remote sensing Article Geostatistical Analysis of CH4 Columns over Monsoon Asia Using Five Years of GOSAT Observations Min Liu 1,2 , Liping Lei 1 , Da Liu 1,2 and Zhao-Cheng Zeng 1,3, * 1 2 3 * Key Laboratory of Digital Earth Science, Institute of Remote Sensing and Digital Earth, Chinese Academy of Sciences, Beijing 100094, China; [email protected] (M.L.); [email protected] (L.L.); [email protected] (D.L.) University of Chinese Academy of Sciences, Beijing 100049, China Institute of Space and Earth Information Science, The Chinese University of Hong Kong, Shatin 999077, Hong Kong, China Correspondence: [email protected]; Tel.: +852-5571-6425 Academic Editors: Xiaofeng Li and Prasad S. Thenkabail Received: 24 January 2016; Accepted: 20 April 2016; Published: 26 April 2016 Abstract: The aim of this study is to evaluate the Greenhouse gases Observation SATellite (GOSAT) column-averaged CH4 dry air mole fraction (XCH4 ) data by using geostatistical analysis and conducting comparisons with model simulations and surface emissions. Firstly, we propose the use of a data-driven mapping approach based on spatio-temporal geostatistics to generate a regular and gridded mapping dataset of XCH4 over Monsoon Asia using five years of XCH4 retrievals by GOSAT from June 2009 to May 2014. The prediction accuracy of the mapping approach is assessed by using cross-validation, which results in a significantly high correlation of 0.91 and a small mean absolute prediction error of 8.77 ppb between the observed dataset and the prediction dataset. Secondly, with the mapping data, we investigate the spatial and temporal variations of XCH4 over Monsoon Asia and compare the results with previous studies on ground and other satellite observations. Thirdly, we compare the mapping XCH4 with model simulations from CarbonTracker-CH4 and find their spatial patterns very consistent, but GOSAT observations are more able to capture the local variability of XCH4 . Finally, by correlating the mapping data with surface emission inventory, we find the geographical distribution of high CH4 values correspond well with strong emissions as indicated in the inventory map. Over the five-year period, the two datasets show a significant high correlation coefficient (0.80), indicating the dominant role of surface emissions in determining the distribution of XCH4 concentration in this region and suggesting a promising statistical way of constraining surface CH4 sources and sinks, which is simple and easy to implement using satellite observations over a long term period. Keywords: GOSAT; XCH4 ; spatio-temporal geostatistics; Monsoon Asia 1. Introduction Atmospheric methane (CH4 ) is the second most important anthropogenic greenhouse gas after carbon dioxide (CO2 ). Under the driving influence of human activities, such as fossil fuel combustion, global averaged CH4 concentration has increased from pre-industrial levels of 722 ppb to 1833 ppb in 2014 [1] and has kept an average growth rate of about 6 ppb per year since 2007 [2]. CH4 has a stronger global warming potential than carbon dioxide; therefore, monitoring CH4 might be a more effective way to mitigate the short-term greenhouse effects [3]. Current ground-based observation station networks have provided long-term greenhouse gas observations with high precision; however, the stations are still sparse and inhomogeneous [4]. Satellite Remote Sens. 2016, 8, 361; doi:10.3390/rs8050361 www.mdpi.com/journal/remotesensing Remote Sens. 2016, 8, 361 2 of 15 observations of CH4 columns, because of their global coverage and high measurement density, can complement the surface network and be used to improve our understanding of carbon cycle and its changes. Current satellite instruments for measuring the atmospheric CH4 total column include the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) onboard the European Space Agency’s Environmental Satellite (ENVISAT) [5] and the Thermal And Near infrared Sensor for carbon Observation Fourier Transform Spectrometer (TANSO-FTS) operated on the Greenhouse gases Observation SATelite (GOSAT) [6]. CH4 retrievals from SCIAMACHY, which began operation in 2003, showed the promising role of satellite observations in understanding the global CH4 distribution and variation [7], but communication with ENVISAT was unfortunately lost in 2012. The Japanese GOSAT, which was successfully launched in 2009, is the world’s first spacecraft dedicated to quantifying the atmospheric CO2 and CH4 concentrations [6]. The column-averaged dry-air mole fractions of atmospheric CH4 (XCH4 ) are retrieved from Short-Wavelength InfraRed (SWIR) solar spectra observed by TANSO-FTS [8]. The GOSAT aims at providing XCH4 measurements with accuracy of 2% at a spatial scale of 1000 km square and in three-month averages [9]. The major sources of CH4 retrieval errors are aerosols and clouds, especially in high altitude, because of their strongly modification of the equivalent optical path length [8]. However, due to the TANSO-FTS footprint observation mode, sky conditions and retrieval constraints, valid XCH4 retrievals from GOSAT are greatly reduced and irregularly distributed in space and time, and have a lot of gaps between them. These limitations make it difficult to directly infer the spatio-temporal variations of XCH4 and meet the requirements of practical application and further scientific research using the data. Therefore, it is essential to develop a gap-filling method for generating regular XCH4 mapping products from the satellite patchy observations. A series of studies have been carried out in mapping GOSAT retrievals based on the effective geostatistics framework [10,11], due to its great advantages in utilizing correlation structure within the greenhouse gas observations and its best linear unbiased prediction capability. The ordinary kriging (OK) approach was first applied by Tomosada et al. [12] to predict global XCO2 concentration, by considering the spatial variability of GOSAT Level 2 XCO2 data in different land types and directions. The method was further adopted by National Institute for Environmental Studies (NIES) GOSAT to generate the GOSAT Level 3 data products of global monthly mean XCO2 and XCH4 [13]. Hammerling et al. [14] improved the OK method by applying a moving window technique to generate global XCO2 distribution map and found that the prediction precisions are the best for temporal resolution in two to four days. Tadić et al. [15,16] further explored the combination of the moving window block kriging technique and ensemble neural networks. To optimize calculation of large satellite datasets, fixed rank kriging (FRK) approach was introduced by Katzfuss et al. [17] to interpolate simulated Orbiting Carbon Observatory (OCO) XCO2 data, combined with expectation maximization (EM) algorithm, which resulted in a more rapid and accurate prediction. Furthermore, to improve the spatial-only geostatistics in mapping by previous studies, Zeng et al. [18–20] proposed the use of the spatio-temporal geostatistical prediction by incorporating the inherent temporal correlation structure between XCO2 observations. The spatio-temporal geostatistical method was carried out to fill the gaps in GOSAT XCO2 data and demonstrated a better predicted precision compared with spatial-only method. More descriptions about spatio-temporal geostatistics and analysis on the mapping data can be found in Guo et al. [21] and Liu et al. [22]. However, these studies mostly focused on XCO2 data, while the effectiveness of these mapping methods on XCH4 data, especially the spatio-temporal geostatistical approach, has not been comprehensively studied yet. Given the important role of atmospheric CH4 dataset in understanding global carbon cycle, our study is dedicated to developing a mapping method for satellite-observed XCH4 data based on spatio-temporal geostatistics and applying the method to five years of GOSAT XCH4 data over most of Monsoon Asia, which covers all or part of east and central Asia, southeast Asia and the Indian sub-continent. As shown in Figure 1a, the study region extends from 18˝ N to 57˝ N in latitude and from 70˝ E to 138˝ E in longitude. Remote Sens. 2016, 8, 361 Remote Sens. 2016, 82016, 8, 361 3 of 15 250 Count 200 150 100 50 0 2010/01 2011/01 2012/01 2013/01 2014/01 Time (a) (b) Figure (a)spatial spatialdistribution distributionof ofavailable available GOSAT GOSAT XCH XCH44 data Figure 1.1.(a) data number number in in each each1° 1˝by by1°1˝grid gridand and(b) temporal variation of available GOSAT XCH 4 data number every three days. (b) temporal variation of available GOSAT XCH4 data number every three days. Previous studies based on satellite and ground-based observations [7,23–25] have showed that Previous studies based on satellite and ground-based observations [7,23–25] have showed that Monsoon Asia is one of the highest CH4 emission regions in the world, due to its strong Monsoon Asia is one of the highest CH4 emission regions in the world, due to its strong anthropogenic anthropogenic emissions, such as those from rice paddies, and natural emissions, such as those from emissions, such as those from rice paddies, and natural emissions, such as those from natural wetlands. natural wetlands. The spatial and temporal variations of CH4 over this region have been investigated The spatial and temporal variations of CH4 over this region have been investigated in several previous in several previous studies. Xiong et al. [26] investigated the CH4 enhancement in the middle to upper studies. Xiong et al. [26] investigated the CH4 enhancement in the middle to upper troposphere in troposphere in South Asia from July to September by comparing satellite CH4 retrievals from the South Asia from July to September by comparing satellite CH4 retrievals from the Atmospheric Infrared Atmospheric Infrared Sounder (AIRS) on the Earth Observing System (EOS)/Aqua platform with the Sounder (AIRS) on the Earth Observing System (EOS)/Aqua platform with the model simulations from model simulations from global tracer transport model version 3 (TM3), and concluded that the global tracer transport model version 3 (TM3), and concluded that the enhancement is contributed by enhancement is contributed by both local surface emissions and convective transport processes. This both local surface emissions and convective transport processes. This study is complemented with the study is complemented with the work by Qin et al. [27], which analyzed the spatio-temporal work by Qin et al. [27], which analyzed the spatio-temporal variations of XCH4 over the Sichuan Basin variations of XCH4 over the Sichuan Basin using GOSAT data, and attributed the consistent high using GOSAT data, and attributed the consistent high XCH4 values in the basin to the strong regional XCH4 values in the basin to the strong regional paddy field emissions and typical closed topography paddy field emissions and typical closed topography of the basin. Moreover, Ishizawa et al. [28] of the basin. Moreover, Ishizawa et al. [28] analyzed the large XCH4 anomaly in summer 2013 over analyzed the large XCH4 anomaly in summer 2013 over Northeast Asia, as observed by GOSAT and Northeast Asia, as observed by GOSAT and ground-based instruments, and attributed the anomaly ground-based instruments, and attributed the anomaly to the transport of CH4 -rich air to Japan from to the transport of CH4-rich air to Japan from strong CH4 source areas in East China. A more strong CH4 source areas in East China. A more comprehensive study by Hayashida et al. [25] conducted comprehensive study by Hayashida et al. [25] conducted detailed analysis on the characteristics of detailed analysis on the characteristics of XCH4 data in Monsoon Asia using SCIAMACHY retrievals, XCH4 data in Monsoon Asia using SCIAMACHY retrievals, and concluded that the distribution of and concluded that the distribution of high XCH4 values agreed well with regional emissions over high XCH4 values agreed well with regional emissions over this region. Though insights on CH4 this region. Though insights on CH4 distribution and variation were gained from these studies, they distribution and variation were gained from these studies, they were only focusing on some specific were only focusing on some specific regions and using simple data binning and averaging methods regions and using simple data binning and averaging methods to generate monthly or seasonal data to generate monthly or seasonal data for their analysis. The binning and averaging method ignores for their analysis. The binning and averaging method ignores the XCH4 variation within the binning the XCH4 variation within the binning blocks and lacks quantitative uncertainty assessment [15]. blocks and lacks quantitative uncertainty assessment [15]. In addition, the GOSAT XCH4 data, which In addition, the GOSAT XCH4 data, which have higher precision than SCIAMACHY data, over the have higher precision than SCIAMACHY data, over the whole Monsoon Asia region, has not been whole Monsoon Asia region, has not been studied and assessed, mainly due to the limitation of the data studied and assessed, mainly due to the limitation of the data coverage. In this study, we aim to coverage. In this study, we aim to evaluate five years of GOSAT XCH4 retrievals over Monsoon Asia by evaluate five years of GOSAT XCH4 retrievals over Monsoon Asia by first proposing the use of spatiofirst proposing the use of spatio-temporal geostatistics for mapping the XCH4 data over the Monsoon temporal geostatistics for mapping the XCH4 data over the Monsoon Asia region using five years of Asia region using five years of GOSAT data. This spatio-temporal geostatistical approach has the GOSAT data. This spatio-temporal geostatistical approach has the advantage of utilizing the joint advantage of utilizing the joint spatial and temporal dependences between observations and including spatial and temporal dependences between observations and including a larger dataset both in space a larger dataset both in space and time to support stable parameter estimation and prediction [11,29]. and time to support stable parameter estimation and prediction [11,29]. With the mapping XCH4 data, With the mapping XCH4 data, we further analyze the spatio-temporal variations of XCH4 , and compare we further analyze the spatio-temporal variations of XCH4, and compare the results with model the results with model simulations and surface CH4 emissions from bottom-up estimation. simulations and surface CH4 emissions from bottom-up estimation. In Section 2, we describe all the used data, and in Section 3, we introduce the spatio-temporal In Section 2, we describe all the used data, and in Section 3, we introduce the spatio-temporal geostatistics and evaluation method of mapping precision. Sections 4 and 5 demonstrate results and geostatistics and evaluation method of mapping precision. Sections 4 and 5 demonstrate results and discussions from analysis of the spatio-temporal XCH4 variations, comparison with model simulations discussions from analysis of the spatio-temporal XCH4 variations, comparison with model and correlation with surface emissions. The summary is presented in Section 6. simulations and correlation with surface emissions. The summary is presented in Section 6. 3 Remote Sens. 2016, 8, 361 4 of 15 2. Data 2.1. GOSAT XCH4 Retrievals We collected five years of GOSAT Level 2 XCH4 data products (version 02.xx) for General Users [8], ranging from June 2009 to May 2014 over the land area of the Monsoon Asia region, as shown in Figure 1a. Validated by the Total Carbon Column Observing Network (TCCON), the GOSAT XCH4 data show a mean global bias of ´5.9 ppb and standard deviation of 12.6 ppb [30]. GOSAT has a recurrent cycle of three days, and, therefore, in this study we set the basic time unit of the mapping data to be three days. The instantaneous field of view of TANSO-FTS is 15.8 mrad, corresponding to a nadir footprint diameter of 10.5 km approximately. Figure 1 shows the spatial distribution and temporal variation of the available data number from satellite observations. The total number of retrievals is irregularly distributed both in space and time. From Figure 1a, it can be seen that the number of retrievals is larger over northern China and India than the western China and high latitude areas, mainly due to the limitations of clear sky conditions or large solar zenith angle. From Figure 1b, we can see the number of retrievals is larger in winter than in summer when Monsoon brings much more cloudiness in this region. 2.2. CH4 Simulations from CarbonTracker CarbonTracker-CH4 is an assimilating system for atmospheric CH4 developed by the National Oceanic and Atmospheric Administration (NOAA). Coupled with the atmospheric tracer transport model version 5 (TM5), CarbonTracker-CH4 assimilates global atmosphere CH4 observations from surface air samples and tall towers to track global CH4 sources and sinks [31,32]. The current release of CarbonTracker-CH4 , CT2010, produces estimates of global atmospheric CH4 mole fractions and surface-atmosphere fluxes from January 2000 to December 2010. The model produces regularly gridded CH4 at a spatial resolution of 4˝ in latitude by 6˝ in longitude with 34 vertical levels, and with a temporal resolution of one day. In comparison with surface observations, the model outputs show a mean bias of ´10.4 ppb [32]. The CH4 mole fractions profile data from the model are transformed to XCH4 by using the pressure-averaged method described by Connor et al. [33]. When comparing XCH4 data from GOSAT and CT2010, the difference due to averaging kernel effect [34] is not considered here, since the difference between applying and not applying the averaging kernel smoothing on model simulations is very small, which is less than 0.1% in XCO2 as shown in Cogan et al. [35]. 2.3. Emission Inventory from EDGAR CH4 Emission inventory data are derived by bottom-up estimates using CH4 emissions statistics from human activities and natural processes, which corresponds to anthropogenic sources and natural sources, respectively. In this study, we collected annual CH4 emissions data in 2010 from Emission Database for Global Atmospheric Research (EDGAR) in version 4.2 FT2010, released by the European Commission’s Joint Research Centre and Netherlands Environmental Assessment Agency [36]. The inventory data have a spatial resolution of 0.1˝ . The EDGAR CH4 emission data have been used as a fundamental reference for many surface emission related studies [37]. 3. Mapping Based on Spatio-Temporal Geostatistics 3.1. Methodology We applied the spatio-temporal geostatistics to the five years of GOSAT XCH4 retrievals to produce the XCH4 mapping data product in spatial resolution of 1˝ by 1˝ and temporal resolution of three days. A theoretical framework of the spatio-temporal geostatistical mapping approach for XCO2 can be found in Zeng et al. [19]. Here, we introduce the essential procedures of implementing spatio-temporal geostatistics and describe some adjustments necessary for XCH4 . Spatio-temporal geostatistical methods are concerned with analyzing the spatial-temporal correlation structure of regional variables Remote Sens. 2016, 8, 361 5 of 15 using the variogram, and optimal prediction (kriging) of the variable at an unsampled location and Remote Sens. 2016, 82016, 8, 361 time [11]. The implementation of spatio-temporal geostatistics in this study can be divided into the following threelocation main steps, XCH and time, modelinggeostatistics of correlationinstructure, 4 trend in space of unsampled and analysis time [11].ofThe implementation spatio-temporal this study and space-time kriging prediction. can be divided into the following three main steps, analysis of XCH4 trend in space and time, modeling of correlation structure, and space-time kriging prediction. 3.1.1. Analysis of XCH4 Trend in Space and Time 3.1.1. of XCH4 Trend in Space Time TheAnalysis spatio-temporal variations ofand XCH 4 data can be represented by a variable Z “ tZ ps, tq|s P S, t P Tu that varies within a spatial domain S and time interval T. We decompose The spatio-temporal variations of XCH4 data can be represented by a variable = { ( , the )| ∈ spatio-temporal variations into an inherent and deterministic trend component m ps, tq and a stochastic , ∈ } that varies within a spatial domain and time interval . We decompose the spatioresidual component R ps, tq, an as shown in and Equation (1), temporal variations into inherent deterministic trend component ( , ) and a stochastic ( , ), as shown in Equation (1), Z ps, tq “ m ps, tq ` R ps, tq . (1) ( , ) = ( , ) + ( , ). (1) The deterministic spatial trend is determined by the spatial distribution of CH4 sources and The deterministic spatial trend is determined by the spatial distribution of CH4 sources and sinks, while the deterministic temporal trend, which consists of the inherent seasonal CH4 cycle and sinks, while the deterministic temporal trend, which consists of the inherent seasonal CH4 cycle and an annual CH4 increase, is determined by temporal variation of CH4 sources and sinks [2]. As in an annual CH4 increase, is determined by temporal variation of CH4 sources and sinks [2]. As in Zeng Zeng et al. [19], we used a linear surface function for modeling the spatial trend, and a set of annual et al. [19], we used a linear surface function for modeling the spatial trend, and a set of annual harmonic functions with a simple linear function for the temporal trend, as shown in Equation (2), harmonic functions with a simple linear function for the temporal trend, as shown in Equation (2), ÿ m ps, tq (“ ,ra)0= ` [a a1 ˚+s ap1q∗` (1) a2 ˚+s p2q ra3 + ˚ t[a` ∗ 4i“ piωtqqs, (2)(2) i cos (β piωtq a ∗s `(2)] +1∑pβi sin sin( ω`)γ+ γ cos( ω ))], residual component ∗π 2 ˚π since the period is 12 months, (1) and (2) are latitude and longitude of the spatial where ω= where ω“ 12 since the period is 12 months, s p1q and s p2q are latitude and longitude of the spatial location, and aa0´3,,ββ1´4and andγγ1´4are areparameters parameters estimated using the toto bebe estimated using the leastlocation,t is t istime timein in months, and least-squares technique. The modeled trend components in space and time are shown in Figure squares technique. The modeled trend components in space and time are shown in Figure 2. 2. An Anincreasing increasingspatial spatialtrend trendfrom from north north to to south south can can be be clearly clearly seen, seen,which whichisisdetermined determinedbybythethe distribution ofof surface emissions [25]. On the other hand, the temporal trend shows a clear annual distribution surface emissions [25]. On the other hand, the temporal trend shows a clear annual increase and a seasonal cycle. The trend component is then subtracted from the full dataset to produce increase and a seasonal cycle. The trend component is then subtracted from the full dataset to produce thethe residual component forfor thethe following analysis. residual component following analysis. CH4 residual (ppb) 50 25 0 -25 -50 2010/01 2011/01 2012/01 2013/01 2014/01 Time (a) (b) Figure 2. (a) spatial trend surface XCH 4 in the study area derived from five years of GOSAT data Figure 2. (a) spatial trend surface of of XCH 4 in the study area derived from five years of GOSAT data from June 2009 to May 2014, and (b) the temporal trend (red line) obtained fitting annual from June 2009 to May 2014; and (b) the temporal trend (red line) obtained byby fitting thethe annual harmonic function and a linear function to the time series of XCH 4 residuals (black dots), which harmonic function and a linear function to the time series of XCH4 residuals (black dots), which is is 4 data in the whole study area. calculated from averaging spatially detrended XCH calculated from averaging thethe spatially detrended XCH 4 data in the whole study area. 3.1.2. Modeling Correlation Structure XCH4 3.1.2. Modeling Correlation Structure of of XCH 4 Thespatio-temporal spatio-temporalcorrelation correlationstructure structureof of the the XCH between any The XCH44 data datadescribes describesthe thecorrelation correlation between two points separated in space and time. The correlation structure can be characterized by the spatioany two points separated in space and time. The correlation structure can be characterized by the temporal variogram model [11].[11]. The The experimental variogram at spatial laglag ℎ hand temporal lag ℎ , spatio-temporal variogram model experimental variogram at spatial s and temporal lag h ,22γ̂(ℎph, ℎ, h),q,isiscomputed computedby byEquation Equation(3), (3), t s t 2 (ℎ , ℎ ) = ( , ) ∑ ( , )[ ( , ) − ( + ℎ , +ℎ )] , (3) where (ℎ , ℎ ) is the number of pairs in the space and time lags. Following Zeng et al. [19], we set the intervals for spatial lag and temporal lag to be 100 km and 3-day, respectively. That is, the 5 Remote Sens. 2016, 8, 361 6 of 15 2γ̂ phs , ht q “ ÿ 1 2 N phs ,ht q rR ps, tq ´ R ps ` hs , t ` ht qs , N phs , ht q (3) where N phs , ht q is the number of pairs in the space and time lags. Following Zeng et al. [19], we set the intervals for spatial lag and temporal lag to be 100 km and 3-day, respectively. That is, the tolerances for spatial and temporal lags, as defined in De Iaco et al. [29], in calculating the variogram, are set to be 50 km and 1.5 days, respectively. In this study, the distance between observations is defined by the great-circle distance based on the latitude and longitude of the observations. Half of Remote Sens. 2016, 82016, 8, 361 a variogram quantity, γ̂ phs , ht q, has been called a semi-variance. A spatio-temporal variogram model, γ phs , ht q, is then fitted to experimental variogram. The spatio-temporal variogram model adopted tolerances for spatial and temporal lags, as defined in De Iaco et al. [29], in calculating the variogram, here is aare combination of the product-sum model [29,38] and an extra global nugget N the set to be 50 km and 1.5 days, respectively. In this study, the distance between observations is ST to capture defined[10], by the great-circle based on nugget effect and is givendistance by Equation (4),the latitude and longitude of the observations. Half of a variogram quantity, (ℎ , ℎ ), has been called a semi-variance. A spatio-temporal variogram model, (ℎ , ℎ ), is then fitted to experimental variogram. variogram model adopted γ ph, uq “ γS phq ` γT puq ´The κ ¨ γspatio-temporal (4) S phq γT puq ` NST , here is a combination of the product-sum model [29,38] and an extra global nugget to capture nugget given by Equation (4), variograms in space and time, and κ is a constant where γthephq and γeffect puq[10], areand theisexponential marginal T S ⋅ (ℎ) ( ) + = (ℎ) + ( ) − κvariogram , study, all parameters (4) to be estimated. For modeling (ℎ, the )spatio-temporal in this are estimated simultaneously in the Zeng et al. [19] instead of sequentially as in Deand Iaco (ℎ) and ( as ) are exponential marginal variograms in space and time, κ isetaal. [29]. where As shown in Zeng al. [19],For this simultaneous estimation method is more for GOSAT constant to be et estimated. modeling the spatio-temporal variogram in this study, precise all parameters are estimated simultaneously as in Zeng et al. [19] instead of sequentially as in De Iaco et al. [29]. As least data than the conventional sequential estimation method. The iterative nonlinear weighted shown in Zeng et al. [19], this simultaneous estimation method is more precise for GOSAT data than squared technique [10] has been used to estimate the model parameters. The calculated experimental the conventional sequential estimation method. The iterative nonlinear weighted least squared spatio-temporal variogram and the corresponding modeled spatio-temporal variogram are shown technique [10] has been used to estimate the model parameters. The calculated experimental spatioin Figure 3. In the variogram, semi-variance values when spatial and temporal lag are closest temporal variogram and thethe corresponding modeled spatio-temporal variogram are shown in Figure to 0 and3. infinity are called nugget and sill, respectively. The ratio of nugget to sill, expressed as In the variogram, the semi-variance values when spatial and temporal lag are closest to 0 and infinity are called nugget and sill, respectively. The ratio of nugget to sill, expressed as a percentage, a percentage, can be used as an indicator to classify data dependence [39]. In general, a ratio less than can be used as an indicator data dependence, dependence [39].between In general, a ratio less thana0.25 indicates spatial 0.25 indicates a strong spatial to orclassify temporal 0.25 and 0.75, moderate a strong spatial or temporal dependence, between 0.25 and 0.75, a moderate spatial or temporal or temporal dependence, and larger than 0.75 a weak spatial or temporal dependence. In this study, dependence, and larger than 0.75 a weak spatial or temporal dependence. In this study, the ratio of the rationugget of nugget to spatial sill, temporal sill and global sill are 0.20, 0.48 and 0.16, respectively, to spatial sill, temporal sill and global sill are 0.20, 0.48 and 0.16, respectively, indicating a indicating a strong dependence XCH4 retrievals space, a dependence moderate dependence strong dependence betweenbetween XCH4 retrievals in space, ainmoderate between XCHbetween 4 XCH4 retrievals in time, and a strong overall spatio-temporal dependence. retrievals in time, and a strong overall spatio-temporal dependence. 2 Semivariance (ppb ) 350 2 Semivariance (ppb ) 350 300 250 200 150 45 Te m 30 por al (da y) 0 200 0 Spati 200 150 Te m 30 por al 400 g al L a 250 45 600 Lag15 300 (km) (a) 600 Lag15 (da y) 0 200 0 Spati 400 g al L a (km) (b) Figure 3. The experimental spatial-temporal variogram surface of the XCH4 residuals in (a) and its Figure 3. The experimental spatial-temporal variogram surface of the XCH4 residuals in (a) and its fitted variogram model in (b). fitted variogram model in (b). 3.1.3. Space-Time Kriging Prediction of XCH4 3.1.3. Space-Time Kriging Prediction of XCH4 variogram, space-time kriging can be implemented to Based on the modeled spatio-temporal predict 4 value at unobserved locations using surrounding observations and produce the Based on the theXCH modeled spatio-temporal variogram, space-time kriging can be implemented to mapping XCH4 over Monsoon Asia. The kriging makes an optimal prediction ( , ) as the linear predict the XCH4 value at unobserved locations using surrounding observations and produce the weighted sum of the surrounding GOSAT XCH4 observations that minimizes the mean squared mapping XCH4 over Asia. The(5), kriging makes an optimal prediction R ps0 , t0 q as the linear prediction error,Monsoon as shown in Equation weighted sum of the surrounding GOSAT XCH4 observations that minimizes the mean squared ( , ) = ∑ [λ ( , )], (5) prediction error, as shown in Equation (5), where λ is the weight assigned to a known sample ( , ). The weights for the observations are determined by the geometry of the observations and the modeled spatio-temporal variogram. The kriging prediction variance, a measurement of prediction uncertainty, is given by Equation (6), 6 Remote Sens. 2016, 8, 361 7 of 15 R̂ ps0 , t0 q “ ÿ n i“1 rλi R psi , ti qs , (5) where λi is the weight assigned to a known sample R psi , ti q. The weights for the observations are determined by the geometry of the observations and the modeled spatio-temporal variogram. The kriging prediction variance, a measurement of prediction uncertainty, is given by Equation (6), ˘2 1T Γ´1 γ0 ´ 1 γ0 ´ , 1T Γ´1 1 ` 2 T ´1 σ “ γ0 Γ (6) ˇ˘ `ˇ where Γ pi, jq “ γ ˇsi ´ s j |, | ti ´ t j ˇ , γ0 pi, 1q “ γ p|si ´ s0 | , |ti ´ t0 |q, and 1 is n ˆ 1 unit vector. In each kriging prediction, theoretically, the optimal prediction is achieved when using all available observations. However, the total number of N = 51742 in this study makes it not practically feasible for the kriging calculation because, to solve the inversion of such N by N matrix for each prediction, is almost computationally impossible. Following Zeng et al. [19], we used the kriging neighborhood, which is a cylinder in space and time, to define the surrounding data. The radii of the neighborhood vary from 200 to 300 km in space and 15 to 45 days in time to make sure the number of observations in the cylinder neighborhood is no less than 20. In order to verify the validity of the used kriging neighborhood in representing local data variability, two key parameters [40], weight of the mean (WM) and slope of the regression (SR) are used in this study. WM indicates the dependency of kriging prediction on the data in the neighborhood, while SR shows whether the neighborhood size is suitable for a valid kriging. The more WM is closer to zero, and the more SR is closer to one will indicate a better kriging neighborhood. Our kriging prediction results in an averaged WM = 0.040 and SR = 0.964 for the used cylinder neighborhood. The results show a low WM closer to zero and high SR closer to one, which indicate that the chosen kriging neighborhood is suitable in representing local variability, and the prediction would not be much improved by searching further. The mapping XCH4 are described in detail in Section 4, and a discussion on prediction uncertainties of the mapping XCH4 is in Section 5. 3.2. Precision Evaluation Using Cross-Validation Cross-validation is a widely used method for assessing prediction accuracy of statistical models [40]. In this study, we used the leave-one-out cross-validation to assess the prediction accuracy of the spatio-temporal geostatistical approach for mapping the GOSAT XCH4 observations. A detailed description of the method can be referred to in Cressie [10]. The cross-validation is carried out by ` ˘ ` ˘ first removing one observation datum Z s j , t j and then making its prediction Ẑ s j , t j using the remaining dataset. This process is repeated for each observation in Z ps, tq. As a result, two datasets, ` ˘ ` ˘ the predicted dataset {Ẑ s j , t j j = 1 . . . N} and the corresponding original dataset {Z s j , t j j = 1 . . . N} can be obtained. The following three summary statistics from the two datasets were derived to assess prediction precision. The correlation coefficient (R) between Z ps, tq and Ẑ ps, tq is 0.91, the ˘ ` ˘ˇ ř ˇˇ ` ˇ mean absolute prediction error (MAE; N j“1 Z s j , t j ´ Ẑ s j , t j {N) is 8.77 ppb, and the percentage of prediction error less than 15 ppb is 82%. These cross-validation results show a significant high correlation coefficient and small prediction errors between the original XCH4 data and the predicted XCH4 data. The histogram of the prediction errors are shown in Figure 4. It indicates that the spatio-temporal geostatistical prediction method developed for GOSAT XCH4 data is effective, and we can therefore generate precise maps of XCH4 over Monsoon Asia using the method from the five years of GOSAT XCH4 observations. Moreover, we compare the prediction accuracy between spatio-temporal and spatial-only method based on the cross-validation statistics. The spatial-only method implemented here is similar to that for generating monthly GOSAT Level 3 data [13]. The whole XCH4 dataset is firstly grouped into monthly datasets (five years = 60 months), and then the variogram for each month is calculated and modeled by the exponential variogram model. Finally, based on the monthly modeled variograms, spatial-only kriging is applied for predictions of XCH4 in each month. As a result, R and MAE for the spatial-only Remote Sens. 2016, 8, 361 8 of 15 method are 0.90 and 8.97 ppb, respectively. Compared with this spatial-only method, we can see that the spatio-temporal method Remote Sens. 2016, 82016, 8, 361 shows a slightly higher correlation coefficient and lower prediction error. 2500 2000 Frequency Frequency Remote Sens. 2016, 82016, 8, 361 MAE= 8.77 ppb ST D =11.80 ppb 1500 2500 1000 2000 MAE= 8.77 ppb ST D =11.80 ppb 1500 500 1000 0 -50 -40 -30 -20 -10 500 0 10 20 30 40 50 Prediction error (ppb) Figure 4. Histogram of the predictionerrors errorsbetween between the values toward the the corresponding Figure 4. Histogram of the prediction thepredicted predicted values toward corresponding 0 observed values in cross-validation. The mean absolute prediction error (MAE) and the standard -50 -40 -30 -20 -10 0 10 20 30 40 50 observed values in cross-validation. The mean absolute prediction error (MAE) and the standard deviation (STD) of the errors are also given. Prediction error (ppb) deviation (STD) of the errors are also given. Figure 4. Histogram of the prediction errors between the predicted values toward the corresponding 4. Assessment of Five Years of the XCH4 Mapping Dataset observed values in cross-validation. mean absolute prediction 4. Assessment of Five Years of the XCHThe 4 Mapping Dataset error (MAE) and the standard deviation (STD) of the errors are also given. 4.1. Spatio-Temporal Variations of XCH4 4.1. Spatio-Temporal Variations of XCH4 4. Figure Assessment of Five ofvariations the XCH4 Mapping Dataset 5 shows the Years overall of mapping XCH4 in space and time. Spatial variation of XCH4 from south the to north andvariations strong seasonal variationXCH can be observed fromtime. FigureSpatial 5a,b. Spatially, Figure 5 shows overall of mapping space and variation of 4 in 4.1. Spatio-Temporal Variations of XCH4 XCH 4 shows obvious latitude, as shown 5a, infrom whichFigure higher5a,b. averaged XCH4the from south to an north and change strong with seasonal variation caninbeFigure observed Spatially, values can be seen in area between 18°N to 32°N. This latitude contrast shows stronger emissions of Figure 5 shows the overall variations of mapping XCH 4 in space and time. Spatial variation of the XCH4 shows an obvious change with latitude, as shown in Figure 5a, in which higher averaged XCH from south to north and strong seasonal variation can be observed from Figure 5a,b. Spatially,the CH 4 in 4southern Asia than northern Asia, which is further shown in Figure 6. Temporally, ˝ ˝ values can be seen in area between 18 N to 32 N. This latitude contrast shows stronger emissions of the XCH 4 shows an obvious from change with as the shown in Figure in which averaged averaged XCH 4 is increasing year tolatitude, year, and annual mean5a, increase is higher 5.97 ppb over the CH4 in southern Asia than northern Asia, which is further shown in Figure 6.stronger Temporally, the averaged values period. can be seen area between 18°N to 32°N. This latitude shows emissions five-year Thisinannual mean increase is consistent with contrast the annual mean increase of 5.60of ppb XCH4 isCH increasing from year to year, and thewhich annual mean shown increase is 5.976.ppb over thethe five-year 4 in southern Asia than is further in Figure Temporally, from surface observations fromnorthern 2007 to Asia, 2013 [41]. Seasonally, the averaged seasonal cycle amplitude period. This annual mean increase isAugust consistent with increase 5.60 ppb from averaged 4 is increasing from year to year, andthe theannual annual mean mean increase 5.97 ppb the surface is 22.47 ppb,XCH with maximum in and minimum around February andisof March, asover shown in five-year period. This annual mean increase is consistent with the annual mean increase of 5.60 ppb observations 2007 the to 2013 [41].cycle Seasonally, the averaged seasonal amplitude is 22.47 Figure 5b.from However, seasonal peak generally varies with latitude,cycle as shown in Figure 5a. In ppb, from surface observations from 2007 toaround 2013 [41]. Seasonally, the averaged seasonalincycle amplitude with maximum and minimum February and March, as shown Figure However, areas southin ofAugust 25°N, the peak appears around September, while in areas north of 30°N, it5b. appears is 22.47 ppb, with maximum in August and minimum around February and March, as shown in around July August. The varies patternwith of seasonal peak isinconsistent the result the seasonal cycleand peak generally latitude,cycle as shown Figure 5a.with In areas southfrom of 25˝ N, Figure 5b. However, the seasonal cycle peak generally varies with latitude, as shown in Figure 5a. In SCIAMACHY as described in Figure 6a ofinHayashida et al. [25]. They found that the Monsoon the peak appears while areas north ofwhile 30˝ N, appears andAsia August. areas southaround of 25°N,September, the peak appears around September, in it areas north around of 30°N, July it appears region includes different phases of seasonal variation of XCH 4, which also corresponds to a wide The pattern of seasonal cycle peak is consistent with the result from SCIAMACHY as described in around July and August. The pattern of seasonal cycle peak is consistent with the result from range of climate zones in this region. Figure 6a of Hayashida et al. [25]. that the Monsoon Asiafound region includes different SCIAMACHY as described in They Figurefound 6a of Hayashida et al. [25]. They that the Monsoon Asia phases region includesof different seasonal variation to of 1860 4, which corresponds to ainwide of seasonal variation XCH4 ,phases whichofalso corresponds aXCH wide rangealso of climate zones this region. CH4 (ppb) CH4 (ppb) range of climate zones in this region. 1860 1820 1820 1780 1780 1740 1740 (a) 2010/01 2011/01 2012/01 2013/01 2014/01 Time 2010/01 2011/01(b) 2012/01 2013/01 2014/01 Time Figure 5. (a) overview of(a) the regional spatio-temporal distribution of XCH4 over (b) Monsoon Asia as a function of latitude and time from five years of mapping XCH4 dataset with a grid resolution of 1° in Figure 5. (a) overview of the regional spatio-temporal distribution of XCH4 over Monsoon Asia as a Figure 5. (a) and overview of the regional spatio-temporal distribution of XCHof Monsoon Asia as latitude one time-unit (three days) in time, and (b) temporal variation monthly averaged 4 over function of latitude and time from five years of mapping XCH4 dataset with a grid resolution of 1° in mapping XCH4 (red dots) over Monsoon Asia and the corresponding standard deviation lines). of 1˝ a function of latitude and time from five years of mapping XCH4 dataset with a grid (grey resolution latitude and one time-unit (three days) in time, and (b) temporal variation of monthly averaged in latitude and one (three days) in time, and (b) temporal variation of monthly averaged mapping XCHtime-unit 4 (red dots) over Monsoon Asia and the corresponding standard deviation (grey lines). mapping XCH4 (red dots) over Monsoon Asia and the corresponding standard deviation (grey lines). 8 8 Remote Sens. 2016, 8, 361 9 of 15 Remote 2016, the 82016,seasonal 8, 361 Figure 6 Sens. shows means of XCH4 over the five-year period. The spatial patterns of XCH4 distribution in the four seasons are similar. Wetlands and rice paddy fields are among Figure 6 shows the seasonal means of XCH4 over the five-year period. The spatial patterns of the primary sources of atmospheric CH4 , which are responsible for the higher XCH arewhich can be XCH4 distribution in the four seasons are similar. Wetlands and rice paddy fields 4, among the observedprimary in all seasons in southern Asia and south-eastern China. This spatial pattern is also sources of atmospheric CH4, which are responsible for the higher XCH4, which can well be consistent with that from a six-year average (2003 2008)China. of SCIAMACHY XCH4 is retrievals observed in all seasons in southern Asia and through south-eastern This spatial pattern also wellas shown inconsistent Figure 14 of that Frankenberg et al.average [7]. Moreover, obvious seasonal variationXCH can4 retrievals be observed. with from a six-year (2003 through 2008) of SCIAMACHY as shown insummer Figure 14and of Frankenberg al. [7]. obvious seasonal variation can and be observed. XCH4 between autumn is et close, asMoreover, well as between winter and spring, XCH4 of betweenare summer and autumn close, as well as latter between winter and spring, XCH4 of the first XCH two 4seasons generally higher isthan that of the two seasons. This isand because, inthe this first two seasons are generally higher than that of the latter two seasons. This is because, in this region, region, summer and autumn are warmer and wetter seasons, as well as the growing seasons of rice, summer and autumn are warmer and wetter seasons, as well as the growing seasons of rice, which which result in stronger emissions from rice paddies and wetlands compared to the dry season in result in stronger emissions from rice paddies and wetlands compared to the dry season in winter winter and spring [25,42]. Several high value areas stand out, including the Pearl River Delta region in and spring [25,42]. Several high value areas stand out, including the Pearl River Delta region in south south China probably due to strong human activity related emissions, the Ganges Delta in south Asia China probably due to strong human activity related emissions, the Ganges Delta in south Asia probablyprobably due to strong wetland emissions, and and the Sichuan Basin inin west Basinshows shows due to strong wetland emissions, the Sichuan Basin westChina. China. Sichuan Sichuan Basin a consistent high anomalous valuevalue in allinseasons, which is related totoitsitsstrong sourceas aswell wellasas a consistent high anomalous all seasons, which is related stronglocal local source the stagnant effect due to due its special basinbasin terrain topography [27]. the stagnant effect to its special terrain topography [27]. (a) Spring (b) Summer (c) Autumn (d) Winter Figure 6. Seasonally averaged XCH4 calculated from five years of spatio-temporal mapping XCH4, Figure 6. Seasonally averaged XCH4 calculated from five years of spatio-temporal mapping XCH4 , including (a) Spring (March to May); (b) Summer (June to August), (c) Autumn (September to including (a) Spring (March to May); (b) Summer (June to August); (c) Autumn (September to November), and (d) Winter (December and January and February the next year). November); and (d) Winter (December and January and February the next year). 4.2. Comparison with Model Simulations of XCH4 4.2. Comparison with Model Simulations of XCH4 Atmospheric modeling of greenhouse gases, such as CarbonTracker, can reproduce large scale features of the atmospheric CH4 distribution well. Figure 7 shows the annual of mapping XCH 4 Atmospheric modeling of greenhouse gases, such as CarbonTracker, canmean reproduce large scale 4 in 2010 from CarbonTracker-CH4. We can data in 2010 and the corresponding model output of XCH features of the atmospheric CH4 distribution well. Figure 7 shows the annual mean of mapping see that the spatial patterns of mapping data and the modeling well agree with each other, with high XCH4 data in 2010 and the corresponding model output of XCH4 in 2010 from CarbonTracker-CH4 . XCH4 in southern and south-eastern Asia and low values in northern and north-western Asia, We can see that the spatial patterns of mapping data and the modeling well agree with each other, especially the high altitude Tibet area. However, the model data shows a lower XCH4 in the low with high XCH4area in southern and south-eastern Asia values in northern north-western latitude than the mapping data, especially inand two low key regions, including theand Sichuan Basin and Asia, especially the high altitude Tibet area. However, the model data shows a lower XCHIn4 in the the Ganges Basin, where CH4 emissions from rice paddy fields and wetlands dominate. high low latitude areaareas, thanthe themodel mapping data, especially twomapping key regions, including the Sichuan Basin latitude simulations are higherin than satellite observations, especially in and the Ganges Basin, where CH4 emissions rice paddy fields andThe wetlands high Tibet, Mongolia and north-eastern China,from where XCH 4 values are low. satellitedominate. data, on theIn other latitude areas, the model simulations are higher than mapping satellite observations, especially in Tibet, Mongolia and north-eastern China, where XCH94 values are low. The satellite data, on the other Remote Sens. 2016, 8, 361 10 of 15 Remote Sens. 2016, 82016, 8, 361 hand, show of XCH can therefore capture the local variability and present 4 and hand,direct show observations direct observations of XCH 4 and can therefore capture the local variability and present a Sens. 2016, 82016, 8, 361 a moreRemote detailed characteristic of XCH variation compared totomodel Morediscussions discussionsareare 4 more detailed characteristic of XCH 4 variation compared modelsimulations. simulations. More presented in Section 5. presented in Section 5. hand, show direct observations of XCH4 and can therefore capture the local variability and present a more detailed characteristic of XCH4 variation compared to model simulations. More discussions are presented in Section 5. (a) Mapping XCH4 (b) CarbonTracker XCH4 (a) Mapping XCH4 (b) CarbonTracker XCH4 Figure 7. (a) the annual averaged XCH4 for the year 2010 from mapping dataset, and (b) the Figure 7.corresponding (a) the annual for the year 2010 from mapping dataset; and (b) the XCH4averaged simulationsXCH from4 CarbonTracker-CH 4 in 2010. corresponding XCH4 simulations from CarbonTracker-CH4 in 2010. Figure 7. (a) the annual averaged XCH4 for the year 2010 from mapping dataset, and (b) the corresponding XCH4 simulations from CarbonTracker-CH4 in 2010. 4.3. Correlation with Surface Emission Inventory 4.3. Correlation with Surface Surface emissionEmission of CH4 isInventory the main driver of the atmospheric XCH4 distributions. Figure 8a 4.3. Correlation with surface Emission Inventory shows the annual CH 4 emission in 2010of derived from EDGARXCH emission inventory. The spatial Surface emission ofSurface CH4 is the main driver the atmospheric 4 distributions. Figure 8a distribution pattern of high CH 4 emissions is determined by both anthropogenic emissions (such as Surface surface emissionCH of 4CH 4 is the main driver of the atmospheric 4 distributions. 8a shows the annual emission in 2010 derived from EDGAR XCH emission inventory.Figure The spatial fossilthe fuel combustion, biomass burning andderived rice paddies) and natural emissions (such asspatial natural shows annual surface CH 4 emission in 2010 from EDGAR emission inventory. The distribution pattern of high CH4 emissions is determined by both anthropogenic emissions (such as wetlands). pattern By comparing 8a and Figure 7a, we can see their spatial patterns agree with each distribution of high Figure CH 4 emissions is determined by both anthropogenic emissions (such as fossil fuel combustion, biomass burning and rice paddies) and natural emissions (such as natural other well. It indicates the variation of multi-year averagedand XCH 4 can well represent the variation of fossil fuel combustion, biomass burning and rice paddies) natural emissions (such as natural wetlands). By comparing Figures 8a and 7a, we can see their spatial patterns agree with each other annual averaged CH 4 surface emissions. Figure 8b shows the relationship between CH4 surface wetlands). By comparing Figure 8a and Figure 7a, we can see their spatial patterns agree with each well. It indicates the variation of multi-year averaged wellannual represent the variation of annual 4 can emissions, hasthe been rearranged into 1° byaveraged 1°XCH grids, and averaged XCH4 value from other well. Itwhich indicates variation of multi-year XCHthe 4 can well represent the variation of averaged CH surface emissions. Figure 8b shows the relationship between CH surface emissions, the mapping dataset as shown in Figure 7a. A significant linear relationship can be observed, with 4 4 annual averaged CH4 surface emissions. Figure 8b shows the relationship between CH4 surface ˝ by ˝ grids,ofand 2) of 0.64 and psignificantly high correlation coefficient 0.80 and the coefficient of determination (R which has been rearranged into 1 1 the annual averaged XCH value from the mapping 4 emissions, which has been rearranged into 1° by 1° grids, and the annual averaged XCH4 value from value lessinthan 0.01. This significant linear relationship indicates the dominant role of surface datasetthe as shown Figure 7a.shown A significant can be observed, with significantly mapping dataset as in Figurelinear 7a. A relationship significant linear relationship can be observed, withhigh emissions in determining the distribution of XCH 4 concentration2over such regions.2 correlation coefficient 0.80 and the coefficient of and determination (R of) of 0.64 and p-value less and thanp-0.01. significantly highofcorrelation coefficient of 0.80 the coefficient determination (R ) of 0.64 value lesslinear than relationship 0.01. This significant relationship theemissions dominantinrole of surface the This significant indicateslinear the dominant roleindicates of surface determining emissions in determining the distribution of XCH4 concentration over such regions. distribution of XCH 4 concentration over such regions. (a) (b) Figure 8. (a) annual CH4 emission in 2010 derived from EDGAR emission inventory in a spatial (b)emissions and the averaged resolution of 0.1° (a) by 0.1°, and (b) The relationship between CH4 surface XCH4 value in 1° by 1° grids drived from the five years of mapping XCH4 data. The color grids (a) annual 4 emission in 2010 derived from EDGAR emission inventory in a spatial FigureFigure 8.represent (a) 8. annual CH4CH emission in 2010 derived emission inaveraged a spatial the density of data distribution. The blackfrom line isEDGAR derived from linear inventory regression of resolution ˝of 0.1° by 0.1°, and (b) The relationship between CH4 surface emissions and the averaged ˝ resolution of 0.1 by(Y) 0.1and ; and (b) The relationship between emissions and the averaged 4 surface(X), 4 data the base 10 logarithm of surface CHCH 4 emissions which shows a significant XCH XCH4 value˝ in 1° ˝by 1° grids drived from the five years of mapping XCH4 data. The color grids 2 equals from XCH4 value 1 by 1 grids the five years of mapping XCH4 data. The color grids linearinrelationship with Rdrived 0.64 (p-value < 0.01). represent the density of data distribution. The black line is derived from linear regression of averaged represent the density of data distribution. The black line is derived from linear regression of averaged XCH4 data (Y) and the base 10 logarithm of surface CH4 emissions (X), which shows a significant 10 emissions (X), which shows a significant linear XCH4 data and the base surface< CH 4 linear(Y) relationship with10 R2logarithm equals 0.64of(p-value 0.01). relationship with R2 equals 0.64 (p-value < 0.01). 10 Remote Sens. 2016, 82016, 8, 361 Remote Sens. 2016, 8, 361 11 of 15 5. Discussion 5. Discussion 5.1. Prediction Uncertainty of Mapping XCH4 Data 5.1. Prediction Uncertainty of Mapping XCHwe In geostatistics, for each prediction, can get a corresponding kriging variance at the same 4 Data time, as shown in Equation (6). The variance is determined by both the density of GOSAT XCH4 In geostatistics, for each prediction, we can get a corresponding kriging variance at the same time, observations and the data homogeneity in the neighborhood of the prediction position. Theoretically, as shown in Equation (6). The variance is determined by both the density of GOSAT XCH4 observations in conditions of denser observations and more homogeneous XCH4 variation surrounding the and the data homogeneity in the neighborhood of the prediction position. Theoretically, in conditions prediction location there will be lower prediction uncertainty [14]. Therefore, the kriging variance of denser observations and more homogeneous XCH4 variation surrounding the prediction location indicates how uncertain each XCH4 prediction is given the available satellite observations. Figure 9 there will be lower prediction uncertainty [14]. Therefore, the kriging variance indicates how uncertain shows the spatial variation of the kriging standard deviation (root of kriging variance) from the each XCH4 prediction is given the available satellite observations. Figure 9 shows the spatial variation mapping XCH4 data in Monsoon Asia averaged over a five-year period. The values change from of the kriging standard deviation (root of kriging variance) from the mapping XCH4 data in Monsoon about 11 ppb to 16 ppb with mean of 13.70 ppb. As expected, in areas with denser observations as Asia averaged over a five-year period. The values change from about 11 ppb to 16 ppb with mean of shown in Figure 1a, including northern China and India, the prediction uncertainty is lower. In some 13.70 ppb. As expected, in areas with denser observations as shown in Figure 1a, including northern parts of south China and west China, the uncertainty is relatively high due to the relatively sparseness China and India, the prediction uncertainty is lower. In some parts of south China and west China, of the satellite observations, and, therefore, more verifications are required for the mapping dataset the uncertainty is relatively high due to the relatively sparseness of the satellite observations, and, in these areas. The spatio-temporal geostatistical approach developed in this study has the advantage therefore, more verifications are required for the mapping dataset in these areas. The spatio-temporal of utilizing a larger dataset both in space and time to support stable parameter estimation and geostatistical approach developed in this study has the advantage of utilizing a larger dataset both in prediction. Therefore, as more observation data will become available in the coming future, we can space and time to support stable parameter estimation and prediction. Therefore, as more observation anticipate that a more robust mapping dataset with lower uncertainty using spatio-temporal data will become available in the coming future, we can anticipate that a more robust mapping dataset geostatistics can be produced. with lower uncertainty using spatio-temporal geostatistics can be produced. Figure 9.9.Spatial distribution of kriging standard deviations, a measurement of prediction Figure Spatial distribution of kriging standard deviations, a measurement of uncertainty, prediction is obtained by averaging the kriging standard deviations over five years of mapping XCH in 4 uncertainty, is obtained by averaging the kriging standard deviations over five years of dataset mapping Monsoon Asia. Blank pixels are grids where less than three of the five annual means are available, in XCH4 dataset in Monsoon Asia. Blank pixels are grids where less than three of the five annual means which the annual meanthe is obtained by averaging at least 11 monthly mean11data. are available, in which annual mean is obtained by averaging at least monthly mean data. 5.2. Discrepancies Discrepancies in in Sichuan Sichuan Basin Basin between 5.2. between Observation Observation and and Modeling Modeling As suggested by Hammerling et al. data with As suggested by Hammerling et al. [43], [43], mapping mapping greenhouse greenhouse gas gas concentration concentration data with uncertainty estimation can be used for comparison with simulation data from the atmospheric transport uncertainty estimation can be used for comparison with simulation data from the atmospheric model coupled with carbonwith flux estimates. Asestimates. shown in Figure 7, theinlargest difference between satellite transport model coupled carbon flux As shown Figure 7, the largest difference observations andobservations model simulations of XCH in the of west China, 4 is located between satellite and model simulations of XCH 4 isSichuan located Basin in the Sichuan Basin ofwhere west a large anomaly is shown in GOSAT data while not in model data. As suggested by Qin et al. China, where a large anomaly is shown in GOSAT data while not in model data. As suggested[27], by CH4etemission from rice paddy fields wetlands andwetlands the stagnant of the basin have Qin al. [27], CH 4 emission from rice and paddy fields and and effect the stagnant effectterrain of the basin the biggest to this anomaly. This same feature can also be seen satellite observations terrain havecontribution the biggest contribution to this anomaly. This same feature canin also be seen in satellite of CO columns and NO columns [44]. However, the model simulations with ground observations 2 observations of CO columns and NO2 columns [44]. However, the model simulations with ground assimilated fail to reproduce local variability overvariability this basin.over Thisthis maybasin. be due to the observations assimilated failthis to reproduce this local This mayineffectiveness be due to the of CarbonTracker [23], which assimilates only the sparse ground based observations in representing the ineffectiveness of CarbonTracker [23], which assimilates only the sparse ground based observations local features of XCH in this area, where, unfortunately, ground-based observations are not available in representing the 4local features of XCH4 in this area, where, unfortunately, ground-based to constrain the fluxes. to constrain the CH4 fluxes. observations areCH not4 available 11 Remote Sens. 2016, 8, 361 12 of 15 5.3. Long Term XCH4 Observations in Constraining Surface Emissions The distribution and variation of column-averaged greenhouse gas can be attributed to spatial distribution of surface emissions, sinks of the gas, and large-scale eddy-driven transport [45]. For XCH4 over the Monsoon region, emissions from human-related activities including paddy fields, and natural wetlands are the dominant emissions, while the reaction of CH4 with hydroxyl radicals (OH), which removes almost 90% of CH4 [46], is the main sink of atmospheric CH4 . For a specific CH4 column, the number of CH4 molecules going out (loss) and coming in (gain) the column due to transport varies from time to time. However, on a yearly basis, the averaged transport component of CH4 leads to net gain or loss and can be approximately quantified as an invariable constant. For the CH4 sinks due to chemical reaction over multi-year periods, the amount of sinks is determined by the total amount and can therefore be quantified as an averaged ratio to the total amount of CH4 molecules in the atmosphere. Therefore, the multi-year averaged XCH4 data observed by GOSAT is approximately a remaining ratio of CH4 emissions from surface after excluding the averaged transport component and chemical sink component. As a result, the distribution of observed XCH4 averaged over a long term period will be indicating the surface sources of CH4 , as we see in Figure 8b. This significant correlation between XCH4 observations and surface emissions provides a promising statistical way, which is simple and easy to implement, of constraining surface CH4 sources using satellite observations over a long term period. 6. Conclusions In this study, we propose the use of a data-driven mapping approach based on spatio-temporal geostatistics to generate a mapping dataset of XCH4 and evaluate the five years of GOSAT XCH4 retrievals over Monsoon Asia from June 2009 to May 2014. The prediction precision using cross-validation results in a significantly high correlation of 0.91 and a small mean absolute prediction error of 8.77 ppb between the original dataset and prediction dataset. Spatio-temporal distribution and variation of XCH4 mapping data agree with results from SCIAMACHY and ground-based observations well. This XCH4 mapping data also provide a new way to assess the model simulations of CH4 coupled with atmospheric transport model. Comparison between XCH4 and model simulations from CarbonTracker-CH4 shows consistent spatial patterns, but the satellite observations are more able to resolve the local variability of XCH4 , such as the constant anomaly shown in the Sichuan Basin. Finally, by comparing the mapping data with surface emission inventory, we found that the geographical distribution of high CH4 values well corresponds to strong emissions as indicated in the inventory map. Over the five-year period, the two datasets show a significantly high correlation coefficient (0.80), indicating the dominant role of surface emissions in determining the distribution of averaged XCH4 concentrations over such regions and a promising statistical way of constraining surface CH4 sources using satellite observations over a long term period. In conclusion, this study provides new mapping datasets of XCH4 over Monsoon Asia derived from satellite observations, and suggests a simple statistical way to constrain the surface CH4 emissions using long term satellite XCH4 retrievals. Moreover, this study provides a complementary work to previous studies using SCIAMACHY, and AIRS over this Monsoon Asia region. However, some assumptions in this study need further verifications. Firstly, spatio-temporal correlation structure is assumed to be similar over the entire Monsoon Asia area, but this is not always true since the spatio-temporal variations in difference locations are different. However, the irregular distribution of the data do not enable us to resolve this problem in this study. Secondly, in geostatistical mapping, we adopted the kriging neighborhood to reduce computational complexity and preserve local variability. Theoretically, the minimum mean square error in kriging is achieved by using a global neighborhood which includes all points. However, a global neighborhood is not practically feasible for kriging calculations because it may lead to a kriging matrix that is too large to be numerically inverted. As a result, the use of a kriging neighborhood might introduce some errors to our results. Remote Sens. 2016, 8, 361 13 of 15 Gaps in observations are common in XCH4 retrievals from greenhouse gas observation satellites, such as GOSAT and SCIAMACHY. Therefore, application of the mapping method to SCIAMACHY and comparison between the two data sources will provide us a new way to investigate their differences in this developed geostatistical way. In comparison of prediction accuracy between spatio-temporal and spatial-only approaches using cross-validation, leaving out larger areas of data would conceivably better highlight the advantage of a spatio-temporal approach because the temporal correlation considered in spatio-temporal approach can provide large benefits given the lack of nearby data. This will be our future work. In addition, although cross-validation gives us a comprehensive statistical assessment of prediction accuracy, it is essential to carry out comparison with independent observations. As some TCCON stations are being set up over this Monsoon Asia region, a comparison with TCCON will also be our work in the coming future. Acknowledgments: This work was supported by the Strategic Priority Research Program–Climate Change (XDA05040401) and the National High Technology Research and Development Program of China (2012AA12A301). We acknowledge the GOSAT retrieved XCH4 data products provided by JAXA/NIES/MOE (https://data.gosat.nies.go.jp/) and EDGAR data (http://edgar.jrc.ec.europa.eu/). The current development of EDGAR is a joint project of the European Commission Joint Research Centre (JRC) and the Netherlands Environmental Assessment Agency (PBL). CarbonTracker-CH4 results are provided by NOAA ESRL, Boulder, Colorado, USA from the website at http://www.esrl.noaa.gov/gmd/ccgg/carbontracker-CH4/. 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