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Article pubs.acs.org/est High-Resolution Satellite-Derived PM 2 . 5 from Optimal Estimation and Geographically
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Article

High-Resolution Satellite-Derived PM 2.5 from Optimal Estimation and Geographically Weighted Regression over North America

Aaron van Donkelaar, * , Randall V. Martin, , Robert J. D. Spurr, § and Richard T. Burnett

Dalhousie University, Halifax, Nova Scotia, Canada Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachusetts, United States § RT Solutions Inc., Cambridge, Massachusetts, United States Health Canada, Ottawa, Ontario, Canada

ABSTRACT: We used a geographically weighted regression (GWR) statistical model to represent bias of fi

ABSTRACT: We used a geographically weighted regression (GWR) statistical model to represent bias of ne particulate matter concentrations (PM 2.5 ) derived from a 1 km optimal estimate (OE) aerosol optical depth (AOD) satellite retrieval that used AOD-to-PM 2.5 relationships from a chemical transport model (CTM) for 20042008 over North America. This hybrid approach combined the geophysical understanding and global applicability intrinsic to the CTM relationships with the knowledge provided by observational constraints. Adjusting the OE PM 2.5 estimates according to the GWR-predicted bias yielded signi cant improvement compared with unadjusted long-term mean values ( R 2 = 0.82 versus R 2 = 0.62), even when a large fraction (70%) of sites were withheld for cross-validation ( R 2 = 0.78) and developed seasonal skill ( R 2 = 0.62 0.89). The eect of individual GWR predictors on OE PM 2.5 estimates additionally provided insight into the sources of uncertainty for global satellite-derived PM 2.5 estimates. These predictor-driven e ects imply that local variability in surface elevation and urban emissions are important sources of uncertainty in geophysical calculations of the AOD-to-PM 2.5 relationship used in satellite-derived PM 2.5 estimates over North America, and potentially worldwide.

2 . 5 relationship used in satellite-derived PM 2 . 5 estimates over North America, and

INTRODUCTION

Fine particulate matter (PM 2.5 ) is associated with an increased risk of mortality and morbidity 1 and globally contributes to an estimated 3.2 million premature deaths each year. 2 Ground- based monitoring networks provide direct observations of PM 2.5 in many developed countries; however, the density and placement of monitors can a ect their ability to characterize concentrations, even for dense networks, such as those in the U.S. Satellite retrievals of aerosol optical depth (AOD) provide insight into the total atmospheric aerosol column, as represented by the extinction of light. The horizontal resolution of these AOD retrievals has traditionally been at 10 km or coarser, 3 , 4 with more recent developments at 3 km 5 and 1 km. 6 These AOD retrievals are being applied to increase the spatial extent of observational constraints on PM 2.5 7 9 for application to exposure assessment and epidemiologic studies. 10 12 The relationship between AOD and PM 2.5 is aected by the aerosol vertical prole and optical properties. Most modern satellite- based PM 2.5 estimates use either statistical or geophysical methods to relate AOD to PM 2.5 . Statistical methods, such as land use regression or geo- graphically weighted regression (GWR), estimate PM 2.5 using predictors that include meteorology, land type, and AOD. Predictor coe cients are tted to optimally represent ground-

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are fi tted to optimally represent ground- 13 − 17 © 2015 American Chemical Society 10482

© 2015 American Chemical Society

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based PM 2.5 monitors. The product of each predictor with its respective coe cient can be summed to provide a spatially continuous PM 2.5 estimate. Statistical methods can more accurately represent ground monitors compared with geo- physical methods, but statistical methods have been limited to regions with dense PM 2.5 monitoring networks to determine relationships between predictors and PM 2.5 . Geophysical methods employ a chemical transport model (CTM) that represents local aerosol vertical pro les and optical properties by combining emission inventories and assimilated meteorology with physical and chemical equations that describe atmospheric composition and its evolution. 18 CTMs simulate both PM 2.5 and AOD, although typically at relatively coarse resolutions on the order of tens to hundreds of kilometers and without direct observational constraint. The CTM-predicted AOD-to-PM 2.5 relationships are being applied to satellite retrievals of AOD to globally estimate PM 2.5 at higher resolution and improved accuracy compared with a CTM alone because of the additional, retrieved information. This approach has demonstrated signi cant accuracy; 19 however,

Received: April 24, 2015 Revised: August 3, 2015

Accepted: August 11, 2015 Published: August 11, 2015

DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

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Environmental Science & Technology Article Figure 1. Flowchart of adjusted optimal estimation (AOE) PM 2 .

Figure 1. Flowchart of adjusted optimal estimation (AOE) PM 2.5 production. The data sources and their resolution are in parentheses.

such CTM-based AOD-to-PM 2.5 relationships underutilize the valuable information available from ground-based measure- ments. In this article, we produced a high-resolution, geophysical, satellite-derived PM 2.5 estimate by developing a 1 km × 1 km resolution optimal estimation (OE) AOD retrieval and adjusted this estimate using a statistical method (GWR) that predicted regional bias across North America. The prediction of bias, rather than of PM 2.5 itself, provided dual bene t. First, the statistical step directly increased the accuracy of the geophysical PM 2.5 estimate by reducing bias. Second, the impact of individual predictors provided insight into geophysical factors aecting the accuracy of the North American geophysical PM 2.5 estimates, guiding future improvements to this globally applicable method. This approach thus maintained a globally applicable data set as needed for global health assessments and indicators, such as the global burden of disease 2 or the environmental performance index ( http://epi.yale.edu/ ), while at the same time improving accuracy over a region with in situ monitoring networks.

MATERIALS AND METHODS

Figure 1 shows an overview of our method to estimate PM 2.5 at 0.01 ° (approximately 1 km) resolution. We began with satellite observations of top-of-atmosphere reectance. Optimal estima- tion was applied to retrieve AOD. A CTM related AOD to PM 2.5 . GWR predicted the bias in the optimal estimate of PM 2.5 , to yield a nal adjusted optimal estimate. Each step is described further below. Extension of Optimal Estimation PM 2.5 to 1km. Optimal estimation (OE) is an inverse-modeling mathematical framework that constrains a retrieval using prior knowledge of the quantity to be retrieved. 20 The uncertainty of that prior is often speci ed relative to an observation. Van Donkelaar et al. 21 developed an OE algorithm at 10 km resolution that used the LIDORT 22 radiative transfer model to retrieve AOD from top- of-atmosphere reectances (collection 5) observed by the MODIS instrument onboard the Terra satellite, constrained by an AOD prior from the GEOS-Chem 23 CTM. Uncertainties were based on comparison with the AERONET 24 sun photometer network. These 10 km OE AOD retrievals generally improved agreement with AERONET compared with the standard dark target MODIS AOD products

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(MOD04), 25 resulting in increased accuracy for satellite- derived PM 2.5 estimates. Here, we extended the OE algorithm of van Donkelaar et al. 21 to produce AOD estimates at 1 km resolution over North America from 2004 to 2008 using MODIS Collection 6 26 level 1 top-of-atmospheric re ectances from the Terra satellite. In addition to the 0.47 and 0.66 μ m MODIS channels used in van Donkelaar et al., 21 we included the 0.41 μ m channel, which can provide a more robust AOD retrieval over bright surfaces, such as deserts, as demonstrated by the MODIS Deep Blue 27 AOD retrieval. Surface reectance relationships were indexed by land type. We used version 2.6 of the vector VLIDORT 22 radiative

transfer code, which includes atmospheric polarization. We did not apply a vertical pro le bias correction term from the CALIOP 28 lidar because this could interfere with interpretation of the statistically based bias adjustment. Pixels at 1 km missing from monthly average values were lled using the average value of the surrounding 10 km. GEOS-Chem Chemical Transport Model. We used GEOS-Chem ( http://geos-chem.org ) v9-01-03 to calculate the prior for OE AOD and applied the simulated AOD-to- PM 2.5 relationship to estimate near-surface PM 2.5 concen- trations, the latter denoted as OE PM 2.5 throughout this manuscript. Our North American nested GEOS-Chem simulation was driven by GEOS-5 assimilated meteorology from the Goddard Earth Observation System (GEOS) of the NASA Global Modeling and Assimilation Oce (GMAO) at 0.5 ° × 0.67 ° with 47 vertical levels for the years 2004 2008. National base inventories were used over Canada (Criteria Air Contaminants) and the U.S. (National Emission Inventory 2005), scaled for interannual variation according to local governmental reports. The GEOS-Chem aerosol simulation included the sulfate nitrate ammonium system, 29 , 30 pri- mary 31 33 and secondary carbonaceous aerosols, 34 mineral

Mie calculations of log-normal size

distributions, growth factors, and refractive indexes, based on the global aerosol data set (GADS) and aircraft measurements, were used to determine the aerosol optical properties of the simulation. 37 39 Details of this simulation are described in Philip et al. 40 Geographically Weighted Regression. We used geo- graphically weighted regression 41 (GWR) to develop a representation of the spatially varying relationship between multiple predictors and the bias between OE and in situ PM 2.5 . GWR is an extension of least-squares regression, which determines the best-tting predictor coecients by minimizing the sum of the squares between observed values and the resultant estimates. GWR extends least-squares regression by allowing predictor coe cients to vary spatially by weighting the estimate-observation pairs at multiple geographic locations according to their inverse-squared distance from individual observational sites. The result is a spatially continuous eld. We applied the GWR-predicted bias to OE PM 2.5 to produce an adjusted optimal estimate (AOE) of PM 2.5 . This approach maintained the geophysical basis intrinsic to the CTM-driven method while incorporating in situ observations to identify local and regional biases caused by errors in the geophysical representation of AOD and the concomitant AOD-to-PM 2.5 relationships. We used urban land cover, subgrid elevation di erence, and aerosol composition as predictors for GWR. Our GWR model was tted at 1 ° × 1° intervals to in situ observations using the glm t function of Matlab R2013a, following the form:

dust, 35 and sea salt.

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DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

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Environmental Science & Technology Article Figure 2. Comparison of mean 1-km OE satellite-derived PM 2 .

Figure 2. Comparison of mean 1-km OE satellite-derived PM 2.5 estimates with ground-based measurements for 2004 2008. The top panel displays OE PM 2.5 . The lower right panel displays in situ PM 2.5 observations. White denotes water or missing data. Gray boxes denote regions highlighted in Figure 6 . Values in the lower left panel include the slope from reduced major axis linear regression ( y), normal distribution of uncertainty N (bias, variance), root mean square di erence (RMSD), coe cient of variation ( r 2 ), and the number of comparison sites (N ). The 1:1 line is solid, and the best t line is dashed.

(in situ PM

2.5

=+U ββ

12

ED

OE PM

2.5

+

β

3

NIT

)

+

β

4

PC

+

β

5

SOA

+

ε

(1)

where β 1 to β 5 represented the spatially varying predictor coecients, and ε represents the error. In situ PM 2.5 and OE PM 2.5 were monthly mean values over the 5-year period 2004 2008. The spatially varying predictor coecients were treated as constant across all years, but varying with month according to separate GWR runs. U was the percent urban land cover according to the 500-m spatial resolution MODIS land cover type product 42 (MCD12Q1), regridded onto a standard 0.01 ° × 0.01 ° grid. Subgrid elevation di erence (ED) denoted the dierence between the local elevation and the mean elevation of the 0.5 ° × 0.67 ° GEOS-Chem grid cell, according to the ETOPO1 Global Relief Model available from the National Geophysical Data Center ( http://www.ngdc.noaa.gov/mgg/ global/seltopo.html ). Speciated PM 2.5 concentrations for nitrate (NIT), primary carbonaceous (PC), and secondary organics (SOA) were represented by applying the simulated relative contribution of each aerosol type to the total OE PM 2.5 , following Philip et al., 40 who demonstrated signicant agreement with speciated

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observations over North America. The highest correlation in that study was found with sulfate ( r = 0.95). The lower correlation of nitrate (r = 0.68), organic matter ( r = 0.45), and black carbon ( r = 0.56) suggests that nitrate and carbonaceous species are more likely sources of regional error. We therefore included as predictors in GWR NIT, PC, and SOA alone. Exclusion of sulfate helps to avoid excessive collinearity with these predictors. Biases associated with these predictors may result from a variety of causes, including regional errors in simulated representation of the chemistry, emission, or transport of these species. Regression pairs were weighted according to the inverse square of their distance from the point of interest, capped between 100 km and an optimally chosen maximum distance of 3000 km, set to minimize the RMSD of the predicted bias with observed values. Grid cells with insu cient rank in the regression, suggesting multicollinearity among predictor variables, were t with a reduced number of predictors with unsolved predictor coe cients set to zero. A 10-fold cross-validation was employed to check for model over tting and to assess uncertainty in AOE PM 2.5 . In Situ PM 2.5 Observations. We used in situ PM 2.5 observations over Canada and the U.S. for evaluation and GWR calibration. Measurements over Canada were taken from

DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

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Environmental Science & Technology Article Figure 3. Comparison of mean bias in OE PM 2 .

Figure 3. Comparison of mean bias in OE PM 2.5 predicted with geographically weighted regression (GWR) and observed with in situ monitors for 20042008. The top panel displays the GWR-predicted di erence between in situ PM 2.5 and OE PM 2.5 . The lower right panel displays the observed

di erence between in situ PM 2.5 and OE PM 2.5 observations. White denotes water or missing data. Gray boxes denote regions highlighted in Figure

6. Values in the lower left panel include the slope from reduced major axis linear regression ( y), normal distribution of uncertainty N (bias, variance), root mean square di erence (RMSD), coe cient of variation ( R 2 ), and the number of comparison sites ( N ). The 1:1 line is solid. and the best t line

is dashed.

the Canadian National Air Pollution Surveillance Network (NAPS; http://www.ec.gc.ca/rnspa-naps/ ; 187 sites) and included tapered element oscillating microbalance (TEOM), beta attenuation mass monitors, and dichotomous samplers. NAPS TEOM instruments were corrected for semivolatile particulate matter losses during air sample heating. 43 U.S. ground-level PM 2.5 data were taken from the U.S. Interagency Monitoring of Protected Visual Environments (IMPROVE; http://vista.cira.colostate. edu/improve/Data/data.htm ; 128 sites) network and from FRM-compliant sites available from the U.S. Environmental Protection Agency Air Quality System (AQS; http://www.epa.gov/airdata/ ; 1125 sites). We treated these in situ observations as truth despite the possibility of measurement errors or representativeness issues arising between these point measurements and area averaged concentrations, such as observed from satellite.

RESULTS AND DISCUSSION

Figure 2 shows OE PM 2.5 and in situ PM 2.5 across North America. Signicant agreement was found ( r 2 = 0.62; RMSD = 2.6 μ g/m 3 ). Elevated PM 2.5 concentrations were observed in

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both data sets over the eastern U.S. and parts of California, with even larger enhancements over the Ohio River Valley. OE PM 2.5 had smoothly varying features in both eastern and western parts of the continent, whereas in situ monitors exhibited more ne-scale variation, particularly in the west. OE PM 2.5 concentrations were often underestimated in the west, resulting in a distinct population in Figure 2 when in situ PM 2.5 measured between 5 and 10 μ g/m 3 . Direct comparison of in situ PM 2.5 with 1 km OE AOD (r 2 = 0.41) outperformed both the standard 3 km MODIS Collection 6 Dark Target retrieval 5 ( r 2 = 0.18), and the 10 km Combined Dark Target-Deep Blue 26 , 27 ( r 2 = 0.34). OE PM 2.5 also outperformed purely simulated PM 2.5 based on aerosol concentrations used for the OE prior constraints (r 2 = 0.57; RMSD = 3.8 μg/m 3 ). Figure 3 (lower right panel) shows the dierence between in situ and OE PM 2.5 , which we used to represent the bias in OE PM 2.5 . In situ values exceeded OE PM 2.5 throughout locations with monitors in the Smokey Mountains, Rocky Mountains, and Cascade Mountains. Parts of the Midwest, by contrast, had comparatively elevated OE PM 2.5 concentrations. Both features were represented within the GWR-predicted bias (top panel),

DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

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Environmental Science & Technology Article Figure 4. Left column contains predictor net impact on the predicted

Figure 4. Left column contains predictor net impact on the predicted bias in OE PM 2.5 shown in Figure 3. Average predictor coecients ( β) and standard errors (S.E.) are given in the middle and right columns. White denotes water or missing data. Gray boxes denote regions highlighted in Figure 6 .

which achieved signi cant agreement with the observed bias (R 2 = 0.62; lower left panel). Figure 4 (left column) shows the contribution of individual predictors to the overall predicted bias. Predictors with a net decrease indicated a positive bias in OE PM 2.5 . One such reduction associated with nitrate occurred in the Canadian prairies and the Ohio River Valley. Broad reductions were also associated with primary carbonaceous aerosol across much of the East. Both of these features were apparent in the PM 2.5 comparison of measured composition versus satellite-model composition in Philip et al., 40 which motivate further investigation. Fine-scale enhancements associated with urban surfaces may indicate local sources unresolved in the simulation

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of the AOD-to-PM 2.5 relationship. Predicted biases over the mountainous regions of the west and southeast U.S. were highly heterogeneous, driven by both subgrid elevation di erences and percent urban land cover. These two predictors may be interpreted as corrective terms that account for the comparatively coarse resolution of the simulation used to constrain the OE AOD retrieval and the AOD-to-PM 2.5 relationship. Geophysically, they appear to represent local PM 2.5 in mountain valleys that may be better represented using higher-resolution simulations of the AOD-to-PM 2.5 relation- ship. Also shown in Figure 4 are average predictor coecients (middle column) and their standard error (right column). Predictor coecients generally show large spatial homogeneity,

DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

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Table 1. Seasonal Variation of Population-Weighted Predictor Coe cients from Eq 1 a

 
 

percent urban ( β 1 )

 

elevation di erence ( β 2 )

 

nitrate ( β 3 )

 

primary carbonaceous ( β 4 )

secondary organic ( β 5 )

coef ( μ g/m 3 / %)

impact ( μg/

coef ( μ g/m 3 /

impact ( μg/

coef

impact ( μ g/

 

coef

impact ( μg/

coef

impact ( μ g/

season

m

3 )

m)

m

3 )

(unitless)

m

3 )

(unitless)

m

3 )

(unitless)

m

3 )

DJF

0.058

2.475

 

0.009

0.293

 

0.906

1.412

 

0.257

1.189

10.528

0.884

MAM

0.019

0.751

0.004

0.101

0.011

0.069

0.167

0.758

0.904

0.295

JJA

0.021

0.842

0.005

0.135

1.557

1.030

0.325

1.553

0.108

0.361

SON

0.032

1.382

0.006

0.182

0.925

0.723

0.024

0.240

0.821

0.092

a Net impact on population-weighted PM 2.5 is also provided.

on population-weighted PM 2 . 5 is also provided. Figure 5. Comparison of mean 1 km

Figure 5. Comparison of mean 1 km AOE satellite-derived PM 2.5 estimates with in situ monitors for 20042008. The lower right panel displays the observed di erence between in situ PM 2.5 and AOE PM 2.5 observations. White denotes water or missing data. Gray boxes denote regions highlighted in Figure 6 . Values in the lower left panel include the slope from reduced major axis linear regression ( y), N (bias, variance), RMSD, R 2 , and the number of comparison sites ( N). The 1:1 line is solid, and the best t line is dashed.

with distinct separation between eastern and western regions. Spatial variation in predictor net impact does not generally follow spatial variation in predictor coe cient, owing to variability in the predictors themselves. Table 1 shows the seasonal variation in predictor values and their net impact. The greatest impact of percent urban was in winter, likely re ecting wintertime sources that were not captured within the simulated AOD-to-PM 2.5 relationship. Elevation dierence also exhibited the greatest impact during winter, possibly representing seasonal woodburning in mountain valleys. Unlike percent urban and elevation di er- ence, which were constant throughout the year, compositional predictors varied seasonally in response to changing emission

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sources and chemistry. Compositional coe cients can therefore be more challenging to interpret. The net impact of these predictors did, however, suggest seasonal maxima in OE PM 2.5 bias associated with nitrate in winter and primary carbonaceous aerosol in summer. The net impact associated with SOA was weakest and less readily interpreted. All three components had contributions throughout most of the year. Figure 5 (top panel) shows AOE PM 2.5 , the result of adding to OE PM 2.5 the sum of the individual predictor bias contributions shown in Figure 4 . The spatial pattern AOD PM 2.5 resembles that in OE PM 2.5 (Figure 1), but with lower PM 2.5 in the Midwest, and additional spatial structure in the mountainous regions. The inclusion of additional predictors,

DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

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such as sulfate or solar zenith angle, did little to increase the explained variance of AOD PM 2.5 with in situ monitors; however, the contributions of these parameters became physically unrealistic. The additional inclusion of road length had little impact on performance. The use of GWR reduced dierences throughout the continent between in situ PM 2.5 and AOE PM 2.5 compared with OE PM 2.5 . In California, observations were generally captured by AOE PM 2.5 (R 2 = 0.67; RMSD = 2.6 μ g/m 3 ), but peak measured values within the San Joaquin Valley remained underestimated, (e.g., 19.6 μ g/m 3 versus 13.9 μ g/m 3 in Bakers eld). Overall agreement was signi cantly improved compared with OE PM 2.5 , with R 2 = 0.82 and RMSD = 1.5 μ g/m 3 . Table 2 shows how the agreement of AOD PM 2.5 with ground monitors was a ected by the number of sites held back

Table 2. E ect of Percentage of Ground Monitors Used for Cross-Validation (CV) during Geographically Weighted Regression on the Agreement of Adjusted Optimal Estimation PM 2.5 with CV sites a

percent CV

R 2

RMSD (μ g/m 3 )

N (bias, variance)

95

0.73

1.9

N ( 0.08, 1.87)

90

0.75

1.8

N ( 0.10, 1.84)

70

0.78

1.7

N ( 0.15, 1.68)

50

0.78

1.7

N ( 0.16, 1.66)

30

0.79

1.6

N ( 0.18, 1.62)

10

0.79

1.7

N ( 0.24, 1.64)

a R 2 , RMSD, and N (bias, variance) are shown when 10 95% of ground monitors are withheld.

for cross-validation. We nd cross-validation sites demonstrated similar agreement when 10% of ground monitors are withheld from the GWR training (R 2 = 0.79; RMSD = 1.7 μ g/m 3 ), suggesting that the GWR-predicted bias was not over t and maintained skill in the absence of in situ monitors. Remarkably, the improvement compared with OE PM 2.5 remained similar when up to 70% of the ground monitors were withheld ( R 2 = 0.78; RMSD = 1.7 μg/m 3 ). The level of agreement continued to be high, even with 95% of ground monitors withheld ( R 2 = 0.73; RMSD = 1.9 μ g/m 3 ). The results suggest value to the combined geophysical statistical approach, even in regions with relatively sparse PM 2.5 monitors, such as found in other countries. Figure 6 shows OE PM 2.5 and AOE PM 2.5 for several North American regions. In western regions, such as San Francisco, Seattle/Vancouver, and Salt Lake City, RMSD with in situ monitors in AOE PM 2.5 was reduced by 2-fold, or more than for OE PM 2.5 . Localized gradients were much stronger in AOE PM 2.5 , again indicative of associations with subgrid elevation changes and urban land cover. Fine-scale enhancements in urban areas were also visible in eastern regions, such as southern Ontario and Philadelphia/New York. OE PM 2.5 and AOE PM 2.5 were more consistent with in situ monitors for eastern regions than western regions. Of interest is the PM 2.5 gradient predicted at urban boundaries in the absence of topographical e ects. Agreement was similar between AOE PM 2.5 and in situ PM 2.5 directly over urban surfaces (RMSD = 1.2 μ g/m 3 ) at sites with little inuence (<0.5 μ g/m 3 ) from subgrid elevation changes, compared with neighboring non- urban pixels (RMSD = 1.3 μ g/m 3 ), suggesting AOE reasonably

(RMSD = 1.3 μ g/m 3 ), suggesting AOE reasonably Figure 6. Regional distribution of 1

Figure 6. Regional distribution of 1 km OE and AOE PM 2.5 . Odd columns correspond to OE PM 2.5 . Even columns correspond to AOE PM 2.5 . Solid circles correspond to in situ monitor locations and values. White denotes water or missing data. Regions are shown as gray boxes in Figures 25.

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Environmental Science & Technology Article Figure 7. Seasonal comparison of 1 km AOE PM 2 .

Figure 7. Seasonal comparison of 1 km AOE PM 2.5 with in situ monitors for 20042008. White denotes water or missing data. Gray boxes denote regions highlighted in Figure 6. The RMSD and R 2 are included in each inset panel. The 1:1 line is solid, and the best t line is dashed.

Table 3. E ect of Spatial Averaging on 1 km OE and 1 km AOE Satellite-Derived PM 2.5 Agreement with Ground-Based Monitors over North America (NA), Eastern North America (ENA; east of 90 ° W), and Western North America (WNA; west of 90° W) a

 

R 2

RMSD (μ g/m 3 )

 

N (bias, variance)

 

data set

area

0.01 °

0.03 °

0.05 °

0.10 °

0.01 ° 0.03 ° 0.05 ° 0.10 °

0.01 °

0.03 °

0.05 °

0.10 °

OE

NA

0.62

0.62

0.62

0.62

2.6

2.6

2.6

2.6

N( 0.87, 2.42)

N (0.92, 2.41)

N( 0.95, 2.41)

N ( 1.00, 2.39)

PM 2.5

 

ENA

0.69

0.70

0.69

0.69

1.6

1.6

1.6

1.6

N( 0.16, 1.63) N( 1.67, 2.88) N( 0.38, 1.49)

N (0.20, 1.62) N (1.72, 2.87) N (0.68, 1.56)

N( 0.23, 1.63) N( 1.75, 2.85) N( 0.91, 1.63)

N ( 0.30, 1.63) N ( 1.79, 2.85) N ( 1.29, 1.74)

WNA

0.40

0.40

0.40

0.39

3.3

3.4

3.4

3.4

AOE

NA

0.82

0.81

0.79

0.76

1.5

1.7

1.9

2.2

PM 2.5

 

ENA

0.83

0.83

0.81

0.78

1.2

1.3

1.5

1.8

N( 0.39, 1.19) N( 0.34, 1.78)

N (0.60, 1.22) N (0.75, 1.87)

N( 0.79, 1.28) N( 1.04, 1.95)

N ( 1.13, 1.35) N ( 1.46, 2.09)

WNA

0.74

0.71

0.68

0.63

1.8

2

2.2

2.6

a R 2 , RMSD, and N (bias, variance) are shown for four spatial resolutions from 0.01 to 0.10° .

predicted PM 2.5 gradients. A similar but weaker pattern was found between the unadjusted OE PM 2.5 and in situ PM 2.5 over urban (RMSD = 1.8 μ g/m 3 ) and nearby nonurban pixels (RMSD = 1.9 μg/m 3 ) at the same locations. Figure 7 shows the seasonal variation in AOE PM 2.5 . Seasonal enhancements were apparent in summer in the southeast and in winter in some cities in mountainous regions, such as Salt Lake City. Signi cant seasonal skill existed between AOE PM 2.5 and in situ monitors ( R 2 = 0.62 0.89; RMSD = 1.4 2.7 μg/m 3 ). The poorest agreement was found during winter, when AOD retrievals were compromised by snow cover and seasonally varying re ectance, but the correlation remained signi cant ( R 2 = 0.62). The production of AOE PM 2.5 over three-year running

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intervals, rather than the ve-year 2004 2008 period, performed similarly; average coe cients of variation with in situ monitors ranged from R 2 = 0.61 (DJF) to R 2 = 0.90 (JJA), and the average RMSD ranged from 2.8 (DJF) to 1.4 μ g/m 3 (MAM). Single year, single month runs also showed signi cance: average coecients of variation with in situ monitors ranged from R 2 = 0.52 (February) to R 2 = 0.83 (August) and average RMSD ranged from 3.7 (January) to 1.7 μ g/m 3 (April). Table 3 describes the e ect of spatial averaging on the consistency between in situ and OE PM 2.5 . The agreement across all resolutions was broadly similar, suggesting that the expected reduction of random error from spatial averaging was

DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491

Environmental Science & Technology

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nearly equivalent to the bene t of increased spatial resolution within the initial OE product. The AOE PM 2.5 coe cient of variation steadily decreased with increasing spatial averaging, which supported the presence of high-resolution features. This eect was enhanced over western North America compared with eastern North America. Next Steps. We developed and presented an approach to incorporate information from in situ monitors into geophysi- cally driven satellite-derived PM 2.5 estimates. Our approach maintains the global applicability of our initial satellite-derived PM 2.5 estimates while taking advantage of local measurements where available. GWR predictors, such as subgrid elevation dierence, urban surfaces, and aerosol composition, oered insight into the sources of uncertainty for the CTM-calculated, geophysical AOD-to-PM 2.5 relationships. This insight can, in turn, direct global improvements to the next generation of satellite-derived PM 2.5 estimates. In addition, adjustment of our 1 km geophysical satellite-derived PM 2.5 estimates over North America by the current GWR-predicted bias provides a signi cantly improved representation of PM 2.5 concentrations in this region for exposure assessment and epidemiological analysis. Data are freely available as a public good at http:// zz. phys.dal.ca/~atmos/ . Future work should seek higher-resolution simulations of the AOD-to-PM 2.5 relationship, especially for regions with large subgrid elevation dierences or urban sources. Additional high- resolution AOD products, such as from the Visible Infrared Radiometer Suite (VIIRS 44 ) or from MODIS, based on the MAIAC 6 , 45 retrieval, may also prove an asset for global satellite- derived PM 2.5 estimates.

AUTHOR INFORMATION

Corresponding Author

* Address: Dept. of Physics and Atmospheric Science, Dalhousie University, 6300 Coburg Road Halifax, NS, Canada B3H 3J5. Phone: (902) 494-1820. E-mail: Aaron.van. Donkelaar@dal.ca .

Notes

The authors declare no competing nancial interest.

ACKNOWLEDGMENTS

The authors are grateful to NASA, the U.S. EPA, and Environment Canada for access to their data products and to Compute Canada for computing resources. This work was supported by Health Canada, the Collaborative Health Research Project of the Natural Sciences and Engineering Research Council of Canada and the Canadian Institute of Health Research, and Environment Canada.

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DOI: 10.1021/acs.est.5b02076 Environ. Sci. Technol. 2015, 49, 10482 10491