Stable isotope composition of atmospheric carbon monoxide : a modelling study

Stable isotope composition of atmospheric carbon monoxide: A modelling study.rnrnThis study aims at an improved understanding of the stable carbon and oxygen isotope composition of the carbon monoxide (CO) in the global atmosphere by means of numerical simulations. At first, a new kinetic chemistry tagging technique for the most complete parameterisation of isotope effects has been introduced into the Modular Earth Submodel System (MESSy) framework. Incorporated into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, an explicit treatment of the isotope effects on the global scale is now possible. The expanded model system has been applied to simulate the chemical system containing up to five isotopologues of all carbon- and oxygen-bearing species, which ultimately determine the δ13C, δ18O and Δ17O isotopic signatures of atmospheric CO. As model input, a new stable isotope-inclusive emission inventory for the relevant trace gases has been compiled. The uncertainties of the emission estimates and of the resulting simulated mixing and isotope ratios have been analysed. The simulated CO mixing and stable isotope ratios have been compared to in-situ measurements from ground-based observatories and from the civil-aircraft-mounted CARIBIC−1 measurement platform.rnrnThe systematically underestimated 13CO/12CO ratios of earlier, simplified modelling studies can now be partly explained. The EMAC simulations do not support the inferences of those studies, which suggest for CO a reduced input of the highly depleted in 13C methane oxidation source. In particular, a high average yield of 0.94 CO per reacted methane (CH4) molecule is simulated in the troposphere, to a large extent due to the competition between the deposition and convective transport processes affecting the CH4 to CO reaction chain intermediates. None of the other factors, assumed or disregarded in previous studies, however hypothesised to have the potential in enriching tropospheric CO in 13C, were found significant when explicitly simulated. The inaccurate surface emissions, likely underestimated over East Asia, are responsible for roughly half of the discrepancies between the simulated and observed 13CO in the northern hemisphere (NH), whereas the remote southern hemisphere (SH) compositions suggest an underestimated fractionation during the oxidation of CO by the hydroxyl radical (OH). A reanalysis of the kinetic isotope effect (KIE) in this reaction contrasts the conventional assumption of a mere pressure dependence, and instead suggests an additional temperature dependence of the 13C KIE, which is driven by changes in the partitioning of the reaction exit channels. This result is yet to be confirmed in the laboratory.rnrnApart from 13CO, for the first time the atmospheric distribution of the oxygen mass-independent fractionation (MIF) in CO, Δ17O, has been consistently simulated on the global scale with EMAC. The applicability of Δ17O(CO) observations to unravelling changes in the tropospheric CH4-CO-OH system has been scrutinised, as well as the implications of the ozone (O3) input to the CO isotope oxygen budget. The Δ17O(CO) is confirmed to be the principal signal for the CO photochemical age, thus providing a measure for the OH chiefly involved in the sink of CO. The highly mass-independently fractionated O3 oxygen is estimated to comprise around 2% of the overall tropospheric CO source, which has implications for the δ18O, but less likely for the Δ17O CO budgets. Finally, additional sensitivity simulations with EMAC corroborate the nearly equal net effects of the present-day CH4 and CO burdens in removing tropospheric OH, as well as the large turnover and stability of the abundance of the latter. The simulated CO isotopologues nonetheless hint at a likely insufficient OH regeneration in the NH high latitudes and the upper troposphere / lower stratosphere (UTLS).rn

Global simulated soil biogenic nitric oxide (NO) emissions: Impact, improvement and innovation

rnNitric oxide (NO) is important for several chemical processes in the atmosphere. Together with nitrogen dioxide (NO2 ) it is better known as nitrogen oxide (NOx ). NOx is crucial for the production and destruction of ozone. In several reactions it catalyzes the oxidation of methane and volatile organic compounds (VOCs) and in this context it is involved in the cycling of the hydroxyl radical (OH). OH is a reactive radical, capable of oxidizing most organic species. Therefore, OH is also called the “detergent” of the atmosphere. Nitric oxide originates from several sources: fossil fuel combustion, biomass burning, lightning and soils. Fossil fuel combustion is the largest source. The others are, depending on the reviewed literature, generally comparable to each other. The individual sources show a different temporal and spatial pattern in their magnitude of emission. Fossil fuel combustion is important in densely populated places, where NO from other sources is less important. In contrast NO emissions from soils (hereafter SNOx) or biomass burning are the dominant source of NOx in remote regions.rnBy applying an atmospheric chemistry global climate model (AC-GCM) I demonstrate that SNOx is responsible for a significant part of NOx in the atmosphere. Furthermore, it increases the O3 and OH mixing ratio substantially, leading to a ∼10% increase in the oxidizing efficiency of the atmosphere. Interestingly, through reduced O3 and OH mixing ratios in simulations without SNOx, the lifetime of NOx increases in regions with other dominating sources of NOx

Simulation of monsoon disturbances in the LMD GCM

The monsoon depressions that form over India during the summer are analyzed using simulations from the Laboratoire de Meteorologie Dynamique general circulation model. This type of synoptic system often occurs with a frequency of one to two per month and can produce a strong Indian rainfall. Two kinds of analyses are conducted in this study. The first one is a subjective analysis based on the evolution of the precipitation rate and the pattern of the sea level pressure. The second one is an objective analysis performed using the TRACK program, which identifies and tracks the minima in the sea level pressure anomaly held and computes the statistics for the distribution of systems. The analysis of a 9-yr control run, which simulates strong precipitation rates over the foothills of the Himalayas and over southern India but weak rates over central India, shows that the number of disturbances is coo low and that they almost never occur during August, when break conditions prevail. The generated disturbances more often move north, toward the foothills of the Himalayas. Another analysis is performed to study the effect of the Tibetan Plateau elevation on these disturbances with a 9-yr run carried out with a Tibetan Plateau at 50% of its current height. It is shown that this later integration simulates more frequent monsoon disturbances, which move rather northwestward, in agreement with the current observations. The comparison between the two runs shows that the June-July-August rainfall difference is in large part due to changes in the occurrence of the monsoon disturbances.

Enhancement of ENSO variability by a weakened Atlantic thermohaline circulation in a coupled GCM

A coupled ocean–atmosphere general circulation model is used to investigate the modulation of El Niño–Southern Oscillation (ENSO) variability due to a weakened Atlantic thermohaline circulation (THC). The THC weakening is induced by freshwater perturbations in the North Atlantic, and leads to a well-known sea surface temperature dipole and a southward shift of the intertropical convergence zone (ITCZ) in the tropical Atlantic. Through atmospheric teleconnections and local coupled air–sea feedbacks, a meridionally asymmetric mean state change is generated in the eastern equatorial Pacific, corresponding to a weakened annual cycle, and westerly anomalies develop over the central Pacific. The westerly anomalies are associated with anomalous warming of SST, causing an eastward extension of the west Pacific warm pool particularly in August–February, and enhanced precipitation. These and other changes in the mean state lead in turn to an eastward shift of the zonal wind anomalies associated with El Niño events, and a significant increase in ENSO variability. In response to a 1-Sv (1 Sv ≡ 106 m3 s−1) freshwater input in the North Atlantic, the THC slows down rapidly and it weakens by 86% over years 50–100. The Niño-3 index standard deviation increases by 36% during the first 100-yr simulation relative to the control simulation. Further analysis indicates that the weakened THC not only leads to a stronger ENSO variability, but also leads to a stronger asymmetry between El Niño and La Niña events. This study suggests a role for an atmospheric bridge that rapidly conveys the influence of the Atlantic Ocean to the tropical Pacific and indicates that fluctuations of the THC can mediate not only mean climate globally but also modulate interannual variability. The results may contribute to understanding both the multidecadal variability of ENSO activity during the twentieth century and longer time-scale variability of ENSO, as suggested by some paleoclimate records.

The Storm-Track Response to Idealized SST Perturbations in an Aquaplanet GCM

The tropospheric response to midlatitude SST anomalies has been investigated through a series of aquaplanet simulations using a high-resolution version of the Hadley Centre atmosphere model (HadAM3) under perpetual equinox conditions. Model integrations show that increases in the midlatitude SST gradient generally lead to stronger storm tracks that are shifted slightly poleward, consistent with changes in the lower-tropospheric baroclinicity. The large-scale atmospheric response is, however, highly sensitive to the position of the SST gradient anomaly relative to that of the subtropical jet in the unperturbed atmosphere. In particular, when SST gradients are increased very close to the subtropical jet, then the Hadley cell and subtropical jet is strengthened while the storm track and eddy-driven jet are shifted equatorward. Conversely, if the subtropical SST gradients are reduced and the midlatitude gradients increased, then the storm track shows a strong poleward shift and a well-separated eddy-driven jet is produced. The sign of the SST anomaly is shown to play a secondary role in determining the overall tropospheric response. These findings are used to provide a new and consistent interpretation of some previous GCM studies concerning the atmospheric response to midlatitude SST anomalies.

Decadal predictability of the Atlantic Ocean in a coupled GCM: forecast skill and optimal perturbations using Linear Inverse Modelling

The decadal predictability of three-dimensional Atlantic Ocean anomalies is examined in a coupled global climate model (HadCM3) using a Linear Inverse Modelling (LIM) approach. It is found that the evolution of temperature and salinity in the Atlantic, and the strength of the meridional overturning circulation (MOC), can be effectively described by a linear dynamical system forced by white noise. The forecasts produced using this linear model are more skillful than other reference forecasts for several decades. Furthermore, significant non-normal amplification is found under several different norms. The regions from which this growth occurs are found to be fairly shallow and located in the far North Atlantic. Initially, anomalies in the Nordic Seas impact the MOC, and the anomalies then grow to fill the entire Atlantic basin, especially at depth, over one to three decades. It is found that the structure of the optimal initial condition for amplification is sensitive to the norm employed, but the initial growth seems to be dominated by MOC-related basin scale changes, irrespective of the choice of norm. The consistent identification of the far North Atlantic as the most sensitive region for small perturbations suggests that additional observations in this region would be optimal for constraining decadal climate predictions.

Mean climate and transience in the tropics of the UGAMP GCM - sensitivity to convective parametrization

The sensitivity of the UK Universities Global Atmospheric Modelling Programme (UGAMP) General Circulation Model (UGCM) to two very different approaches to convective parametrization is described. Comparison is made between a Kuo scheme, which is constrained by large-scale moisture convergence, and a convective-adjustment scheme, which relaxes to observed thermodynamic states. Results from 360-day integrations with perpetual January conditions are used to describe the model's tropical time-mean climate and its variability. Both convection schemes give reasonable simulations of the time-mean climate, but the representation of the main modes of tropical variability is markedly different. The Kuo scheme has much weaker variance, confined to synoptic frequencies near 4 days, and a poor simulation of intraseasonal variability. In contrast, the convective-adjustment scheme has much more transient activity at all time-scales. The various aspects of the two schemes which might explain this difference are discussed. The particular closure on moisture convergence used in this version of the Kuo scheme is identified as being inappropriate.

Effect of ENSO phase on large-scale snow water equivalent distribution in a GCM

Understanding links between the El Nino-Southern Oscillation (ENSO) and snow would be useful for seasonal forecasting, but also for understanding natural variability and interpreting climate change predictions. Here, a 545-year run of the general circulation model HadCM3, with prescribed external forcings and fixed greenhouse gas concentrations, is used to explore the impact of ENSO on snow water equivalent (SWE) anomalies. In North America, positive ENSO events reduce the mean SWE and skew the distribution towards lower values, and vice versa during negative ENSO events. This is associated with a dipole SWE anomaly structure, with anomalies of opposite sign centered in western Canada and the central United States. In Eurasia, warm episodes lead to a more positively skewed distribution and the mean SWE is raised. Again, the opposite effect is seen during cold episodes. In Eurasia the largest anomalies are concentrated in the Himalayas. These correlations with February SWE distribution are seen to exist from the previous June-July-August (JJA) ENSO index onwards, and are weakly detected in 50-year subsections of the control run, but only a shifted North American response can be detected in the anaylsis of 40 years of ERA40 reanalysis data. The ENSO signal in SWE from the long run could still contribute to regional predictions although it would be a weak indicator only

Annular variability and eddy-zonal flow interactions in a simplified atmospheric GCM. Part 1: Characterization of high and low frequency behaviour

Experiments have been performed using a simplified, Newtonian forced, global circulation model to investigate how variability of the tropospheric jet can be characterized by examining the combined fluctuations of the two leading modes of annular variability. Eddy forcing of this variability is analyzed in the phase space of the leading modes using the vertically integrated momentum budget. The nature of the annular variability and eddy forcing depends on the time scale. At low frequencies the zonal flow and baroclinic eddies are in quasi equilibrium and anomalies propagate poleward. The eddies are shown primarily to reinforce the anomalous state and are closely balanced by the linear damping, leaving slow evolution as a residual. At high frequencies the flow is strongly evolving and anomalies are initiated on the poleward side of the tropospheric jet and propagate equatorward. The eddies are shown to drive this evolution strongly: eddy location and amplitude reflect the past baroclinicity, while eddy feedback on the zonal flow may be interpreted in terms of wave breaking associated with baroclinic life cycles in lateral shear.

Atmosphere feedbacks during ENSO in a coupled GCM with a modified atmospheric convection scheme

The too diverse representation of ENSO in a coupled GCM limits one’s ability to describe future change of its properties. Several studies pointed to the key role of atmosphere feedbacks in contributing to this diversity. These feedbacks are analyzed here in two simulations of a coupled GCM that differ only by the parameterization of deep atmospheric convection and the associated clouds. Using the Kerry–Emanuel (KE) scheme in the L’Institut Pierre-Simon Laplace Coupled Model, version 4 (IPSL CM4; KE simulation), ENSO has about the right amplitude, whereas it is almost suppressed when using the Tiedke (TI) scheme. Quantifying both the dynamical Bjerknes feedback and the heat flux feedback in KE, TI, and the corresponding Atmospheric Model Intercomparison Project (AMIP) atmosphere-only simulations, it is shown that the suppression of ENSO in TI is due to a doubling of the damping via heat flux feedback. Because the Bjerknes positive feedback is weak in both simulations, the KE simulation exhibits the right ENSO amplitude owing to an error compensation between a too weak heat flux feedback and a too weak Bjerknes feedback. In TI, the heat flux feedback strength is closer to estimates from observations and reanalysis, leading to ENSO suppression. The shortwave heat flux and, to a lesser extent, the latent heat flux feedbacks are the dominant contributors to the change between TI and KE. The shortwave heat flux feedback differences are traced back to a modified distribution of the large-scale regimes of deep convection (negative feedback) and subsidence (positive feedback) in the east Pacific. These are further associated with the model systematic errors. It is argued that a systematic and detailed evaluation of atmosphere feedbacks during ENSO is a necessary step to fully understand its simulation in coupled GCMs.

Using idealized snow forcing to test teleconnections with the Indian summer monsoon in the Hadley Centre GCM

Anomalous heavy snow during winter or spring has long been regarded as a possible precursor of deficient Indian monsoon rainfall during the subsequent summer. However previous work in this field is inconclusive, in terms of the mechanism that communicates snow anomalies to the monsoon summer, and even the region from which snow has the most impact. In this study we explore these issues in coupled and atmosphere-only versions of the Hadley Centre model. A 1050-year control integration of the HadCM3 coupled model, which well represents the seasonal cycle of snow cover over the Eurasian continent, is analysed and shows evidence for weakened monsoons being preceded by strong snow forcing (in the absence of ENSO) over either the Himalaya/Tibetan Plateau or north/west Eurasia regions. However, empirical orthogonal function (EOF) analysis of springtime interannual variability in snow depth shows the leading mode to have opposite signs between these two regions, suggesting that competing mechanisms may be possible. To determine the dominant region, ensemble integrations are carried out using HadAM3, the atmospheric component of HadCM3, and a variety of anomalous snow forcing initial conditions obtained from the control integration of the coupled model. Forcings are applied during spring in separate experiments over the Himalaya/Tibetan Plateau and north/west Eurasia regions, in conjunction with climatological SSTs in order to avoid the direct effects of ENSO. With the aid of idealized forcing conditions in sensitivity tests, we demonstrate that forcing from the Himalaya region is dominant in this model via a Blanford-type mechanism involving reduced surface sensible heat and longwave fluxes, reduced heating of the troposphere over the Tibetan Plateau and consequently a reduced meridional tropospheric temperature gradient which weakens the monsoon during early summer. Snow albedo is shown to be key to the mechanism, explaining around 50% of the perturbation in sensible heating over the Tibetan Plateau, and accounting for the majority of cooling through the troposphere.