For the past decade, observations of carbonyl sulfide (OCS or COS) have been investigated as a proxy for carbon uptake by plants. OCS is destroyed by enzymes that interact with CO2 during photosynthesis, namely carbonic anhydrase (CA) and RuBisCO, where CA is the more important one. The majority of sources of OCS to the atmosphere are geographically separated from this large plant sink, whereas the sources and sinks of CO2 are co-located in ecosystems. The drawdown of OCS can therefore be related to the uptake of CO2 without the added complication of co-located emissions comparable in magnitude. Here we review the state of our understanding of the global OCS cycle and its applications to ecosystem carbon cycle science. OCS uptake is correlated well to plant carbon uptake, especially at the regional scale. OCS can be used in conjunction with other independent measures of ecosystem function, like solar-induced fluorescence and carbon and water isotope studies. More work needs to be done to generate global coverage for OCS observations and to link this powerful atmospheric tracer to systems where fundamental questions concerning the carbon and water cycle remain.
17 April 2020 in Atmospheric Chemistry and Physics
The Copernicus Atmosphere Monitoring Service (CAMS) operated by the European Centre for Medium-Range Weather Forecasts (ECMWF) has produced a global reanalysis of aerosol and reactive gases (called CAMSRA) for the period 2003–2016. Space observations of ozone, carbon monoxide, NO2 and aerosol optical depth are assimilated by a 4D-Var method in the 60-layer ECMWF global atmospheric model, which for the reanalysis is operated at a horizontal resolution of about 80 km. As a contribution to the evaluation of the reanalysis, we compare atmospheric concentrations of different reactive species provided by the CAMS reanalysis with independent observational data gathered by airborne instrumentation during the field campaigns INTEX-A, INTEX-B, NEAQS-ITCT, ITOP, AMMA, ARCTAS, VOCALS, YAK-AEROSIB, HIPPO and KORUS-AQ. We show that the reanalysis rather successfully reproduces the observed concentrations of chemical species that are assimilated in the system, including O3 and CO with biases generally less than 20 %, but generally underestimates the concentrations of the primary hydrocarbons and secondary organic species. In some cases, large discrepancies also exist for fast-reacting radicals such as OH and HO2.
To perform realistic high-resolution air quality modeling in a polluted urban area, the Weather Research and Forecasting (WRF) model is used with an embedded large-eddy simulation (LES) module and online chemistry. As an illustration, a numerical experiment is conducted in the megacity of Hong Kong, which is characterized by multi-type inhomogeneous pollution sources and complex topography. The results from the multi-resolution simulations at mesoscale and LES scales are evaluated by comparing them with ozone sounding profiles and surface observations. The comparisons show that both mesoscale and LES simulations reproduce the mean concentrations of the chemical species and their diurnal variations at the background stations well. However, the mesoscale simulations largely underestimate the NOx concentrations and overestimate O3 at the roadside stations due to the coarse representation of the traffic emissions. The LES simulations improve the agreement with the measurements near the road traffic, and the LES with the highest spatial resolution (33.3 m) provides the best results. The large-eddy simulations show more detailed structures in the spatial distributions of chemical species than the mesoscale simulations, highlighting the capability of LES to resolve high-resolution photochemical transformations in urban areas. Compared to the mesoscale model results, the LES simulations show similar evolutions in the profiles of the chemical species as a function of the boundary layer development over a diurnal cycle.
25 February 2016 in Atmospheric Chemistry and Physics
Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world.
28 July 2022 in International Journal of Heat and Mass Transfer
We investigate factors that drive the variability in total column CO2 at the Total Carbon Column Observing Network sites in the Southern Hemisphere using fluxes tagged by process and by source region from the CarbonTracker analysed product as well as the Simple Biosphere model. We show that the terrestrial biosphere is the largest driver of variability in the Southern Hemisphere column CO2. However, it does not dominate in the same fashion as in the Northern Hemisphere. Local- and hemispheric-scale biomass burning can also play an important role, particularly at the tropical site, Darwin. The magnitude of seasonal variability in the column-average dry-air mole fraction of CO2, XCO2, is also much smaller in the Southern Hemisphere and comparable in magnitude to the annual increase. Comparison of measurements to the model simulations highlights that there is some discrepancy between the two time series, especially in the early part of the Darwin data record. We show that this mismatch is most likely due to erroneously estimated local fluxes in the Australian tropical region, which are associated with enhanced photosynthesis caused by early rainfall during the tropical monsoon season.