Description: Reanalysis data sets are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. In this paper, we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere–troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. We also provide a systematic documentation of the treatment of WV and O3 in current reanalyses to aid future research and guide the interpretation of differences amongst reanalysis fields. The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. However, significant biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses. In contrast to O3, reanalysis estimates of stratospheric WV are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore mainly dependent on the reanalyses' representation of the physical drivers that influence stratospheric WV, such as temperatures in the tropical tropopause layer, methane oxidation, and the stratospheric overturning circulation. The lack of assimilated observations and known deficiencies in the representation of stratospheric transport in reanalyses result in much poorer agreement amongst observational and reanalysis estimates of stratospheric WV. Hence, stratospheric WV products from the current generation of reanalyses should generally not be used in scientific studies.

Description: A quality assessment of the CFC-11 (CCl3F), CFC-12 (CCl2F2), HF, and SF6 products from limb-viewing satellite instruments is provided by means of a detailed intercomparison. The climatologies in the form of monthly zonal mean time series are obtained from HALOE, MIPAS, ACE-FTS, and HIRDLS within the time period 1991–2010. The intercomparisons focus on the mean biases of the monthly and annual zonal mean fields and aim to identify their vertical, latitudinal and temporal structure. The CFC evaluations (based on MIPAS, ACE-FTS and HIRDLS) reveal that the uncertainty in our knowledge of the atmospheric CFC-11 and CFC-12 mean state, as given by satellite data sets, is smallest in the tropics and mid-latitudes at altitudes below 50 and 20 hPa, respectively, with a 1σ multi-instrument spread of up to ±5 %. For HF, the situation is reversed. The two available data sets (HALOE and ACE-FTS) agree well above 100 hPa, with a spread in this region of ±5 to ±10 %, while at altitudes below 100 hPa the HF annual mean state is less well known, with a spread ±30 % and larger. The atmospheric SF6 annual mean states derived from two satellite data sets (MIPAS and ACE-FTS) show only very small differences with a spread of less than ±5 % and often below ±2.5 %. While the overall agreement among the climatological data sets is very good for large parts of the upper troposphere and lower stratosphere (CFCs, SF6) or middle stratosphere (HF), individual discrepancies have been identified. Pronounced deviations between the instrument climatologies exist for particular atmospheric regions which differ from gas to gas. Notable features are differently shaped isopleths in the subtropics, deviations in the vertical gradients in the lower stratosphere and in the meridional gradients in the upper troposphere, and inconsistencies in the seasonal cycle. Additionally, long-term drifts between the instruments have been identified for the CFC-11 and CFC-12 time series. The evaluations as a whole provide guidance on what data sets are the most reliable for applications such as studies of atmospheric transport and variability, model–measurement comparisons and detection of long-term trends. The data sets will be publicly available from the SPARC Data Centre and through PANGAEA (doi:10.1594/PANGAEA.849223).

Description: The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated, simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993-2012). The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes.Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA’s long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements - including high altitude observations from the NASA Global Hawk platform. The models generally capture the seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model-measurement correlation (r ≥ 0.7) and a low sensitivity to the choice of emission inventory, at most sites. In a given model, the absolute model-measurement agreement is highly sensitive to the choice of emissions and inter-model differences are also apparent, even when using the same inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve optimal agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2 Br2). In general, the models are able to reproduce well observations of CHBr3 and CH2 Br2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr3 (and to a lesser extent CH2 Br2) most elevated over the tropical West Pacific during boreal winter. The models also indicate the Asian Monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr3 and CH2 Br2 of 2.0 (1.2-2.5) ppt, ≫ 57% larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. However, transport-driven inter-annual variability in the annual mean bromine SGI is of the order of a ±5%, with SGI exhibiting a strong positive correlation with ENSO in the East Pacific.

Description: Halocarbons are produced naturally in the oceans by biological and chemical processes. They are emitted from surface seawater into the atmosphere, where they take part in numerous chemical processes such as ozone destruction and the oxidation of mercury and dimethyl sulfide. Here we present oceanic and atmospheric halocarbon data for the Peruvian upwelling zone obtained during the M91 cruise onboard the research vessel METEOR in December 2012. Surface waters during the cruise were characterized by moderate concentrations of bromoform (CHBr3) and dibromomethane (CH2Br2) correlating with diatom biomass derived from marker pigment concentrations, which suggests this phytoplankton group is a likely source. Concentrations measured for the iodinated compounds methyl iodide (CH3I) of up to 35.4 pmol L−1, chloroiodomethane (CH2ClI) of up to 58.1 pmol L−1 and diiodomethane (CH2I2) of up to 32.4 pmol L−1 in water samples were much higher than previously reported for the tropical Atlantic upwelling systems. Iodocarbons also correlated with the diatom biomass and even more significantly with dissolved organic matter (DOM) components measured in the surface water. Our results suggest a biological source of these compounds as a significant driving factor for the observed large iodocarbon concentrations. Elevated atmospheric mixing ratios of CH3I (up to 3.2 ppt), CH2ClI (up to 2.5 ppt) and CH2I2 (3.3 ppt) above the upwelling were correlated with seawater concentrations and high sea-to-air fluxes. During the first part of the cruise, the enhanced iodocarbon production in the Peruvian upwelling contributed significantly to tropospheric iodine levels, while this contribution was considerably smaller during the second part.

Description: Changes in incoming solar ultraviolet radiation over the 11-year solar cycle affect stratospheric ozone abundances. It is important to quantify the magnitude, structure, and seasonality of the associated solar-ozone response (SOR) to understand the impact of the 11-year solar cycle on climate. Part 1 of this two-part study uses multiple linear regression analysis to extract the SOR in a number of recently updated satellite ozone datasets covering different periods within the epoch 1970 to 2013. The annual mean SOR in the updated version 7.0 (v7.0) Stratospheric Aerosol and Gas Experiment (SAGE) II number density dataset (1984–2004) is very consistent with that found in the previous v6.2. In contrast, we find a substantial decrease in the magnitude of the SOR in the tropical upper stratosphere in the SAGE II v7.0 mixing ratio dataset (∼ 1 %) compared to the v6.2 (∼ 4 %). This difference is shown to be largely attributable to the change in the independent stratospheric temperature dataset used to convert SAGE II ozone number densities to mixing ratios. Since these temperature records contain substantial uncertainties, we suggest that datasets based on SAGE II number densities are currently most reliable for evaluating the SOR. We further analyse three extended ozone datasets that combine SAGE II v7.0 number densities with more recent GOMOS (Global Ozone Monitoring by Occultation of Stars) or OSIRIS (Optical Spectrograph and Infrared Imager System) measurements. The extended SAGE–OSIRIS dataset (1984–2013) shows a smaller and less statistically significant SOR across much of the tropical upper stratosphere compared to the SAGE II data alone. In contrast, the two SAGE–GOMOS datasets (1984–2011) show SORs that are in closer agreement with the original SAGE II data and therefore appear to provide a more reliable estimate of the SOR. We also analyse the SOR in the recent Solar Backscatter Ultraviolet Instrument (SBUV) Merged Ozone Dataset (SBUVMOD) version 8.6 (VN8.6) (1970–2012) and SBUV Merged Cohesive VN8.6 (1978–2012) datasets and compare them to the previous SBUVMOD VN8.0 (1970–2009). Over their full lengths, the three records generally agree in terms of the broad magnitude and structure of the annual mean SOR. The main difference is that SBUVMOD VN8.6 shows a smaller and less significant SOR in the tropical upper stratosphere and therefore more closely resembles the SAGE II v7.0 mixing ratio data than does the SBUV Merged Cohesive VN8.6, which has a more continuous SOR of ∼ 2 % in this region. The sparse spatial and temporal sampling of limb satellite instruments prohibits the extraction of sub-annual variations in the SOR from SAGE-based datasets. However, the SBUVMOD VN8.6 dataset suggests substantial month-to-month variations in the SOR, particularly in the winter extratropics, which may be important for the proposed high-latitude dynamical response to the solar cycle. Overall, the results highlight substantial uncertainties in the magnitude and structure of the observed SOR from different satellite records. The implications of these uncertainties for understanding and modelling the effects of solar variability on climate should be explored.

Description: Halogenated organic compounds are naturally produced in the ocean and emitted to the atmosphere. The halogenated very short-lived substances (VSLS), such as bromoform, have atmospheric lifetimes of less than half a year. When VSLS reach the stratosphere, they enhance ozone depletion and thus impact the climate. During boreal summer, the Asian monsoon circulation transfers air masses from the Asian troposphere to the global stratosphere. Still, the extent to which VSLS from the Indian Ocean contribute to the stratospheric halogen burden and their exact origin is unclear. Here we show that the monsoon circulation transports VSLS from the Indian Ocean to the stratosphere. During the research cruises SO234-2 and SO235 in July-August 2014 onboard RV SONNE, we measured oceanic and atmospheric concentrations of bromoform (tropical lifetime at 10 km = 17 days), dibromomethane (150 days) and methyl iodide (3.5 days) in the subtropical and tropical West Indian Ocean and calculated their emission strengths. We use the Langrangian transport model FLEXPART driven by ERA-Interim meteorological fields to investigate the transport of oceanic emissions in the atmosphere. We analyze the direct contribution of observed bromoform emissions to the stratospheric halogen budget with forward trajectories. Furthermore, we investigate the connection between the Asian monsoon anticyclone and the oceanic source regions using backward trajectories. The West Indian Ocean is a strong source region of VSLS to the atmosphere and the monsoon transport is fast enough for bromoform to reach the stratosphere. However, the main source regions for the entrainment of oceanic air masses through the Asian monsoon anticyclone are the West Pacific and Bay of Bengal as well as the Arabian Sea. Our findings indicate that changes in emission or circulation in this area due to climate change can directly affect the stratospheric halogen burden and thus the ozone layer.