scholarly journals iFit: An intensity-based retrieval for SO<sub>2</sub> and BrO from scattered sunlight ultraviolet volcanic plume absorption spectra

Author(s):  
M. R. Burton ◽  
G. M. Sawyer

Abstract. iFit is a new intensity-based retrieval algorithm for direct fitting of measured UV spectra, specifically developed for use in volcanology. It has been designed with a focus on minimising processing of the measured spectra prior to analysis. Here, we report a detailed presentation of the iFit algorithm, and test it in 4 case studies, examining clear sky spectra, SO2 calibration cell experiments and volcanic SO2 and BrO retrievals from traverse measurements performed on Mt. Etna volcano, Italy. We show that the major source of fit error in the intensity fitting come from air mass factor independent solar spectrum errors, which are, however, easily characterised and removed by dividing the measured spectrum by a pre-calculated solar spectrum residual. Furthermore, we have quantified the magnitude of the flat spectrum in two spectrometers, and shown that this spectrum is strongly spectrometer dependent but temperature independent, opening the possibility for robust analysis and and BrO without the need for temperature stabilisation of quantification of both SO2 the spectrometer. We find that iFit can be robustly and easily applied to traverse measurements of volcanic plumes, producing bias-free profiles of SO2 , and high quality SO2 /BrO ratios without the need for clear sky background spectra. Fit residuals are typically pure instrumental noise when the residual solar spectrum is removed. We believe that the iFit approach, which avoids the need for a clear sky spectrum and which achieves noise-limited fits, is ideally suited to the automated analysis of spectra produced by networks of scanning UV spectrometers around volcanoes.

2015 ◽  
Vol 57 ◽  
Author(s):  
Massimo Aranzulla ◽  
Flavio Cannavò ◽  
Simona Scollo

<p>The detection of volcanic plumes produced during explosive eruptions is important to improve our understanding on dispersal processes and reduce risks to aviation operations. The ability of Global Position-ing System (GPS) to retrieve volcanic plumes is one of the new challenges of the last years in volcanic plume detection. In this work, we analyze the Signal to Noise Ratio (SNR) data from 21 permanent stations of the GPS network of the Istituto Nazionale di Geofisica e Vulcanologia, Osservatorio Etneo, that are located on the Mt. Etna (Italy) flanks. Being one of the most explosive events since 2011, the eruption of November 23, 2013 was chosen as a test-case. Results show some variations in the SNR data that can be correlated with the presence of an ash-laden plume in the atmosphere. Benefits and limitations of the method are highlighted.</p>


2014 ◽  
Vol 14 (18) ◽  
pp. 25213-25280
Author(s):  
J. Gliß ◽  
N. Bobrowski ◽  
L. Vogel ◽  
U. Platt

Abstract. Spatial and temporal profiles of chlorine dioxide (OClO), bromine monoxide (BrO) and sulphur dioxide (SO2) were measured in the plume of Mt. Etna, Italy, in September 2012 using Multi-Axis-Differential-Optical-Absorption-Spectroscopy (MAX-DOAS). OClO (BrO) was detected in 119 (452) individual measurements covering plume ages up to 6 (23) minutes. The retrieved slant column densities (SCDs) reached values up to 2.0 × 1014 molecules cm−2 (OClO) and 1.1 × 1015 molecules cm−2 (BrO). In addition, the spectra were analysed for signatures of IO, OIO and OBrO, none of these species could be detected. The corresponding detection limits for IO / SO2, OIO / SO2 and OBrO / SO2 were 1.8 × 10−6, 2.0 × 10−5 and 1.1 × 10−5 respectively. The measurements were performed at plume ages (τ) from zero to 23 min downwind the emission source. The chemical variability of BrO and OClO in the plume was studied analysing the OClO / SO2 and BrO / SO2-ratio. A marked increase of both ratios was observed in the young plume (τ < 3 min) and a levelling off at larger plume ages (τ > 3 min) with mean abundances of 3.17 × 10−5 (OClO / SO2), 1.55 × 10−4 (BrO / SO2) and 0.16 (OClO / BrO). Furthermore, enhanced BrO/SO2-ratios were found at the plume edges (by ~30–37%) and a strong indication of enhanced OClO / SO2-ratios as well (~10–250%). A measurement performed in the early morning (05:20–06:20 UTC, sunrise: 04:40 UTC) showed an BrO / SO2-ratio increasing with time until 05:35 UTC and a constant ratio afterwards. Observing this increase was only possible due to a correction for stratospheric BrO signals in the plume spectra. The corresponding OClO / SO2-ratio showed a similar trend stabilising around 06:13 UTC, approximately 40 min later than BrO. This is another strong indication for the photochemical nature of the reactions involved in the formation of oxidised halogens in volcanic plumes. In particular, these findings support the current understanding of the underlying chemistry, namely, that BrO is formed in an autocatalytic reaction mechanism in literature often referred to as "bromine explosion" and that OClO is formed in the "BrO + ClO"-reaction. BrO and OClO concentrations were estimated from the measured SCDs assuming a circular plume shape. In addition, mixing ratios of ClO were determined from the retrieved OClO and BrO-SCDs assuming chemical equilibrium between formation of OClO (BrO + ClO) and its destruction (photolysis). Mean abundances in the young plume (τ<4 min) were BrO = 1.35 ppb, OClO = 300 ppt and ClO = 139 ppt with peak values of 600 ppt (OClO), 2.7 ppb (BrO) and 235 ppt (ClO) respectively. The prevailing Cl-atom concentrations in the plume could be estimated from the rate of increase of OClO and BrO in the young plume and the determined ClO and OClO concentrations. Values between 5.1 × 106 cm−3 (at 40 ppb O3) and 2.1 × 108 cm−3 (at 1 ppb O3) were found. Based on that, a potential – chlorine induced – depletion of tropospheric methane (CH4) in the plume was investigated. CH4-lifetimes between 13 h (at 1 ppb O3) and 23 days (at 40 ppb O3) were found. These are considerably small compared to the atmospheric lifetime of CH4. However, the impact of gaseous chlorine on the CH4-budget in the plume environment was assessed to be relatively small, mainly due to plume dispersion (decrease of Cl number densities) and permanent mixing of the plume with the surrounding atmosphere (net supply of O3 and CH4).


2015 ◽  
Vol 15 (10) ◽  
pp. 5659-5681 ◽  
Author(s):  
J. Gliß ◽  
N. Bobrowski ◽  
L. Vogel ◽  
D. Pöhler ◽  
U. Platt

Abstract. Spatial and temporal profiles of chlorine dioxide (OClO), bromine monoxide (BrO) and sulfur dioxide (SO2) of the volcanic plume at Mt. Etna, Italy, were investigated in September 2012 using Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS). OClO was detected in 119 individual measurements covering plume ages up to 6 min. BrO could be detected in 452 spectra up to 23 min downwind. The retrieved slant column densities (SCDs) reached maximum values of 2.0 × 1014 molecules cm-2 (OClO) and 1.1 × 1015 molecules cm-2 (BrO). Mean mixing ratios of BrO and OClO were estimated assuming a circular plume cross section. Furthermore, ClO mixing ratios were derived directly from the BrO and OClO-SCDs. Average abundances of BrO = 1.35 ppb, OClO = 300 ppt and ClO = 139 ppt were found in the young plume (plume age τ < 4 min) with peak values of 2.7 ppb (BrO), 600 ppt (OClO) and 235 ppt (ClO) respectively. The chemical evolution of BrO and OClO in the plume was investigated in great detail by analysing the OClO/SO2 and BrO/SO2 ratios as a function of plume age τ. A marked increase of both ratios was observed in the young plume (τ < 142 s) and a levelling off at larger plume ages showing mean SO2 ratios of 3.17 × 10-5 (OClO/SO2) and 1.65 × 10-4 (BrO/SO2). OClO was less abundant in the plume compared to BrO with a mean OClO/BrO ratio of 0.16 at plume ages exceeding 3 min. A measurement performed in the early morning at low solar radiances revealed BrO/SO2 and OClO/SO2 ratios increasing with time. This observation substantiates the importance of photochemistry regarding the formation of BrO and OClO in volcanic plumes. These findings support the current understanding of the underlying chemistry, namely, that BrO is formed in an autocatalytic, heterogeneous reaction mechanism (in literature often referred to as "bromine explosion") and that OClO is formed in the reaction of OClO with BrO. These new findings, especially the very detailed observation of the BrO and OClO formation in the young plume, were used to infer the prevailing Cl-atom concentrations in the plume. Relatively small values ranging from [Cl] = 2.5 × 106 cm-3 (assuming 80 ppb background O3) to [Cl] = 2.0 × 108 cm-3 (at 1 ppb O3) were calculated at plume ages of about 2 min. Based on these Cl abundances, a potential – chlorine-induced – depletion of tropospheric methane (CH4) in the plume was investigated. CH4 lifetimes between 14 h (at 1 ppb O3) and 47 days (at 80 ppb O3) were derived. While these lifetimes are considerably shorter than the atmospheric lifetime of CH4, the impact of gaseous chlorine on the CH4 budget in the plume environment should nevertheless be relatively small due to plume dispersion (decreasing Cl concentrations) and ongoing mixing of the plume with the surrounding atmosphere (replenishing O3 and CH4). In addition, all spectra were analysed for signatures of IO, OIO and BrO. None of these species could be detected. Upper limits for IO/SO2, OIO/SO2 and OBrO/SO2 are 1.8 × 10-6, 2.0 × 10-5 and 1.1 × 10-5 respectively.


2019 ◽  
Vol 11 (10) ◽  
pp. 1175 ◽  
Author(s):  
Nathalie Huret ◽  
Charlotte Segonne ◽  
Sébastien Payan ◽  
Giuseppe Salerno ◽  
Valéry Catoire ◽  
...  

Quantification of gaseous emission fluxes from volcanoes can yield valuable insights on processes occurring in the Earth’s interior as part of hazard monitoring. It is also an important task in the framework of climate change, in order to refine estimates of natural emissions. Passive open-path UltraViolet (UV) scattered observation by UV camera allows the imaging of volcanic plumes and evaluation of sulfur dioxide (SO2) fluxes at high temporal resolution during daytime. Another technique of imaging is now available in the InfraRed (IR) spectral domain. Infrared hyperspectral imagers have the potential to overcome the boundary of daytime sampling of the UV, providing measurements also during the night and giving access simultaneously to additional relevant gas species. In this context the IMAGETNA campaign of measurements took place at Mt Etna (Italy) in June 2015. Three different IR imagers (commercial and under developments) were deployed, together with a Fourier Transform InfraRed spectrometer (FTIR) instrument, a UV camera, a Long Wavelength InfraRed (LWIR) camera and a radiometer. We present preliminary results obtained by the two IR cameras under development, and then the IR hyperspectral imager results, coming from full physics retrieval, are compared to those of the UV camera. The comparison points out an underestimation of the SO2 Slant Column Densities (SCD) of the UV camera by a factor of 3.6. The detailed study of the retrieved SO2 SCD highlights the promising application of IR imaging in volcanology for remotely volcanic plume gas measurements. It also provides a way to investigate uncertainties in the SO2 SCD imaging in the UV and the IR.


2017 ◽  
Vol 10 (3) ◽  
pp. 759-782 ◽  
Author(s):  
Alba Lorente ◽  
K. Folkert Boersma ◽  
Huan Yu ◽  
Steffen Dörner ◽  
Andreas Hilboll ◽  
...  

Abstract. Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (<  0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that it is mainly caused by the assumptions and choices made to represent the state of the atmosphere. In order to decide which approach and which ancillary data are best for AMF calculations, we call for well-designed validation exercises focusing on polluted conditions in which AMF structural uncertainty has the highest impact on NO2 and HCHO retrievals.


2020 ◽  
Vol 12 (24) ◽  
pp. 4107
Author(s):  
Charlotte Segonne ◽  
Nathalie Huret ◽  
Sébastien Payan ◽  
Mathieu Gouhier ◽  
Valéry Catoire

Fast and accurate quantification of gas fluxes emitted by volcanoes is essential for the risk mitigation of explosive eruption, and for the fundamental understanding of shallow eruptive processes. Sulphur dioxide (SO2), in particular, is a reliable indicator to predict upcoming eruptions, and its systemic characterization allows the rapid assessment of sudden changes in eruptive dynamics. In this regard, infrared (IR) hyperspectral imaging is a promising new technology for accurately measure SO2 fluxes day and night at a frame rate down to 1 image per second. The thermal infrared region is not very sensitive to particle scattering, which is an asset for the study of volcanic plume. A ground based infrared hyperspectral imager was deployed during the IMAGETNA campaign in 2015 and provided high spectral resolution images of the Mount Etna (Sicily, Italy) plume from the North East Crater (NEC), mainly. The LongWave InfraRed (LWIR) hyperspectral imager, hereafter name Hyper-Cam, ranges between 850–1300 cm−1 (7.7–11.8 µm). The LATMOS (Laboratoire Atmosphères Milieux Observations Spatiales) Atmospheric Retrieval Algorithm (LARA), which is used to retrieve the slant column densities (SCD) of SO2, is a robust and a complete radiative transfer model, well adapted to the inversion of ground-based remote measurements. However, the calculation time to process the raw data and retrieve the infrared spectra, which is about seven days for the retrieval of one image of SO2 SCD, remains too high to infer near real-time (NRT) SO2 emission fluxes. A spectral image classification methodology based on two parameters extracting spectral features in the O3 and SO2 emission bands was developed to create a library. The relevance is evaluated in detail through tests. From data acquisition to the generation of SO2 SCD images, this method requires only ~40 s per image, which opens the possibility to infer NRT estimation of SO2 emission fluxes from IR hyperspectral imager measurements.


2009 ◽  
Vol 26 (4) ◽  
pp. 704-718 ◽  
Author(s):  
Bart De Paepe ◽  
Steven Dewitte

Abstract The authors present a new algorithm to retrieve aerosol optical depth (AOD) over a desert using the window channels centered at 8.7, 10.8, and 12.0 μm of the Spinning Enhanced Visible and Infrared Imager (SEVIRI) instrument on board the Meteosat Second Generation satellite. The presence of dust aerosols impacts the longwave outgoing radiation, allowing the aerosols over the desert surfaces to be detected in the thermal infrared (IR) wavelengths. To retrieve the aerosol properties over land, the surface contribution to the satellite radiance measured at the top of the atmosphere has to be taken into account. The surface radiation depends on the surface temperature, which is characterized by a strong diurnal variation over the desert, and the surface emissivity, which is assumed to be constant over a time span of 24 h. The surface emissivity is based on clear-sky observations that are corrected for atmospheric absorption and emission. The clear-sky image is a composite of pixels that is characterized by the highest brightness temperature (BT) of the SEVIRI channel at 10.8 μm, and by a negative BT difference between the channels at 8.7 and 10.8 μm. Because of the lower temperatures of clouds and aerosols compared to clear-sky conditions, the authors assume that the selected pixel values are obtained for a clear-sky day. A forward model is used to simulate the thermal IR radiation transfer in the dust layer. The apparent surface radiation for the three window channels in the presence of aerosols is calculated as a function of the surface emissivity and the surface temperature, the aerosol layer temperature, and the AOD for different aerosol loadings. From these simulations two emissivity ratios, which are stored in lookup tables (LUT), are calculated. The retrieval algorithm consists of processing the clear-sky image and computing the surface emissivity, processing the instantaneous image, and computing the apparent surface radiation for the three window channels. The two emissivity ratios are computed using the radiances at 8.7 and 10.8 μm and at 8.7 and 12.0 μm, respectively. The SEVIRI AOD is obtained by the inversion of these emissivity ratios using the corresponding LUT. The algorithm is applied to a minor dust event over the Sahara between 19 and 22 June 2007. For the validation the SEVIRI AOD is compared with the AOD from the Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) along the satellite track.


2008 ◽  
Vol 8 (24) ◽  
pp. 7723-7734 ◽  
Author(s):  
L. Clarisse ◽  
P. F. Coheur ◽  
A. J. Prata ◽  
D. Hurtmans ◽  
A. Razavi ◽  
...  

Abstract. In this paper we demonstrate the potential of the infrared Fourier transform spectrometer IASI in analysing volcanic eruptions, using the September 2007 eruption at Jebel at Tair as an illustrative example. Detailed radiative transfer calculations are presented, simulating IASI-like transmittance spectra for a variety of volcanic plumes. We analyse the sensitivity of IASI to SO2 at different altitudes and demonstrate that IASI is in principle capable of sensing SO2 down to the surface. Using the brightness temperature difference of well chosen SO2 channels as a filter, we are able to track the plume of the Jebel at Tair eruption for 12 days, on a par with state of the art UV sounders. A method is presented for quickly estimating the altitude of a volcanic plume based on the relative intensities of the SO2 absorption lines. Despite recent advances, it is still very challenging to retrieve vertical profiles of SO2 from nadir viewing satellites. Currently the most accurate profiles in nadir are retrieved using backtracking of the plume with atmospheric transport models. Via full inverse retrievals using the optimal estimation method, we show the possibility of extracting medium coarse vertical profiles from IASI data. The retrieval allows us to present an evolution of the total mass of SO2 in the plume for the Jebel at Tair eruption. An analytical relation is derived between brightness temperature differences and concentrations, which fits the experimental data very well. The spectral range of IASI also allows retrieval of volcanic aerosols. In the initial plume of the Jebel at Tair eruption, volcanic aerosols were found in the form of ice particles, for which we derived particle sizes.


2019 ◽  
Vol 0 (0) ◽  
Author(s):  
Ahmad Nawaz ◽  
Aneek Kuila ◽  
Nirmalendu Sekhar Mishra ◽  
Kah Hon Leong ◽  
Lan Ching Sim ◽  
...  

Abstract Conventional metal oxide and its composites embrace the long-standing problem of using the combined visible and near-infrared (NIR) light. Doping with suitable impurities of metal, nonmetal, or its combinations for visible light enhancement is very well studied. However, the quantum efficiency of these photocatalysts does not produce an exciting appearance toward visible and NIR light when irradiated through either artificial or natural light. Furthermore, owing to the limited availability of solar light, challenges arise from the implication of these developed nano-photocatalysts. Therefore, the hybridized concept was developed for the effective use of either full or partial solar spectrum, even functioning in dark conditions. The present review focuses on the challenges of hybridized photocatalysts in storing and discharging the harvested photons obtained from the solar spectrum. The review vividly emphasizes the evolution of light-driven nanomaterials since its innovation and significant breakthroughs in brief, while a detailed presentation of the implications of hybrid photocatalysts for full solar applications, including the mechanistic features, charging-discharging characteristics, work function, charge carrier mobility, and interactions, follows. The article also delivers the substantial contribution of these materials in regard to energy and environmental application.


2014 ◽  
Vol 14 (4) ◽  
pp. 2015-2038 ◽  
Author(s):  
J. M. Livingston ◽  
J. Redemann ◽  
Y. Shinozuka ◽  
R. Johnson ◽  
P. B. Russell ◽  
...  

Abstract. Airborne sunphotometer measurements acquired by the NASA Ames Airborne Tracking Sunphotometer (AATS-14) aboard the NASA P-3 research aircraft are used to evaluate dark-target over-land retrievals of extinction aerosol optical depth (AOD) from spatially and temporally near-coincident measurements by the Moderate Resolution Imaging Spectroradiometer (MODIS) during the summer 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. The new MODIS Collection 6 aerosol data set includes retrievals of AOD at both 10 km × 10 km and 3 km × 3 km (at nadir) resolution. In this paper we compare MODIS and AATS AOD at 553 nm in 58 10 km and 134 3 km retrieval grid cells. These AOD values were derived from data collected over Canada on four days during short time segments of five (four Aqua and one Terra) satellite overpasses of the P-3 during low-altitude P-3 flight tracks. Three of the five MODIS–AATS coincidence events were dominated by smoke: one included a P-3 transect of a well-defined smoke plume in clear sky, but two were confounded by the presence of scattered clouds above smoke. The clouds limited the number of MODIS retrievals available for comparison, and led to MODIS AOD retrievals that underestimated the corresponding AATS values. This happened because the MODIS aerosol cloud mask selectively removed 0.5 km pixels containing smoke and clouds before the aerosol retrieval. The other two coincidences (one Terra and one Aqua) occurred during one P-3 flight on the same day and in the same general area, in an atmosphere characterized by a relatively low AOD (< 0.3), spatially homogeneous regional haze from smoke outflow with no distinguishable plume. For the ensemble data set for MODIS AOD retrievals with the highest-quality flag, MODIS AOD agrees with AATS AOD within the expected MODIS over-land AOD uncertainty in 60% of the retrieval grid cells at 10 km resolution and 69% at 3 km resolution. These values improve to 65 % and 74%, respectively, when the cloud-affected case with the strongest plume is excluded. We find that the standard MODIS dark-target over-land retrieval algorithm fails to retrieve AOD for thick smoke, not only in cloud-contaminated regions but also in clear sky. We attribute this to deselection, by the cloud and/or bright surface masks, of 0.5 km resolution pixels that contain smoke.


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