You are on page 1of 10


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

Fine particulate matter (PM2.5) is associated with an increased
based PM2.5 monitors. The product of each predictor with its
respective coefficient can be summed to provide a spatially
risk of mortality and morbidity1 and globally contributes to an continuous PM2.5 estimate. Statistical methods can more
estimated 3.2 million premature deaths each year.2 Ground- accurately represent ground monitors compared with geo-
based monitoring networks provide direct observations of physical methods, but statistical methods have been limited to
PM2.5 in many developed countries; however, the density and regions with dense PM2.5 monitoring networks to determine
placement of monitors can affect their ability to characterize relationships between predictors and PM2.5.
concentrations, even for dense networks, such as those in the Geophysical methods employ a chemical transport model
U.S. (CTM) that represents local aerosol vertical profiles and optical
Satellite retrievals of aerosol optical depth (AOD) provide properties by combining emission inventories and assimilated
insight into the total atmospheric aerosol column, as meteorology with physical and chemical equations that describe
represented by the extinction of light. The horizontal resolution atmospheric composition and its evolution.18 CTMs simulate
of these AOD retrievals has traditionally been at 10 km or both PM2.5 and AOD, although typically at relatively coarse
coarser,3,4 with more recent developments at 3 km5 and 1 km.6 resolutions on the order of tens to hundreds of kilometers and
These AOD retrievals are being applied to increase the spatial without direct observational constraint. The CTM-predicted
extent of observational constraints on PM2.57−9 for application AOD-to-PM2.5 relationships are being applied to satellite
to exposure assessment and epidemiologic studies.10−12 The retrievals of AOD to globally estimate PM2.5 at higher
relationship between AOD and PM2.5 is affected by the aerosol resolution and improved accuracy compared with a CTM
vertical profile and optical properties. Most modern satellite- alone because of the additional, retrieved information. This
based PM2.5 estimates use either statistical or geophysical approach has demonstrated significant accuracy;19 however,
methods to relate AOD to PM2.5.
Statistical methods, such as land use regression or geo- Received: April 24, 2015
graphically weighted regression (GWR), estimate PM2.5 using Revised: August 3, 2015
predictors that include meteorology, land type, and AOD.13−17 Accepted: August 11, 2015
Predictor coefficients are fitted to optimally represent ground- 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 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
Figure 1. Flowchart of adjusted optimal estimation (AOE) PM2.5 from monthly average values were filled using the average value
production. The data sources and their resolution are in parentheses. of the surrounding 10 km.
GEOS-Chem Chemical Transport Model. We used
GEOS-Chem ( v9-01-03 to calculate
such CTM-based AOD-to-PM2.5 relationships underutilize the the prior for OE AOD and applied the simulated AOD-to-
valuable information available from ground-based measure- PM2.5 relationship to estimate near-surface PM2.5 concen-
ments. trations, the latter denoted as OE PM2.5 throughout this
In this article, we produced a high-resolution, geophysical, manuscript. Our North American nested GEOS-Chem
satellite-derived PM2.5 estimate by developing a 1 km × 1 km simulation was driven by GEOS-5 assimilated meteorology
resolution optimal estimation (OE) AOD retrieval and adjusted from the Goddard Earth Observation System (GEOS) of the
this estimate using a statistical method (GWR) that predicted NASA Global Modeling and Assimilation Office (GMAO) at
regional bias across North America. The prediction of bias, 0.5° × 0.67° with 47 vertical levels for the years 2004−2008.
rather than of PM2.5 itself, provided dual benefit. First, the National base inventories were used over Canada (Criteria Air
statistical step directly increased the accuracy of the geophysical Contaminants) and the U.S. (National Emission Inventory
PM2.5 estimate by reducing bias. Second, the impact of 2005), scaled for interannual variation according to local
individual predictors provided insight into geophysical factors governmental reports. The GEOS-Chem aerosol simulation
affecting the accuracy of the North American geophysical PM2.5 included the sulfate−nitrate−ammonium system,29,30 pri-
estimates, guiding future improvements to this globally mary31−33 and secondary carbonaceous aerosols,34 mineral
applicable method. This approach thus maintained a globally dust,35 and sea salt.36 Mie calculations of log-normal size
applicable data set as needed for global health assessments and distributions, growth factors, and refractive indexes, based on
indicators, such as the global burden of disease2 or the the global aerosol data set (GADS) and aircraft measurements,
environmental performance index (, while were used to determine the aerosol optical properties of the
at the same time improving accuracy over a region with in situ simulation.37−39 Details of this simulation are described in
monitoring networks. Philip et al.40


Figure 1 shows an overview of our method to estimate PM2.5 at
Geographically Weighted Regression. We used geo-
graphically weighted regression41 (GWR) to develop a
representation of the spatially varying relationship between
0.01° (approximately 1 km) resolution. We began with satellite multiple predictors and the bias between OE and in situ PM2.5.
observations of top-of-atmosphere reflectance. Optimal estima- GWR is an extension of least-squares regression, which
tion was applied to retrieve AOD. A CTM related AOD to determines the best-fitting predictor coefficients by minimizing
PM2.5. GWR predicted the bias in the optimal estimate of the sum of the squares between observed values and the
PM2.5, to yield a final adjusted optimal estimate. Each step is resultant estimates. GWR extends least-squares regression by
described further below. allowing predictor coefficients to vary spatially by weighting the
Extension of Optimal Estimation PM2.5 to 1km. estimate-observation pairs at multiple geographic locations
Optimal estimation (OE) is an inverse-modeling mathematical according to their inverse-squared distance from individual
framework that constrains a retrieval using prior knowledge of observational sites. The result is a spatially continuous field.
the quantity to be retrieved.20 The uncertainty of that prior is We applied the GWR-predicted bias to OE PM2.5 to produce
often specified relative to an observation. Van Donkelaar et al.21 an adjusted optimal estimate (AOE) of PM2.5. This approach
developed an OE algorithm at 10 km resolution that used the maintained the geophysical basis intrinsic to the CTM-driven
LIDORT22 radiative transfer model to retrieve AOD from top- method while incorporating in situ observations to identify
of-atmosphere reflectances (collection 5) observed by the local and regional biases caused by errors in the geophysical
MODIS3 instrument onboard the Terra satellite, constrained by representation of AOD and the concomitant AOD-to-PM2.5
an AOD prior from the GEOS-Chem23 CTM. Uncertainties relationships.
were based on comparison with the AERONET24 sun We used urban land cover, subgrid elevation difference, and
photometer network. These 10 km OE AOD retrievals aerosol composition as predictors for GWR. Our GWR model
generally improved agreement with AERONET compared was fitted at 1° × 1° intervals to in situ observations using the
with the standard dark target MODIS AOD products glmfit function of Matlab R2013a, following the form:
10483 DOI: 10.1021/acs.est.5b02076
Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

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) observations over North America. The highest correlation in
that study was found with sulfate (r = 0.95). The lower
= β1U + β2 ED + β3 NIT + β4 PC + β5SOA + ε (1) correlation of nitrate (r = 0.68), organic matter (r = 0.45), and
black carbon (r = 0.56) suggests that nitrate and carbonaceous
where β1 to β5 represented the spatially varying predictor species are more likely sources of regional error. We therefore
coefficients, and ε represents the error. In situ PM2.5 and OE included as predictors in GWR NIT, PC, and SOA alone.
PM2.5 were monthly mean values over the 5-year period 2004− Exclusion of sulfate helps to avoid excessive collinearity with
2008. The spatially varying predictor coefficients were treated these predictors. Biases associated with these predictors may
as constant across all years, but varying with month according result from a variety of causes, including regional errors in
to separate GWR runs. U was the percent urban land cover simulated representation of the chemistry, emission, or
according to the 500-m spatial resolution MODIS land cover transport of these species. Regression pairs were weighted
type product42 (MCD12Q1), regridded onto a standard 0.01° according to the inverse square of their distance from the point
× 0.01° grid. Subgrid elevation difference (ED) denoted the of interest, capped between 100 km and an optimally chosen
difference between the local elevation and the mean elevation maximum distance of ∼3000 km, set to minimize the RMSD of
of the 0.5° × 0.67° GEOS-Chem grid cell, according to the the predicted bias with observed values. Grid cells with
ETOPO1 Global Relief Model available from the National insufficient rank in the regression, suggesting multicollinearity
Geophysical Data Center ( among predictor variables, were fit with a reduced number of
global/seltopo.html). predictors with unsolved predictor coefficients set to zero. A
Speciated PM2.5 concentrations for nitrate (NIT), primary 10-fold cross-validation was employed to check for model over
carbonaceous (PC), and secondary organics (SOA) were fitting and to assess uncertainty in AOE PM2.5.
represented by applying the simulated relative contribution of In Situ PM2.5 Observations. We used in situ PM2.5
each aerosol type to the total OE PM2.5, following Philip et observations over Canada and the U.S. for evaluation and
al.,40 who demonstrated significant agreement with speciated GWR calibration. Measurements over Canada were taken from
10484 DOI: 10.1021/acs.est.5b02076
Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

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 both data sets over the eastern U.S. and parts of California, with
(NAPS;; 187 sites) and even larger enhancements over the Ohio River Valley. OE
included tapered element oscillating microbalance (TEOM), PM2.5 had smoothly varying features in both eastern and
beta attenuation mass monitors, and dichotomous samplers. western parts of the continent, whereas in situ monitors
NAPS TEOM instruments were corrected for semivolatile exhibited more fine-scale variation, particularly in the west. OE
particulate matter losses during air sample heating.43 U.S. PM2.5 concentrations were often underestimated in the west,
ground-level PM2.5 data were taken from the U.S. Interagency resulting in a distinct population in Figure 2 when in situ PM2.5
Monitoring of Protected Visual Environments (IMPROVE; measured between 5 and 10 μg/m3. Direct comparison of in; 128 situ PM2.5 with 1 km OE AOD (r2 = 0.41) outperformed both
sites) network and from FRM-compliant sites available from the standard 3 km MODIS Collection 6 Dark Target retrieval5
the U.S. Environmental Protection Agency Air Quality System (r2 = 0.18), and the 10 km Combined Dark Target-Deep
(AQS;; 1125 sites). We treated Blue26,27 ( r2 = 0.34). OE PM2.5 also outperformed purely
these in situ observations as “truth” despite the possibility of simulated PM2.5 based on aerosol concentrations used for the
measurement errors or representativeness issues arising OE prior constraints (r2 = 0.57; RMSD = 3.8 μg/m3).
between these point measurements and area averaged Figure 3 (lower right panel) shows the difference between in
concentrations, such as observed from satellite. situ and OE PM2.5, which we used to represent the bias in OE


Figure 2 shows OE PM2.5 and in situ PM2.5 across North
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
America. Significant agreement was found (r2 = 0.62; RMSD = comparatively elevated OE PM2.5 concentrations. Both features
2.6 μg/m3). Elevated PM2.5 concentrations were observed in were represented within the GWR-predicted bias (top panel),
10485 DOI: 10.1021/acs.est.5b02076
Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

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 of the AOD-to-PM2.5 relationship. Predicted biases over the
(R2 = 0.62; lower left panel). mountainous regions of the west and southeast U.S. were
Figure 4 (left column) shows the contribution of individual highly heterogeneous, driven by both subgrid elevation
predictors to the overall predicted bias. Predictors with a net differences and percent urban land cover. These two predictors
decrease indicated a positive bias in OE PM2.5. One such may be interpreted as corrective terms that account for the
reduction associated with nitrate occurred in the Canadian comparatively coarse resolution of the simulation used to
prairies and the Ohio River Valley. Broad reductions were also constrain the OE AOD retrieval and the AOD-to-PM2.5
associated with primary carbonaceous aerosol across much of relationship. Geophysically, they appear to represent local
the East. Both of these features were apparent in the PM2.5 PM2.5 in mountain valleys that may be better represented using
comparison of measured composition versus satellite-model higher-resolution simulations of the AOD-to-PM2.5 relation-
composition in Philip et al.,40 which motivate further ship. Also shown in Figure 4 are average predictor coefficients
investigation. Fine-scale enhancements associated with urban (middle column) and their standard error (right column).
surfaces may indicate local sources unresolved in the simulation Predictor coefficients generally show large spatial homogeneity,
10486 DOI: 10.1021/acs.est.5b02076
Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

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
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. sources and chemistry. Compositional coefficients can therefore
Spatial variation in predictor net impact does not generally be more challenging to interpret. The net impact of these
follow spatial variation in predictor coefficient, owing to predictors did, however, suggest seasonal maxima in OE PM2.5
variability in the predictors themselves. bias associated with nitrate in winter and primary carbonaceous
Table 1 shows the seasonal variation in predictor values and aerosol in summer. The net impact associated with SOA was
their net impact. The greatest impact of percent urban was in weakest and less readily interpreted. All three components had
winter, likely reflecting wintertime sources that were not contributions throughout most of the year.
captured within the simulated AOD-to-PM2.5 relationship. Figure 5 (top panel) shows AOE PM2.5, the result of adding
Elevation difference also exhibited the greatest impact during to OE PM2.5 the sum of the individual predictor bias
winter, possibly representing seasonal woodburning in contributions shown in Figure 4. The spatial pattern AOD
mountain valleys. Unlike percent urban and elevation differ- PM2.5 resembles that in OE PM2.5 (Figure 1), but with lower
ence, which were constant throughout the year, compositional PM2.5 in the Midwest, and additional spatial structure in the
predictors varied seasonally in response to changing emission mountainous regions. The inclusion of additional predictors,
10487 DOI: 10.1021/acs.est.5b02076
Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

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
Environmental Science & Technology Article

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)
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)
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 intervals, rather than the five-year 2004−2008 period,
found between the unadjusted OE PM2.5 and in situ PM2.5 over performed similarly; average coefficients of variation with in
urban (RMSD = 1.8 μg/m3) and nearby nonurban pixels situ monitors ranged from R2 = 0.61 (DJF) to R2 = 0.90 (JJA),
(RMSD = 1.9 μg/m3) at the same locations. and the average RMSD ranged from 2.8 (DJF) to 1.4 μg/m3
Figure 7 shows the seasonal variation in AOE PM2.5. Seasonal (MAM). Single year, single month runs also showed
enhancements were apparent in summer in the southeast and in significance: average coefficients of variation with in situ
winter in some cities in mountainous regions, such as Salt Lake monitors ranged from R2 = 0.52 (February) to R2 = 0.83
City. Significant seasonal skill existed between AOE PM2.5 and (August) and average RMSD ranged from 3.7 (January) to 1.7
in situ monitors (R2 = 0.62−0.89; RMSD = 1.4−2.7 μg/m3). μg/m3 (April).
The poorest agreement was found during winter, when AOD Table 3 describes the effect of spatial averaging on the
retrievals were compromised by snow cover and seasonally consistency between in situ and OE PM2.5. The agreement
varying reflectance, but the correlation remained significant (R2 across all resolutions was broadly similar, suggesting that the
= 0.62). The production of AOE PM2.5 over three-year running expected reduction of random error from spatial averaging was
10489 DOI: 10.1021/acs.est.5b02076
Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

nearly equivalent to the benefit of increased spatial resolution (4) Kahn, R.; Gaitley, B. J.; Garay, M. J.; Diner, D. J.; Eck, T. F.;
within the initial OE product. The AOE PM2.5 coefficient of Smirnov, A.; Holben, B. N. Multiangle Imaging SpectroRadiometer
variation steadily decreased with increasing spatial averaging, global aerosol product assessment by comparison with the Aerosol
which supported the presence of high-resolution features. This Robotic Network. J. Geophys. Res. 2010, 115, 1−28.
effect was enhanced over western North America compared (5) Remer, L. A.; Mattoo, S.; Levy, R. C.; Munchak, L. A. MODIS 3
km aerosol product: algorithm and global perspective. Atmos. Meas.
with eastern North America.
Tech. 2013, 6, 1829−1844.
Next Steps. We developed and presented an approach to (6) Lyapustin, A.; Wang, Y.; Laszlo, I.; Kahn, R.; Korkin, S.; Remer,
incorporate information from in situ monitors into geophysi- L.; Levy, R.; Reid, J. S. Multiangle implementation of atmospheric
cally driven satellite-derived PM2.5 estimates. Our approach correction (MAIAC): 2. Aerosol algorithm. J. Geophys. Res. 2011, 116,
maintains the global applicability of our initial satellite-derived 10.1029/2010JD014986
PM2.5 estimates while taking advantage of local measurements (7) Kloog, I.; Chudnovsky, A. A.; Just, A. C.; Nordio, F.; Koutrakis,
where available. GWR predictors, such as subgrid elevation P.; Coull, B. A.; Lyapustin, A.; Wang, Y.; Schwartz, J. A new hybrid
difference, urban surfaces, and aerosol composition, offered spatio-temporal model for estimating daily mutli-year PM 2.5
insight into the sources of uncertainty for the CTM-calculated, concentrations across northeastern USA using high resolution aerosol
geophysical AOD-to-PM2.5 relationships. This insight can, in optical depth data. Atmos. Environ. 2014, 95, 581−590.
turn, direct global improvements to the next generation of (8) van Donkelaar, A.; Martin, R. V.; Brauer, M.; Kahn, R.; Levy, R.;
satellite-derived PM2.5 estimates. In addition, adjustment of our Verduzco, C.; Villeneuve, P. J. Global Estimates of Ambient Fine
1 km geophysical satellite-derived PM2.5 estimates over North Particulate Matter Concentrations from Satellite-Based Aerosol
America by the current GWR-predicted bias provides a Optical Depth: Development and Application. Environ. Health Perspect.
2010, 118 (6), 847−855.
significantly improved representation of PM2.5 concentrations (9) Hu, X.; Waller, L. A.; Lyapustin, A.; Wang, Y.; Al-Hamdan, M. Z.;
in this region for exposure assessment and epidemiological Crosson, W. L.; Estes, M. G.; Estes, S. M.; Quattrochi, D. A.;
analysis. Data are freely available as a public good at http://fizz. Puttaswamy, S. J.; Liu, Y. Estimating ground-level PM2.5 concen- trations in the Southeastern United States using MAIAC AOD
Future work should seek higher-resolution simulations of the retrievals and a two-stage model. Remote Sens. Environ. 2014, 140,
AOD-to-PM2.5 relationship, especially for regions with large 220−232.
subgrid elevation differences or urban sources. Additional high- (10) Crouse, D. L.; Peters, P. A.; van Donkelaar, A.; Goldberg, M. S.;
resolution AOD products, such as from the Visible Infrared Villeneuve, P. J.; Brion, O.; Khan, S.; Atari, D. O.; Jerrett, M.; Pope, C.
Radiometer Suite (VIIRS44) or from MODIS, based on the A.; Brauer, M.; Brook, R. D.; Martin, R. V.; Stieb, D.; Burnett, R. T.
MAIAC6,45 retrieval, may also prove an asset for global satellite- Risk of Nonaccidental and Cardiovascular Mortality in Relation to
derived PM2.5 estimates. Long-term Exposure to Low Concentrations of Fine Particulate

Matter: A Canadian National-level Cohort Study. Environ. Health
AUTHOR INFORMATION Perspect. 2012, 120 (5), 708−714.
(11) Brauer, M.; Amann, M.; Burnett, R. T.; Cohen, A.; Dentener, F.
Corresponding Author J.; Ezzati, M.; Henderson, S.; Krzyzanowski, M.; Martin, R. V.; van
*Address: Dept. of Physics and Atmospheric Science, Dingenen, R.; van Donkelaar, A.; Thurston, G. Exposure assessment
Dalhousie University, 6300 Coburg Road Halifax, NS, Canada for the estimation of the global burden of disease attributable to
B3H 3J5. Phone: (902) 494-1820. E-mail: Aaron.van. outdoor air pollution. Environ. Sci. Technol. 2012, 2012 (46), 652−660. (12) Hyder, A.; Lee, H. J.; Ebisu, K.; Koutrakis, P.; Belanger, K.; Bell,
M. L. PM2.5 exposure and bith outcomes: Use of satellite- and
Notes monitor-based data. Epidemiology 2014, 25 (1), 58−67.
The authors declare no competing financial interest.

(13) Kloog, I.; Koutrakis, P.; Coull, B. A.; Lee, H. J.; Schwartz, J.
Assessing temporally and spatially resolved PM2.5 exposures for
ACKNOWLEDGMENTS epidemiological studies using satellite aerosol optical depth measure-
The authors are grateful to NASA, the U.S. EPA, and ments. Atmos. Environ. 2011, 45, 6267−6275.
Environment Canada for access to their data products and to (14) Ma, Z.; Hu, X.; Huang, L.; Bi, J.; Liu, Y. Estimating ground-level
PM2.5 in China using satellite remote sensing. Environ. Sci. Technol.
Compute Canada for computing resources. This work was
2014, 48 (13), 7436−7444.
supported by Health Canada, the Collaborative Health (15) Hoek, G.; Beelen, R.; De Hoogh, K.; Vienneau, D.; Gulliver, J.;
Research Project of the Natural Sciences and Engineering Fischer, P.; Briggs, D. A review of land-use regression models to assess
Research Council of Canada and the Canadian Institute of spatial variation of outdoor air pollution. Atmos. Environ. 2008, 42,
Health Research, and Environment Canada.

(16) Hystad, P.; Setton, E.; Cervantes, A.; Poplawski, K.; Deschenes,
REFERENCES S.; Brauer, M.; Martin, R. V.; van Donkelaar, A.; Lamsal, L. N.; Jerrett,
(1) Pope, C. A.; Ezzati, M.; Dockery, D. W. Fine-Particulate Air M.; Demers, P. Creating National Air Pollution Models for Population
Pollution and Life Expectancy in the United States. N. Engl. J. Med. Exposure Assessment in Canada. Environ. Health Perspect. 2011, 119
2009, 360, 376−386. (8), 1123−1129.
(2) Lim, S. S.; Vos, T.; Flaxman, A. D. F.; Danaei, G.; Shibuya, K.; (17) Vienneau, D.; de Hoogh, K.; Bechle, M. J.; Beelen, R.; van
et al. A comparative risk assessment of burden of disease and injury Donkelaar, A.; Martin, R. V.; Millet, D. B.; Hoek, G.; Marshall, J. D.
attributable to 67 risk factors and risk factor clusters in 21 regions, Western European land use regression incorporating satellite- and
1990−2010: a systematic analysis for the Global Burden of Disease ground-based measurements of NO2 and PM10. Environ. Sci. Technol.
Study 2010. Lancet 2012, 380, 2224−2260. 2013, 47 (23), 13555−13564.
(3) Levy, R. C.; Remer, L. A.; Mattoo, S.; Vermote, E. F.; Kaufman, (18) Liu, Y.; Park, R. J.; Jacob, D. J.; Li, Q. B.; Kilaru, V.; Sarnat, J. A.
Y. J. Second-generation operational algorithm: Retrieval of aerosol Mapping annual mean ground-level PM2.5 concentrations using
properties over land from inversion of Moderate Resolution Imaging Multiangle Imaging Spectroradiometer aerosol optical thickness over
Spectroradiometer spectral reflectance. J. Geophys. Res. 2007, 112 the contiguous United States. J. Geophys. Res. 2004, 109 (D22),
(D13),10.1029/2006JD007811 10.1029/2004JD005025

10490 DOI: 10.1021/acs.est.5b02076

Environ. Sci. Technol. 2015, 49, 10482−10491
Environmental Science & Technology Article

(19) van Donkelaar, A.; Martin, R. V.; Brauer, M.; Boys, B. L., Use of (36) Jaegle, L.; Quinn, P. K.; Bates, T.; Alexander, B.; Lin, J.-T.
Satellite Observations for Long-Term Exposure Assessment of Global Global distribution of seas salt aerosols: New constraints from in situ
Concentrations of Fine Particulate Matter. Environ. Health Perspect. and remote sensing observations. Atmos. Chem. Phys. 2011, 11, 3137−
2015, 123 (2), 10.1289/ehp.1408646. 3157.
(20) Rodgers, C. D. Inverse Methods for Atmospheric Sounding: Theory (37) Martin, R. V.; Jacob, D. J.; Yantosca, R. M.; Chin, M.; Ginoux, P.
and Practice; World Scientific: Singapore, River Edge, NJ, 2000; Series Global and regional decreases in tropospheric oxidants from
of Atmospheric Oceanic and Planetary Physics; Vol. 2. photochemical effects of aerosols. J. Geophys. Res. 2003, 108 (D3)
(21) van Donkelaar, A.; Martin, R. V.; Spurr, R. J. D.; Drury, E.; 10.1029/2002JD002622.
Remer, L. A.; Levy, R. C.; Wang, J. Optimal estimation for global (38) Drury, E.; Jacob, D. J.; Wang, J.; Spurr, R. J. D.; Chance, K.
ground-level fine particulate matter concentrations. J. Geophys. Res. Improved algorithm for MODIS satellite retrievals of aerosol optical
2013, 118, 5621−5636. depths over western North America. J. Geophys. Res. 2008, 113 (D16)
(22) Spurr, R. LIDORT and VLIDORT: Linearized pseudo-spherical 10.1029/2007JD009573.
scalar and vector discrete ordinate radiative transfer models for use in (39) Ridley, D. A.; Heald, C. L.; Ford, B. J. North African dust export
remote sensing retrieval problems; Springer: New York, 2008; Vol. 3. and deposition: A satellite and model perspective. J. Geophys. Res.
(23) Bey, I.; Jacob, D. J.; Yantosca, R. M.; Logan, J. A.; Field, B. D.; 2012, 117 (D2) 10.1029/2011JD016794.
Fiore, A. M.; Li, Q. B.; Liu, H. G. Y.; Mickley, L. J.; Schultz, M. G. (40) Philip, S.; Martin, R. V.; Van Donkelaar, A.; Lo, J. W.-H.; Wang,
Global modeling of tropospheric chemistry with assimilated Y.; Chen, D.; Zhang, L.; Kasibhatla, P.; Wang, S.; Zhang, Q.; Lu, Z.;
meteorology: Model description and evaluation. J. Geophys. Res. Streets, D. G.; Bittman, S.; Macdonald, D. J. Global chemical
2001, 106 (D19), 23073−23095. composition of ambient fine particulate matter for exposure
(24) Holben, B. N.; Eck, T. F.; Slutsker, I.; Tanre, D.; Buis, J. P.; assessment. Environ. Sci. Technol. 2014, 48, 13060−13068.
Setzer, A.; Vermote, E.; Reagan, J. A.; Kaufman, Y. J.; Nakajima, T.; (41) Brunsdon, C.; Fotheringham, A. S.; Charlton, M. E. Geo-
Lavenu, F.; Jankowiak, I.; Smirnov, A. AERONET - A federated graphically Weighted Regression: A method for exploring spatial
instrument network and data archive for aerosol characterization. nonstationarity. Geographic Analysis 1996, 28 (4), 281−298.
Remote Sens. Environ. 1998, 66 (1), 1−16. (42) Friedl, M. A.; Sulla-Menashe, D.; Tan, B.; Schneider, A.;
(25) Levy, R. C.; Remer, L. A.; Kleidman, R. G.; Mattoo, S.; Ichoku, Ramankutty, N.; Sibley, A.; Huang, X. MODIS Collection 5 global
C.; Kahn, R.; Eck, T. F. Global Evaluation of the Collection 5 MODIS land cover: Algorithm refinements and characterization of new
dark-target aerosol product over land. Atmos. Chem. Phys. 2010, 10, datasets. Remote Sens. Environ. 2010, 114, 168−182.
10399−10420. (43) Allen, G. Evaluation of Transformation Methods for Adjustment of
(26) Levy, R. C.; Mattoo, S.; Munchak, L. A.; Remer, L. A.; Sayer, A. Historial TEOM Data in the NAPS Network; Analysis and Air Quality
M.; Patadia, F.; Hsu, N. C. The Collection 6 MODIS aerosol products Section, Environment Canada: Gatineau QC, 2010.
over land and ocean. Atmos. Meas. Tech. 2013, 6, 2989−3034. (44) Justice, C. O.; Román, M. O.; Csiszar, I.; Vermote, E. F.; Wolfe,
(27) Hsu, N. C.; Jeong, M. J.; Bettenhausen, C.; Sayer, A. M.; R. E.; Hook, S. J.; Friedl, M.; Wang, Z.; Schaaf, C. B.; Miura, T.;
Hansell, R.; Seftor, C. S.; Huang, J.; Tsay, S. C. Enhanced Deep Blue Tschudi, M.; Riggs, G.; Hall, D. K.; Lyapustin, A. I.; Devadiga, S.;
aerosol retrieval algorithm: The second generation. J. Geophys. Res. Davidson, C.; Masuoka, E. J. Land and cryosphere products from
2013, 118, 9296−9315. Suomi NPP VIIRS: Overview and status. Journal of Geophysical
(28) Winker, D. M.; Vaughan, M. A.; Omar, A.; Hu, Y.; Powell, K. A. Research: Atmospheres 2013, 118 (17), 9753−9765.
Overview of the CALIPSO mission and CALIOP data processing (45) Lyapustin, A.; Martonchik, J.; Wang, Y. J.; Laszlo, I.; Korkin, S.
algorithms. J. Atmos. Oceanic Technol. 2009, 26, 2310−2323. Multiangle implementation of atmospheric correction (MAIAC): 1.
(29) Park, R. J.; Jacob, D. J.; Field, B. D.; Yantosca, R. M.; Chin, M. Radiative transfer basis and look-up tables. J. Geophys. Res. 2011, 116,
Natural and transboundary pollution influences on sulfate−nitrate− 10.1029/2010JD014985.
ammonium aerosols in the United States: Implications for policy. J.
Geophys. Res. 2004, 109 (D15), 10.1029/2003JD004473.
(30) Pye, H. O. T.; Liao, H.; Wu, S.; Mickley, L. J.; Jacob, D. J.;
Henze, D. K.; Seinfeld, J. H. Effect of changes in climate and emissions
on future sulfate−nitrate−ammonium aerosol levels in the United
States. J. Geophys. Res. 2009, 114 (D01205), 10.1029/2008JD010701.
(31) Heald, C. L.; Coe, H.; Jimenez, J. L.; Weber, R. J.; Bahreini, R.;
Middlebrook, A. M.; Russell, L. M.; Jolleys, M.; Fu, T.-M.; Allan, J. D.;
Bower, K. N.; Capes, G.; Crosier, J.; Morgan, W. T.; Robinson, N. H.;
Williams, P. I.; Cubison, M. J.; DeCarlo, P. F.; Dunlea, E. J. Exploring
the vertical profile of atmospheric organic aerosol: comparing 17
aircraft field campaigns with a global model. Atmos. Chem. Phys. 2011,
11, 12673−12696.
(32) Park, R. J.; Jacob, D. J.; Chin, M.; Martin, R. V. Sources of
carbonaceous aerosols over the United States and implications for
natural visibility. J. Geophys. Res. 2003, 108 (D12),10.1029/
(33) Wang, Q.; Jacob, D. J.; Fisher, J. A.; Mao, J. T.; Leibensperger,
E. M.; Carouge, C. C.; Le Sager, P.; Kondo, Y.; Jimenez, J. L.; Cubison,
M. J.; Doherty, S. J. Sources of carbonaceous aerosol and deposited
black carbon in the Arctic in winter-spring: implications for radiative
forcing. Atmos. Chem. Phys. 2011, 11, 12453−12473.
(34) Liao, H.; Henze, D. K.; Seinfeld, J. H.; Wu, S. L.; Mickley, L. J.
Biogenic secondary organic aerosol over the United States:
Comparison of climatological simulations with observations. J.
Geophys. Res. 2007, 112 (D6), 10.1029/2006JD007813.
(35) Fairlie, T. D.; Jacob, D. J.; Park, R. J. The impact of transpacific
transport of mineral dust in the United States. Atmos. Environ. 2007,
41 (6), 1251−1266.

10491 DOI: 10.1021/acs.est.5b02076

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