scholarly journals How much information do extinction and backscattering measurements contain about the chemical composition of atmospheric aerosol?

2017 ◽  
Vol 17 (5) ◽  
pp. 3423-3444 ◽  
Author(s):  
Michael Kahnert ◽  
Emma Andersson

Abstract. We theoretically and numerically investigate the problem of assimilating multiwavelength lidar observations of extinction and backscattering coefficients of aerosols into a chemical transport model. More specifically, we consider the inverse problem of determining the chemical composition of aerosols from these observations. The main questions are how much information the observations contain to determine the particles' chemical composition, and how one can optimize a chemical data assimilation system to make maximum use of the available information. We first quantify the information content of the measurements by computing the singular values of the scaled observation operator. From the singular values we can compute the number of signal degrees of freedom, Ns, and the reduction in Shannon entropy, H. As expected, the information content as expressed by either Ns or H grows as one increases the number of observational parameters and/or wavelengths. However, the information content is strongly sensitive to the observation error. The larger the observation error variance, the lower the growth rate of Ns or H with increasing number of observations. The right singular vectors of the scaled observation operator can be employed to transform the model variables into a new basis in which the components of the state vector can be partitioned into signal-related and noise-related components. We incorporate these results in a chemical data assimilation algorithm by introducing weak constraints that restrict the assimilation algorithm to acting on the signal-related model variables only. This ensures that the information contained in the measurements is fully exploited, but not overused. Numerical tests show that the constrained data assimilation algorithm provides a solution to the inverse problem that is considerably less noisy than the corresponding unconstrained algorithm. This suggests that the restriction of the algorithm to the signal-related model variables suppresses the assimilation of noise in the observations.

2016 ◽  
Author(s):  
Michael Kahnert ◽  
Emma Andersson

Abstract. We theoretically and numerically investigate the problem of assimilating lidar observations of extinction and backscattering coefficients of aerosols into a chemical transport model. More specifically, we consider the inverse problem of determining the chemical composition of aerosols from these observations. The main questions are how much information the observations contain to constrain the particles' chemical composition, and how one can optimise a chemical data assimilation system to make maximum use of the available information. We first quantify the information content of the measurements by computing the singular values of the observation operator. From the singular values we can compute the number of signal degrees of freedom and the reduction in Shannon entropy. For an observation standard deviation of 10 %, it is found that simultaneous measurements of extinction and backscattering allows us to constrain twice as many model variables as extinction measurements alone. The same holds for measurements at two wavelengths compared to measurements at a single wavelength. However, when we extend the set of measurements from two to three wavelengths then we observe only a small increase in the number of signal degrees of freedom, and a minor change in the Shannon entropy. The information content is strongly sensitive to the observation error; both the number of signal degrees of freedom and the reduction in Shannon entropy steeply decrease as the observation standard deviation increases in the range between 1 and 100 %. The right singular vectors of the observation operator can be employed to transform the model variables into a new basis in which the components of the state vector can be divided into signal-related and noise-related components. We incorporate these results in a chemical data assimilation algorithm by introducing weak constraints that restrict the assimilation algorithm to acting on the signal-related model variables only. This ensures that the information contained in the measurements is fully exploited, but not over-used. Numerical experiments confirm that the constrained data assimilation algorithm solves the inverse problem in a way that automatises the choice of control variables, and that restricts the minimisation of the costfunction to the signal-related model variables.


2009 ◽  
Vol 9 (2) ◽  
pp. 6691-6737 ◽  
Author(s):  
S. Massart ◽  
C. Clerbaux ◽  
D. Cariolle ◽  
A. Piacentini ◽  
S. Turquety ◽  
...  

Abstract. The Infrared Atmospheric Sounding Interferometer (IASI) is one of the five European new generation instruments carried by the polar-orbiting MetOp-A satellite. Data assimilation is a powerful tool to combine these data with a numerical model. This paper presents the first steps made towards the assimilation of the total ozone columns from the IASI measurements into a chemistry transport model. The IASI ozone data used are provided by an inversion of radiances performed at the LATMOS (Laboratoire Atmosphères, Milieux, Observations Spatiales). As a contribution to the validation of this dataset, the LATMOS-IASI data are compared to a four dimensional ozone field, with low systematic and random errors compared to ozonesondes and OMI-DOAS data. This field results from the combined assimilation of ozone profiles from the MLS instrument and of total ozone columns from the SCIAMACHY instrument. It is found that on average, the LATMOS-IASI data tends to overestimate the total ozone columns by 2% to 8%. The random observation error of the LATMOS-IASI data is estimated to about 6%, except over polar regions and deserts where it is higher. Using this information, the LATMOS-IASI data are then assimilated, combined with the MLS data. This first LATMOS-IASI data assimilation experiment shows that the resulting analysis is quite similar to the one obtained from the combined MLS and SCIAMACHY data assimilation.


2016 ◽  
Vol 9 (8) ◽  
pp. 2893-2908 ◽  
Author(s):  
Sergey Skachko ◽  
Richard Ménard ◽  
Quentin Errera ◽  
Yves Christophe ◽  
Simon Chabrillat

Abstract. We compare two optimized chemical data assimilation systems, one based on the ensemble Kalman filter (EnKF) and the other based on four-dimensional variational (4D-Var) data assimilation, using a comprehensive stratospheric chemistry transport model (CTM). This work is an extension of the Belgian Assimilation System for Chemical ObsErvations (BASCOE), initially designed to work with a 4D-Var data assimilation. A strict comparison of both methods in the case of chemical tracer transport was done in a previous study and indicated that both methods provide essentially similar results. In the present work, we assimilate observations of ozone, HCl, HNO3, H2O and N2O from EOS Aura-MLS data into the BASCOE CTM with a full description of stratospheric chemistry. Two new issues related to the use of the full chemistry model with EnKF are taken into account. One issue is a large number of error variance parameters that need to be optimized. We estimate an observation error variance parameter as a function of pressure level for each observed species using the Desroziers method. For comparison purposes, we apply the same estimate procedure in the 4D-Var data assimilation, where both scale factors of the background and observation error covariance matrices are estimated using the Desroziers method. However, in EnKF the background error covariance is modelled using the full chemistry model and a model error term which is tuned using an adjustable parameter. We found that it is adequate to have the same value of this parameter based on the chemical tracer formulation that is applied for all observed species. This is an indication that the main source of model error in chemical transport model is due to the transport. The second issue in EnKF with comprehensive atmospheric chemistry models is the noise in the cross-covariance between species that occurs when species are weakly chemically related at the same location. These errors need to be filtered out in addition to a localization based on distance. The performance of two data assimilation methods was assessed through an 8-month long assimilation of limb sounding observations from EOS Aura MLS. This paper discusses the differences in results and their relation to stratospheric chemical processes. Generally speaking, EnKF and 4D-Var provide results of comparable quality but differ substantially in the presence of model error or observation biases. If the erroneous chemical modelling is associated with moderately fast chemical processes, but whose lifetimes are longer than the model time step, then EnKF performs better, while 4D-Var develops spurious increments in the chemically related species. If, however, the observation biases are significant, then 4D-Var is more robust and is able to reject erroneous observations while EnKF does not.


2016 ◽  
Author(s):  
Sergey Skachko ◽  
Richard Menard ◽  
Quentin Errera ◽  
Yves Christophe ◽  
Simon Chabrillat

Abstract. We compare two optimized chemical data assimilation systems, one based on the ensemble Kalman filter (EnKF) and the other based on four-dimensional variational (4D-Var), using a comprehensive stratospheric chemistry transport model (CTM). The work is an extension of the Belgian Assimilation System for Chemical ObsErvations (BASCOE), initially designed to work with a 4D-Var data assimilation. A strict comparison of both methods in the case of chemical tracer transport was done in a previous study and indicated that both methods provide essentially similar results. In the present work, we assimilate observations of ozone, HCl, HNO3, H2O and N2O from EOS Aura-MLS data into the BASCOE CTM with a full description of stratospheric chemistry. Two new issues related to the use of full chemistry model with EnKF are taken into account. One issue concerns to a large number of error variance parameters that need to be optimized. We estimate an observation error parameter as function of pressure level for each observed species using the Desroziers' method. For comparison reasons, we apply the same estimate procedure in the 4D-Var data assimilation, where we keep both estimates: the background and observation error variances. However in EnKF, the background error covariance is modelled using the full chemistry model and a model error term. We found that it is adequate to have a single model error based on the chemical tracer formulation that is applied for all species. This is an indication that the main source of model error in chemical transport model is due to the transport. The second issue in EnKF with comprehensive atmospheric chemistry models is the sampling errors between species. When species are weakly chemically related, cross-species sampling noise errors occur at the same location. These errors need to be filtered out, in addition to a localization based on distance. The performance of two data assimilation methods was assessed through an eight-month long assimilation of limb sounding observations from EOS Aura-MLS. The paper discusses the differences in results and their relation to stratospheric chemical processes. Generally speaking, EnKF and 4D-Var provide results of comparable quality but differ substantially in presence of model error or observation biases. If the erroneous chemical modelling is associated with not too small chemical life-times, then EnKF performs better, while 4D-Var develops spurious increments in the chemically related species. If, on the other hand, the observation biases are significant, then 4D-Var is more robust and is able to reject erroneous observations, while EnKF does not.


2016 ◽  
Author(s):  
Julius Vira ◽  
Elisa Carboni ◽  
Roy G. Grainger ◽  
Mikhail Sofiev

Abstract. This study focuses on two new aspects on inverse modelling of volcanic emissions. First, we derive an observation operator for satellite retrievals of plume height, and second, we solve the inverse problem using the 4D-Var method. The approach is demonstrated by assimilating IASI SO2 plume height and total column retrievals in a source term inversion for the 2010 eruption of Eyjafjallajökull. The inversion resulted in temporal and vertical reconstruction of the SO2 emissions during the 1–20 May, 2010 with formal vertical and temporal resolutions of 500 m and 12 hours. The plume height observation operator is based on simultaneous assimilation of the plume height and total column retrievals. The plume height is taken to represent the vertical centre of mass, which is transformed into the first moment of mass. This makes the observation operator linear and simple to implement. The necessary modifications to the observation error covariance matrix are derived. Regularisation by truncated iteration is investigated as a simple and efficient regularisation method for the 4D-Var based inversion. In an experiment with synthetic observations, the truncated iteration was found to perform similarly to the commonly used Tikhonov regularisation. However, the truncated iteration allows the amount of regularisation to be varied a posteriori, without repeating the inversion. For inverting the Eyjafjallajökull SO2 emission at the temporal and vertical resolution used in this study, the 4D-Var method required about 70 % less computational effort than commonly used methods based on performing a separate model simulation for each degree of freedom in the estimated source term. Compared to the inversion using only total column retrievals, assimilating the plume height resulted in a vertical emission profile more closely matching the ash plume heights observed by radar. The a posteriori source term gave an estimate of 0.29 Tg erupted SO2 of which 95 % was injected below 11 km.


2017 ◽  
Vol 10 (5) ◽  
pp. 1985-2008 ◽  
Author(s):  
Julius Vira ◽  
Elisa Carboni ◽  
Roy G. Grainger ◽  
Mikhail Sofiev

Abstract. This study focuses on two new aspects of inverse modelling of volcanic emissions. First, we derive an observation operator for satellite retrievals of plume height, and second, we solve the inverse problem using an algorithm based on the 4D-Var data assimilation method. The approach is first tested in a twin experiment with simulated observations and further evaluated by assimilating IASI SO2 plume height and total column retrievals in a source term inversion for the 2010 eruption of Eyjafjallajökull. The inversion resulted in temporal and vertical reconstruction of the SO2 emissions during 1–20 May 2010 with formal vertical and temporal resolutions of 500 m and 12 h.The plume height observation operator is based on simultaneous assimilation of the plume height and total column retrievals. The plume height is taken to represent the vertical centre of mass, which is transformed into the first moment of mass (centre of mass times total mass). This makes the observation operator linear and simple to implement. The necessary modifications to the observation error covariance matrix are derived.Regularization by truncated iteration is investigated as a simple and efficient regularization method for the 4D-Var-based inversion. In the twin experiments, the truncated iteration was found to perform similarly to the commonly used Tikhonov regularization, which in turn is equivalent to a Gaussian a priori source term. However, the truncated iteration allows the level of regularization to be determined a posteriori without repeating the inversion.In the twin experiments, assimilating the plume height retrievals resulted in a 5–20 % improvement in root mean squared error but simultaneously introduced a 10–20 % low bias on the total emission depending on assumed emission profile. The results are consistent with those obtained with real data. For Eyjafjallajökull, comparisons with observations showed that assimilating the plume height retrievals reduced the overestimation of injection height during individual periods of 1–3 days, but for most of the simulated 20 days, the injection height was constrained by meteorological conditions, and assimilation of the plume height retrievals had only small impact. The a posteriori source term for Eyjafjallajökull consisted of 0.29 Tg (with total column and plume height retrievals) or 0.33 Tg (with total column retrievals only) erupted SO2 of which 95 % was injected below 11 or 12 km, respectively.


2014 ◽  
Vol 7 (1) ◽  
pp. 283-302 ◽  
Author(s):  
B. Gaubert ◽  
A. Coman ◽  
G. Foret ◽  
F. Meleux ◽  
A. Ung ◽  
...  

Abstract. An ensemble Kalman filter (EnKF) has been coupled to the CHIMERE chemical transport model in order to assimilate ozone ground-based measurements on a regional scale. The number of ensembles is reduced to 20, which allows for future operational use of the system for air quality analysis and forecast. Observation sites of the European ozone monitoring network have been classified using criteria on ozone temporal variability, based on previous work by Flemming et al. (2005). This leads to the choice of specific subsets of suburban, rural and remote sites for data assimilation and for evaluation of the reference run and the assimilation system. For a 10-day experiment during an ozone pollution event over Western Europe, data assimilation allows for a significant improvement in ozone fields: the RMSE is reduced by about a third with respect to the reference run, and the hourly correlation coefficient is increased from 0.75 to 0.87. Several sensitivity tests focus on an a posteriori diagnostic estimation of errors associated with the background estimate and with the spatial representativeness of observations. A strong diurnal cycle of both these errors with an amplitude up to a factor of 2 is made evident. Therefore, the hourly ozone background error and the observation error variances are corrected online in separate assimilation experiments. These adjusted background and observational error variances provide a better uncertainty estimate, as verified by using statistics based on the reduced centered random variable. Over the studied 10-day period the overall EnKF performance over evaluation stations is found relatively unaffected by different formulations of observation and simulation errors, probably due to the large density of observation sites. From these sensitivity tests, an optimal configuration was chosen for an assimilation experiment extended over a three-month summer period. It shows a similarly good performance as the 10-day experiment.


Atmosphere ◽  
2021 ◽  
Vol 12 (1) ◽  
pp. 91
Author(s):  
Santiago Lopez-Restrepo ◽  
Andres Yarce ◽  
Nicolás Pinel ◽  
O.L. Quintero ◽  
Arjo Segers ◽  
...  

The use of low air quality networks has been increasing in recent years to study urban pollution dynamics. Here we show the evaluation of the operational Aburrá Valley’s low-cost network against the official monitoring network. The results show that the PM2.5 low-cost measurements are very close to those observed by the official network. Additionally, the low-cost allows a higher spatial representation of the concentrations across the valley. We integrate low-cost observations with the chemical transport model Long Term Ozone Simulation-European Operational Smog (LOTOS-EUROS) using data assimilation. Two different configurations of the low-cost network were assimilated: using the whole low-cost network (255 sensors), and a high-quality selection using just the sensors with a correlation factor greater than 0.8 with respect to the official network (115 sensors). The official stations were also assimilated to compare the more dense low-cost network’s impact on the model performance. Both simulations assimilating the low-cost model outperform the model without assimilation and assimilating the official network. The capability to issue warnings for pollution events is also improved by assimilating the low-cost network with respect to the other simulations. Finally, the simulation using the high-quality configuration has lower error values than using the complete low-cost network, showing that it is essential to consider the quality and location and not just the total number of sensors. Our results suggest that with the current advance in low-cost sensors, it is possible to improve model performance with low-cost network data assimilation.


Atmosphere ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 900
Author(s):  
Ioanna Skoulidou ◽  
Maria-Elissavet Koukouli ◽  
Arjo Segers ◽  
Astrid Manders ◽  
Dimitris Balis ◽  
...  

In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively).


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