We present a comprehensive description and benchmark evaluation of the tropospheric chemistry version of the global chemistry transport model TM5 (Tracer Model 5, version TM5-chem-v3.0). A full ...description is given concerning the photochemical mechanism, the interaction with aerosol, the treatment of the stratosphere, the wet and dry deposition parameterizations, and the applied emissions. We evaluate the model against a suite of ground-based, satellite, and aircraft measurements of components critical for understanding global photochemistry for the year 2006. The model exhibits a realistic oxidative capacity at a global scale. The methane lifetime is ~8.9 years with an associated lifetime of methyl chloroform of 5.86 years, which is similar to that derived using an optimized hydroxyl radical field. The seasonal cycle in observed carbon monoxide (CO) is well simulated at different regions across the globe. In the Northern Hemisphere CO concentrations are underestimated by about 20 ppbv in spring and 10 ppbv in summer, which is related to missing chemistry and underestimated emissions from higher hydrocarbons, as well as to uncertainties in the seasonal variation of CO emissions. The model also captures the spatial and seasonal variation in formaldehyde tropospheric columns as observed by SCIAMACHY. Positive model biases over the Amazon and eastern United States point to uncertainties in the isoprene emissions as well as its chemical breakdown. Simulated tropospheric nitrogen dioxide columns correspond well to observations from the Ozone Monitoring Instrument in terms of its seasonal and spatial variability (with a global spatial correlation coefficient of 0.89), but TM5 fields are lower by 25–40%. This is consistent with earlier studies pointing to a high bias of 0–30% in the OMI retrievals, but uncertainties in the emission inventories have probably also contributed to the discrepancy. TM5 tropospheric nitrogen dioxide profiles are in good agreement (within ~0.1 ppbv) with in situ aircraft observations from the INTEX-B campaign over (the Gulf of) Mexico. The model reproduces the spatial and seasonal variation in background surface ozone concentrations and tropospheric ozone profiles from the World Ozone and Ultraviolet Radiation Data Centre to within 10 ppbv, but at several tropical stations the model tends to underestimate ozone in the free troposphere. The presented model results benchmark the TM5 tropospheric chemistry version, which is currently in use in several international cooperation activities, and upon which future model improvements will take place.
Using both thermal infrared (TIR) and near infrared (NIR) channels of MOPITT (Measurements of Pollution in the Troposphere) on EOS‐Terra, we demonstrate the first coincident multispectral retrievals ...of carbon monoxide (CO) from space. Exploiting both TIR and NIR channels has been possible due to recent progress in characterizing NIR channel radiance errors. This has allowed us to trade off sensitivity to near surface CO for larger random errors in the combined retrieval. By examining retrieval diagnostics such as DFS (degrees of freedom for signal) and averaging kernels for the multispectral retrieval (TIR + NIR) as compared to the TIR‐only retrieval, we find that adding the NIR channel to the retrieval significantly increases sensitivity to CO, especially near the surface, but with high spatial variability due to surface albedo variations. The cases with the largest increases in DFS are over regions with low thermal contrast between the surface and lower atmosphere. In the tropics (23.4°S–23.4°N), the fraction of daytime land cases with at least 0.4 DFS in the surface layer (surface to 800 hPa) is 20% for TIR‐only retrievals compared to 59% for multispectral retrievals. Vertical resolution for the surface layer is also improved, in some cases from around 6 km for TIR‐only to roughly 1 km for TIR + NIR. Since we apply a single a priori CO profile (unlike MOPITT V4) and error covariance in all the retrievals reported here, these increases are due solely to the addition of the NIR channel. Enhanced sensitivity to near surface CO is especially evident in a case study for central/east Asia where source regions for urban areas with high population density are clearly identifiable. Although these retrievals are still a research product and require further validation and scientific evaluation, they demonstrate the increased sensitivity to CO in the lowermost troposphere that can be obtained from multispectral MOPITT data.
Ozone (O3) profiles recorded over Beijing from 1995 to 2005 by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program were analyzed to provide a first climatology of ...tropospheric O3 over Beijing and the North China Plains (NCPs), one of the most populated and polluted regions in China. A pooled method was adopted in the data analysis to reduce the influence of irregular sampling frequency. The tropospheric O3 over Beijing shows a seasonal and vertical distribution typical of mid-latitude locations in the Northern Hemisphere, but has higher daytime concentrations in the lower troposphere, when compared to New York City, Tokyo, and Paris at similar latitude. The tropospheric O3 over Beijing exhibits a common summer maximum and a winter minimum, with a broad summer maximum in the middle troposphere and a narrower early summer (June) peak in the lower troposphere. Examination of meteorological and satellite data suggests that the lower tropospheric O3 maximum in June is a result of strong photochemical production, transport of regional pollution, and possibly also more intense burnings of biomass in Central-Eastern China. Trajectory analysis indicates that in summer the regional pollution from the NCPs, maybe mixed with urban plumes from Beijing, played important roles on the high O3 concentrations in the boundary layer, but had limited impact on the O3 concentrations in the middle troposphere. A comparison of the data recorded before and after 2000 reveals that O3 in the lower troposphere over Beijing had a strong positive trend (approximately 2% per year from 1995 to 2005) in contrast to a flat or a decreasing trend over Tokyo, New York City, and Paris, indicating worsening photochemical pollution in Beijing and the NCPs.
High‐altitude ozone measurements at the Jungfraujoch observatory, Switzerland (JFJ, 3850 asl), covering the period 1990–2008 are investigated in this study. Anthropogenic ozone precursor emissions ...decreased over Europe and North America since the early 1990s. However, ozone concentrations at JFJ over the 19 year period show significant positive trends in the 1990s and no significant trends after 1999. Ozone trends were further studied with respect to air mass origin using 20 day back trajectories. The ozone increase during winter was particularly large in air masses with recent contact with the European planetary boundary layer (PBL), most probably in response to the steady decrease in European NO emissions leading to less ozone titration. On the other hand, the corresponding summer ozone increase was small, possibly attributable to the balancing effects of decreasing European ozone precursor emissions and increasing baseline ozone concentrations. Ozone from all source regions other than European PBL has a similar temporal pattern, exhibiting an increase for about the first 10 years, then leveling off to either no trend or insignificant decrease. This suggests that the physical processes determining the trend are beyond the time scale of the used backward trajectories or not described adequately by the simplified transport description in individual trajectories.
Key Points
Ozone at Jungfraujoch in 1990–2008 was investigated
Ozone trends shift from positive in 1990s to no significant trends afterward
Trends in individual source regions show similar pattern
The objective of this paper is to deliver the most accurate ozone (O3) and carbon monoxide (CO) climatology for the pure troposphere only, i.e. exclusively from the ground to the dynamical tropopause ...on an individual profile basis. The results (profiles and columns) are derived solely from the Measurements of OZone and water vapour by in-service Alrbus airCraft programme (MOZAIC) over 15 years (1994–2009). The study, focused on the northern mid-latitudes 24–50° N and 119° W–140° E, includes more than 40 000 profiles over 11 sites to give a quasi-global zonal picture. Considering all the sites, the pure tropospheric column peak-to-peak seasonal cycle ranges are 23.7–43.2 DU for O3 and 1.7–6.9 × 10 18 molecules cm−2 for CO. The maxima of the seasonal cycles are not in phase, occurring in February–April for CO and May–July for O3. The phase shift is related to the photochemistry and OH removal efficiencies. The purely tropospheric seasonal profiles are characterized by a typical autumn–winter/spring–summer O3 dichotomy (except in Los Angeles, Eastmed – a cluster of Cairo and Tel Aviv – and the regions impacted by the summer monsoon) and a summer–autumn/winter–spring CO dichotomy. We revisit the boundary-layer, mid-tropospheric (MT) and upper-tropospheric (UT) partial columns using a~new monthly varying MT ceiling. Interestingly, the seasonal cycle maximum of the UT partial columns is shifted from summer to spring for O3 and to very early spring for CO. Conversely, the MT maximum is shifted from spring to summer and is associated with a summer (winter) MT thickening (thinning). Lastly, the pure tropospheric seasonal cycles derived from our analysis are consistent with the cycles derived from spaceborne measurements, the correlation coefficients being r=0.6–0.9 for O3 and r>0.9 for CO. The cycles observed from space are nevertheless greater than MOZAIC for O3 (by 9–18 DU) and smaller for CO (up to 1 × 10 18 molecules cm−2). The larger winter O3 difference between the two data sets suggests probable stratospheric contamination in satellite data due to the tropopause position. The study underlines the importance of rigorously discriminating between the stratospheric and tropospheric reservoirs and avoiding use of a~monthly averaged tropopause position without this strict discrimination in order to assess the pure O3 and CO tropospheric trends.
We present our new measurement of the cross-section for charm dimuon production in neutrino–iron interactions based upon the full statistics collected by the NOMAD experiment. After background ...subtraction we observe 15 344 charm dimuon events, providing the largest sample currently available. The analysis exploits the large inclusive charged current sample – about 9×106 events after all analysis cuts – and the high resolution NOMAD detector to constrain the total systematic uncertainty on the ratio of charm dimuon to inclusive Charged Current (CC) cross-sections to ∼2%. We also perform a fit to the NOMAD data to extract the charm production parameters and the strange quark sea content of the nucleon within the NLO QCD approximation. We obtain a value of mc(mc)=1.159±0.075 GeV/c2 for the running mass of the charm quark in the MS¯ scheme and a strange quark sea suppression factor of κs=0.591±0.019 at Q2=20 GeV2/c2.
The precise measurement of forces is one way to obtain deep insight into the fundamental interactions present in nature. In the context of neutral antimatter, the gravitational interaction is of high ...interest, potentially revealing new forces that violate the weak equivalence principle. Here we report on a successful extension of a tool from atom optics--the moiré deflectometer--for a measurement of the acceleration of slow antiprotons. The setup consists of two identical transmission gratings and a spatially resolving emulsion detector for antiproton annihilations. Absolute referencing of the observed antimatter pattern with a photon pattern experiencing no deflection allows the direct inference of forces present. The concept is also straightforwardly applicable to antihydrogen measurements as pursued by the AEgIS collaboration. The combination of these very different techniques from high energy and atomic physics opens a very promising route to the direct detection of the gravitational acceleration of neutral antimatter.
Comparisons of aircraft measurements of carbon monoxide (CO) to the retrievals of CO using observations from the Measurements of Pollution in The Troposphere (MOPITT) instrument onboard the Terra ...satellite are presented. Observations made as part of the NASA INTEX-B and NSF MIRAGE field campaigns during March–May 2006 are used to validate the MOPITT CO retrievals, along with routine samples from 2001 through 2006 from NOAA and the MOZAIC measurements from commercial aircraft. A significant positive bias, around 20% for total column CO, in MOPITT CO was found in the comparison to in situ measurements during 2006. Comparisons to the long-term records of measurements from NOAA and MOZAIC revealed an increasing bias in the V3 MOPITT CO retrievals over time. The impact of an instrumental drift is illustrated through retrieval simulations.
We assimilate stratospheric ozone profiles from MLS (Microwave Limb Sounder) into the MOCAGE Chemistry Transport Model (CTM) to study Stratosphere-Troposphere Exchange (STE). This study uses two ...horizontal grid resolutions of 2° and 0.2°. The combined impacts of MLS ozone assimilation and high horizontal resolution are illustrated in two case studies where STE events occurred (23 June 2009 and 17 July 2009). At high resolution the filamentary structures of stratospheric air which characterise STE events are captured by the model. To test the impact of the assimilation and the resolution, we compare model outputs from different experiments (high resolution and low resolution; MLS assimilation run and free run) with independent data (MOZAIC aircraft ozone data; WOUDC ozone sonde network data). MLS ozone analyses show a better description of the Upper Troposphere Lower Stratosphere (UTLS) region and the stratospheric intrusions than the free model run. In particular, at high horizontal resolution the MLS ozone analyses present realistic filamentary ozone structures in the UTLS and laminae structures in the ozone profile. Despite a low aspect ratio between horizontal resolution and vertical resolution in the UTLS at high horizontal resolution, MLS ozone analyses improve the vertical structures of the ozone fields. Results from backward trajectories and ozone forecasts show that assimilation at high horizontal resolution of MLS ozone profiles between 10 hPa and 215 hPa has an impact on tropospheric ozone.
Measurements of carbon monoxide (CO) made as part of three aircraft experiments during the summer of 2004 over North America have been used for the continued validation of the CO retrievals from the ...Measurements of Pollution in the Troposphere (MOPITT) instrument on board the Terra satellite. Vertical profiles measured during the NASA INTEX‐A campaign, designed to be coincident with MOPITT overpasses, as well as measurements made during the COBRA‐2004 and MOZAIC experiments, provided valuable validation comparisons. On average, the MOPITT CO retrievals are biased slightly high for these North America locations. While the mean bias differs between the different aircraft experiments (e.g., 7.0 ppbv for MOZAIC to 18.4 ppbv for COBRA at 700 hPa), the standard deviations are quite large, so the results for the three data sets can be considered consistent. On average, it is estimated that MOPITT is 7–14% high at 700 hPa and ∼3% high at 350 hPa. These results are consistent with the validation results for the Carr, Colorado, Harvard Forest, Massachusetts, and Poker Flats, Alaska, aircraft profiles for “phase 2” presented by Emmons et al. (2004) and are generally within the design criteria of 10% accuracy.
PDF
