scholarly journals Evaluation of simulated photochemical partitioning of oxidized nitrogen in the upper troposphere

2010 ◽  
Vol 10 (8) ◽  
pp. 20125-20165 ◽  
Author(s):  
B. H. Henderson ◽  
R. W. Pinder ◽  
J. Crooks ◽  
R. C. Cohen ◽  
W. T. Hutzell ◽  
...  

Abstract. Regional and global chemical transport models underpredict NOx (NO+NO2) in the upper troposphere where it is a precursor to the greenhouse gas ozone. The NOx bias been shown in model evaluations using aircraft data (Singh et al., 2007) and total column NO2 (molecules cm−2) from satellite observations (Napelenok et al., 2008). The causes of NOx underpredictions have yet to be fully understood due to the interconnected nature of simulated emission, transport, and chemistry processes. Recent observation-based studies suggest that, in the upper troposphere, simulated chemistry overpredicts hydrogen radicals (OH• and HO2•) and would convert NOx to HNO3 too quickly (Olson et al., 2006; Bertram et al., 2007; Ren et al., 2008). Since typical chemistry evaluation techniques are not available for upper tropospheric conditions, this study develops an evaluation platform from in situ observations, stochastic convection, and deterministic chemistry. We derive a stochastic convection model and optimize it using two simulated datasets of time since convection, one based on meteorology and the other on chemistry. The chemistry surrogate for time since convection is calculated using seven different chemical mechanisms, all of which predict shorter time since convection than our meteorological analysis. We evaluate chemical simulations by inter-comparison and by pairing results with observations based on NOx:HNO3, a photochemical aging indicator. Inter-comparison reveals individual chemical mechanism biases and recommended updates. Evaluation against observations shows that all chemical mechanisms overpredict NOx removal relative to long-lived methanol and carbon monoxide. All chemical mechanisms underpredict observed NOx by at least 30%, and further evaluation is necessary to refine simulation sensitivities to initial conditions and chemical rate uncertainties.

2011 ◽  
Vol 11 (1) ◽  
pp. 275-291 ◽  
Author(s):  
B. H. Henderson ◽  
R. W. Pinder ◽  
J. Crooks ◽  
R. C. Cohen ◽  
W. T. Hutzell ◽  
...  

Abstract. Regional and global chemical transport models underpredict NOx (NO + NO2) in the upper troposphere where it is a precursor to the greenhouse gas ozone. The NOx bias has been shown in model evaluations using aircraft data (Singh et al., 2007) and total column NO2 (molecules cm−2) from satellite observations (Napelenok et al., 2008). The causes of NOx underpredictions have yet to be fully understood due to the interconnected nature of simulated emission, transport, and chemistry processes. Recent observation-based studies, in the upper troposphere, identify chemical rate coefficients as a potential source of error (Olson et al., 2006; Ren et al., 2008). Since typical chemistry evaluation techniques are not available for upper tropospheric conditions, this study develops an evaluation platform from in situ observations, stochastic convection, and deterministic chemistry. We derive a stochastic convection model and optimize it using two simulated datasets of time since convection, one based on meteorology, and the other on chemistry. The chemistry surrogate for time since convection is calculated using seven different chemical mechanisms, all of which predict shorter time since convection than our meteorological analysis. We evaluate chemical simulations by inter-comparison and by pairing results with observations based on NOx:HNO3, a photochemical aging indicator. Inter-comparison reveals individual chemical mechanism biases and recommended updates. Evaluation against observations shows that all chemical mechanisms overpredict NOx removal relative to long-lived methanol and carbon monoxide. All chemical mechanisms underpredict observed NOx by at least 30%, and further evaluation is necessary to refine simulation sensitivities to initial conditions and chemical rate uncertainties.


2019 ◽  
Vol 491 (4) ◽  
pp. 5595-5620 ◽  
Author(s):  
Sanson T S Poon ◽  
Richard P Nelson ◽  
Seth A Jacobson ◽  
Alessandro Morbidelli

ABSTRACT The NASA’s Kepler mission discovered ∼700 planets in multiplanet systems containing three or more transiting bodies, many of which are super-Earths and mini-Neptunes in compact configurations. Using N-body simulations, we examine the in situ, final stage assembly of multiplanet systems via the collisional accretion of protoplanets. Our initial conditions are constructed using a subset of the Kepler five-planet systems as templates. Two different prescriptions for treating planetary collisions are adopted. The simulations address numerous questions: Do the results depend on the accretion prescription?; do the resulting systems resemble the Kepler systems, and do they reproduce the observed distribution of planetary multiplicities when synthetically observed?; do collisions lead to significant modification of protoplanet compositions, or to stripping of gaseous envelopes?; do the eccentricity distributions agree with those inferred for the Kepler planets? We find that the accretion prescription is unimportant in determining the outcomes. The final planetary systems look broadly similar to the Kepler templates adopted, but the observed distributions of planetary multiplicities or eccentricities are not reproduced, because scattering does not excite the systems sufficiently. In addition, we find that ∼1 per cent of our final systems contain a co-orbital planet pair in horseshoe or tadpole orbits. Post-processing the collision outcomes suggests that they would not significantly change the ice fractions of initially ice-rich protoplanets, but significant stripping of gaseous envelopes appears likely. Hence, it may be difficult to reconcile the observation that many low-mass Kepler planets have H/He envelopes with an in situ formation scenario that involves giant impacts after dispersal of the gas disc.


2012 ◽  
Vol 53 (60) ◽  
pp. 257-266 ◽  
Author(s):  
E. Rignot ◽  
I. Fenty ◽  
D. Menemenlis ◽  
Y. Xu

AbstractWe examine the pattern of spreading of warm subtropical-origin waters around Greenland for the years 1992–2009 using a high-resolution (4km horizontal grid) coupled ocean and sea-ice simulation. The simulation, provided by the Estimating the Circulation and Climate of the Ocean, Phase II (ECCO2) project, qualitatively reproduces the observed warming of subsurface waters in the subpolar gyre associated with changes of the North Atlantic atmospheric state that occurred in the mid-1990s. The modeled subsurface ocean temperature warmed by 1.5˚C in southeast and southwest Greenland during 1994–2005 and subsequently cooled by 0.5˚C; modeled subsurface ocean temperature increased by 2–2.5˚C in central and then northwest Greenland during 1997–2005 and stabilized thereafter, while it increased after 2005 by <0.5˚C in north Greenland. Comparisons with in situ measurements off the continental shelf in the Labrador and Irminger Seas indicate that the model initial conditions were 0.4˚C too warm in the south but the simulated warming is correctly reproduced; while measurements from eastern Baffin Bay reveal that the model initial conditions were 1.0˚C too cold in the northwest but the simulated ocean warming brought modeled temperature closer to observations, i.e. the simulated warming is 1.0˚C too large. At several key locations, the modeled oceanic changes off the shelf and below the seasonal mixed layer were rapidly transmitted to the shelf within troughs towards (model-unresolved) fjords. Unless blocked in the fjords by shallow sills, these warm subsurface waters had potential to propagate down the fjords and melt the glacier fronts. Based on model sensitivity simulations from an independent study (Xu and others, 2012), we show that the oceanic changes have very likely increased the subaqueous melt rates of the glacier fronts, and in turn impacted the rates of glacier flow.


2014 ◽  
Vol 53 (6) ◽  
pp. 1416-1432 ◽  
Author(s):  
R. D. Sharman ◽  
L. B. Cornman ◽  
G. Meymaris ◽  
J. Pearson ◽  
T. Farrar

AbstractThe statistical properties of turbulence at upper levels in the atmosphere [upper troposphere and lower stratosphere (UTLS)] are still not well known, partly because of the lack of adequate routine observations. This is despite the obvious benefit that such observations would have for alerting aircraft of potentially hazardous conditions, either in real time or for route planning. To address this deficiency, a research project sponsored by the Federal Aviation Administration has developed a software package that automatically estimates and reports atmospheric turbulence intensity levels (as EDR ≡ ε1/3, where ε is the energy or eddy dissipation rate). The package has been tested and evaluated on commercial aircraft. The amount of turbulence data gathered from these in situ reports is unprecedented. As of January 2014, there are ~200 aircraft outfitted with this system, contributing to over 137 million archived records of EDR values through 2013, most of which were taken at cruise levels of commercial aircraft, that is, in the UTLS. In this paper, techniques used for estimating EDR are outlined and comparisons with pilot reports from the same or nearby aircraft are presented. These reports allow calibration of EDR in terms of traditionally reported intensity categories (“light,” “moderate,” or “severe”). The results of some statistical analyses of EDR values are also presented. These analyses are restricted to the United States for now, but, as this program is expanded to international carriers, such data will begin to become available over other areas of the globe.


2015 ◽  
Vol 15 (13) ◽  
pp. 7667-7684 ◽  
Author(s):  
Fuqing Zhang ◽  
Junhong Wei ◽  
Meng Zhang ◽  
K. P. Bowman ◽  
L. L. Pan ◽  
...  

Abstract. This study analyzes in situ airborne measurements from the 2008 Stratosphere–Troposphere Analyses of Regional Transport (START08) experiment to characterize gravity waves in the extratropical upper troposphere and lower stratosphere (ExUTLS). The focus is on the second research flight (RF02), which took place on 21–22 April 2008. This was the first airborne mission dedicated to probing gravity waves associated with strong upper-tropospheric jet–front systems. Based on spectral and wavelet analyses of the in situ observations, along with a diagnosis of the polarization relationships, clear signals of mesoscale variations with wavelengths ~ 50–500 km are found in almost every segment of the 8 h flight, which took place mostly in the lower stratosphere. The aircraft sampled a wide range of background conditions including the region near the jet core, the jet exit and over the Rocky Mountains with clear evidence of vertically propagating gravity waves of along-track wavelength between 100 and 120 km. The power spectra of the horizontal velocity components and potential temperature for the scale approximately between ~ 8 and ~ 256 km display an approximate −5/3 power law in agreement with past studies on aircraft measurements, while the fluctuations roll over to a −3 power law for the scale approximately between ~ 0.5 and ~ 8 km (except when this part of the spectrum is activated, as recorded clearly by one of the flight segments). However, at least part of the high-frequency signals with sampled periods of ~ 20–~ 60 s and wavelengths of ~ 5–~ 15 km might be due to intrinsic observational errors in the aircraft measurements, even though the possibilities that these fluctuations may be due to other physical phenomena (e.g., nonlinear dynamics, shear instability and/or turbulence) cannot be completely ruled out.


2011 ◽  
Vol 11 (5) ◽  
pp. 1961-1977 ◽  
Author(s):  
J. Flemming ◽  
A. Inness ◽  
L. Jones ◽  
H. J. Eskes ◽  
V. Huijnen ◽  
...  

Abstract. The 2008 Antarctic ozone hole was one of the largest and most long-lived in recent years. Predictions of the ozone hole were made in near-real time (NRT) and hindcast mode with the Integrated Forecast System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The forecasts were carried out both with and without assimilation of satellite observations from multiple instruments to provide more realistic initial conditions. Three different chemistry schemes were applied for the description of stratospheric ozone chemistry: (i) a linearization of the ozone chemistry, (ii) the stratospheric chemical mechanism of the Model of Ozone and Related Chemical Tracers, version 3, (MOZART-3) and (iii) the relaxation to climatology as implemented in the Transport Model, version 5, (TM5). The IFS uses the latter two schemes by means of a two-way coupled system. Without assimilation, the forecasts showed model-specific shortcomings in predicting start time, extent and duration of the ozone hole. The assimilation of satellite observations from the Microwave Limb Sounder (MLS), the Ozone Monitoring Instrument (OMI), the Solar Backscattering Ultraviolet radiometer (SBUV-2) and the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY) led to a significant improvement of the forecasts when compared with total columns and vertical profiles from ozone sondes. The combined assimilation of observations from multiple instruments helped to overcome limitations of the ultraviolet (UV) sensors at low solar elevation over Antarctica. The assimilation of data from MLS was crucial to obtain a good agreement with the observed ozone profiles both in the polar stratosphere and troposphere. The ozone analyses by the three model configurations were very similar despite the different underlying chemistry schemes. Using ozone analyses as initial conditions had a very beneficial but variable effect on the predictability of the ozone hole over 15 days. The initialized forecasts with the MOZART-3 chemistry produced the best predictions of the increasing ozone hole whereas the linear scheme showed the best results during the ozonehole closure.


2015 ◽  
Vol 8 (6) ◽  
pp. 2473-2489 ◽  
Author(s):  
J. Ungermann ◽  
J. Blank ◽  
M. Dick ◽  
A. Ebersoldt ◽  
F. Friedl-Vallon ◽  
...  

Abstract. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 High Altitude LOng Range (HALO) research aircraft during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra that are spectrally sampled every 0.625 cm−1. A total of 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line of sight. Simultaneous in situ observations by the Basic Halo Measurement and Sensor System (BAHAMAS), the Fast In-situ Stratospheric Hygrometer (FISH), an ozone detector named Fairo, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in situ trace gas data, and discrepancies can to a large extent be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.


2017 ◽  
Author(s):  
Florian Berkes ◽  
Patrick Neis ◽  
Martin G. Schultz ◽  
Ulrich Bundke ◽  
Susanne Rohs ◽  
...  

Abstract. Despite several studies on temperature trends in the tropopause region, a comprehensive understanding of the evolution of temperatures in this climate-sensitive region of the atmosphere remains elusive. Here we present a unique global-scale, long-term data set of high-resolution in-situ temperature data measured aboard passenger aircraft within the European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System, www.iagos.org). This data set is used to investigate temperature trends within the global upper troposphere and lowermost stratosphere (UTLS) for the period 1995 to 2012 in different geographical regions and vertical layers of the UTLS. The largest amount of observations is available over the North Atlantic. Here, a neutral temperature trend is found within the lowermost stratosphere. This contradicts the temperature trend in the European Centre for Medium Range Weather Forecast (ECMWF) ERA-Interim reanalysis, where a significant (95 % confidence) temperature increase of +0.56 K/decade is obtained. Differences between trends derived from observations and reanalysis data can be traced back to changes in the temperature bias between observation and model data over the studied period. This study demonstrates the value of the IAGOS temperature observations as anchor point for the evaluation of reanalyses and its suitability for independent trend analyses.


2018 ◽  
Vol 11 (10) ◽  
pp. 4155-4174 ◽  
Author(s):  
Benjamin Brown-Steiner ◽  
Noelle E. Selin ◽  
Ronald Prinn ◽  
Simone Tilmes ◽  
Louisa Emmons ◽  
...  

Abstract. While state-of-the-art complex chemical mechanisms expand our understanding of atmospheric chemistry, their sheer size and computational requirements often limit simulations to short lengths or ensembles to only a few members. Here we present and compare three 25-year present-day offline simulations with chemical mechanisms of different levels of complexity using the Community Earth System Model (CESM) Version 1.2 CAM-chem (CAM4): the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) mechanism, the Reduced Hydrocarbon mechanism, and the Super-Fast mechanism. We show that, for most regions and time periods, differences in simulated ozone chemistry between these three mechanisms are smaller than the model–observation differences themselves. The MOZART-4 mechanism and the Reduced Hydrocarbon are in close agreement in their representation of ozone throughout the troposphere during all time periods (annual, seasonal, and diurnal). While the Super-Fast mechanism tends to have higher simulated ozone variability and differs from the MOZART-4 mechanism over regions of high biogenic emissions, it is surprisingly capable of simulating ozone adequately given its simplicity. We explore the trade-offs between chemical mechanism complexity and computational cost by identifying regions where the simpler mechanisms are comparable to the MOZART-4 mechanism and regions where they are not. The Super-Fast mechanism is 3 times as fast as the MOZART-4 mechanism, which allows for longer simulations or ensembles with more members that may not be feasible with the MOZART-4 mechanism given limited computational resources.


2021 ◽  
Author(s):  
Victor Lannuque ◽  
Bastien Sauvage ◽  
Brice Barret ◽  
Hannah Clark ◽  
Gilles Athier ◽  
...  

Abstract. Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the IASI instrument onboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10° from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5° N in DJFM and 128 to 149 ppb at 3–7° S in JJASO), and decreasing values south- and north-ward. The O3 meridional transects are characterized by mixing ratio minima of ~ 42–54 ppb at the ITCZ (10–16° S in DJFM and 5–8° N in JJASO) framed by local maxima (~ 53–71 ppb) coincident with the wind shear zones North and South of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution, drive the location of the observed UT CO maxima, and are related to the following transport pathway: CO emitted at the surface is transported towards the ITCZ by the trade winds and further convectively uplifted. Then UT CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maxima are located. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability, and is related to similar transport circulation than fire air masses. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high altitude air masses uplifted from either local or long distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO), and must be created during transport by photochemistry. This analysis of meridional transects contribute to a better understanding of distributions of CO and O3 in the intertropical African upper troposphere and the processes which drive these distributions. Therefore, it provides a solid basis for comparison and improvement of models and satellite products in order to get the good O3 for the good reasons.


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