The chemical transport model Oslo CTM3

Abstract. We present here the global chemical transport model Oslo CTM3, an update of the Oslo CTM2. The update comprises a faster transport scheme, an improved wet scavenging scheme for large scale rain, updated photolysis rates and a new lightning parameterization. Oslo CTM3 is better parallelized and allows for stable, large time steps for advection, enabling more complex or high resolution simulations. Thorough comparisons between the Oslo CTM3, Oslo CTM2 and measurements are performed, and in general the Oslo CTM3 is found to reproduce measurements well. Inclusion of tropospheric sulfur chemistry and nitrate aerosols in CTM3 is shown to be important to reproduce tropospheric O3, OH and the CH4 lifetime well. Using the same meteorology to drive the two models, shows that some features related to transport are better resolved by the CTM3, such as polar cap transport, while features like transport close to the vortex edge are resolved better in the Oslo CTM2 due to its required shorter transport time step. The longer transport time steps in CTM3 result in larger errors e.g. near the jets, and when necessary, this can be remedied by using a shorter time step. An additional, more accurate and time consuming, treatment of polar cap transport is presented, however, both perform acceptably. A new treatment of the horizontal distribution of lightning is presented and found to compare well with measurements. Vertical distributions of lighting are updated, and tested against the old vertical distribution. The new profiles are found to produce more NOx in the tropical middle troposphere, and less at the surface and at high altitudes.

Download Full-text

The chemical transport model Oslo CTM3

Geoscientific Model Development ◽

10.5194/gmd-5-1441-2012 ◽

2012 ◽

Vol 5 (6) ◽

pp. 1441-1469 ◽

Cited By ~ 40

Author(s):

O. A. Søvde ◽

M. J. Prather ◽

I. S. A. Isaksen ◽

T. K. Berntsen ◽

F. Stordal ◽

...

Keyword(s):

Large Scale ◽

Transport Model ◽

Chemical Transport ◽

Horizontal Distribution ◽

Small Scale ◽

Chemical Transport Model ◽

Polar Cap ◽

Time Step ◽

Transport Time ◽

Fractional Cloud

Abstract. We present here the global chemical transport model Oslo CTM3, an update of the Oslo CTM2. The update comprises a faster transport scheme, an improved wet scavenging scheme for large scale rain, updated photolysis rates and a new lightning parameterization. Oslo CTM3 is better parallelized and allows for stable, large time steps for advection, enabling more complex or high spatial resolution simulations. A new treatment of the horizontal distribution of lightning is presented and found to compare well with measurements. The vertical distribution of lightning is updated and found to be a large contributor to CTM2–CTM3 differences, producing more NOx in the tropical middle troposphere, and less at the surface and at high altitudes. Compared with Oslo CTM2, Oslo CTM3 is faster, more capable and has better conceptual models for scavenging, vertical transport and fractional cloud cover. CTM3 captures stratospheric O3 better than CTM2, but shows minor improvements in terms of matching atmospheric observations in the troposphere. Use of the same meteorology to drive the two models shows that some features related to transport are better resolved by the CTM3, such as polar cap transport, while features like transport close to the vortex edge are resolved better in the Oslo CTM2 due to its required shorter transport time step. The longer transport time steps in CTM3 result in larger errors, e.g., near the jets, and when necessary the errors can be reduced by using a shorter time step. Using a time step of 30 min, the new transport scheme captures both large-scale and small-scale variability in atmospheric circulation and transport, with no loss of computational efficiency. We present a version of the new transport scheme which has been specifically tailored for polar studies, resulting in more accurate polar cap transport than the standard CTM3 transport, confirmed by comparison to satellite observations. Inclusion of tropospheric sulfur chemistry and nitrate aerosols in CTM3 is shown to be important to reproduce tropospheric O3, OH and the CH4 lifetime well.

Download Full-text

Inversion of long-lived trace gas emissions using combined Eulerian and Lagrangian chemical transport models

Atmospheric Chemistry and Physics ◽

10.5194/acp-11-9887-2011 ◽

2011 ◽

Vol 11 (18) ◽

pp. 9887-9898 ◽

Cited By ~ 49

Author(s):

M. Rigby ◽

A. J. Manning ◽

R. G. Prinn

Keyword(s):

High Resolution ◽

Large Scale ◽

Transport Model ◽

Initial Conditions ◽

Dispersion Model ◽

Chemical Transport ◽

Particle Dispersion ◽

Global Network ◽

Lagrangian Model ◽

Chemical Transport Model

Abstract. We present a method for estimating emissions of long-lived trace gases from a sparse global network of high-frequency observatories, using both a global Eulerian chemical transport model and Lagrangian particle dispersion model. Emissions are derived in a single step after determining sensitivities of the observations to initial conditions, the high-resolution emissions field close to observation points, and larger regions further from the measurements. This method has the several advantages over inversions using one type of model alone, in that: high-resolution simulations can be carried out in limited domains close to the measurement sites, with lower resolution being used further from them; the influence of errors due to aggregation of emissions close to the measurement sites can be minimized; assumptions about boundary conditions to the Lagrangian model do not need to be made, since the entire emissions field is estimated; any combination of appropriate models can be used, with no code modification. Because the sensitivity to the entire emissions field is derived, the estimation can be carried out using traditional statistical methods without the need for multiple steps in the inversion. We demonstrate the utility of this approach by determining global SF6 emissions using measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) between 2007 and 2009. The global total and large-scale patterns of the derived emissions agree well with previous studies, whilst allowing emissions to be determined at higher resolution than has previously been possible, and improving the agreement between the modeled and observed mole fractions at some sites.

Download Full-text

Clouds, photolysis and regional tropospheric ozone budgets

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-9-13889-2009 ◽

2009 ◽

Vol 9 (3) ◽

pp. 13889-13916 ◽

Cited By ~ 1

Author(s):

A. Voulgarakis ◽

O. Wild ◽

N. H. Savage ◽

G. D. Carver ◽

J. A. Pyle

Keyword(s):

Tropospheric Ozone ◽

Large Scale ◽

Transport Model ◽

Regional Scale ◽

Three Dimensional ◽

Global Scale ◽

Chemical Production ◽

Chemical Transport Model ◽

Photolysis Rates ◽

Boundary Layer Ozone

Abstract. We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity on regional scales.

Download Full-text

Street-in-Grid modeling of gas-phase pollutants in Paris city

10.5194/acp-2019-1087 ◽

2019 ◽

Cited By ~ 1

Author(s):

Lya Lugon ◽

Karine Sartelet ◽

Youngseob Kim ◽

Jérémy Vigneron ◽

Olivier Chrétien

Keyword(s):

Transport Model ◽

Regional Scale ◽

Chemical Transport ◽

Scale Model ◽

Background Concentrations ◽

Chemical Transport Model ◽

Time Step ◽

Multi Scale ◽

Pollutant Concentrations ◽

Stationary Approach

Abstract. Regional-scale chemistry-transport models have coarse spatial resolution, and thus can only simulate background concentrations. They fail to simulate the high concentrations observed close to roads and in streets, i.e. where a large part of the urban population lives. Local-scale models may be used to simulate concentrations in streets. They often assume that background concentrations are constant and/or use simplified chemistry. Recently developed, the multi-scale model Street-in-Grid (SinG) estimates gaseous pollutant concentrations simultaneously at local and regional scales, coupling them dynamically. This coupling combines the regional-scale chemistry-transport model Polair3D and the street network model MUNICH (Model of Urban Network of Intersecting Canyons and Highway). MUNICH models explicitly street canyons and intersections, and it is coupled to the first vertical level of the chemical-transport model, enabling the transfer of pollutant mass between the street canyon roof and the atmosphere. The original versions of SinG and MUNICH adopt a stationary hypothesis to estimate pollutant concentrations in streets. Although the computation of NOx concentration is numerically stable with the stationary approach, the partitioning between NO and NO2 is highly dependent on the time step of coupling between transport and chemistry processes. In this study, a new non-stationary approach is presented with a fine coupling between transport and chemistry, leading to numerically stable partitioning between NO and NO2. Simulations of NO, NO2 and NOx concentrations over Paris city with SinG, MUNICH and Polair3D are compared to observations at traffic and urban stations to estimate the added value of multi-scale modeling with a dynamical coupling between the regional and local scales. As expected, the regional chemical-transport model underestimates NO and NO2 concentrations in the streets. However, there is a good agreement between the measurements and the concentrations simulated with MUNICH and SinG. The dynamic coupling between the local and regional scales tends to be important for streets with an intermediate aspect ratio and with high traffic emissions.

Download Full-text

Modeling lightning-NO<sub><i>x</i></sub> chemistry at sub-grid scale in a global chemical transport model

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-15-34091-2015 ◽

2015 ◽

Vol 15 (23) ◽

pp. 34091-34147 ◽

Cited By ~ 1

Author(s):

A. Gressent ◽

B. Sauvage ◽

D. Cariolle ◽

M. Evans ◽

M. Leriche ◽

...

Keyword(s):

Large Scale ◽

Transport Model ◽

Chemical Transport ◽

Horizontal Resolution ◽

Parameter Estimates ◽

Plume Dispersion ◽

Chemical Transport Model ◽

Tropical Regions ◽

The Impact ◽

Lightning Nox

Abstract. For the first time, a plume-in-grid approach is implemented in a chemical transport model (CTM) to parameterize the effects of the non-linear reactions occurring within high concentrated NOx plumes from lightning NOx emissions (LNOx) in the upper troposphere. It is characterized by a set of parameters including the plume lifetime, the effective reaction rate constant related to NOx-O3 chemical interactions and the fractions of NOx conversion into HNO3 within the plume. Parameter estimates were made using the DSMACC chemical box model, simple plume dispersion simulations and the mesoscale 3-D Meso-NH model. In order to assess the impact of the LNOx plume approach on the NOx and O3 distributions at large scale, simulations for the year 2006 were performed using the GEOS-Chem global model with a horizontal resolution of 2° × 2.5°. The implementation of the LNOx parameterization implies NOx and O3 decrease at large scale over the region characterized by a strong lightning activity (up to 25 and 8 %, respectively, over Central Africa in July) and a relative increase downwind of LNOx emissions (up to 18 and 2 % for NOx and O3, respectively, in July) are derived. The calculated variability of NOx and O3 mixing ratios around the mean value according to the known uncertainties on the parameter estimates is maximum over continental tropical regions with ΔNOx [−33.1; +29.7] ppt and ΔO3 [−1.56; +2.16] ppb, in January, and ΔNOx [−14.3; +21] ppt and ΔO3 [−1.18; +1.93] ppb, in July, mainly depending on the determination of the diffusion properties of the atmosphere and the initial NO mixing ratio injected by lightning. This approach allows (i) to reproduce a more realistic lightning NOx chemistry leading to better NOx and O3 distributions at the large scale and (ii) focus on other improvements to reduce remaining uncertainties from processes related to NOx chemistry in CTM.

Download Full-text

Simulation of radon-222 with the GEOS-Chem global model: Emissions, seasonality, and convective transport

10.5194/acp-2020-804 ◽

2020 ◽

Author(s):

Bo Zhang ◽

Hongyu Liu ◽

James H. Crawford ◽

Gao Chen ◽

T. Duncan Fairlie ◽

...

Keyword(s):

Large Scale ◽

Transport Model ◽

Lower Troposphere ◽

Chemical Transport ◽

Surface Concentration ◽

Vertical Gradient ◽

Convective Transport ◽

Chemical Transport Model ◽

Earth Observing System ◽

Land Surfaces

Abstract. Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surfaces, and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model to improve our understanding of 222Rn emissions and surface concentration seasonality, and characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, MERRA and GEOS-FP. We evaluate four global 222Rn emission scenarios by comparing model results with observations at 51 surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with surface observations globally ( 80 % data within a factor of 2), and reasonable agreement in Asia (close to 70 %). Further constraints on 222Rn emissions would require additional concentration and emission flux observations in the central U.S., Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles in northern mid-latitude summer, and from three short-term airborne campaigns. While simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0–4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared with GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations. This has important implications for using chemical transport models to interpret the transport of other trace species when these GEOS products are used as driving meteorology.

Download Full-text

Clouds, photolysis and regional tropospheric ozone budgets

Atmospheric Chemistry and Physics ◽

10.5194/acp-9-8235-2009 ◽

2009 ◽

Vol 9 (21) ◽

pp. 8235-8246 ◽

Cited By ~ 32

Author(s):

A. Voulgarakis ◽

O. Wild ◽

N. H. Savage ◽

G. D. Carver ◽

J. A. Pyle

Keyword(s):

Tropospheric Ozone ◽

Large Scale ◽

Transport Model ◽

Regional Scale ◽

Three Dimensional ◽

Lower Troposphere ◽

Global Scale ◽

Chemical Production ◽

Chemical Transport Model ◽

Photolysis Rates

Abstract. We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene, through decreases of OH in the lower troposphere, is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity of the ozone budget components on regional scales.

Download Full-text

Evaluation of cloud convection and tracer transport in a three-dimensional chemical transport model

Atmospheric Chemistry and Physics ◽

10.5194/acp-11-5783-2011 ◽

2011 ◽

Vol 11 (12) ◽

pp. 5783-5803 ◽

Cited By ~ 21

Author(s):

W. Feng ◽

M. P. Chipperfield ◽

S. Dhomse ◽

B. M. Monge-Sanz ◽

X. Yang ◽

...

Keyword(s):

Mass Flux ◽

Large Scale ◽

Transport Model ◽

Chemical Transport ◽

Convective Transport ◽

Convective Precipitation ◽

Tracer Transport ◽

Chemical Transport Model ◽

Mass Fluxes ◽

Spatial And Seasonal Variation

Abstract. We investigate the performance of cloud convection and tracer transport in a global off-line 3-D chemical transport model. Various model simulations are performed using different meteorological (re)analyses (ERA-40, ECMWF operational and ECMWF Interim) to diagnose the updraft mass flux, convective precipitation and cloud top height. The diagnosed upward mass flux distribution from TOMCAT agrees quite well with the ECMWF reanalysis data (ERA-40 and ERA-Interim) below 200 hPa. Inclusion of midlevel convection improves the agreement at mid-high latitudes. However, the reanalyses show strong convective transport up to 100 hPa, well into the tropical tropopause layer (TTL), which is not captured by TOMCAT. Similarly, the model captures the spatial and seasonal variation of convective cloud top height although the mean modelled value is about 2 km lower than observed. The ERA-Interim reanalyses have smaller archived upward convective mass fluxes than ERA-40, and smaller convective precipitation, which is in better agreement with satellite-based data. TOMCAT captures these relative differences when diagnosing convection from the large-scale fields. The model also shows differences in diagnosed convection with the version of the operational analyses used, which cautions against using results of the model from one specific time period as a general evaluation. We have tested the effect of resolution on the diagnosed modelled convection with simulations ranging from 5.6° × 5.6° to 1° × 1°. Overall, in the off-line model, the higher model resolution gives stronger vertical tracer transport, however, it does not make a large change to the diagnosed convective updraft mass flux (i.e., the model results using the convection scheme fail to capture the strong convection transport up to 100 hPa as seen in the archived convective mass fluxes). Similarly, the resolution of the forcing winds in the higher resolution CTM does not make a large improvement compared to the archived mass fluxes. Including a radon tracer in the model confirms the importance of convection for reproducing observed midlatitude profiles. The model run using archived mass fluxes transports significantly more radon to the upper troposphere but the available data does not strongly discriminate between the different model versions.

Download Full-text

Simulation of radon-222 with the GEOS-Chem global model: emissions, seasonality, and convective transport

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-1861-2021 ◽

2021 ◽

Vol 21 (3) ◽

pp. 1861-1887

Author(s):

Bo Zhang ◽

Hongyu Liu ◽

James H. Crawford ◽

Gao Chen ◽

T. Duncan Fairlie ◽

...

Keyword(s):

Large Scale ◽

Emission Scenario ◽

Transport Model ◽

Lower Troposphere ◽

Chemical Transport ◽

Surface Concentration ◽

Convective Transport ◽

Emission Flux ◽

Chemical Transport Model ◽

Emission Fluxes

Abstract. Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surfaces and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model to improve our understanding of 222Rn emissions and surface concentration seasonality and characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, the Modern-Era Retrospective analysis for Research and Applications (MERRA) and GEOS Forward Processing (GEOS-FP). We evaluate four global 222Rn emission scenarios by comparing model results with observations at 51 surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with surface observations globally (68.9 % of data within a factor of 2) and a large underestimate of winter surface 222Rn concentrations at Northern Hemisphere midlatitudes and high latitudes due to an oversimplified formulation of 222Rn emission fluxes (1 atom cm−2 s−1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global 222Rn emission scenario based on Zhang et al. (2011) and demonstrate its potential to improve simulated surface 222Rn concentrations and seasonality. The regional components of this scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors in determining 222Rn emission flux rates. However, large model underestimates of surface 222Rn concentrations still exist in Asia, suggesting unusually high regional 222Rn emissions. We therefore propose a conservative upscaling factor of 1.2 for 222Rn emission fluxes in China, which was also constrained by observed deposition fluxes of 210Pb (a progeny of 222Rn). With this modification, the model shows better agreement with observations in Europe and North America (> 80 % of data within a factor of 2) and reasonable agreement in Asia (close to 70 %). Further constraints on 222Rn emissions would require additional concentration and emission flux observations in the central United States, Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles in northern midlatitude summer and from three short-term airborne campaigns. While simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0–4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared with GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated for by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations. This has important implications for using chemical transport models to interpret the transport of other trace species when these GEOS products are used as driving meteorology.

Download Full-text