Article

pubs.acs.org/est

High-Resolution Satellite-Derived PM2.5 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 fine particulate
matter concentrations (PM2.5) derived from a 1 km optimal
estimate (OE) aerosol optical depth (AOD) satellite retrieval
that used AOD-to-PM2.5 relationships from a chemical transport
model (CTM) for 2004−2008 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 PM2.5 estimates according to the GWR-predicted bias
yielded significant improvement compared with unadjusted
long-term mean values (R2 = 0.82 versus R2 = 0.62), even when
a large fraction (70%) of sites were withheld for cross-validation
(R2 = 0.78) and developed seasonal skill (R2 = 0.62−0.89). The effect of individual GWR predictors on OE PM2.5 estimates
additionally provided insight into the sources of uncertainty for global satellite-derived PM2.5 estimates. These predictor-driven
effects imply that local variability in surface elevation and urban emissions are important sources of uncertainty in geophysical
calculations of the AOD-to-PM2.5 relationship used in satellite-derived PM2.5 estimates over North America, and potentially
worldwide.

■ INTRODUCTION
Fine particulate matter (PM2.5) is associated with an increased
risk of mortality and morbidity1 and globally contributes to an
estimated 3.2 million premature deaths each year.2 Ground-
based monitoring networks provide direct observations of
PM2.5 in many developed countries; however, the density and
placement of monitors can affect 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 km5 and 1 km.6
These AOD retrievals are being applied to increase the spatial
extent of observational constraints on PM2.57−9 for application
to exposure assessment and epidemiologic studies.10−12 The
relationship between AOD and PM2.5 is affected by the aerosol
vertical profile and optical properties. Most modern satellite-
based PM2.5 estimates use either statistical or geophysical
methods to relate AOD to PM2.5.
Statistical methods, such as land use regression or geo-
graphically weighted regression (GWR), estimate PM2.5 using
predictors that include meteorology, land type, and AOD.13−17
Predictor coefficients are fitted to optimally represent ground-
based PM2.5 monitors. The product of each predictor with its
respective coefficient can be summed to provide a spatially
continuous PM2.5 estimate. Statistical methods can more
accurately represent ground monitors compared with geo-
physical methods, but statistical methods have been limited to
regions with dense PM2.5 monitoring networks to determine
relationships between predictors and PM2.5.
Geophysical methods employ a chemical transport model
(CTM) that represents local aerosol vertical profiles 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 PM2.5 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-PM2.5 relationships are being applied to satellite
retrievals of AOD to globally estimate PM2.5 at higher
resolution and improved accuracy compared with a CTM
alone because of the additional, retrieved information. This
approach has demonstrated significant accuracy;19 however,
Received: April 24, 2015
Revised: August 3, 2015
Accepted: August 11, 2015
Published: August 11, 2015

© 2015 American Chemical Society 10482 DOI: 10.1021/acs.est.5b02076

Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology
Figure 1. Flowchart of adjusted optimal estimation (AOE) PM2.5
production. The data sources and their resolution are in parentheses.
such CTM-based AOD-to-PM2.5 relationships underutilize the
valuable information available from ground-based measure-
ments.
In this article, we produced a high-resolution, geophysical,
satellite-derived PM2.5 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 PM2.5 itself, provided dual benefit. First, the
statistical step directly increased the accuracy of the geophysical
PM2.5 estimate by reducing bias. Second, the impact of
individual predictors provided insight into geophysical factors
affecting the accuracy of the North American geophysical PM2.5
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 disease2 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 PM2.5 at
0.01° (approximately 1 km) resolution. We began with satellite
observations of top-of-atmosphere reflectance. Optimal estima-
tion was applied to retrieve AOD. A CTM related AOD to
PM2.5. GWR predicted the bias in the optimal estimate of
PM2.5, to yield a final adjusted optimal estimate. Each step is
described further below.
Extension of Optimal Estimation PM2.5 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 specified relative to an observation. Van Donkelaar et al.21
developed an OE algorithm at 10 km resolution that used the
LIDORT22 radiative transfer model to retrieve AOD from top-
of-atmosphere reflectances (collection 5) observed by the
MODIS3 instrument onboard the Terra satellite, constrained by
an AOD prior from the GEOS-Chem23 CTM. Uncertainties
were based on comparison with the AERONET24 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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Article
(MOD04),25 resulting in increased accuracy for satellite-
derived PM2.5 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 626 level
1 top-of-atmospheric reflectances from the Terra satellite. In
addition to the 0.47 and 0.66 μm MODIS channels used in van
Donkelaar et al.,21 we included the 0.41 μm channel, which can
provide a more robust AOD retrieval over bright surfaces, such
as deserts, as demonstrated by the MODIS Deep Blue27 AOD
retrieval. Surface reflectance relationships were indexed by land
type. We used version 2.6 of the vector VLIDORT22 radiative
transfer code, which includes atmospheric polarization. We did
not apply a vertical profile bias correction term from the
CALIOP28 lidar because this could interfere with interpretation
of the statistically based bias adjustment. Pixels at 1 km missing
from monthly average values were filled 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-
PM2.5 relationship to estimate near-surface PM2.5 concen-
trations, the latter denoted as OE PM2.5 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 Office (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-
mary31−33 and secondary carbonaceous aerosols,34 mineral
dust,35 and sea salt.36 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 regression41 (GWR) to develop a
representation of the spatially varying relationship between
multiple predictors and the bias between OE and in situ PM2.5.
GWR is an extension of least-squares regression, which
determines the best-fitting predictor coefficients by minimizing
the sum of the squares between observed values and the
resultant estimates. GWR extends least-squares regression by
allowing predictor coefficients 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 field.
We applied the GWR-predicted bias to OE PM2.5 to produce
an adjusted optimal estimate (AOE) of PM2.5. 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-PM2.5
relationships.
We used urban land cover, subgrid elevation difference, and
aerosol composition as predictors for GWR. Our GWR model
was fitted at 1° × 1° intervals to in situ observations using the
glmfit function of Matlab R2013a, following the form:
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Figure 2. Comparison of mean 1-km OE satellite-derived PM2.5 estimates with ground-based measurements for 2004−2008. The top panel displays
OE PM2.5. The lower right panel displays in situ PM2.5 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 difference (RMSD), coefficient of variation (r2), and the number of comparison sites (N). The 1:1 line is solid, and the
best fit line is dashed.

(in situ PM 2.5 − OE PM 2.5)
= β1U + β2 ED + β3 NIT + β4 PC + β5SOA + ε
where β1 to β5 represented the spatially varying predictor
coefficients, and ε represents the error. In situ PM2.5 and OE
PM2.5 were monthly mean values over the 5-year period 2004−
2008. The spatially varying predictor coefficients 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 product42 (MCD12Q1), regridded onto a standard 0.01°
× 0.01° grid. Subgrid elevation difference (ED) denoted the
difference 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 PM2.5 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 PM2.5, following Philip et
al.,40 who demonstrated significant agreement with speciated
observations over North America. The highest correlation in
that study was found with sulfate (r = 0.95). The lower
(1) 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
insufficient rank in the regression, suggesting multicollinearity
among predictor variables, were fit with a reduced number of
predictors with unsolved predictor coefficients set to zero. A
10-fold cross-validation was employed to check for model over
fitting and to assess uncertainty in AOE PM2.5.
In Situ PM2.5 Observations. We used in situ PM2.5
observations over Canada and the U.S. for evaluation and
GWR calibration. Measurements over Canada were taken from
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Figure 3. Comparison of mean bias in OE PM2.5 predicted with geographically weighted regression (GWR) and observed with in situ monitors for
2004−2008. The top panel displays the GWR-predicted difference between in situ PM2.5 and OE PM2.5. The lower right panel displays the observed
difference between in situ PM2.5 and OE PM2.5 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 difference (RMSD), coefficient of variation (R2), and the number of comparison sites (N). The 1:1 line is solid. and the best fit 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 PM2.5 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.
both data sets over the eastern U.S. and parts of California, with
even larger enhancements over the Ohio River Valley. OE
PM2.5 had smoothly varying features in both eastern and
western parts of the continent, whereas in situ monitors
exhibited more fine-scale variation, particularly in the west. OE
PM2.5 concentrations were often underestimated in the west,
resulting in a distinct population in Figure 2 when in situ PM2.5
measured between 5 and 10 μg/m3. Direct comparison of in
situ PM2.5 with 1 km OE AOD (r2 = 0.41) outperformed both
the standard 3 km MODIS Collection 6 Dark Target retrieval5
(r2 = 0.18), and the 10 km Combined Dark Target-Deep
Blue26,27 ( r2 = 0.34). OE PM2.5 also outperformed purely
simulated PM2.5 based on aerosol concentrations used for the
OE prior constraints (r2 = 0.57; RMSD = 3.8 μg/m3).
Figure 3 (lower right panel) shows the difference between in
situ and OE PM2.5, which we used to represent the bias in OE

■ RESULTS AND DISCUSSION

Figure 2 shows OE PM2.5 and in situ PM2.5 across North
America. Significant agreement was found (r2 = 0.62; RMSD =
2.6 μg/m3). Elevated PM2.5 concentrations were observed in
10485
PM2.5. In situ values exceeded OE PM2.5 throughout locations
with monitors in the Smokey Mountains, Rocky Mountains,
and Cascade Mountains. Parts of the Midwest, by contrast, had
comparatively elevated OE PM2.5 concentrations. Both features
were represented within the GWR-predicted bias (top panel),
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Figure 4. Left column contains predictor net impact on the predicted bias in OE PM2.5 shown in Figure 3. Average predictor coefficients (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 significant agreement with the observed bias
(R2 = 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 PM2.5. 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 PM2.5
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
10486
of the AOD-to-PM2.5 relationship. Predicted biases over the
mountainous regions of the west and southeast U.S. were
highly heterogeneous, driven by both subgrid elevation
differences 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-PM2.5
relationship. Geophysically, they appear to represent local
PM2.5 in mountain valleys that may be better represented using
higher-resolution simulations of the AOD-to-PM2.5 relation-
ship. Also shown in Figure 4 are average predictor coefficients
(middle column) and their standard error (right column).
Predictor coefficients generally show large spatial homogeneity,
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Table 1. Seasonal Variation of Population-Weighted Predictor Coefficients from Eq 1a

percent urban (β1) elevation difference (β2) nitrate (β3) primary carbonaceous (β4) secondary organic (β5)
coef (μg/m3/ impact (μg/ coef (μg/m3/ impact (μg/ coef impact (μg/ coef impact (μg/ coef impact (μg/
season %) m3 ) m) m3) (unitless) m3) (unitless) m3 ) (unitless) m3)
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 PM2.5 is also provided.

Figure 5. Comparison of mean 1 km AOE satellite-derived PM2.5 estimates with in situ monitors for 2004−2008. The lower right panel displays the
observed difference between in situ PM2.5 and AOE PM2.5 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, R2, and the
number of comparison sites (N). The 1:1 line is solid, and the best fit 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 coefficient, 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 reflecting wintertime sources that were not
captured within the simulated AOD-to-PM2.5 relationship.
Elevation difference also exhibited the greatest impact during
winter, possibly representing seasonal woodburning in
mountain valleys. Unlike percent urban and elevation differ-
ence, which were constant throughout the year, compositional
predictors varied seasonally in response to changing emission
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sources and chemistry. Compositional coefficients can therefore
be more challenging to interpret. The net impact of these
predictors did, however, suggest seasonal maxima in OE PM2.5
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 PM2.5, the result of adding
to OE PM2.5 the sum of the individual predictor bias
contributions shown in Figure 4. The spatial pattern AOD
PM2.5 resembles that in OE PM2.5 (Figure 1), but with lower
PM2.5 in the Midwest, and additional spatial structure in the
mountainous regions. The inclusion of additional predictors,
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such as sulfate or solar zenith angle, did little to increase the for cross-validation. We find cross-validation sites demonstrated
explained variance of AOD PM2.5 with in situ monitors; similar agreement when 10% of ground monitors are withheld
however, the contributions of these parameters became from the GWR training (R2 = 0.79; RMSD = 1.7 μg/m3),
physically unrealistic. The additional inclusion of road length suggesting that the GWR-predicted bias was not overfit and
had little impact on performance. The use of GWR reduced maintained skill in the absence of in situ monitors. Remarkably,
differences throughout the continent between in situ PM2.5 and the improvement compared with OE PM2.5 remained similar
AOE PM 2.5 compared with OE PM2.5 . In California, when up to 70% of the ground monitors were withheld (R2 =
observations were generally captured by AOE PM2.5 (R2 = 0.78; RMSD = 1.7 μg/m3). The level of agreement continued
0.67; RMSD = 2.6 μg/m3), but peak measured values within to be high, even with 95% of ground monitors withheld (R2 =
the San Joaquin Valley remained underestimated, (e.g., 19.6 0.73; RMSD = 1.9 μg/m3). The results suggest value to the
μg/m3 versus 13.9 μg/m3 in Bakersfield). Overall agreement combined geophysical−statistical approach, even in regions
was significantly improved compared with OE PM2.5, with R2 = with relatively sparse PM2.5 monitors, such as found in other
0.82 and RMSD = 1.5 μg/m3. countries.
Table 2 shows how the agreement of AOD PM2.5 with Figure 6 shows OE PM2.5 and AOE PM2.5 for several North
ground monitors was affected by the number of sites held back American regions. In western regions, such as San Francisco,
Seattle/Vancouver, and Salt Lake City, RMSD with in situ
Table 2. Effect of Percentage of Ground Monitors Used for monitors in AOE PM2.5 was reduced by ∼2-fold, or more than
Cross-Validation (CV) during Geographically Weighted for OE PM2.5. Localized gradients were much stronger in AOE
Regression on the Agreement of Adjusted Optimal PM2.5, again indicative of associations with subgrid elevation
Estimation PM2.5 with CV sitesa changes and urban land cover. Fine-scale enhancements in
percent CV R2 RMSD (μg/m3) N (bias, variance) urban areas were also visible in eastern regions, such as
95 0.73 1.9 N (−0.08, 1.87) southern Ontario and Philadelphia/New York. OE PM2.5 and
90 0.75 1.8 N (−0.10, 1.84) AOE PM2.5 were more consistent with in situ monitors for
70 0.78 1.7 N (−0.15, 1.68) eastern regions than western regions. Of interest is the PM2.5
50 0.78 1.7 N (−0.16, 1.66) gradient predicted at urban boundaries in the absence of
30 0.79 1.6 N (−0.18, 1.62) topographical effects. Agreement was similar between AOE
10 0.79 1.7 N (−0.24, 1.64) PM2.5 and in situ PM2.5 directly over urban surfaces (RMSD =
a 2
R , RMSD, and N (bias, variance) are shown when 10−95% of 1.2 μg/m3) at sites with little influence (<0.5 μg/m3) from
ground monitors are withheld. subgrid elevation changes, compared with neighboring non-
urban pixels (RMSD = 1.3 μg/m3), suggesting AOE reasonably

Figure 6. Regional distribution of 1 km OE and AOE PM2.5. Odd columns correspond to OE PM2.5. Even columns correspond to AOE PM2.5. Solid
circles correspond to in situ monitor locations and values. White denotes water or missing data. Regions are shown as gray boxes in Figures 2−5.

10488 DOI: 10.1021/acs.est.5b02076

Environ. Sci. Technol. 2015, 49, 10482−10491
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Figure 7. Seasonal comparison of 1 km AOE PM2.5 with in situ monitors for 2004−2008. White denotes water or missing data. Gray boxes denote
regions highlighted in Figure 6. The RMSD and R2 are included in each inset panel. The 1:1 line is solid, and the best fit line is dashed.

Table 3. Effect of Spatial Averaging on 1 km OE and 1 km AOE Satellite-Derived PM2.5 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
R2 RMSD (μg/m3) 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)
PM2.5
ENA 0.69 0.70 0.69 0.69 1.6 1.6 1.6 1.6 N(−0.16, 1.63) N(−0.20, 1.62) N(−0.23, 1.63) N(−0.30, 1.63)
WNA 0.40 0.40 0.40 0.39 3.3 3.4 3.4 3.4 N(−1.67, 2.88) N(−1.72, 2.87) N(−1.75, 2.85) N(−1.79, 2.85)
AOE NA 0.82 0.81 0.79 0.76 1.5 1.7 1.9 2.2 N(−0.38, 1.49) N(−0.68, 1.56) N(−0.91, 1.63) N(−1.29, 1.74)
PM2.5
ENA 0.83 0.83 0.81 0.78 1.2 1.3 1.5 1.8 N(−0.39, 1.19) N(−0.60, 1.22) N(−0.79, 1.28) N(−1.13, 1.35)
WNA 0.74 0.71 0.68 0.63 1.8 2 2.2 2.6 N(−0.34, 1.78) N(−0.75, 1.87) N(−1.04, 1.95) N(−1.46, 2.09)
a 2
R , RMSD, and N (bias, variance) are shown for four spatial resolutions from 0.01 to 0.10°.

predicted PM2.5 gradients. A similar but weaker pattern was
found between the unadjusted OE PM2.5 and in situ PM2.5 over
urban (RMSD = 1.8 μg/m3) and nearby nonurban pixels
(RMSD = 1.9 μg/m3) at the same locations.
Figure 7 shows the seasonal variation in AOE PM2.5. Seasonal
enhancements were apparent in summer in the southeast and in
winter in some cities in mountainous regions, such as Salt Lake
City. Significant seasonal skill existed between AOE PM2.5 and
in situ monitors (R2 = 0.62−0.89; RMSD = 1.4−2.7 μg/m3).
The poorest agreement was found during winter, when AOD
retrievals were compromised by snow cover and seasonally
varying reflectance, but the correlation remained significant (R2
= 0.62). The production of AOE PM2.5 over three-year running
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intervals, rather than the five-year 2004−2008 period,
performed similarly; average coefficients of variation with in
situ monitors ranged from R2 = 0.61 (DJF) to R2 = 0.90 (JJA),
and the average RMSD ranged from 2.8 (DJF) to 1.4 μg/m3
(MAM). Single year, single month runs also showed
significance: average coefficients of variation with in situ
monitors ranged from R2 = 0.52 (February) to R2 = 0.83
(August) and average RMSD ranged from 3.7 (January) to 1.7
μg/m3 (April).
Table 3 describes the effect of spatial averaging on the
consistency between in situ and OE PM2.5. The agreement
across all resolutions was broadly similar, suggesting that the
expected reduction of random error from spatial averaging was
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nearly equivalent to the benefit of increased spatial resolution
within the initial OE product. The AOE PM2.5 coefficient of
variation steadily decreased with increasing spatial averaging,
which supported the presence of high-resolution features. This
effect 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 PM2.5 estimates. Our approach
maintains the global applicability of our initial satellite-derived
PM2.5 estimates while taking advantage of local measurements
where available. GWR predictors, such as subgrid elevation
difference, urban surfaces, and aerosol composition, offered
insight into the sources of uncertainty for the CTM-calculated,
geophysical AOD-to-PM2.5 relationships. This insight can, in
turn, direct global improvements to the next generation of
satellite-derived PM2.5 estimates. In addition, adjustment of our
1 km geophysical satellite-derived PM2.5 estimates over North
America by the current GWR-predicted bias provides a
significantly improved representation of PM2.5 concentrations
in this region for exposure assessment and epidemiological
analysis. Data are freely available as a public good at http://fizz.
phys.dal.ca/~atmos/.
Future work should seek higher-resolution simulations of the
AOD-to-PM2.5 relationship, especially for regions with large
subgrid elevation differences or urban sources. Additional high-
resolution AOD products, such as from the Visible Infrared
Radiometer Suite (VIIRS44) or from MODIS, based on the
MAIAC6,45 retrieval, may also prove an asset for global satellite-
derived PM2.5 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 financial 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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10491 DOI: 10.1021/acs.est.5b02076

Environ. Sci. Technol. 2015, 49, 10482−10491