scholarly journals A three-dimensional-model inversion of methyl chloroform to constrain the atmospheric oxidative capacity

2021 ◽  
Vol 21 (6) ◽  
pp. 4809-4824
Author(s):  
Stijn Naus ◽  
Stephen A. Montzka ◽  
Prabir K. Patra ◽  
Maarten C. Krol
Keyword(s):  
Large Scale ◽  
Transport Model ◽  
Oxidative Capacity ◽  
Added Value ◽  
Interannual Variations ◽  
Three Dimensional Model ◽  
Model Inversion ◽  
Methyl Chloroform ◽  
Convergence Problems ◽  
Global Mean

Abstract. Variations in the atmospheric oxidative capacity, largely determined by variations in the hydroxyl radical (OH), form a key uncertainty in many greenhouse and other pollutant budgets, such as that of methane (CH4). Methyl chloroform (MCF) is an often-adopted tracer to indirectly put observational constraints on large-scale variations in OH. We investigated the budget of MCF in a 4DVAR inversion using the atmospheric transport model TM5, for the period 1998–2018, with the objective to derive information on large-scale, interannual variations in atmospheric OH concentrations. While our main inversion did not fully converge, we did derive interannual variations in the global oxidation of MCF that bring simulated mole fractions of MCF within 1 %–2 % of the assimilated observations from the NOAA-GMD surface network at most sites. Additionally, the posterior simulations better reproduce aircraft observations used for independent validation compared to the prior simulations. The derived OH variations showed robustness with respect to the prior MCF emissions and the prior OH distribution over the 1998 to 2008 period. Although we find a rapid 8 % increase in global mean OH concentrations between 2010 and 2012 that quickly declines afterwards, the derived interannual variations were typically small (< 3 %/yr), with no significant long-term trend in global mean OH concentrations. The inverse system found strong adjustments to the latitudinal distribution of OH, relative to widely used prior distributions, with systematic increases in tropical and decreases in extra-tropical OH concentrations (both up to 30 %). These spatial adjustments were driven by intrahemispheric biases in simulated MCF mole fractions, which have not been identified in previous studies. Given the large amplitude of these adjustments, which exceeds spread between literature estimates, and a residual bias in the MCF intrahemispheric gradients, we suggest a reversal in the extratropical ocean sink of MCF in response to declining atmospheric MCF abundance (as hypothesized in Wennberg et al., 2004). This ocean source provides a more realistic explanation for the biases, possibly complementary to adjustments in the OH distribution. We identified significant added value in the use of a 3D transport model, since it implicitly accounts for variable transport and optimizes the observed spatial gradients of MCF, which is not possible in simpler models. However, we also found a trade-off in computational expense and convergence problems. Despite these convergence problems, the derived OH variations do result in an improved match with MCF observations relative to an interannually repeating prior for OH. Therefore, we consider that variations in OH derived from MCF inversions with 3D models can add value to budget studies of long-lived gases like CH4.

scholarly journals A 3D-model inversion of methyl chloroform to constrain the atmospheric oxidative capacity

2020 ◽  
Author(s):  
Stijn Naus ◽  
Stephen A. Montzka ◽  
Prabir K. Patra ◽  
Maarten C. Krol
Keyword(s):  
3D Model ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Oxidative Capacity ◽  
Interannual Variations ◽  
Model Inversion ◽  
Methyl Chloroform ◽  
Aircraft Observations ◽  
Surface Network ◽  
Atmospheric Transport Model

Abstract. Variations in the atmospheric oxidative capacity, largely determined by variations in the hydroxyl radical (OH), form a key uncertainty in many greenhouse and other pollutant budgets, such as that of methane (CH4). Methyl chloroform (MCF) is an often-adopted tracer to indirectly put observational constraints on variations in OH. We investigated the budget of MCF in a 4DVAR inversion using the atmospheric transport model TM5, for the period 1998–2018, with the objective to derive information on interannual variations in OH and in its spatial distribution. We derived interannual variations in the global oxidation of MCF that bring simulated mole fractions of MCF within 1–2 % of the assimilated observations from the NOAA-GMD surface network at most sites. Additionally, the posterior simulations better reproduce aircraft observations used for independent validation. The derived OH variations showed robustness with respect to the prior MCF emissions and the prior OH distribution. The interannual variations were typically small (

scholarly journals Constraints and biases in a tropospheric two-box model of OH

2019 ◽  
Vol 19 (1) ◽  
pp. 407-424 ◽  
Author(s):  
Stijn Naus ◽  
Stephen A. Montzka ◽  
Sudhanshu Pandey ◽  
Sourish Basu ◽  
Ed J. Dlugokencky ◽  
...  
Keyword(s):  
Transport Model ◽  
Absolute Magnitude ◽  
Oxidative Capacity ◽  
Box Model ◽  
Surface Measurement ◽  
Positive Trend ◽  
Model Inversion ◽  
Methyl Chloroform ◽  
The Impact ◽  
Bias Corrections

Abstract. The hydroxyl radical (OH) is the main atmospheric oxidant and the primary sink of the greenhouse gas CH4. In an attempt to constrain atmospheric levels of OH, two recent studies combined a tropospheric two-box model with hemispheric-mean observations of methyl chloroform (MCF) and CH4. These studies reached different conclusions concerning the most likely explanation of the renewed CH4 growth rate, which reflects the uncertain and underdetermined nature of the problem. Here, we investigated how the use of a tropospheric two-box model can affect the derived constraints on OH due to simplifying assumptions inherent to a two-box model. To this end, we derived species- and time-dependent quantities from a full 3-D transport model to drive two-box model simulations. Furthermore, we quantified differences between the 3-D simulated tropospheric burden and the burden seen by the surface measurement network of the National Oceanic and Atmospheric Administration (NOAA). Compared to commonly used parameters in two-box models, we found significant deviations in the magnitude and time-dependence of the interhemispheric exchange rate, exposure to OH, and stratospheric loss rate. For MCF these deviations can be large due to changes in the balance of its sources and sinks over time. We also found that changes in the yearly averaged tropospheric burden of CH4 and MCF can be obtained within 0.96 ppb yr−1 and 0.14 % yr−1 by the NOAA surface network, but that substantial systematic biases exist in the interhemispheric mixing ratio gradients that are input to two-box model inversions. To investigate the impact of the identified biases on constraints on OH, we accounted for these biases in a two-box model inversion of MCF and CH4. We found that the sensitivity of interannual OH anomalies to the biases is modest (1 %–2 %), relative to the uncertainties on derived OH (3 %–4 %). However, in an inversion where we implemented all four bias corrections simultaneously, we found a shift to a positive trend in OH concentrations over the 1994–2015 period, compared to the standard inversion. Moreover, the absolute magnitude of derived global mean OH, and by extent, that of global CH4 emissions, was affected much more strongly by the bias corrections than their anomalies (∼10 %). Through our analysis, we identified and quantified limitations in the two-box model approach as well as an opportunity for full 3-D simulations to address these limitations. However, we also found that this derivation is an extensive and species-dependent exercise and that the biases were not always entirely resolvable. In future attempts to improve constraints on the atmospheric oxidative capacity through the use of simple models, a crucial first step is to consider and account for biases similar to those we have identified for the two-box model.

scholarly journals Ambiguity in the causes for decadal trends in atmospheric methane and hydroxyl

2017 ◽  
Vol 114 (21) ◽  
pp. 5367-5372 ◽  
Author(s):  
Alexander J. Turner ◽  
Christian Frankenberg ◽  
Paul O. Wennberg ◽  
Daniel J. Jacob
Keyword(s):  
Greenhouse Gas ◽  
Recent Literature ◽  
Atmospheric Methane ◽  
Model Inversion ◽  
Sources And Sinks ◽  
Methyl Chloroform ◽  
Competing Hypotheses ◽  
Time Invariant ◽  
Global Mean ◽  
Methane Concentrations

Methane is the second strongest anthropogenic greenhouse gas and its atmospheric burden has more than doubled since 1850. Methane concentrations stabilized in the early 2000s and began increasing again in 2007. Neither the stabilization nor the recent growth are well understood, as evidenced by multiple competing hypotheses in recent literature. Here we use a multispecies two-box model inversion to jointly constrain 36 y of methane sources and sinks, using ground-based measurements of methane, methyl chloroform, and the C13/C12 ratio in atmospheric methane (δ13CH4) from 1983 through 2015. We find that the problem, as currently formulated, is underdetermined and solutions obtained in previous work are strongly dependent on prior assumptions. Based on our analysis, the mathematically most likely explanation for the renewed growth in atmospheric methane, counterintuitively, involves a 25-Tg/y decrease in methane emissions from 2003 to 2016 that is offset by a 7% decrease in global mean hydroxyl (OH) concentrations, the primary sink for atmospheric methane, over the same period. However, we are still able to fit the observations if we assume that OH concentrations are time invariant (as much of the previous work has assumed) and we then find solutions that are largely consistent with other proposed hypotheses for the renewed growth of atmospheric methane since 2007. We conclude that the current surface observing system does not allow unambiguous attribution of the decadal trends in methane without robust constraints on OH variability, which currently rely purely on methyl chloroform data and its uncertain emissions estimates.

scholarly journals Estimating the Earth’s Outgoing Longwave Radiation Measured from a Moon-Based Platform

2021 ◽  
Vol 13 (11) ◽  
pp. 2201
Author(s):  
Hanlin Ye ◽  
Huadong Guo ◽  
Guang Liu ◽  
Jinsong Ping ◽  
Lu Zhang ◽  
...  
Keyword(s):  
Outgoing Longwave Radiation ◽  
Large Scale ◽  
Single Point ◽  
Longwave Radiation ◽  
Earth Observation ◽  
Artificial Satellites ◽  
Earth Observations ◽  
The Earth ◽  
Observation Geometry ◽  
Global Mean

Moon-based Earth observations have attracted significant attention across many large-scale phenomena. As the only natural satellite of the Earth, and having a stable lunar surface as well as a particular orbit, Moon-based Earth observations allow the Earth to be viewed as a single point. Furthermore, in contrast with artificial satellites, the varied inclination of Moon-based observations can improve angular samplings of specific locations on Earth. However, the potential for estimating the global outgoing longwave radiation (OLR) from the Earth with such a platform has not yet been fully explored. To evaluate the possibility of calculating OLR using specific Earth observation geometry, we constructed a model to estimate Moon-based OLR measurements and investigated the potential of a Moon-based platform to acquire the necessary data to estimate global mean OLR. The primary method of our study is the discretization of the observational scope into various elements and the consequent integration of the OLR of all elements. Our results indicate that a Moon-based platform is suitable for global sampling related to the calculation of global mean OLR. By separating the geometric and anisotropic factors from the measurement calculations, we ensured that measured values include the effects of the Moon-based Earth observation geometry and the anisotropy of the scenes in the observational scope. Although our results indicate that higher measured values can be achieved if the platform is located near the center of the lunar disk, a maximum difference between locations of approximately 9 × 10−4 W m−2 indicates that the effect of location is too small to remarkably improve observation performance of the platform. In conclusion, our analysis demonstrates that a Moon-based platform has the potential to provide continuous, adequate, and long-term data for estimating global mean OLR.

Drivers of (non-)linear Eocene surface warming in the DeepMIP ensemble

2021 ◽  
Author(s):  
Sebastian Steinig ◽  
Jiang Zhu ◽  
Ran Feng ◽  
Keyword(s):  
Temperature Gradient ◽  
Heat Transport ◽  
Climate Sensitivity ◽  
Radiative Forcing ◽  
Large Scale ◽  
Surface Albedo ◽  
Early Eocene ◽  
Meridional Heat Transport ◽  
Surface Warming ◽  
Global Mean

&lt;p&gt;The early Eocene greenhouse represents the warmest interval of the Cenozoic and therefore provides a unique opportunity to understand how the climate system operates under elevated atmospheric CO&lt;sub&gt;2&lt;/sub&gt; levels similar to those projected for the end of the 21st century. Early Eocene geological records indicate a large increase in global mean surface temperatures compared to present day (by ~14&amp;#176;C) and a greatly reduced meridional temperature gradient (by ~30% in SST). However, reproducing these large-scale climate features at reasonable CO&lt;sub&gt;2&lt;/sub&gt; levels still poses a challenge for current climate models. Recent modelling studies indicate an important role for shortwave (SW) cloud feedbacks to drive increases in climate sensitivity with global warming, which helps to close the gap between simulated and reconstructed Eocene global warmth and temperature gradient. Nevertheless, the presence of such state-dependent feedbacks and their relative strengths in other models remain unclear.&lt;/p&gt;&lt;p&gt;In this study, we perform a systematic investigation of the simulated surface warming and the underlying mechanisms in the recently published DeepMIP ensemble. The DeepMIP early Eocene simulations use identical paleogeographic boundary conditions and include six models with suitable output: CESM1.2_CAM5, GFDL_CM2.1, HadCM3B_M2.1aN, IPSLCM5A2, MIROC4m and NorESM1_F. We advance previous energy balance analysis by applying the approximate partial radiative perturbation (APRP) technique to quantify the individual contributions of surface albedo, cloud and non-cloud atmospheric changes to the simulated Eocene top-of-the-atmosphere SW flux anomalies. We further compare the strength of these planetary albedo feedbacks to changes in the longwave atmospheric emissivity and meridional heat transport in the warm Eocene climate. Particular focus lies in the sensitivity of the feedback strengths to increasing global mean temperatures in experiments at a range of atmospheric CO&lt;sub&gt;2&lt;/sub&gt; concentrations between x1 to x9 preindustrial levels.&lt;/p&gt;&lt;p&gt;Preliminary results indicate that all models that provide data for at least 3 different CO&lt;sub&gt;2&lt;/sub&gt; levels show an increase of the equilibrium climate sensitivity at higher global mean temperatures. This is associated with an increase of the overall strength of the positive SW cloud feedback with warming in those models. This nonlinear behavior seems to be related to both a reduction and optical thinning of low-level clouds, albeit with intermodel differences in the relative importance of the two mechanisms. We further show that our new APRP results can differ significantly from previous estimates based on cloud radiative forcing alone, especially in high-latitude areas with large surface albedo changes. We also find large intermodel variability and state-dependence in meridional heat transport modulated by changes in the atmospheric latent heat transport. Ongoing work focuses on the spatial patterns of the climate feedbacks and the implications for the simulated meridional temperature gradients.&lt;/p&gt;

Form Follows Experience - Notes on the Functionality of Footbridges

2021 ◽  
Author(s):  
Michel Schreinemachers ◽  
Wiebe Strick
Keyword(s):  
The Netherlands ◽  
Large Scale ◽  
Water Levels ◽  
Added Value ◽  
Highway Bridge ◽  
Or Efficiency ◽  
Pedestrian Bridges ◽  
The City ◽  
Prime Location ◽  
Natural Way

<p>Should a bridge always be functional and accessible? Should it always fulfil its purpose? This seemingly self- evident question is a key question in footbridge design that is oriented towards creating experiences.</p><p>Footbridges are able to successfully enriches our experience of a certain context or landscape, it cannot be functional all the time, under all environmental conditions, weather and seasons. A good example is the Zalige bridge designed as part of the Room for the River, a large-scale national program for inland flood- protection in the Netherlands. Build upon the floodplains within a newly created river-park by the city of Nijmegen, the Zalige bridge’s curved shape stands in direct relationship to the fluctuating water levels of the river. When water levels rise, the bridge partially submerges, becoming only accessible through steppingstones. At peak heights, the bridge disappears completely, becoming a metaphor for our relationship to the water.</p><p>“Building a bridge that fails to fulfil its sole purpose of containing the water; this can only be pulled off in the Netherlands.” – jury Dutch Design Awards about the Zalige bridge.</p><p>The loss of functionality is directly related to the creation of an experience. When the water levels rose in January 2018, the bridge became the prime location to experience the changing landscape. It shows that engineering a bridge is not solely focussed on the most efficient engineering, but for the purpose it fulfils as for society. For most pedestrian bridges where the perception of the user is on a different level as for a highway bridge, functionality provides more than just cost driven or efficiency driven parameters. It is more related to the added value for the community. When design not solemnly derives from the sheer taste and predilection of the designer but is based on the user’s experience, it generates a durable relation with a feeling of ownership of its users. The key is to create this experience in an elegant and natural way and not forced or dictated. It should be people's own unique discovery and should not be imposed.</p>

scholarly journals Analysis of a rapid increase of stratospheric ozone during late austral summer 2008 over Kerguelen (49.4° S, 70.3° E)

2011 ◽  
Vol 11 (1) ◽  
pp. 363-373 ◽  
Author(s):  
H. Bencherif ◽  
L. El Amraoui ◽  
G. Kirgis ◽  
J. Leclair De Bellevue ◽  
A. Hauchecorne ◽  
...  
Keyword(s):  
Potential Vorticity ◽  
Large Scale ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Three Dimensional ◽  
Austral Summer ◽  
Air Masses ◽  
Global Mapping ◽  
The Tropics

Abstract. This paper reports on an increase of ozone event observed over Kerguelen (49.4° S, 70.3° E) in relationship with large-scale isentropic transport. This is evidenced by ground-based observations (co-localised radiosonde and SAOZ experiments) together with satellite global observations (Aura/MLS) assimilated into MOCAGE, a Méteo-France model. The study is based on the analyses of the first ozonesonde experiment never recorded at the Kerguelen site within the framework of a French campaign called ROCK that took place from April to August 2008. Comparisons and interpretations of the observed event are supported by co-localised SAOZ observations, by global mapping of tracers (O3, N2O and columns of O3) from Aura/MLS and Aura/OMI experiments, and by model simulations of Ertel Potential Vorticity initialised by the ECMWF (European Centre for Medium-Range Weather Forecasts) data reanalyses. Satellite and ground-based observational data revealed a consistent increase of ozone in the local stratosphere by mid-April 2008. Additionally, Ozone (O3) and nitrous oxide (N2O) profiles obtained during January–May 2008 using the Microwave Limb Sounder (MLS) aboard the Aura satellite are assimilated into MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle), a global three-dimensional chemistry transport model of Météo-France. The assimilated total O3 values are consistent with SAOZ ground observations (within ±5%), and isentropic distributions of O3 match well with maps of advected potential vorticity (APV) derived from the MIMOSA model, a high-resolution advection transport model, and from the ECMWF reanalysis. The event studied seems to be related to the isentropic transport of air masses that took place simultaneously in the lower- and middle-stratosphere, respectively from the polar region and from the tropics to the mid-latitudes. In fact, the ozone increase observed by mid April 2008 resulted simultaneously: (1) from an equator-ward departure of polar air masses characterised with a high-ozone layer in the lower stratosphere (near the 475 K isentropic level), and (2) from a reverse isentropic transport from the tropics to mid- and high-latitudes in the upper stratosphere (nearby the 700 K level). The increase of ozone observed over Kerguelen from the 16-April ozonesonde profile is thus attributed to a concomitant isentropic transport of ozone in two stratospheric layers: the tropical air moving southward and reaching over Kerguelen in the upper stratosphere, and the polar air passing over the same area but in the lower stratosphere.

scholarly journals Evolution of the Distribution of Upper-Tropospheric Humidity over the Indian Ocean: Connection with Large-Scale Advection and Local Cloudiness

2017 ◽  
Vol 56 (7) ◽  
pp. 2035-2052 ◽  
Author(s):  
Thomas Garot ◽  
Hélène Brogniez ◽  
Renaud Fallourd ◽  
Nicolas Viltard
Keyword(s):  
Indian Ocean ◽  
Large Scale ◽  
Transport Model ◽  
Intraseasonal Variability ◽  
Back Trajectory ◽  
Time Step ◽  
Air Masses ◽  
Upper Troposphere ◽  
Upper Tropospheric Humidity ◽  
The Indian Ocean

AbstractThe spatial and temporal distribution of upper-tropospheric humidity (UTH) observed by the Sounder for Atmospheric Profiling of Humidity in the Intertropics by Radiometry (SAPHIR)/Megha-Tropiques radiometer is analyzed over two subregions of the Indian Ocean during October–December over 2011–14. The properties of the distribution of UTH were studied with regard to the phase of the Madden–Julian oscillation (active or suppressed) and large-scale advection versus local production of moisture. To address these topics, first, a Lagrangian back-trajectory transport model was used to assess the role of the large-scale transport of air masses in the intraseasonal variability of UTH. Second, the temporal evolution of the distribution of UTH is analyzed using the computation of the higher moments of its probability distribution function (PDF) defined for each time step over the domain. The results highlight significant differences in the PDF of UTH depending on the phase of the MJO. The modeled trajectories ending in the considered domain originate from an area that strongly varies depending on the phases of the MJO: during the active phases, the air masses are spatially constrained within the tropical Indian Ocean domain, whereas a distinct upper-tropospheric (200–150 hPa) westerly flow guides the intraseasonal variability of UTH during the suppressed phases. Statistical relationships between the cloud fractions and the UTH PDF moments of are found to be very similar regardless of the convective activity. However, the occurrence of thin cirrus clouds is associated with a drying of the upper troposphere (enhanced during suppressed phases), whereas the occurrence of thick cirrus anvil clouds appears to be significantly related to a moistening of the upper troposphere.

Sign in / Sign up

Export Citation Format

Share Document