Westhuysen ◽  
Zaizhong Ma ◽  
Avichal Mehra ◽  
Aron Roland ◽  
...  
Keyword(s):  
Extreme Event ◽  
Numerical Models ◽  
Model Performance ◽  
Ground Truth ◽  
Wave Model ◽  
Atmospheric Model ◽  
Stationary Source ◽  
Source Point ◽  
Spectral Wave Model ◽  
Model Ensembles

AbstractVarious uncertainties exist in a hindcast due to the inabilities of numerical models to resolve all the complicated atmosphere-sea interactions, and the lack of certain ground truth observations. Here, a comprehensive analysis of an atmospheric model performance in hindcast mode (Hurricane Weather and Research Forecasting model—HWRF) and its 40 ensembles during severe events is conducted, evaluating the model accuracy and uncertainty for hurricane track parameters, and wind speed collected along satellite altimeter tracks and at stationary source point observations. Subsequently, the downstream spectral wave model WAVEWATCH III is forced by two sets of wind field data, each includes 40 members. The first ones are randomly extracted from original HWRF simulations and the second ones are based on spread of best track parameters. The atmospheric model spread and wave model error along satellite altimeters tracks and at stationary source point observations are estimated. The study on Hurricane Irma reveals that wind and wave observations during this extreme event are within ensemble spreads. While both Models have wide spreads over areas with landmass, maximum uncertainty in the atmospheric model is at hurricane eye in contrast to the wave model.

A new ensemble-based statistical methodology to verify changes in weather and climate models

2021 ◽  
Author(s):  
Christian Zeman ◽  
Christoph Schär
Keyword(s):  
Climate Models ◽  
Climate Model ◽  
Numerical Models ◽  
Hypothesis Test ◽  
Model Development ◽  
Atmospheric Model ◽  
Statistical Hypothesis ◽  
Model Parameters ◽  
Rounding Errors ◽  
Weather And Climate

<p>Since their first operational application in the 1950s, atmospheric numerical models have become essential tools in weather and climate prediction. As such, they are a constant subject to changes, thanks to advances in computer systems, numerical methods, and the ever increasing knowledge about the atmosphere of Earth. Many of the changes in today's models relate to seemingly unsuspicious modifications, associated with minor code rearrangements, changes in hardware infrastructure, or software upgrades. Such changes are meant to preserve the model formulation, yet the verification of such changes is challenged by the chaotic nature of our atmosphere - any small change, even rounding errors, can have a big impact on individual simulations. Overall this represents a serious challenge to a consistent model development and maintenance framework.</p><p>Here we propose a new methodology for quantifying and verifying the impacts of minor atmospheric model changes, or its underlying hardware/software system, by using ensemble simulations in combination with a statistical hypothesis test. The methodology can assess effects of model changes on almost any output variable over time, and can also be used with different hypothesis tests.</p><p>We present first applications of the methodology with the regional weather and climate model COSMO. The changes considered include a major system upgrade of the supercomputer used, the change from double to single precision floating-point representation, changes in the update frequency of the lateral boundary conditions, and tiny changes to selected model parameters. While providing very robust results, the methodology also shows a large sensitivity to more significant model changes, making it a good candidate for an automated tool to guarantee model consistency in the development cycle.</p>

scholarly journals Investigation of water adsorption and hygroscopicity of atmospherically relevant particles using a commercial vapor sorption analyzer

2017 ◽  
Vol 10 (10) ◽  
pp. 3821-3832 ◽  
Author(s):  
Wenjun Gu ◽  
Yongjie Li ◽  
Jianxi Zhu ◽  
Xiaohong Jia ◽  
Qinhao Lin ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Water Adsorption ◽  
Theoretical Data ◽  
Atmospheric Particles ◽  
Relative Mass ◽  
Nonspherical Particles ◽  
Vapor Sorption ◽  
Hygroscopic Growth ◽  
Dry Conditions

Abstract. Water adsorption and hygroscopicity are among the most important physicochemical properties of aerosol particles, largely determining their impacts on atmospheric chemistry, radiative forcing, and climate. Measurements of water adsorption and hygroscopicity of nonspherical particles under subsaturated conditions are nontrivial because many widely used techniques require the assumption of particle sphericity. In this work we describe a method to directly quantify water adsorption and mass hygroscopic growth of atmospheric particles for temperature in the range of 5–30 °C, using a commercial vapor sorption analyzer. A detailed description of instrumental configuration and experimental procedures, including relative humidity (RH) calibration, is provided first. It is then demonstrated that for (NH4)2SO4 and NaCl, deliquescence relative humidities and mass hygroscopic growth factors measured using this method show good agreements with experimental and/or theoretical data from literature. To illustrate its ability to measure water uptake by particles with low hygroscopicity, we used this instrument to investigate water adsorption by CaSO4 ⋅ 2H2O as a function of RH at 25 °C. The mass hygroscopic growth factor of CaSO4 ⋅ 2H2O at 95 % RH, relative to that under dry conditions (RH  < 1 %), was determined to be (0.450±0.004) % (1σ). In addition, it is shown that this instrument can reliably measure a relative mass change of 0.025 %. Overall, we have demonstrated that this commercial instrument provides a simple, sensitive, and robust method to investigate water adsorption and hygroscopicity of atmospheric particles.

scholarly journals Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans
Keyword(s):  
Rate Constant ◽  
Atmospheric Chemistry ◽  
Rate Constants ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Photolysis Rates ◽  
The Impact ◽  
Chemical Rate

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.

scholarly journals Sensitivity of aerosol radiative effects to different mixing assumptions in the AEROPT 1.0 submodel of the EMAC atmospheric-chemistry–climate model

2014 ◽  
Vol 7 (5) ◽  
pp. 2503-2516 ◽  
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld
Keyword(s):  
Optical Properties ◽  
Radiative Transfer ◽  
Black Carbon ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Climate Model ◽  
Mixing Rule ◽  
Aerosol Optical Properties ◽  
Internal Mixing ◽  
Aerosol Radiative

Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well-mixed aerosol is a good approximation for particles with a black-carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005, we calculate that the global aerosol direct radiative forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.

scholarly journals A new radiation infrastructure for the Modular Earth Submodel System (MESSy, based on version 2.51)

2016 ◽  
Author(s):  
Simone Dietmüller ◽  
Patrick Jöckel ◽  
Holger Tost ◽  
Markus Kunze ◽  
Cathrin Gellhorn ◽  
...  
Keyword(s):  
Optical Properties ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Circulation Model ◽  
Shortwave Radiation ◽  
Aerosol Optical Properties ◽  
On Line ◽  
User Friendly ◽  
Radiation Scheme

Abstract. The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a basemodel via a highly flexible data management facility (Jöckel et al., 2010). In the present paper we present the four new radiation related submodels RAD, AEROPT, CLOUDOPT and ORBIT. The submodel RAD (with shortwave radiation scheme RAD_FUBRAD) simulates the radiative transfer, the submodel AEROPT calculates the aerosol optical properties, the submodel CLOUDOPT calculates the cloud optical properties, and the submodel ORBIT is responsible for Earth orbit calculations. These submodels are coupled via the standard MESSy infrastructure and are largely based on the original radiation scheme of the general circulation model ECHAM5, however, expanded with additional features. These features comprise, among others, user-friendly and flexibly controllable (by namelists) on-line radiative forcing calculations by multiple diagnostic calls of the radiation routines. With this, it is now possible to calculate radiative forcing (instantaneous as well as stratosphere adjusted) of various greenhouse gases simultaneously in only one simulation, as well as the radiative forcing of cloud perturbations. Examples of on-line radiative forcing calculations in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model are presented.

scholarly journals Comparison of ice particle characteristics simulated by the Community Atmosphere Model (CAM5) with in-situ observations

2014 ◽  
Vol 14 (6) ◽  
pp. 7637-7681 ◽  
Author(s):  
T. Eidhammer ◽  
H. Morrison ◽  
A. Bansemer ◽  
A. Gettelman ◽  
A. J. Heymsfield
Keyword(s):  
Size Distribution ◽  
Radiative Forcing ◽  
Climate Model ◽  
Global Climate ◽  
Global Climate Model ◽  
Atmospheric Model ◽  
Slope Parameter ◽  
Cloud Radiative Forcing ◽  
Threshold Size ◽  
Cloud Ice

Abstract. Detailed measurements of ice crystals in cirrus clouds were used to compare with results from the Community Atmospheric Model Version 5 (CAM5) global climate model. The observations are from two different field campaigns with contrasting conditions: Atmospheric Radiation Measurements Spring Cloud Intensive Operational Period in 2000 (ARM-IOP), which was characterized primarily by midlatitude frontal clouds and cirrus, and Tropical Composition, Cloud and Climate Coupling (TC4), which was dominated by anvil cirrus. Results show that the model typically overestimates the slope parameter of the exponential size distributions of cloud ice and snow, while the variation with temperature (height) is comparable. The model also overestimates the ice/snow number concentration (0th moment of the size distribution) and underestimates higher moments (2nd through 5th), but compares well with observations for the 1st moment. Overall the model shows better agreement with observations for TC4 than for ARM-IOP in regards to the moments. The mass-weighted terminal fallspeed is lower in the model compared to observations for both ARM-IOP and TC4, which is partly due to the overestimation of the size distribution slope parameter. Sensitivity tests with modification of the threshold size for cloud ice to snow autoconversion (Dcs) do not show noticeable improvement in modeled moments, slope parameter and mass weighed fallspeed compared to observations. Further, there is considerable sensitivity of the cloud radiative forcing to Dcs, consistent with previous studies, but no value of Dcs improves modeled cloud radiative forcing compared to measurements. Since the autoconversion of cloud ice to snow using the threshold size Dcs has little physical basis, future improvement to combine cloud ice and snow into a single category, eliminating the need for autoconversion, is suggested.

scholarly journals Characterising the seasonal and geographical variability in tropospheric ozone, stratospheric influence and recent changes

2019 ◽  
Vol 19 (6) ◽  
pp. 3589-3620 ◽  
Author(s):  
Ryan S. Williams ◽  
Michaela I. Hegglin ◽  
Brian J. Kerridge ◽  
Patrick Jöckel ◽  
Barry G. Latter ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Data Availability ◽  
Ozone Production ◽  
Upper Troposphere ◽  
The World

Abstract. The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability, and its changes and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified-dynamics chemistry–climate model (CCM) simulations from the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the International Global Atmospheric Chemistry – Stratosphere-troposphere Processes And their Role in Climate (IGAC-SPARC) (IGAC–SPARC) Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozone-sonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (∼0–5.5 km) sub-column ozone is found for EMAC, ranging from 2 to 8 Dobson units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (∼±4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozone-sondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with a negative bias in the troposphere resulting from a likely underestimation of photochemical ozone production. This has ramifications for diagnosing the level of model–measurement agreement. Model variability is found to be more similar in magnitude to that implied from ozone-sondes in comparison with OMI, which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is inferred that CMAM simulates a faster and shallower Brewer–Dobson circulation (BDC) compared to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is significant and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long-term changes in the CCM ozone tracers are calculated for different seasons. An overall statistically significant increase in tropospheric ozone is found across much of the world but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5 %–10 %) between 1980–1989 and 2001–2010. Our model study implies that attribution from stratosphere–troposphere exchange (STE) to such ozone changes ranges from 25 % to 30 % at the surface to as much as 50 %–80 % in the upper troposphere–lower stratosphere (UTLS) across some regions of the world, including western Eurasia, eastern North America, the South Pacific and the southern Indian Ocean. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere.

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