Observing and modelling the impact of arctic and tropical cirrus clouds on far-infrared radiance spectra

The work described in this thesis concerns the effect of cirrus clouds on far-infrared (FIR) radiance spectra. Though the importance of both FIR radiation and cirrus clouds to the Earth’s energy budget is well recognised, few high spectral resolution measurements have been made at FIR wavelengths to date. Observations taken during two diverse field campaigns, along with spectra simulated using a radiative transfer model, are used here to investi- gate the FIR signature of cirrus. The FIR observations presented are made using the TAFTS spectrometer, which measures spectral radiances from ei- ther an aircraft or the ground. The deployment of TAFTS during the RHUBC campaign based in Barrow, Alaska is described. TAFTS was used to make ground-based FIR observations of the arctic atmosphere, both with and without cirrus. Comparing these with modelled spectra, which assume a parameterised particle size distribution (PSD) when describing the cirrus microphysics, suggested that the PSD parameterisation underestimates the fraction of ice water content contributed by small ice crystals. This conclusion is corroborated by AERI-ER observations made simultaneously at the Barrow site during RHUBC. TAFTS observations of convective tropical cirrus made during EMERALD- II near Darwin, Australia are also presented here. During EMERALD-II TAFTS was deployed on an aircraft, enabling spectral measurements of cirrus at wavenumbers between 100 and 200cm−1 to be made for the first time. Comparisons with LBLDIS spectra calculated using PSDs measured using cloud probes indicate that the number of small crystals measured may be too high by a factor of three. This result is in agreement with previous studies suggesting that small crystal populations are over-counted by in-situ cloud probes, due to shattering of larger crystals on the probe inlets. The results from both campaigns illustrate the sensitivity of FIR radiances to cirrus properties, with particular emphasis on the effect of small ice crystals

Evaluation of wetland CH4 in the Joint UK Land Environment Simulator (JULES) land surface model using satellite observations

Wetlands are the largest natural source of methane. The ability to model the emissions of methane from natural wetlands accurately is critical to our understanding of the global methane budget and how it may change under future climate scenarios. The simulation of wetland methane emissions involves a complicated system of meteorological drivers coupled to hydrological and biogeochemical processes. The Joint UK Land Environment Simulator (JULES) is a process-based land surface model that underpins the UK Earth System Model (UKESM) and is capable of generating estimates of wetland methane emissions. In this study, we use GOSAT satellite observations of atmospheric methane along with the TOMCAT global 3-D chemistry transport model to evaluate the performance of JULES in reproducing the seasonal cycle of methane over a wide range of tropical wetlands. By using an ensemble of JULES simulations with differing input data and process configurations, we investigate the relative importance of the meteorological driving data, the vegetation, the temperature dependency of wetland methane production and the wetland extent. We find that JULES typically performs well in replicating the observed methane seasonal cycle. We calculate correlation coefficients to the observed seasonal cycle of between 0.58 and 0.88 for most regions; however, the seasonal cycle amplitude is typically underestimated (by between 1.8 and 19.5 ppb). This level of performance is comparable to that typically provided by state-of-the-art data-driven wetland CH4 emission inventories. The meteorological driving data are found to be the most significant factor in determining the ensemble performance, with temperature dependency and vegetation having moderate effects. We find that neither wetland extent configuration outperforms the other, but this does lead to poor performance in some regions. We focus in detail on three African wetland regions (Sudd, Southern Africa and Congo) where we find the performance of JULES to be poor and explore the reasons for this in detail. We find that neither wetland extent configuration used is sufficient in representing the wetland distribution in these regions (underestimating the wetland seasonal cycle amplitude by 11.1, 19.5 and 10.1 ppb respectively, with correlation coefficients of 0.23, 0.01 and 0.31). We employ the Catchment-based Macro-scale Floodplain (CaMa-Flood) model to explicitly represent river and floodplain water dynamics and find that these JULES-CaMa-Flood simulations are capable of providing a wetland extent that is more consistent with observations in this regions, highlighting this as an important area for future model development.</p

Co-ordinated Airborne Studies in the Tropics (CAST)

This is the author accepted manuscript. The final version is available from the American Meteorological Society via http://dx.doi.org/10.1175/BAMS-D-14-00290.1The Co-ordinated Airborne Studies in the Tropics (CAST) project is studying the chemical composition of the atmosphere in the Tropical Warm Pool region to improve understanding of trace gas transport in convection. The main field activities of the CAST (Co-ordinated Airborne Studies in the Tropics) campaign took place in the West Pacific in January/February 2014. The field campaign was based in Guam (13.5°N, 144.8°E) using the UK FAAM BAe-146 atmospheric research aircraft and was coordinated with the ATTREX project with the unmanned Global Hawk and the CONTRAST campaign with the Gulfstream V aircraft. Together, the three aircraft were able to make detailed measurements of atmospheric structure and composition from the ocean surface to 20 km. These measurements are providing new information about the processes influencing halogen and ozone levels in the tropical West Pacific as well as the importance of trace gas transport in convection for the upper troposphere and stratosphere. The FAAM aircraft made a total of 25 flights between 1°S-14°N and 130°-155°E. It was used to sample at altitudes below 8 km with much of the time spent in the marine boundary layer. It measured a range of chemical species, and sampled extensively within the region of main inflow into the strong West Pacific convection. The CAST team also made ground-based measurements of a number of species (including daily ozonesondes) at the Atmospheric Radiation Measurement program site on Manus Island, Papua New Guinea (2.1°S, 147.4°E). This article presents an overview of the CAST project focussing on the design and operation of the West Pacific experiment. It additionally discusses some new developments in CAST, including flights of new instruments on the Global Hawk in February/March 2015.CAST is funded by NERC and STFC, with grant NE/ I030054/1 (lead award), NE/J006262/1, NE/J006238/1, NE/J006181/1, NE/J006211/1, NE/J006061/1, NE/J006157/1, NE/J006203/1, NE/J00619X/1, and NE/J006173/1. N. R. P. Harris was supported by a NERC Advanced Research Fellowship (NE/G014655/1). P. I. Palmer acknowledges his Royal Society Wolfson Research Merit Award. The BAe-146-301 Atmospheric Research Aircraft is flown by Directflight Ltd and managed by the Facility for Airborne Atmospheric Measurements, which is a joint entity of the Natural Environment Research Council and the Met Office. The authors thank the staff at FAAM, Directflight and Avalon Aero who worked so hard toward the success of the aircraft deployment in Guam, especially for their untiring efforts when spending an unforeseen 9 days in Chuuk. We thank the local staff at Chuuk and Palau, as well as the authorities in the Federated States of Micronesia for their help in facilitating our research flights. Special thanks go to the personnel associated with the ARM facility at Manus, Papua New Guinea without whose help the ground-based measurements would not have been possible. Thanks to the British Atmospheric Data Centre (BADC) for hosting our data and the NCAS Atmospheric Measurement Facility for providing the radiosonde and ground-based ozone equipment. Chlorophyll-a data used in Figure 1 were extracted using the Giovanni online data system, maintained by the NASA GES DISC. We also acknowledge the MODIS mission scientists and associated NASA personnel for the production of this data set. Finally we thank many individual associated with the ATTREX and CONTRAST campaigns for their help in the logistical planning, and we would like to single out Jim Bresch for his excellent and freely provided meteorological advice

Evaluation of wetland CH4 in the Joint UK Land Environment Simulator (JULES) land surface model using satellite observations

Wetlands are the largest natural source of methane. The ability to model the emissions of methane from natural wetlands accurately is critical to our understanding of the global methane budget and how it may change under future climate scenarios. The simulation of wetland methane emissions involves a complicated system of meteorological drivers coupled to hydrological and biogeochemical processes. The Joint UK Land Environment Simulator (JULES) is a process-based land surface model that underpins the UK Earth System Model (UKESM) and is capable of generating estimates of wetland methane emissions. In this study, we use GOSAT satellite observations of atmospheric methane along with the TOMCAT global 3-D chemistry transport model to evaluate the performance of JULES in reproducing the seasonal cycle of methane over a wide range of tropical wetlands. By using an ensemble of JULES simulations with differing input data and process configurations, we investigate the relative importance of the meteorological driving data, the vegetation, the temperature dependency of wetland methane production and the wetland extent. We find that JULES typically performs well in replicating the observed methane seasonal cycle. We calculate correlation coefficients to the observed seasonal cycle of between 0.58 and 0.88 for most regions; however, the seasonal cycle amplitude is typically underestimated (by between 1.8 and 19.5 ppb). This level of performance is comparable to that typically provided by state-of-the-art data-driven wetland CH4 emission inventories. The meteorological driving data are found to be the most significant factor in determining the ensemble performance, with temperature dependency and vegetation having moderate effects. We find that neither wetland extent configuration outperforms the other, but this does lead to poor performance in some regions. We focus in detail on three African wetland regions (Sudd, Southern Africa and Congo) where we find the performance of JULES to be poor and explore the reasons for this in detail. We find that neither wetland extent configuration used is sufficient in representing the wetland distribution in these regions (underestimating the wetland seasonal cycle amplitude by 11.1, 19.5 and 10.1 ppb respectively, with correlation coefficients of 0.23, 0.01 and 0.31). We employ the Catchment-based Macro-scale Floodplain (CaMa-Flood) model to explicitly represent river and floodplain water dynamics and find that these JULES-CaMa-Flood simulations are capable of providing a wetland extent that is more consistent with observations in this regions, highlighting this as an important area for future model development

Improved calibration procedures for the EM27/SUN spectrometers of the COllaborative Carbon Column Observing Network (COCCON)

In this study, an extension on the previously reported status of the COllaborative Carbon Column Observing Network\u27s (COCCON) calibration procedures incorporating refined methods is presented. COCCON is a global network of portable Bruker EM27/SUN FTIR spectrometers for deriving column-averaged atmospheric abundances of greenhouse gases. The original laboratory open-path lamp measurements for deriving the instrumental line shape (ILS) of the spectrometer from water vapour lines have been refined and extended to the secondary detector channel incorporated in the EM27/SUN spectrometer for detection of carbon monoxide (CO). The refinements encompass improved spectroscopic line lists for the relevant water lines and a revision of the laboratory pressure measurements used for the analysis of the spectra. The new results are found to be in good agreement with those reported by Frey et al. (2019) and discussed in detail. In addition, a new calibration cell for ILS measurements was designed, constructed and put into service. Spectrometers calibrated since January 2020 were tested using both methods for ILS characterization, open-path (OP) and cell measurements. We demonstrate that both methods can detect the small variations in ILS characteristics between different spectrometers, but the results of the cell method indicate a systematic bias of the OP method. Finally, a revision and extension of the COCCON network instrument-to-instrument calibration factors for XCO2, XCO and XCH4 is presented, incorporating 47 new spectrometers (of 83 in total by now). This calibration is based on the reference EM27/SUN spectrometer operated by the Karlsruhe Institute of Technology (KIT) and spectra collected by the collocated TCCON station Karlsruhe. Variations in the instrumental characteristics of the reference EM27/SUN from 2014 to 2017 were detected, probably arising from realignment and the dual-channel upgrade performed in early 2018. These variations are considered in the evaluation of the instrument-specific calibration factors in order to keep all tabulated calibration results consistent

LINE BROADENING PARAMETERS OF METHANE AT 6000 CM−1^{-1}

Author Institution: Insitute of Environmental Physics, University of Bremen, Germany; Earth Observation Science Group, University of Leicester, UKBeing one of the most important greenhouse gases, methane (CH$_4$) is also modified by anthropogenic activity. Nowadays, it can be monitored globally from space on the long-term scale using combinations of different remote sensing instruments. The critical point for the retrieval algorithms is the knowledge of the spectroscopic parameters. Although a significant amount of spectroscopic data on CH$_4$ is available, the information on the line parameters in mid infrared (MIR) spectral region is inadequate for accurate remote sensing applications and there is a need for improved spectroscopic line parameters. We report on the improved spectroscopic line parameters for CH$_4$ in the spectral regions used by SCIAMACHY and TANSO instruments around 6000 cm$^{-1}$. New data were obtained using high resolution absorption spectra of CH$_4$, perturbed by oxygen, nitrogen and air. Spectra were measured using Fourier transform spectrometer in a broad range of total pressures from 2 to 1000 mbar and temperatures down to 196 K. Calculations of broadening parameters were performed using Reference Forward Model assuming Voigt line profile within international collaboration between the Molecular Spectroscopy Laboratory in IUP Bremen, and Earth Observation Science Group, University of Leicester, UK. Accuracy of the new data matches the level of the demands of modern datasets and remote sensing. The new data were compared with the data included in the latest HITRAN edition and other published works. Before release for the general scientific community, the new data was tested on the TANSO and SCIAMACHY retrievals

GreenHouse gas Observations of the Stratosphere and Troposphere (GHOST): an airborne shortwave-infrared spectrometer for remote sensing of greenhouse gases

GHOST is a novel, compact shortwave-infrared grating spectrometer, designed for remote sensing of tropospheric columns of greenhouse gases (GHGs) from an airborne platform. It observes solar radiation at medium to high spectral resolution (better than 0.3nm), which has been reflected by the Earth's surface using similar methods to those used by polar-orbiting satellites such as the JAXA GOSAT mission, NASA's OCO-2, and the Copernicus Sentinel-5 Precursor. By using an original design comprising optical fibre inputs along with a single diffraction grating and detector array, GHOST is able to observe CO2 absorption bands centred around 1.61 and 2.06µm (the same wavelength regions used by OCO-2 and GOSAT) whilst simultaneously measuring CH4 absorption at 1.65µm (also observed by GOSAT) and CH4 and CO at 2.30µm (observed by Sentinel-5P). With emissions expected to become more concentrated towards city sources as the global population residing in urban areas increases, there emerges a clear requirement to bridge the spatial scale gap between small-scale urban emission sources and global-scale GHG variations. In addition to the benefits achieved in spatial coverage through being able to remotely sense GHG tropospheric columns from an aircraft, the overlapping spectral ranges and comparable spectral resolutions mean that GHOST has unique potential for providing validation opportunities for these platforms, particularly over the ocean, where ground-based validation measurements are not available. In this paper we provide an overview of the GHOST instrument, calibration, and data processing, demonstrating the instrument's performance and suitability for GHG remote sensing. We also report on the first GHG observations made by GHOST during its maiden science flights on board the NASA Global Hawk unmanned aerial vehicle, which took place over the eastern Pacific Ocean in March 2015 as part of the CAST/ATTREX joint Global Hawk flight campaign