Meteorol Atmos Phys (2011) 113:139–152
DOI 10.1007/s00703-011-0153-9
ORIGINAL PAPER
Spatiotemporal analysis of particulate matter, sulfur dioxide
and carbon monoxide concentrations over the city
of Rio de Janeiro, Brazil
Marcelo Zeri • José Francisco Oliveira-Júnior •
Gustavo Bastos Lyra
Received: 29 March 2011 / Accepted: 10 July 2011 / Published online: 24 July 2011
Ó Springer-Verlag 2011
Abstract Time series of pollutants and weather variables
measured at four sites in the city of Rio de Janeiro, Brazil,
between 2002 and 2004, were used to characterize tem-
poral and spatial relationships of air pollution. Concentra-
tions of particulate matter (PM10), sulfur dioxide (SO2) and
carbon monoxide (CO) were compared to national and
international standards. The annual median concentration
of PM10 was higher than the standard set by the World
Health Organization (WHO) on all sites and the 24 h
means exceeded the standards on several occasions on two
sites. SO2 and CO did not exceed the limits, but the daily
maximum of CO in one of the stations was 27% higher on
weekends compared to weekdays, due to increased activity
in a nearby Convention Center. Air temperature and vapor
pressure deficit have both presented the highest correla-
tions with pollutant’s concentrations. The concentrations of
SO2 and CO were not correlated between sites, suggesting
that local sources are more important to those pollutants
compared to PM10. The time series of pollutants and air
temperature were decomposed in time and frequency by
wavelet analysis. The results revealed that the common
variability of air temperature and PM10 is dominated by
Responsible editor: S. Trini Castelli.
M. Zeri (&)
Energy Biosciences Institute, University of Illinois
at Urbana-Champaign, 1206 West Gregory Drive,
Urbana, IL 61801, USA
e-mail: mzeri@illinois.edu
J. F. Oliveira-Júnior
Department of Mechanical Engineering, COPPE, Federal
University of Rio de Janeiro, Rio de Janeiro, Brazil
G. B. Lyra
Federal Rural University of Rio de Janeiro, Seropédica, Brazil
temporal scales of 1–8 days, time scales that are associated
with the passage of weather events, such as cold fronts.
1 Introduction
Air pollution in urban areas is associated with health
problems and increase in mortality rates in several parts of
the world (De Leon et al. 1996; Schwartz 1996; Gonçalves
et al. 2005). For that reason, concentration of particulate
matter and other gaseous air pollutants [e.g., carbon mon-
oxide (CO), sulfur dioxide (SO2), nitrogen dioxide and
ozone] has been the subject of air quality policies and
government regulation (e.g., United States’ Clean Air Act).
The concentration of air pollutants is associated with
meteorological variables, such as air temperature, humid-
ity, wind speed and direction, rainfall and solar radiation.
This latter variable is mainly related to the formation of
secondary pollutants. Synoptic systems such as fronts,
cyclones, anti-cyclones, stationary and quasi-stationary
high-pressure systems also affect the dispersion of pollu-
tants in the lower troposphere in a scale of one to several
days. Such systems have the potential to disperse or to
confine pollutants over large areas. Strong winds contribute
to dispersion of pollutants, while an increase in concen-
tration is observed during atmospheric inversion events,
when cold air is trapped near the surface (Elminir 2007;
Sánchez-Ccoyllo and Andrade 2002). Fronts are important
for dispersion processes since they are associated with
cloud formation, wet deposition, and strong winds caused
by pressure gradients. On the other hand, subsidence
caused by stationary and quasi-stationary high-pressure
systems confines pollutants to a shallow layer near the
surface. Besides that, the presence of such systems
reduces atmospheric circulation, contributing to rising
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140
concentration of pollutants, and also reduces cloud for-
mation, which affects dispersion and wet deposition. His-
torically, the stagnation caused by stationary systems was
responsible for all extreme events of pollution over urban
areas (Arya 1999).
Particulate matter (PMx), CO and SO2 are among the
most common air pollutants. Particulate matter refer to
suspended particles in the air that can be originated from
natural processes, like sea spray or volcanoes, industrial
processes or human activities, such as burning of fossil
fuels and forest and agricultural fires (Andreae et al. 2004;
Lara et al. 2005; Cançado et al. 2006). Particulate matter is
also associated with re-suspension of dust caused by traffic
of cars, for example. These particles are classified
according to their aerodynamic size, which range from
10-9 to 10-6 m. Particles of 10 lm or smaller, commonly
referred as PM10, are of especial importance since they
have the potential to be inhaled and penetrate human lungs,
causing respiratory problems such as asthma or lung cancer
(Samet et al. 2000). Fine particulate matter is composed of
particles smaller than 2.5 lm, commonly referred as PM2.5,
which can penetrate even deeper into the respiratory sys-
tem. Besides that, particulate matter reduces atmospheric
visibility, contribute to the corrosion of materials and act as
a catalyst of primary pollutants to other harmful pollutants
(Seinfield and Pandis 1997).
Carbon monoxide is a colorless and odorless gas
released by the combustion of fossil fuels. The main source
of CO is vehicular exhaust, but forest fires and industrial
processes, such as chemical manufacturing, are also major
contributors of this pollutant to the atmosphere. The impact
on the respiratory system is related to the formation of a
stable component between CO and hemoglobin, carboxy-
hemoglobin, which slows down the exchanges of oxygen.
Another gaseous pollutant commonly present in urban
environments is SO2. Emissions of SO2 are associated with
volcanoes, but also with the combustion of fossil fuels,
since coal and petroleum contain sulfur compounds. The
oxidation of sulfur dioxide can lead to the formation of acid
rain and, similarly to PMx and CO, the exposure to SO2 can
increase asthma symptoms among other health problems
(Braga et al. 2006; Gonçalves et al. 2005; Pereira et al.
2009) and contribute to corrosion of materials and metallic
structures.
Rio de Janeiro is the second largest city of Brazil, with
about 6.3 million inhabitants, and located over a complex
topography near the coast. The city was ranked 6th
between the most polluted capitals in Brazil in 2007
(Balazina 2007), with levels of fine particulate matter well
above (21.2 lg m-3) the concentration recommended by
the World Health Organization (WHO) (10 lg m-3).
Sources of pollution can be stationary (power plants or oil
refineries), mobile (traffic of cars) or temporary, such as
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M. Zeri et al.
forest fires. For the metropolitan area of Rio de Janeiro,
mobile sources are the dominant factor influencing the
levels of pollution (Ferreira 2005).
The objective of this work is to investigate the con-
centrations of PM10, CO and SO2 measured at four loca-
tions (air quality stations) over the city’s urban area. The
stations cover an area of approximately 100 km2 and the
locations include sites close to the ocean, next to Guana-
bara Bay, at the downtown area, and one close to a 1,000 m
high massif and an urban forest. The concentration of each
pollutant was characterized for each station for different
time scales (annually, weekly) and their correlation with
meteorological variables was also investigated. Finally,
wavelet spectral analysis was used to determine the tem-
poral scales responsible for significant correlations between
stations and also between pollutants and meteorological
variables.
2 Materials and methods
2.1 Site
The city of Rio de Janeiro is located in the southeast region
of Brazil, between latitudes 22°450 0500 S and 23°040 1000 S
and longitudes 43°060 3000 W and 43°470 4000 W. According to
the Köppen climate classification, the city’s climate is of
the kind Aw, characterized by dry and cool winters and wet
and rainy summers. The air temperature ranges from
21.1°C (average minimum temperatures) during winter to
27.3°C (average maximum temperatures) during summer.
The annual average temperature is 23.9°C, precipitation is
approximately 1,258 mm year-1 and the average number
of days with precipitation is 124. The topography is char-
acterized by the Tijuca and Pedra Branca massifs, as can be
seen in Fig. 1. Those massifs act like a barrier to the
incoming winds (sea breeze), dampening the air circulation
on the areas behind them and also forcing the flow into
‘‘wind corridors’’ (Ferreira 2005).
The most important conditions that contribute to the
increase in the concentration of pollutants are the complex
topography, mesoscale events (sea breeze and mountain–
valley breeze), the occurrence of the South Atlantic Sub-
tropical Anticyclone (SASA) and fronts (Ferreira 2005).
The location and intensity of the SASA changes seasonally,
while the passage of fronts is more frequent during the
winter and spring. During summer, the SASA is located
over the ocean and contributes to the formation of warm
and wet air masses, which interact with cold fronts
reaching the city, resulting in the main cause of precipi-
tation during this period. During the winter, the SASA is
closer to the continent, causing subsidence of dry air and
consequently less precipitation (Oliveira Júnior 2008).
Spatiotemporal analysis of particulate matter, SO2 and CO concentrations
Fig. 1 Map of monitoring stations and topography. Meteorological station located at the São Cristóvão site. Site marked Downtown referred as
Centro in the text
Another influence to the local weather is the occurrence of
the South Atlantic Convergence Zone (SACZ), an axis of
clouds across Brazil which is oriented northwest–southeast,
frequently observed during summer and associated with
higher frequency of rain events (Liebmann et al. 1999;
Muza et al. 2009; Carvalho et al. 2004).
2.2 Air pollution and weather data
Measurements of PM10, SO2 and CO were made at four
sites (Fig. 1) in the city of Rio de Janeiro, Brazil, from
January 2002 to December 2004 (March 2004, for SO2).
The Copacabana neighborhood is located at the south
region of Rio de Janeiro, facing the Atlantic Ocean to the
south, the Tijuca massif to the west and Guanabara Bay to
the east. The area has approximately 150,000 inhabitants
and the highest population density in the city. The
Copacabana station (22°570 45.000 S, 43°100 38.000 E, 28 m above
sea level) is located at the Cardeal Arcoverde square, near
Copacabana’s first subway terminal and at approximately
500 m from the shoreline (Copacabana Beach). The station
at the downtown area (hereafter referred as Centro) is
located near the Largo da Carioca square (22°540 27.600 S,
43°100 40.500 E, 34 m a.s.l.), a region of intense commercial
activity near the city’s financial center (Rio Branco Street),
and 1 km west of Santos Dumont airport, the second major
141
airport in the city and one of the busiest in the country. The
São Cristóvão station (22°530 47.000 S, 43°130 11.000 E, 19 m
a.s.l.) is located in the northern district of São Cristóvão, at
approximately 600 m from the Guanabara Bay shoreline.
The site was established next to a Convention Center that
hosts, from Friday to Sunday, cultural events and a market
of traditional foods and craftsmanship items. This station is
also located next to Linha Vermelha and Avenida Brasil
express lanes, two highways that connect several areas of
Rio de Janeiro. The last station was located on the northern
neighborhood of Tijuca, a district with about 150,000
inhabitants. The measurements were performed near the
Saens Peña Square (22°550 25.000 S, 43°130 57.000 E, 27 m
a.s.l.), at about 1 km north of the border to the Tijuca
Forest, the world’s largest urban forest, covering approxi-
mately 32 km2.
Particulate matter was measured based on the Beta
radiation absorption method (sensor BAM 1020, MET
ONE, Grants Pass, OR, USA). The inlet was placed at
4.5 m above the ground and the air was pumped into the
analyzer at a rate of 16.6 l min-1. Carbon monoxide was
measured using an infrared sensor (EC9830 CO Gas
Analyzers, ECOTECH, Victoria, Australia), while SO2 was
measured by a fluorescent method (EC9850B SO2 Gas
Analyzers, ECOTECH, Victoria, Australia). Measurements
were made every 10 min and recorded in a datalogger
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142
(model 9400DAS, ECOTECH, VIC, Australia). An auto-
matic weather station (model S-1000, Squitter Electronics
Inc., Deerfield Beach, USA) was located at the São Cris-
tóvão station, measuring air temperature, relative humidity,
wind speed, wind direction and rainfall. Measurements
were made every 15 min and latter averaged (summed, for
rainfall) over 24 h periods. The periods of 24 h ranged
from 15:00 of the previous day to 15:00 of the current day.
The data for carbon monoxide represent the daily maxi-
mum (COmax) for the same period. The frequency of
occurrence of synoptic events that reached the city from
2002 to 2004 was obtained (Climanálise 2005) and plotted
in Fig. 3. All data processing, statistics and plotting was
done using MATLAB 7.11 (The MathWorks, Inc.), and
significance tests reported were calculated using a t test
statistic.
2.3 Wavelet analysis
The wavelet transform is a mathematical tool used to
decompose a time series in several temporal scales (or
frequencies), enabling the determination of the contribution
of different frequencies to the total variance. The decom-
position is the result of the convolution (in the frequency
space) of the original signal with variants of a function
called the mother wavelet (Daubechies 1992). Fourier
analysis can also be used to determine the spectrum of
frequencies contributing to the variance of a time series.
However, wavelet analysis preserves the location in time of
features of the signal, like non-periodic variability. Con-
trary to the infinite sines and cosines used in Fourier
analysis, wavelet analysis makes use of functions that are
finite in time. This tool has been used in many geophysical
studies that deal with periodic and non-periodic oscillations
in time series of wind speed, air temperature, CO2 con-
centration, etc. (Farge 1992; Torrence and Compo 1998; Sá
et al. 1998; Krusche and Machado 2000; Grinsted et al.
2004; Zeri and Sá 2010). The Morlet wavelet function was
used in this work since it has been shown to correctly
identify modes of variability in geophysical time series
(Torrence and Compo 1998). This function is defined as:
2 WSW sector, likely associated with the higher terrain
WðgÞ ¼ p1=4 eix0 g eg =2 ð1Þ
where g is the non-dimensional time parameter and x0 is
the non-dimensional frequency. The wavelet transform of
the time series x is then calculated as:
Z1
1 s  t
W ðt; aÞ ¼ pffiffiffi xðsÞW ds ð2Þ
a a
1
where t is the time, a is the dilatation parameter, s is the
integration variable and * denotes the complex conjugate.
123
M. Zeri et al.
The common variability in time and frequency of two time
series x and y can be determined by the wavelet cross-
spectrum, calculated as Wxy ¼ Wx Wy , where Wx and Wy are
the wavelet transforms of x and y, respectively. The
absolute value of Wxy is the cross-wavelet power, which is
proportional to the covariance between the two signals at
each scale, while the complex part of Wxy contains infor-
mation about the phase relationship between the time ser-
ies. In this work, scripts for the MATLAB program
developed by Grinsted et al. (2004) and by Torrence and
Compo (1998) were used. The significance levels in the
cross-wavelet analysis were not corrected for auto-corre-
lation due to the presence of seasonal variation in the time
series. Longer time-series would make it possible to
remove the annual trends, which was not possible in this
study due the limited data availability.
3 Results and discussion
3.1 Meteorological data
According to the windrose histogram in Fig. 2, the main
wind directions at the São Cristóvão station were east–
southeast (ESE), northwest (NW), west (W) and west–
southwest (WSW), depending on the season. The sector
ESE is associated with the sea breeze, while sector NW is
influenced by the land breeze. Those two sectors are the
most important during spring and winter, although the land
and sea breezes are associated with higher wind speeds
during springtime compared to wintertime. The sector ESE
is not as important during summer, when winds from W are
the second most important sector after NW. The WSW and
W winds are associated with the passage of fronts in the
region. Besides the influence of sea and land breezes, the
sectors NW and ESE point to directions that are not
obstructed by the local topography, suggesting that those
are preferential channels for the wind field over the region.
Indeed, the highest wind speeds were observed for those
sectors (U [ 4 m s-1). Conversely, the lowest values of
wind speed (0 \ U B 1 m s-1) were observed for the
elevation in that direction.
Average wind speed ranged from 1 to 3 m s21, with
different seasonal variability in 2002 and 2003 (Fig. 3a).
While the monthly averages were approximately constant
throughout 2002, the year of 2003 presented a more pro-
nounced increase in the average wind speed from July to
November. These seasonal changes are expected since the
wind speed is related to the frequency of occurrence of
synoptic events (discussed later in this section), which in
turn are influenced by other large scale factors such as El
Spatiotemporal analysis of particulate matter, SO2 and CO concentrations 143

(a) Spring (b) Summer

NORTH NORTH

20% 20%

10% 10%

WEST EAST WEST EAST

5−6 5−6
4−5 4−5
3−4 3−4
2−3 2−3
1−2 1−2
SOUTH 0−1 SOUTH 0−1

(c) Autumn (d) Winter

NORTH NORTH

20% 20%

10% 10%

WEST EAST WEST EAST

Wind speed
(ms−1)
5−6 >=5
4−5 4−5
3−4 3−4
2−3 2−3
1−2 1−2
SOUTH 0−1 SOUTH 0−1

Fig. 2 Windrose histogram for each season, using data measured at the São Cristóvão station from 2002 to 2004. Relative contribution of each
sector shown in the polar axis for different classes of wind speed

Niño (Oliveira Júnior 2008). The seasonal cycle was more
pronounced in the time series of air temperature (Tair), for
all years (Fig. 3b). The average air temperature during the
winter months, from July to September, was &21°C,
which was approximately 6°C lower than the average of
&27°C for the summer months (January–March). Air
humidity was characterized using the vapor pressure deficit
(VPD, Fig. 3c), which revealed an annual variability not
seen for the relative humidity (not shown). Vapor pressure
deficit was highest during the summer months (January–
March), the same period when air temperature was highest.
The decrease in average air temperature in May was likely
the cause of the decrease in VPD around the same time.
Accumulated rainfall (R) was lowest during the winter
(June–August) and highest during the summer. The distri-
bution of rain events was different for the summer months.
While February and May had the highest values for 2002
and 2004, the accumulated rainfall in 2003 was highest in
March and decreased afterwards. The different variability
of rainfall can be explained by the different frequency of
occurrence of synoptic events like fronts, SASA and SACZ
(Fig. 3f–h). The higher sums of rainfall (and rain days,
Fig. 3e) in March, April and also in late spring were cor-
related with higher number of front events. The different
distribution of rain in 2002 and 2003 was also associated
with different variability of Tair and VPD. Average Tair and
VPD were highest in March of 2002, a period between the
two maxima in rainfall during that year. For 2003, the
maxima in Tair and VPD occurred in February, a month
before March, when the highest accumulated rainfall in the
year was registered. In summary, the variability of weather
parameters was related to the natural annual cycles (i.e.,
different seasons), but also to the different frequency of
occurrence of synoptic events, such as the higher occur-
rence of fronts or SASA events during the winter and
spring.
3.2 Characterization of pollutants
Time series of 24 h and monthly averages of PM10, SO2
and CO for all sites are displayed in Fig. 4. All three
pollutants presented higher values during the winter period,
when lower wind speeds and the higher occurrence of
thermal inversions dampen the dispersion processes.
However, the amplitude of the maximum values is different
between stations. The São Cristóvão site had the highest
number of extreme values of PM10, due to its proximity to
the main traffic corridors in the city (Brazil Avenue and

123
144 M. Zeri et al.

Fig. 3 Monthly averages 6 35

(a wind speed, b air temperature (a) Wind speed 2002 (b) Air temperature
and c vapor pressure deficit) and 2003
4 30
totals [d rainfall, e rain days, 2004

U (m s−1)

(°C)
f number of fronts, and
25
g number of events of South

air
2

T
Atlantic Subtropical
Anticyclone (SASA), and 20
h South America Convergence 0
Zone (SACZ)] using data 15
measured from 2002 to 2004
20 250
(c) Vapor pressure deficit (d) Rainfall
200
15
VPD (hPa)

R (mm)
150
10
100
5
50

0 0

25 6
(e) Rain days (f) Fronts
20

# of events (−)
# of days (−)

4
15

10
2
5

0 0

6 4
(g) SASA (h) SACZ
# of events (−)

# of events (−)
3
4

2
1

0 0
J F M A M J J A S O N D J F M A M J J A S O N D
Month Month

Linha Vermelha express ways). In fact, the extreme values
that exceeded 150 lg m-3 were more frequent at this site
(nine cases marked with dots in Fig. 4) in comparison with
the others. The level of 150 lg m-3 for 24 h average is the
value that should not be exceeded more than once per year,
according to the standards defined by the Brazilian Com-
mission for the Environment (CONAMA) (CONAMA
1990) and the United States Environmental Protection
Agency (US-EPA). The only sites where the number of
extreme values did not exceed the maximum recommended
by CONAMA and US-EPA were Tijuca and Copacabana.
The 24 h average of SO2 was lower than the standard
defined by CONAMA (365 lg m-3) in all sites. The var-
iability for SO2 was similar for all sites, except for Tijuca,
which had the lowest variance. The lower variance can be
associated to the proximity to the Tijuca massif, which
causes higher precipitation and consequent wet deposition
of pollutants. The evolution of the time series of COmax
was similar for the Copacabana and Tijuca stations, while
São Cristóvão had well defined maxima around wintertime.
According to CONAMA, the daily maximum for CO
should not exceed 10 ppm more than once per year, which
did not happen for any of the sites.
The statistical properties of all pollutants were summa-
rized using boxplots, as presented in Fig. 5. The median
concentration of PM10 was lowest for Copacabana
(&45 lg m-3) and highest for Centro (&65 lg m-3). The
four stations can be grouped in two sets: heavily polluted
areas affected by traffic or industrial activities (Centro and
São Cristóvão) and areas primarily residential or away
from downtown (Copacabana and Tijuca). The average
concentration of PM10 for all sites, except Copacabana,

123
Spatiotemporal analysis of particulate matter, SO2 and CO concentrations
Copacabana Centro
(a) (b)
PM10 (µg m−3)
150
100
50
40
(e) (f)
SO2 (µg m−3)
30
20
10
(i) (j)
3
CO (ppm)
Jan02 Jan03 Jan04 Jan02 Jan03 Jan04
Fig. 4 Time series of pollutants for all stations from 2002 to 2004.
Monthly averages displayed as thick lines and time series of daily
averages shown in the background. Cases of PM10 that exceeded the
exceeded the Brazilian national annual mean standard of
50 lg m-3, marked with a dashed line in Fig. 5a. The
Copacabana site is distant from main traffic corridors in the
city, what justifies the lower concentration of PM10. The
concentration of SO2 was not significantly different
between Tijuca and São Cristóvão (median of
&8 lg m-3), while Copacabana and Centro had concen-
trations that were approximately 13% higher and lower,
respectively, when compared to that value. All sites had
average concentration lower than the annual mean standard
of 80 lg m-3 defined by CONAMA (1990). The similarity
between sites suggests a homogeneous source for all areas
(vehicular exhaust, industrial processes). Indeed, all sites
are located close to shopping malls, convention centers or
busy avenues. For carbon monoxide, the medians of COmax
were not significantly different between three of the four
stations (Copacabana, Centro and Tijuca), indicating sim-
ilar source strength, as observed for SO2. Although the
median was lowest for São Cristóvão, this site had the
highest outliers. The analysis of COmax outliers higher than
2.5 ppm for São Cristóvão station revealed that 53% of the
cases (26 total) occurred on weekends (Saturday and
Sunday), while the remaining cases were distributed during
weekdays. This result can be explained by the occurrence
of cultural events (concerts and other presentations) at the
Convention Center next to the measurement site.
145
Tijuca Sao Cristovao
(c) (d)
(g) (h)
(k) (l)
Jan02 Jan03 Jan04 Jan02 Jan03 Jan04
standard of 150 lg m-3 marked with dots. Carbon monoxide
represents the daily maximum (COmax)
In spite of differences in average concentrations, all
pollutants were significantly correlated between stations
(Table 1). The average correlation coefficient between
PM10, SO2 and COmax at all the stations was approximately
0.8, 0.64 and 0.65, respectively. The correlation among
stations suggests that the concentrations of pollutants are
affected by large-scale transport phenomena (e.g., weather
patterns, sea breeze), which influences all the stations
simultaneously. For example, the proximity to the coast is
certain to influence the levels of PM10, since sea salt is an
important component of particulate matter. In fact, marine
sources were identified to be the main contributors to wet
deposition of pollutants at the stations used in this work,
with Na?, Cl-, Mg2?, K? and SO42- the most important
chemical compounds (Albuquerque et al. 2006). The
dependence of correlation with distance between stations
was reported in a study of urban PM10 for several sites in
Finland (Anttila and Salmi 2006). According to that study,
stations separated by &10 km had an average correlation
coefficient of &0.8, which agrees with the value reported
here. For the current study, the distance between stations
ranged from 3.2 km (Tijuca—São Cristóvão) to 8.5 km
(Copacabana—São Cristóvão). A linear relationship was
found (y = -0.01x ? 0.86; r2 = 0.8) between the corre-
lation coefficients for PM10 in Table 1 and the distance
between pairs of stations. The correlation coefficient for
123
146 M. Zeri et al.

Fig. 5 Boxplots for the data (a) PM10 40 (b) SO 2

displayed in Fig. 4 grouped by (c) CO
180
pollutant. Stations abbreviated 3.5
as Copacabana (Cp), Centro 35
(Ct), Tijuca (Tj) and São 160
Cristóvão (SC). Median denoted 3
by the horizontal line inside the 30
140
boxes. Boxes edges represent the
first (q1) and third (q3) 2.5
quartiles, respectively. Whiskers 120 25

(µg m )

SO (µg m )
−3

−3
extend from the edges to 1.5

CO (ppm)
times the interquartile range 2
100 20
(q3–q1). Cases outside this
10

2
range are outliers and are
PM
marked with ?signs. Standard 80 15 1.5
of 50 lg m-3 for PM10
(a) marked with the dashed line
60
10 1

40
5 0.5

20
0 0

Cp Ct Tj SC Cp Ct Tj SC Cp Ct Tj SC

this relationship was -0.9, which was statistically signifi- of higher values on weekdays and lower concentrations on
cant at the 5% level. The lower correlation coefficients for weekends, due to reduced traffic of vehicles and conse-
SO2 and COmax in Table 1 indicate that local sources are quent reduction in re-suspension of dust and particulate
likely more important to those pollutants as compared to matter. On average, the relative change of the concentra-
PM10. In fact, higher values of COmax are observed on tions during the weekend (Saturday and Sunday) in com-
weekends at the São Cristóvão station, contrary to the other parison to weekdays (Tuesday–Friday) was approximately
sites, as described in the next paragraph. -13, -30 and -25%, for PM10, SO2 and COmax, respec-
The concentrations of all pollutants were grouped by tively. However, the average for COmax excludes the São
day of week and averaged, revealing the common pattern Cristóvão station, which presented an increase in concen-
tration on weekends (?27%). This result can be explained
Table 1 Correlation coefficient between stations (Cp, Copacabana; by the fact that the Convention Center near the São Cris-
Ct, Centro; Tj, Tijuca; SC, São Cristóvão) for each pollutant (par- tóvão station has increased activity on weekends, when
ticulate matter, PM10; sulfur dioxide, SO2; carbon monoxide, CO) cultural events attract many visitors and consequent
Cp Ct Tj SC increase in traffic flow.
Finally, it should be noted that the correlation coeffi-
PM10
cients and significance tests reported here, and in other
Cp 1.00 0.78 0.80 0.77 studies (Elminir 2007; Anttila and Salmi 2006), were not
Dt – 1.00 0.80 0.81 corrected for seasonal variation or day-to-day persistence.
Tj – – 1.00 0.83 The unbiased correlation between stations would have to
SC – – – 1.00 be calculated by removing the annual trends from the time
CO series, which would require longer signals of pollutants and
Cp 1.00 0.68 0.60 0.65 meteorological variables.
Dt – 1.00 0.66 0.72
Tj – – 1.00 0.59
3.3 Relationship with meteorological variables
SC – – – 1.00
at the São Cristóvão site
SO2
Cp 1.00 0.74 0.58 0.62
The concentration of pollutants is strongly correlated with
Dt – 1.00 0.56 0.59
meteorological variables or weather patterns (Gonçalves
Tj – – 1.00 0.72
et al. 2005; Elminir 2007; Demuzere et al. 2009). Wind
SC – – – 1.00
speed, air temperature, relative humidity (or vapor pressure
All values are statistically significant at the 99% level deficit) and rainfall are the most common drivers of

123
Spatiotemporal analysis of particulate matter, SO2 and CO concentrations 147

Fig. 6 Monthly values (a) r(U,PM10) (b) r(U,SO2) (c) r(U,CO)

(averages of 2002–2004) of the 0.2 r2
correlation coefficient (left axis)
and r squared (right axis) for 0

r (−)
pairs of pollutants and −0.2
meteorological variables, as
−0.4 1
indicated by the notation r(x,y)
in the subplots. Significant −0.6 0.5
correlations (at 99% level) −0.8 0
denoted by filled symbols
(d) r(T a,PM10) (e) r(T a,SO2) (f) r(Ta,CO)
2
r
0.6
r (−)
0.4
1
0.2
0.5

0 0

0.8 (g) r(VPD,PM10) (h) r(VPD,SO2) (i) r(VPD,CO) 2

r
0.6
r (−)

0.4

0.2
1
0 0.5

−0.2 0
1 3 5 7 9 11 1 3 5 7 9 11 1 3 5 7 9 11
Month Month Month

changes in concentrations. In this work, the effects of those
variables, measured at the São Cristóvão site, on the con-
centrations of PM10, SO2 and COmax were quantified by
calculating the correlation coefficient between each mete-
orological variable and the pollutants, grouped by month
(Fig. 6). No annual trend was observed for any pair of
pollutant and meteorological variable. The statistically
significant correlations (closed symbols) of wind speed
with pollutants were irregularly distributed during the year.
All statistically significant correlations between wind speed
and pollutants for the São Cristóvão site were negative,
implying that lower wind speeds lead to higher concen-
tration of pollutants. Particulate matter was negatively
correlated with wind speed (Fig. 6), suggesting that less
dispersion of particulates by the wind led to higher con-
centrations, in agreement with a study of pollutants in
Holland (Demuzere et al. 2009). The relationship between
SO2 and COmax with wind speed revealed that significant
correlations (all negative) occurred during the winter (June
and July), and again in October and December, for COmax.
Air temperature and vapor pressure deficit were the most
important variables regarding the correlation with pollu-
tants, having the highest correlation coefficient and
explaining most of the variance in the linear relationships
(high r2). The significant correlations were all positive and
no annual trend was observed. The correlation of PM10
with air temperature was statistically significant for the
whole year. On the other hand, the concentration of SO2
and COmax were not significant during some of the south-
ern hemisphere summer months (December, for SO2, and
January–March and May, for COmax). According to the
time series in Fig. 4, summer is the period with the lowest
values of SO2 and COmax. That can be explained consid-
ering that during the summer the surface gets warmer by
solar heating and, consequently, the air in contact with the
surface is heated and, by convection, moves upwards,
mixing the surface layer (Stull 1988). The warmer the
surface is, the more intense the exchange of heat with the
overlaying air will be, thus increasing the mixing and
the size of eddies that help to disperse pollutants. The corre-
lation coefficient between air temperature and all three
pollutants dropped around May. Moreover, the correlations
were not statistically significant (open circles) for SO2 and
COmax. That period coincided with the rainfall events,
which help to clean the atmosphere of particulates and
other pollutants by process of ‘‘washout’’. A warmer
environment leads to a higher VPD (drier conditions),
enabling the re-suspension of dust if wind speed is strong.
Since air temperature was used in the calculation of VPD,
the correlation coefficient between VPD and the pollutants
followed the trends observed for Tair, with a few
exceptions.
Although the correlation coefficient was statistically
significant between Tair and pollutants, the fraction of the
variance explained by the linear relationship rarely
exceeded 50%. This result indicates that other factors

123
148 M. Zeri et al.

contribute to the variability of those pollutants at this site.
A comprehensive analysis of the weather-concentrations
relationships would require the use of stepwise regression
analysis and the inclusion of other variables (Demuzere
et al. 2009). Such analysis is beyond the scope of this paper
and should be explored in future works by using data from
other stations and over extended periods of time.
The process of pollutants removal by rainfall can happen
by absorption, for gaseous pollutants, or by entrapment into
raindrops, for particulate matter (Hales 1972; Shukla et al.
2008). The relationship between pollutants and rainfall at
the São Cristóvão site was determined by calculating the
median concentration for rain and no-rain days. Rain days
were determined as those with daily-accumulated rainfall
higher than zero. According to our results, PM10 was
successfully removed from the atmosphere by rainfall.
Rain days presented a concentration of PM10 that was
approximately 30% lower compared to no-rain days. The
median concentrations of PM10 for rain and no-rain days
were 46.0 and 64.0 lg m-3, respectively (the medians
were significantly different at the 5% level). The two
gaseous pollutants (SO2 and COmax) presented a different
response to rainfall. The average concentration of SO2 for
rain days was 40% lower compared to the average con-
centration for no-rain days (the concentrations for rain and
no-rain days were 6.0 and 10.0 lg m-3, respectively, and
the medians were also different at the 5% level). On the
other hand, the median values of COmax for rain and no-
rain days (0.53 and 0.51 ppm, respectively) were not sta-
tistically different, indicating no effect of rainfall in
washing out the atmosphere of CO. The different response
of SO2 and CO to rainfall is likely associated with different
rates of absorption of these gases by water droplets. The
solubility in water for carbon monoxide is 0.0026 g/
100 mL (at 20°C), a rate that is several orders of magnitude
lower compared to the solubility in water for SO2 (11.58 g/
100 mL, at 20°C). In order to investigate that, the data for
rain days was filtered so that only days with more than
10 mm of accumulated rainfall were selected. As a result,
the average of COmax was 10% lower than the value for no-
rain days (0.48 and 0.51 ppm, respectively), but the dif-
ference was still not statistically significant. Filtering for
stronger rainfall events reduced the sample size even more
and did not revealed significant differences. The insensi-
tivity of the average concentration of COmax to precipita-
tion suggests that policies that regulate this pollutant
should be stricter compared to other pollutants, since the
natural cleaning process (rainfall) will be of no help to
alleviate emergency situations when the concentration near
the surface exceeds safe limits.
The relationships between wind direction and concen-
tration of PM10 are presented in Fig. 7. Those results, when

(a) Spring (b) Summer

NORTH NORTH

20% 20%

10% 10%

WEST EAST −3 WEST EAST −3

PM10 (µg m ) PM10 (µg m )
>=130 130 − 150
110 − 130 110 − 130
90 − 110 90 − 110
70 − 90 70 − 90
50 − 70 50 − 70
30 − 50 30 − 50
SOUTH 10 − 30 SOUTH 10 − 30

(c) Autumn (d) Winter

NORTH NORTH

20% 20%

10% 10%

WEST EAST −3 WEST EAST −3

PM (µg m ) PM (µg m )
10 10
>=130 >=130
110 − 130 110 − 130
90 − 110 90 − 110
70 − 90 70 − 90
50 − 70 50 − 70
30 − 50 30 − 50
SOUTH 10 − 30 SOUTH 10 − 30

Fig. 7 Pollution-rose histogram for each season, using PM10 data measured at the São Cristóvão station from 2002 to 2004. Relative
contribution of each sector shown in the polar axis for different classes of PM10 concentration

123
Spatiotemporal analysis of particulate matter, SO2 and CO concentrations
combined with the windrose in Fig. 2, reveal that strong
winds contribute to disperse PM10 while conditions with
low wind speeds are associated with higher concentrations
of particulate matter. For example, springtime is dominated
by winds from sectors SE and NW, with southeastern
winds stronger than northwestern winds (Fig. 2a). As a
result, the concentration of PM10 is higher for sector NW in
spring (Fig. 7a). A second example of such relationship can
be seen during summertime (Fig. 2b). During that period of
the year, sector SE is still associated with the stronger wind
speeds and sectors WSW and W are dominated by lower
wind speeds. Consequently, the pollution-rose of PM10 for
summertime (Fig. 7b) shows higher concentrations for
sectors WSW and W, and lower for sector SE. During
autumn and winter this relationship between wind speed
and dispersion of PM10 is still present but weaker. Overall,
higher wind speeds are less frequent, resulting in high
levels of PM10 for all the most important sectors, such as
during winter (Fig. 7d). Another interesting feature of the
pollution-roses in Fig. 7 is that winds from the sectors
WSW and W are more frequent during summer and
autumn, associated with the passage of fronts. However,
those winds are weaker compared to other sectors (Fig. 2),
resulting in higher levels of PM10 during the passage of
fronts. This is in agreement with the results presented in the
next section, which demonstrated that PM10 and air tem-
perature are correlated in a time scale of 1–8 days, which is
approximately the duration of passing fronts. The rela-
tionship between concentrations of both SO2 and COmax
with wind direction (results not shown) was not so evident
compared to PM10. Lower wind speeds contributed to
higher concentrations of SO2 and COmax, especially during
winter, but the contribution of different sectors was
approximately the same.
No meteorological measurements were available for the
other sites, but based on the relationships between wind
direction and PM10 for São Cristóvão we hypothesize that
lower wind speeds will contribute to higher levels of PM10
in other areas of the city of Rio de Janeiro. More meteo-
rological measurements should be carried out at the other
sites in order to identify specific conditions that contribute
to increase in pollution levels in those areas. For example,
the site at Tijuca is close to high altitude areas and could be
affected by mountain and valley breezes, while dispersion
by sea and land breezes are important at the Copacabana
station due to the proximity to the ocean. Indeed, those
sites had the lowest levels of PM10 (Fig. 5a).
Pollution roses can also be used to identify sources of
pollutants. Northern winds were relatively frequent during
autumn and winter, and were associated with high levels of
PM10, SO2 and CO. We investigated the area surrounding
the São Cristóvão site and we hypothesize that the Galeão
Airport, approximately 5 km to the north, is the probable
149
source of pollutants measured at the site during conditions
of northern winds. In addition, another likely source of
pollutants is the oil refinery REDUC, the largest oil refinery
owned by the Brazilian oil company (Petrobras), located at
approximately 15 km to the north and north–northwest, at
the city of Duque de Caxias. Centro and Tijuca are likely
influenced by the same sources affecting São Cristóvão due
to the relatively short distance between these stations
(*3 km). However, a detailed analysis for the sites at
Centro, Tijuca and Copacabana would require measure-
ments of wind direction, which were not available when
pollutants were measured.
3.4 Temporal characteristics of pollutants
using wavelet analysis
The time series of PM10 and air temperature were analyzed
using the cross wavelet technique in order to identify the
temporal scales that are significantly correlated between
the two signals (Fig. 8). According to this analysis most of
the significant correlation occurs on the time scales of
1–8 days, as denoted by the regions enclosed in the black
contour in Fig. 8c. Other contributions can also be seen at
the scale of 8–16 days (July–October 2003) and around
64 days (July–October 2002). The angle of the arrows
(*0°) indicates that the signals of PM10 and Tair were in
phase, which results in positive correlation. The variability
between 1 and 8 days was intermittent and clustered
around wintertime for both years. The time scale of those
events suggests that they were associated with the passage
of fronts and other synoptic weather systems (ASAS,
SACZ) that were more frequent during this time of the year
(Fig. 3f, g). The variability of 64 days occurred simulta-
neously to the changes in PM10 at lower temporal scales,
indicating that several time scales influence the concen-
trations at the same time. The relationship of PM10 with
wind speed revealed few significant contributions while the
analysis using VPD resulted in similar results compared to
Tair.
The correlation coefficient between PM10 measured at
the São Cristóvão and Tijuca sites was 0.87 (Table 1). To
investigate this relationship on the time and temporal scales
domain, the cross wavelet analysis was applied to the time
series of PM10 measured at the two sites (Fig. 9). As
expected, the two sites had significant correlations at sev-
eral temporal scales. Similarly to the analysis between
PM10 and Tair, the dominant temporal scale was that of
1–8 days. A gap in contributions is also seen between the
scales of 16–32 days and the seasonal variation of 64 days
was observed for both sites during wintertime of 2002. An
important difference here is the variability on the scale of
128 days, which was absent on the time series of air tem-
perature. This result illustrates why the simple correlation
123
150 M. Zeri et al.

Fig. 8 Time series of PM10

a and air temperature b for the
São Cristóvão station between
2002 and 2004. Periodogram of
cross-wavelet power between
PM10 and Tair displayed in
c. The color axis in c represents
the cross-wavelet power.
Arrows angle (trigonometric
convention) indicate the phase
relationship, thick contour lines
enclose regions that are
statistically significant, and light
shaded regions mark the area
where edge effects due to time-
series limited size distort the
results

Fig. 9 Cross-wavelet analysis between PM10 at the Tijuca and São Cristóvão stations between 2002 and 2004

analysis with weather variables sometimes results in low 4 Conclusions

correlation coefficients or r2. Some time scales in the time
series of the pollutant might not be present in any of the The concentrations of PM10, SO2 and COmax were mea-
weather variables, leaving part of the pollutant variance sured from 2002 to 2004 at four locations over the city
unexplained. of Rio de Janeiro, Brazil. The lowest annual median

123
Spatiotemporal analysis of particulate matter, SO2 and CO concentrations
concentration of PM10 was &45 lg m-3, registered at the
Copacabana site. This value is more than twice the level
recommended by the WHO, which is 20 lg m-3, but still
lower than the CONAMA standard of 50 lg m-3. Aver-
ages of 24 h exceeded both CONAMA’s and US-EPA’s
standard of 150 lg m-3 on several occasions during the
two years analyzes in this study. For SO2, the annual
median concentration was lower than 10 lg m-3, which is
well below WHO’s recommended level of 20 lg m-3, as
well as lower than the Brazilian standard of 80 lg m-3.
Carbon monoxide was not a reason of concern, since
COmax did not exceed the Brazilian standard of 10 ppm.
However, care should be taken about the COmax at the São
Cristóvão station, which was *27% higher on weekends
in comparison to weekdays due to increased activities
(cultural events) in this region.
No annual trend was observed in the correlation of
weather variables with the pollutants. Wind speed was
significantly correlated only in few cases (monthly aver-
ages) over the year. The highest (and statistically signifi-
cant) correlation coefficients between weather and
pollutants were observed for air temperature and vapor
pressure deficit. However, the fraction of variance
explained by each variable (r2) was rarely higher than 50%,
suggesting that multilinear regression analysis should be
used in future studies in order to investigate the simulta-
neous influence of other weather variables. The removal of
pollutants by rainfall was efficient for PM10 and SO2
(reduction of 30 and 40%, respectively, compared to
no-rain days), but ineffective for CO.
The correlation coefficient between PM10 measured at
different sites ranged from 0.77 to 0.83. The correlations
were very well explained by a linear relationship (y =
-0.01x ? 0.86; r2 = 0.8) between the correlation coeffi-
cient and the distance between pairs of stations. The
relation was not statistically significant for SO2 and
COmax, suggesting that local sources are more important
for those pollutants in comparison to the large-scale
influence of PM10.
The wavelet analysis between air temperature and PM10
revealed that most of the variability in their relationship
occurs at the temporal scales of 1–8 days, the approximate
time scale of weather patterns that influence the city (e.g.,
cold fronts; SASA). A temporal variability with a period of
64 days was observed for 2002 but not for 2003. Addi-
tional data would be required to investigate the occurrence
of that temporal scale. The wavelet analysis was applied to
PM10 measured at the São Cristóvão and Tijuca stations,
revealing the same dominant temporal scale of 1–8 days
and the 64 days variability in 2002. However, a significant
time scale of 128 days was present in both signals, which
was not observed in any of the weather variables. This
result illustrates why the linear regression analysis of
151
weather and pollutants fails to explain part of the variance
in the relationship, since part of the variability in the pol-
lutants are not explained by the commonly used weather
variables. We demonstrated that the wavelet analysis is a
useful tool to reveal the missing temporal scales that might
influence pollutants concentrations over urban areas.
Additional meteorological measurements should be carried
out in order to improve the knowledge of the variability
that influences pollutants concentrations.
Acknowledgments We thank the Coordenadoria de Despoluição
dos Recursos Ambientais da Secretaria Municipal de Meio Ambiente
do Rio de Janeiro for the pollutants data and the Fundação Instituto de
Geotécnica for the São Cristóvão meteorological data.
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