ALBERT

Beschreibung: Halogenated very short-lived substances (VSLSs), such as bromoform (CHBr3), can be transported to the stratosphere and contribute to the halogen loading and ozone depletion. Given their highly variable emission rates and their short atmospheric lifetimes, the exact amount as well as the spatio-temporal variability of their contribution to the stratospheric halogen loading are still uncertain. We combine observational data sets with Lagrangian atmospheric modelling in order to analyse the spatial and temporal variability of the CHBr3 injection into the stratosphere for the time period 1979–2013. Regional maxima with mixing ratios of up to 0.4–0.5 ppt at 17 km altitude are diagnosed to be over Central America (1) and over the Maritime Continent–west Pacific (2), both of which are confirmed by high-altitude aircraft campaigns. The CHBr3 maximum over Central America is caused by the co-occurrence of convectively driven short transport timescales and strong regional sources, which in conjunction drive the seasonality of CHBr3 injection. Model results at a daily resolution reveal isolated, exceptionally high CHBr3 values in this region which are confirmed by aircraft measurements during the ACCENT campaign and do not occur in spatially or temporally averaged model fields. CHBr3 injection over the west Pacific is centred south of the Equator due to strong oceanic sources underneath prescribed by the here-applied bottom-up emission inventory. The globally largest CHBr3 mixing ratios at the cold point level of up to 0.6 ppt are diagnosed to occur over the region of India, Bay of Bengal, and Arabian Sea (3); however, no data from aircraft campaigns are available to confirm this finding. Inter-annual variability of stratospheric CHBr3 injection of 10 %–20 % is to a large part driven by the variability of coupled ocean–atmosphere circulation systems. Long-term changes, on the other hand, correlate with the regional sea surface temperature trends resulting in positive trends of stratospheric CHBr3 injection over the west Pacific and Asian monsoon region and negative trends over the east Pacific. For the tropical mean, these opposite regional trends balance each other out, resulting in a relatively weak positive trend of 0.017±0.012 ppt Br per decade for 1979–2013, corresponding to 3 % Br per decade. The overall contribution of CHBr3 together with CH2Br2 to the stratospheric halogen loading accounts for 4.7 ppt Br, in good agreement with existing studies, with 50 % and 50 % being injected in the form of source and product gases, respectively.

Beschreibung: We examine differences among reanalysis high-cloud products in the tropics, assess the impacts of these differences on radiation budgets at the top of the atmosphere and within the tropical upper troposphere and lower stratosphere (UTLS), and discuss their possible origins in the context of the reanalysis models. We focus on the ERA5 (fifth-generation European Centre for Medium-range Weather Forecasts – ECMWF – reanalysis), ERA-Interim (ECMWF Interim Reanalysis), JRA-55 (Japanese 55-year Reanalysis), MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, Version 2), and CFSR/CFSv2 (Climate Forecast System Reanalysis/Climate Forecast System Version 2) reanalyses. As a general rule, JRA-55 produces the smallest tropical high-cloud fractions and cloud water contents among the reanalyses, while MERRA-2 produces the largest. Accordingly, long-wave cloud radiative effects are relatively weak in JRA-55 and relatively strong in MERRA-2. Only MERRA-2 and ERA5 among the reanalyses produce tropical-mean values of outgoing long-wave radiation (OLR) close to those observed, but ERA5 tends to underestimate cloud effects, while MERRA-2 tends to overestimate variability. ERA5 also produces distributions of long-wave, short-wave, and total cloud radiative effects at the top of the atmosphere that are very consistent with those observed. The other reanalyses all exhibit substantial biases in at least one of these metrics, although compensation between the long-wave and short-wave effects helps to constrain biases in the total cloud radiative effect for most reanalyses. The vertical distribution of cloud water content emerges as a key difference between ERA-Interim and other reanalyses. Whereas ERA-Interim shows a monotonic decrease of cloud water content with increasing height, the other reanalyses all produce distinct anvil layers. The latter is in better agreement with observations and yields very different profiles of radiative heating in the UTLS. For example, whereas the altitude of the level of zero net radiative heating tends to be lower in convective regions than in the rest of the tropics in ERA-Interim, the opposite is true for the other four reanalyses. Differences in cloud water content also help to explain systematic differences in radiative heating in the tropical lower stratosphere among the reanalyses. We discuss several ways in which aspects of the cloud and convection schemes impact the tropical environment. Discrepancies in the vertical profiles of temperature and specific humidity in convective regions are particularly noteworthy, as these variables are directly constrained by data assimilation, are widely used, and feed back to convective behaviour through their relationships with thermodynamic stability.

Beschreibung: The tropical tropopause layer (TTL) is the transition region between the well-mixed convective troposphere and the radiatively controlled stratosphere with air masses showing chemical and dynamical properties of both regions. The representation of the TTL in meteorological reanalysis data sets is important for studying the complex interactions of circulation, convection, trace gases, clouds, and radiation. In this paper, we present the evaluation of climatological and long-term TTL temperature and tropopause characteristics in the reanalysis data sets ERA-Interim, ERA5, JRA-25, JRA-55, MERRA, MERRA-2, NCEP-NCAR (R1), and CFSR. The evaluation has been performed as part of the SPARC (Stratosphere–troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The most recent atmospheric reanalysis data sets (ERA-Interim, ERA5, JRA-55, MERRA-2, and CFSR) all provide realistic representations of the major characteristics of the temperature structure within the TTL. There is good agreement between reanalysis estimates of tropical mean temperatures and radio occultation data, with relatively small cold biases for most data sets. Temperatures at the cold point and lapse rate tropopause levels, on the other hand, show warm biases in reanalyses when compared to observations. This tropopause-level warm bias is related to the vertical resolution of the reanalysis data, with the smallest bias found for data sets with the highest vertical resolution around the tropopause. Differences in the cold point temperature maximize over equatorial Africa, related to Kelvin wave activity and associated disturbances in TTL temperatures. Interannual variability in reanalysis temperatures is best constrained in the upper TTL, with larger differences at levels below the cold point. The reanalyses reproduce the temperature responses to major dynamical and radiative signals such as volcanic eruptions and the quasi-biennial oscillation (QBO). Long-term reanalysis trends in temperature in the upper TTL show good agreement with trends derived from adjusted radiosonde data sets indicating significant stratospheric cooling of around −0.5 to −1 K per decade. At 100 hPa and the cold point, most of the reanalyses suggest small but significant cooling trends of −0.3 to −0.6 K per decade that are statistically consistent with trends based on the adjusted radiosonde data sets. Advances of the reanalysis and observational systems over the last decades have led to a clear improvement in the TTL reanalysis products over time. Biases of the temperature profiles and differences in interannual variability clearly decreased in 2006, when densely sampled radio occultation data started being assimilated by the reanalyses. While there is an overall good agreement, different reanalyses offer different advantages in the TTL such as realistic profile and cold point temperature, continuous time series, or a realistic representation of signals of interannual variability. Their use in model simulations and in comparisons with climate model output should be tailored to their specific strengths and weaknesses.

Beschreibung: A suite of oxygenated volatile organic compounds (OVOCs – acetaldehyde, acetone, propanal, butanal and butanone) were measured concurrently in the surface water and atmosphere of the South China Sea and Sulu Sea in November 2011. A strong correlation was observed between all OVOC concentrations in the surface seawater along the entire cruise track, except for acetaldehyde, suggesting similar sources and sinks in the surface ocean. Additionally, several phytoplankton groups, such as haptophytes or pelagophytes, were also correlated to all OVOCs, indicating that phytoplankton may be an important source of marine OVOCs in the South China and Sulu seas. Humic- and protein-like fluorescent dissolved organic matter (FDOM) components seemed to be additional precursors for butanone and acetaldehyde. The measurement-inferred OVOC fluxes generally showed an uptake of atmospheric OVOCs by the ocean for all gases, except for butanal. A few important exceptions were found along the Borneo coast, where OVOC fluxes from the ocean to the atmosphere were inferred. The atmospheric OVOC mixing ratios over the northern coast of Borneo were relatively high compared with literature values, suggesting that this coastal region is a local hotspot for atmospheric OVOCs. The calculated amount of OVOCs entrained into the ocean seemed to be an important source of OVOCs to the surface ocean. When the fluxes were out of the ocean, marine OVOCs were found to be enough to control the locally measured OVOC distribution in the atmosphere. Based on our model calculations, at least 0.4 ppb of marine-derived acetone and butanone can reach the upper troposphere, where they may have an important influence on hydrogen oxide radical formation over the western Pacific Ocean.

Beschreibung: The impact of changes in incoming solar irradiance on stratospheric ozone abundances should be included in climate simulations to aid in capturing the atmospheric response to solar cycle variability. This study presents the first systematic comparison of the representation of the 11-year solar cycle ozone response (SOR) in chemistry–climate models (CCMs) and in pre-calculated ozone databases specified in climate models that do not include chemistry, with a special focus on comparing the recommended protocols for the Coupled Model Intercomparison Project Phase 5 and Phase 6 (CMIP5 and CMIP6). We analyse the SOR in eight CCMs from the Chemistry–Climate Model Initiative (CCMI-1) and compare these with results from three ozone databases for climate models: the Bodeker Scientific ozone database, the SPARC/Atmospheric Chemistry and Climate (AC&C) ozone database for CMIP5 and the SPARC/CCMI ozone database for CMIP6. The peak amplitude of the annual mean SOR in the tropical upper stratosphere (1–5 hPa) decreases by more than a factor of 2, from around 5 to 2 %, between the CMIP5 and CMIP6 ozone databases. This substantial decrease can be traced to the CMIP5 ozone database being constructed from a regression model fit to satellite and ozonesonde measurements, while the CMIP6 database is constructed from CCM simulations. The SOR in the CMIP6 ozone database therefore implicitly resembles the SOR in the CCMI-1 models. The structure in latitude of the SOR in the CMIP6 ozone database and CCMI-1 models is considerably smoother than in the CMIP5 database, which shows unrealistic sharp gradients in the SOR across the middle latitudes owing to the paucity of long-term ozone measurements in polar regions. The SORs in the CMIP6 ozone database and the CCMI-1 models show a seasonal dependence with enhanced meridional gradients at mid- to high latitudes in the winter hemisphere. The CMIP5 ozone database does not account for seasonal variations in the SOR, which is unrealistic. Sensitivity experiments with a global atmospheric model without chemistry (ECHAM6.3) are performed to assess the atmospheric impacts of changes in the representation of the SOR and solar spectral irradiance (SSI) forcing between CMIP5 and CMIP6. The larger amplitude of the SOR in the CMIP5 ozone database compared to CMIP6 causes a likely overestimation of the modelled tropical stratospheric temperature response between 11-year solar cycle minimum and maximum by up to 0.55 K, or around 80 % of the total amplitude. This effect is substantially larger than the change in temperature response due to differences in SSI forcing between CMIP5 and CMIP6. The results emphasize the importance of adequately representing the SOR in global models to capture the impact of the 11-year solar cycle on the atmosphere. Since a number of limitations in the representation of the SOR in the CMIP5 ozone database have been identified, we recommend that CMIP6 models without chemistry use the CMIP6 ozone database and the CMIP6 SSI dataset to better capture the climate impacts of solar variability. The SOR coefficients from the CMIP6 ozone database are published with this paper.

Beschreibung: 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.

Beschreibung: Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. When transported to the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise on RV Sonne in the subtropical and tropical west Indian Ocean in July and August 2014, we measured the VSLSs, methyl iodide (CH3I) and for the first time bromoform (CHBr3) and dibromomethane (CH2Br2), in surface seawater and the marine atmosphere to derive their emission strengths. Using the Lagrangian particle dispersion model FLEXPART with ERA-Interim meteorological fields, we calculated the direct contribution of observed VSLS emissions to the stratospheric halogen burden during the Asian summer monsoon. Furthermore, we compare the in situ calculations with the interannual variability of transport from a larger area of the west Indian Ocean surface to the stratosphere for July 2000–2015. We found that the west Indian Ocean is a strong source for CHBr3 (910 pmol m−2 h−1), very strong source for CH2Br2 (930 pmol m−2 h−1), and an average source for CH3I (460 pmol m−2 h−1). The atmospheric transport from the tropical west Indian Ocean surface to the stratosphere experiences two main pathways. On very short timescales, especially relevant for the shortest-lived compound CH3I (3.5 days lifetime), convection above the Indian Ocean lifts oceanic air masses and VSLSs towards the tropopause. On a longer timescale, the Asian summer monsoon circulation transports oceanic VSLSs towards India and the Bay of Bengal, where they are lifted with the monsoon convection and reach stratospheric levels in the southeastern part of the Asian monsoon anticyclone. This transport pathway is more important for the longer-lived brominated compounds (17 and 150 days lifetime for CHBr3 and CH2Br2). The entrainment of CHBr3 and CH3I from the west Indian Ocean to the stratosphere during the Asian summer monsoon is lower than from previous cruises in the tropical west Pacific Ocean during boreal autumn and early winter but higher than from the tropical Atlantic during boreal summer. In contrast, the projected CH2Br2 entrainment was very high because of the high emissions during the west Indian Ocean cruise. The 16-year July time series shows highest interannual variability for the shortest-lived CH3I and lowest for the longest-lived CH2Br2. During this time period, a small increase in VSLS entrainment from the west Indian Ocean through the Asian monsoon to the stratosphere is found. Overall, this study confirms that the subtropical and tropical west Indian Ocean is an important source region of halogenated VSLSs, especially CH2Br2, to the troposphere and stratosphere during the Asian summer monsoon.

Beschreibung: The climate research community uses atmospheric reanalysis data sets to understand a wide range of processes and variability in the atmosphere, yet different reanalyses may give very different results for the same diagnostics. The Stratosphere–troposphere Processes And their Role in Climate (SPARC) Reanalysis Intercomparison Project (S-RIP) is a coordinated activity to compare reanalysis data sets using a variety of key diagnostics. The objectives of this project are to identify differences among reanalyses and understand their underlying causes, to provide guidance on appropriate usage of various reanalysis products in scientific studies, particularly those of relevance to SPARC, and to contribute to future improvements in the reanalysis products by establishing collaborative links between reanalysis centres and data users. The project focuses predominantly on differences among reanalyses, although studies that include operational analyses and studies comparing reanalyses with observations are also included when appropriate. The emphasis is on diagnostics of the upper troposphere, stratosphere, and lower mesosphere. This paper summarizes the motivation and goals of the S-RIP activity and extensively reviews key technical aspects of the reanalysis data sets that are the focus of this activity. The special issue The SPARC Reanalysis Intercomparison Project (S-RIP) in this journal serves to collect research with relevance to the S-RIP in preparation for the publication of the planned two (interim and full) S-RIP reports.