scholarly journals TransCom N<sub>2</sub>O model inter-comparison – Part 1: Assessing the influence of transport and surface fluxes on tropospheric N<sub>2</sub>O variability

2014 ◽  
Vol 14 (2) ◽  
pp. 2307-2362 ◽  
Author(s):  
R. L. Thompson ◽  
P. K. Patra ◽  
K. Ishijima ◽  
E. Saikawa ◽  
M. Corazza ◽  
...  

Abstract. We present a comparison of chemistry-transport models (TransCom-N2O) to examine the importance of atmospheric transport and surface fluxes on the variability of N2O mixing ratios in the troposphere. Six different models and two model variants participated in the inter-comparison and simulations were made for the period 2006 to 2009. In addition to N2O, simulations of CFC-12 and SF6 were made by a subset of four of the models to provide information on the models proficiency in stratosphere-troposphere exchange (STE) and meridional transport, respectively. The same prior emissions were used by all models to restrict differences among models to transport and chemistry alone. Four different N2O flux scenarios totalling between 14 and 17 Tg N yr−1 (for 2005) globally were also compared. The modelled N2O mixing ratios were assessed against observations from in-situ stations, discrete air sampling networks, and aircraft. All models adequately captured the large-scale patterns of N2O and the vertical gradient from the troposphere to the stratosphere and most models also adequately captured the N2O tropospheric growth rate. However, all models underestimated the inter-hemispheric N2O gradient by at least 0.33 ppb (equivalent to 1.5 Tg N), which, even after accounting for an overestimate of emissions in the Southern Ocean of circa 1.0 Tg N, points to a likely underestimate of the Northern Hemisphere source by up to 0.5 Tg N and/or an overestimate of STE in the Northern Hemisphere. Comparison with aircraft data reveal that the models overestimate the amplitude of the N2O seasonal cycle at Hawaii (21° N, 158° W) below circa 6000 m, suggesting an overestimate of the importance of stratosphere to troposphere transport in the lower troposphere at this latitude. In the Northern Hemisphere, most of the models that provided CFC-12 simulations captured the phase of the CFC-12, seasonal cycle, indicating a reasonable representation of the timing of STE. However, for N2O all models simulated a too early minimum by 2 to 3 months owing to errors in the seasonal cycle in the prior soil emissions, which is still not adequately represented by terrestrial biosphere models. In the Southern Hemisphere, most models failed to capture the N2O and CFC-12 seasonality at Cape Grim, Tasmania, and all failed at the South Pole, whereas for SF6, all models could capture the seasonality at all sites, suggesting that there are large errors in modeled vertical transport in high southern latitudes.

2014 ◽  
Vol 14 (8) ◽  
pp. 4349-4368 ◽  
Author(s):  
R. L. Thompson ◽  
P. K. Patra ◽  
K. Ishijima ◽  
E. Saikawa ◽  
M. Corazza ◽  
...  

Abstract. We present a comparison of chemistry-transport models (TransCom-N2O) to examine the importance of atmospheric transport and surface fluxes on the variability of N2O mixing ratios in the troposphere. Six different models and two model variants participated in the inter-comparison and simulations were made for the period 2006 to 2009. In addition to N2O, simulations of CFC-12 and SF6 were made by a subset of four of the models to provide information on the models' proficiency in stratosphere–troposphere exchange (STE) and meridional transport, respectively. The same prior emissions were used by all models to restrict differences among models to transport and chemistry alone. Four different N2O flux scenarios totalling between 14 and 17 TgN yr−1 (for 2005) globally were also compared. The modelled N2O mixing ratios were assessed against observations from in situ stations, discrete air sampling networks and aircraft. All models adequately captured the large-scale patterns of N2O and the vertical gradient from the troposphere to the stratosphere and most models also adequately captured the N2O tropospheric growth rate. However, all models underestimated the inter-hemispheric N2O gradient by at least 0.33 parts per billion (ppb), equivalent to 1.5 TgN, which, even after accounting for an overestimate of emissions in the Southern Ocean of circa 1.0 TgN, points to a likely underestimate of the Northern Hemisphere source by up to 0.5 TgN and/or an overestimate of STE in the Northern Hemisphere. Comparison with aircraft data reveal that the models overestimate the amplitude of the N2O seasonal cycle at Hawaii (21° N, 158° W) below circa 6000 m, suggesting an overestimate of the importance of stratosphere to troposphere transport in the lower troposphere at this latitude. In the Northern Hemisphere, most of the models that provided CFC-12 simulations captured the phase of the CFC-12, seasonal cycle, indicating a reasonable representation of the timing of STE. However, for N2O all models simulated a too early minimum by 2 to 3 months owing to errors in the seasonal cycle in the prior soil emissions, which was not adequately represented by the terrestrial biosphere model. In the Southern Hemisphere, most models failed to capture the N2O and CFC-12 seasonality at Cape Grim, Tasmania, and all failed at the South Pole, whereas for SF6, all models could capture the seasonality at all sites, suggesting that there are large errors in modelled vertical transport in high southern latitudes.


2014 ◽  
Vol 11 (10) ◽  
pp. 14587-14637 ◽  
Author(s):  
A. Berchet ◽  
I. Pison ◽  
F. Chevallier ◽  
J.-D. Paris ◽  
P. Bousquet ◽  
...  

Abstract. Eight surface observation sites providing quasi-continuous measurements of atmospheric methane mixing ratios have been operated since the mid-2000's in Siberia. For the first time in a single work, we assimilate all of these in situ data in an atmospheric inversion. Our objective is to quantify methane surface fluxes from anthropogenic and wetland sources at the meso-scale in the Siberian Lowlands for the year 2010. To do so, we first inquire into the way the inversion uses the observations and the fluxes are constrained by the observation sites. As atmospheric inversions at the meso-scale suffer from mis-quantified sources of uncertainties, we follow recent innovations in inversion techniques and use a new inversion approach which quantifies the uncertainties more objectively than the previous inversions. We find that, due to errors in the representation of the atmospheric transport and redundant pieces of information, only one observation every few days is found valuable by the inversion. The remaining high-resolution signals are representative of very local emission patterns. An analysis of the use of information by the inversion also reveals that the observation sites constrain methane emissions within a radius of 500 km. More observation sites are necessary to constrain the whole Siberian Lowlands. Still, the fluxes within the constrained areas are quantified with objectified uncertainties. At the end, the tolerance intervals for posterior methane fluxes are of roughly 20% (resp. 50%) of the fluxes for anthropogenic (resp. wetland) sources. About 50–70% of emissions are constrained by the inversion on average on an annual basis. Extrapolating the figures on the constrained areas to the whole Siberian Lowlands, we find a regional methane budget of 5–28 Tg CH4 for the year 2010, i.e. 1–5% of the global methane emissions. As very few in situ observations are available in the region of interest, observations of methane total columns from the Greenhouse Gas Observing SATellite (GOSAT) are used for the evaluation of the inversion results, but they exhibit marginal signal from the fluxes within the region of interest.


2016 ◽  
Author(s):  
Mike J. Newland ◽  
Patricia Martinerie ◽  
Emmanuel Witrant ◽  
Detlev Helmig ◽  
David R. Worton ◽  
...  

Abstract. The NOX (NO and NO2) and HOX (OH and HO2) budgets of the atmosphere exert a major influence on atmospheric composition, controlling removal of primary pollutants and formation of a wide range of secondary products, including ozone, that can influence human health and climate. However, there remain large uncertainties in the changes to these budgets over recent decades. Due to their short atmospheric lifetimes, NOX and HOX are highly variable in space and time, and so the measurements of these species are of very limited value for examining long term, large scale changes to their budgets. Here, we take an alternative approach by examining long-term atmospheric trends of alkyl nitrates, the formation of which is dependent on the atmospheric NO / HO2 ratio. We derive long term trends in the alkyl nitrates from measurements in firn air from the NEEM site, Greenland. Their mixing ratios increased by a factor of 4–5 between the 1970s and 1990s. This was followed by a steep decline to the sampling date of 2008. Moreover, we examine how the trends in the alkyl nitrates compare to similarly derived trends in their parent alkanes (i.e. the alkanes which, when oxidised in the presence of NOX, lead to the formation of the alkyl nitrates). The ratios of the alkyl nitrates to their parent alkanes increase from around 1970 to the late 1990's consistent with large changes to the [NO] / [HO2] ratio in the northern hemisphere atmosphere during this period. These could represent historic changes to NOX sources and sinks. Alternatively, they could represent changes to concentrations of the hydroxyl radical, OH, or to the transport time of the air masses from source regions to the Arctic.


2014 ◽  
Vol 14 (20) ◽  
pp. 27663-27729 ◽  
Author(s):  
T. Launois ◽  
P. Peylin ◽  
S. Belviso ◽  
B. Poulter

Abstract. Clear analogies between carbonyl sulfide (OCS) and carbon dioxide (CO2) diffusion pathways through leaves have been revealed by experimental studies with plant uptake playing an important role for the atmospheric budget of both species. Here we use atmospheric OCS to evaluate the gross primary production (GPP) of three dynamic global vegetation models (LPJ, NCAR-CLM4 and ORCHIDEE). Vegetation uptake of OCS is modeled as a linear function of GPP and LRU, the ratio of OCS to CO2 deposition velocities to plants. New parameterizations for the non-photosynthetic sinks (oxic soils, atmospheric oxidation) and biogenic sources (oceans and anoxic soils) of OCS are also provided. Despite new large oceanic emissions, global OCS budgets created with each vegetation model show exceeding sinks by several hundreds of Gg S yr−1. An inversion of the surface fluxes (optimization of a global scalar which accounts for flux uncertainties) led to balanced OCS global budgets, as atmospheric measurements suggest, mainly by drastic reduction (−30%) of soil and vegetation uptakes. The amplitude of variations in atmospheric OCS mixing ratios is mainly dictated by the vegetation sink over the Northern Hemisphere. This allows for bias recognition in the GPP representations of the three selected models. Main bias patterns are (i) the terrestrial GPP of ORCHIDEE at high Northern latitudes is currently over-estimated, (ii) the seasonal variations of the GPP are out of phase in the NCAR-CLM4 model, showing a maximum carbon uptake too early in spring in the northernmost ecosystems, (iii) the overall amplitude of the seasonal variations of GPP in NCAR-CLM4 is too small, and (iv) for the LPJ model, the GPP is slightly out of phase for northernmost ecosystems and the respiration fluxes might be too large in summer in the Northern Hemisphere.


2011 ◽  
Vol 11 (2) ◽  
pp. 421-437 ◽  
Author(s):  
S. Wang ◽  
L. W. O'Neill ◽  
Q. Jiang ◽  
S. P. de Szoeke ◽  
X. Hong ◽  
...  

Abstract. This paper presents an evaluation and validation of the Naval Research Laboratory's COAMPS® real-time forecasts during the VOCALS-REx over the area off the west coast of Chile/Peru in the Southeast Pacific during October and November 2008. The analyses focus on the marine boundary layer (MBL) structure. These forecasts are compared with lower troposphere soundings, in situ surface measurements, and satellite observations. The predicted mean MBL cloud and surface wind spatial distributions are in good agreement with the satellite observations. The large-scale longitudinal variation of the MBL structure along 20° S is captured by the forecasts. That is, the MBL height increases westward toward the open ocean, the moisture just above the inversion decreases, and the MBL structure becomes more decoupled offshore. The observed strong wind shear across the cloud-top inversion near 20° S was correctly predicted by the model. The model's cloud spatial and temporal distribution in the 15 km grid mesh is sporadic compared to satellite observations. Our results suggest that this is caused by grid-scale convection likely due to a lack of a shallow cumulus convection parameterization in the model. Both observations and model forecasts show wind speed maxima near the top of MBL along 20° S, which is consistent with the westward upslope of the MBL heights based on the thermal wind relationship. The forecasts produced well-defined diurnal variations in the spatially-averaged MBL structure, although the overall signal is weaker than those derived from the in situ measurements and satellite data. The MBL heights are generally underpredicted in the nearshore area. An analysis of the sensitivity of the MBL height to horizontal and vertical grid resolution suggests that the underprediction is likely associated with overprediction of the mesoscale downward motion and cold advection near the coast.


2014 ◽  
Vol 14 (17) ◽  
pp. 9249-9258 ◽  
Author(s):  
S. O'Doherty ◽  
M. Rigby ◽  
J. Mühle ◽  
D. J. Ivy ◽  
B. R. Miller ◽  
...  

Abstract. High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant hydrofluorocarbons (HFCs) respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 ± 0.04 and 0.7 ± 0.02 mW m−2 in 2012 respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1σ) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing by 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.


2018 ◽  
Vol 18 (5) ◽  
pp. 3839-3864 ◽  
Author(s):  
Christian Hogrefe ◽  
Peng Liu ◽  
George Pouliot ◽  
Rohit Mathur ◽  
Shawn Roselle ◽  
...  

Abstract. This study analyzes simulated regional-scale ozone burdens both near the surface and aloft, estimates process contributions to these burdens, and calculates the sensitivity of the simulated regional-scale ozone burden to several key model inputs with a particular emphasis on boundary conditions derived from hemispheric or global-scale models. The Community Multiscale Air Quality (CMAQ) model simulations supporting this analysis were performed over the continental US for the year 2010 within the context of the Air Quality Model Evaluation International Initiative (AQMEII) and Task Force on Hemispheric Transport of Air Pollution (TF-HTAP) activities. CMAQ process analysis (PA) results highlight the dominant role of horizontal and vertical advection on the ozone burden in the mid-to-upper troposphere and lower stratosphere. Vertical mixing, including mixing by convective clouds, couples fluctuations in free-tropospheric ozone to ozone in lower layers. Hypothetical bounding scenarios were performed to quantify the effects of emissions, boundary conditions, and ozone dry deposition on the simulated ozone burden. Analysis of these simulations confirms that the characterization of ozone outside the regional-scale modeling domain can have a profound impact on simulated regional-scale ozone. This was further investigated by using data from four hemispheric or global modeling systems (Chemistry – Integrated Forecasting Model (C-IFS), CMAQ extended for hemispheric applications (H-CMAQ), the Goddard Earth Observing System model coupled to chemistry (GEOS-Chem), and AM3) to derive alternate boundary conditions for the regional-scale CMAQ simulations. The regional-scale CMAQ simulations using these four different boundary conditions showed that the largest ozone abundance in the upper layers was simulated when using boundary conditions from GEOS-Chem, followed by the simulations using C-IFS, AM3, and H-CMAQ boundary conditions, consistent with the analysis of the ozone fields from the global models along the CMAQ boundaries. Using boundary conditions from AM3 yielded higher springtime ozone columns burdens in the middle and lower troposphere compared to boundary conditions from the other models. For surface ozone, the differences between the AM3-driven CMAQ simulations and the CMAQ simulations driven by other large-scale models are especially pronounced during spring and winter where they can reach more than 10 ppb for seasonal mean ozone mixing ratios and as much as 15 ppb for domain-averaged daily maximum 8 h average ozone on individual days. In contrast, the differences between the C-IFS-, GEOS-Chem-, and H-CMAQ-driven regional-scale CMAQ simulations are typically smaller. Comparing simulated surface ozone mixing ratios to observations and computing seasonal and regional model performance statistics revealed that boundary conditions can have a substantial impact on model performance. Further analysis showed that boundary conditions can affect model performance across the entire range of the observed distribution, although the impacts tend to be lower during summer and for the very highest observed percentiles. The results are discussed in the context of future model development and analysis opportunities.


2013 ◽  
Vol 141 (2) ◽  
pp. 690-706 ◽  
Author(s):  
Masaki Katsumata ◽  
Hiroyuki Yamada ◽  
Hisayuki Kubota ◽  
Qoosaku Moteki ◽  
Ryuichi Shirooka

Abstract This report describes the in situ observed evolution of the atmospheric profile during an event of the boreal summer intraseasonal variation (BSISV) in the tropical western Pacific Ocean. The convectively active region of the BSISV proceeded northward over the sounding and radar network. Over the array, the situation changed from a convectively inactive period to an active period. Inspection of the sounding data revealed the gradual moistening of the lower troposphere during the convectively inactive period. The sounding-derived heat and moisture budget analyses indicated that both the convective- and large-scale processes caused moistening of the lower and middle troposphere where the radar echo tops were observed most frequently. This study is the first to identify such a “preconditioning” process for the BSISV in the western Pacific using detailed in situ observational data. During the preconditioning, an increase in CAPE was observed, as in previous studies of the MJO. An increase of moisture in the boundary layer was responsible for the increase of CAPE. The large-scale horizontal convergence in the boundary layer may be a key factor to moisten the boundary layer through the convective-scale processes, as well as through the large-scale processes to moisten the lower and middle troposphere.


2014 ◽  
Vol 7 (3) ◽  
pp. 743-755 ◽  
Author(s):  
C. Dyroff ◽  
A. Zahn ◽  
S. Sanati ◽  
E. Christner ◽  
A. Rauthe-Schöch ◽  
...  

Abstract. A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.


2011 ◽  
Vol 8 (4) ◽  
pp. 7475-7524 ◽  
Author(s):  
G. Keppel-Aleks ◽  
P. O. Wennberg ◽  
R. A. Washenfelder ◽  
D. Wunch ◽  
T. Schneider ◽  
...  

Abstract. New observations of the vertically integrated CO2 mixing ratio, ⟨CO2⟩, from ground-based remote sensing show that variations in ⟨CO2⟩ are primarily determined by large-scale flux patterns. They therefore provide fundamentally different information than observations made within the boundary layer, which reflect the combined influence of large scale and local fluxes. Observations of both ⟨CO2⟩ and CO2 concentrations in the free troposphere show that large-scale spatial gradients induce synoptic-scale temporal variations in ⟨CO2⟩ in the Northern Hemisphere midlatitudes through horizontal advection. Rather than obscure the signature of surface fluxes on atmospheric CO2, these synoptic-scale variations provide useful information that can be used to reveal the meridional flux distribution. We estimate the meridional gradient in ⟨CO2⟩ from covariations in ⟨CO2⟩ and potential temperature, θ, a dynamical tracer, on synoptic timescales to evaluate surface flux estimates commonly used in carbon cycle models. We find that Carnegie Ames Stanford Approach (CASA) biospheric fluxes underestimate both the ⟨CO2⟩ seasonal cycle amplitude throughout the Northern Hemisphere midlatitudes as well as the meridional gradient during the growing season. Simulations using CASA net ecosystem exchange (NEE) with increased and phase-shifted boreal fluxes better reflect the observations. Our simulations suggest that boreal growing season NEE (between 45–65° N) is underestimated by ~40 % in CASA. We describe the implications for this large seasonal exchange on inference of the net Northern Hemisphere terrestrial carbon sink.


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