Atmospheric Environment 42 (2008) 6523–6534

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Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Influence of sea breeze circulation and road traffic emissions on the

relationship between particle number, black carbon, PM1, PM2.5 and
PM2.5–10 concentrations in a coastal city
Sergio Rodrı́guez a, b, *, Emilio Cuevas a, Yenny González a, Ramón Ramos a,
Pedro Miguel Romero a, Noemı́ Pérez c, Xavier Querol c, Andrés Alastuey c
a
Izaña Atmospheric Research Centre, AEMet, Associated Unit to CSIC ‘‘Studies on Atmospheric Pollution’’, C/ La Marina, 20,
6a Planta, E38001 Santa Cruz de Tenerife, Canary Islands, Spain
b
Department of Geology, University of Huelva, Associated Unit to CSIC on ‘‘Air Pollution’’, Campus El Carmen, E21071 Huelva, Spain
c
Institute of Earth Science ‘‘Jaume Almera’’, CSIC, Lluis Solé i Sabaris S/N, E08028 Barcelona, Spain

a r t i c l e i n f o a b s t r a c t

Article history: The physical characterisation of metrics representative of ambient air particle concentra-
Received 19 February 2008 tion is becoming a topic of great interest for urban air quality monitoring and human ex-
Received in revised form 26 March 2008 posure assessment. In this article, the influence of sea breeze circulation and primary road
Accepted 2 April 2008
traffic emissions on the relationship between the urban aerosol number (N3, particles
>3 nm), black carbon <10 mm (BC), PM1, PM2.5, PM2.5–10 (PMx) concentrations was stud-
Keywords:
ied in a coastal city (Santa Cruz de Tenerife, Canary Islands). The daily cycles of sea and
Ultrafine particles
mountain breezes (inland during daylight and seaward at night) and road traffic emissions
New particle formation
Black carbon exerted a great, and well differentiated, influence on the BC, N3 and PMx concentrations. In
Soot this scenario, the following major aerosol features were observed: (1) fresh vehicle exhaust
Vehicle exhausts emissions resulted in high BC and N3 concentrations, in such a way that these two metrics
increased when the ‘‘road traffic intensity (vehicles h1)/wind speed’’ ratio increased, (2)
PM1 and PM2.5 levels were lower during daylight (due to inland entry of relatively clean
marine air masses) than at night (due to the seaward drainage airflow resulting in the
transport of aged particulate pollutants from the city), (3) although N3 and BC concentra-
tions exhibited a significant correlation during the whole study period, the N3/BC ratio ex-
perienced a daily evolution with a maximum during daylight. Thus, high N3
concentrations associated with high N3/BC ratios and high solar irradiance conditions
were recorded during the daylight inland breeze period due to an enhancement of pro-
cesses favouring new particle formation. Data analysis points out that this enhancement
in the new particle formation processes is strongly related to the nucleation of photo-
oxidized vapours under the relatively low PMx (and consequently low aerosol surface
area) concentrations prompted by the inland entry of clean marine air due to the daylight
breeze blowing. The results obtained show that, in addition to the vehicle exhaust emis-
sions, new particle formation in coastal urban areas due to photo-oxidation processes
may significantly contribute to the ultrafine particle concentration.
Crown Copyright Ó 2008 Published by Elsevier Ltd. All rights reserved.

1. Introduction
* Corresponding author. Izaña Atmospheric Research Centre, AEMet,
Associated Unit to CSIC ‘‘Studies on Atmospheric Pollution’’, C/ La
Marina, 20, 6a Planta, E38001 Santa Cruz de Tenerife, Canary Islands,
Studies performed over the last two decades related
Spain. Tel.: þ34 922151718; fax: þ34 922574475. exposure to urban ambient PM10 and PM2.5 (mass concen-
E-mail address: srodriguez@inm.es (S. Rodrı́guez). trations of particulate matter-PM <10 mm and <2.5 mm

1352-2310/$ – see front matter Crown Copyright Ó 2008 Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2008.04.022
6524 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534
aerodynamic diameter, respectively) with an increased risk
to sufferers of respiratory and cardiovascular diseases
(Dockery and Pope, 1996). As a result of this, PM10 and
PM2.5 are currently used as urban air quality reference
‘‘metrics’’. More recent research has highlighted the high
potential toxicity of some PM components. For example, ul-
trafine particles (<0.1 mm) are considered especially detri-
mental to human health (Peters et al., 1997). These
particles easily reach the alveoli, enter the blood circulatory
system and may be distributed throughout the whole hu-
man body, with this distribution being greater for insoluble
material. Moreover, fresh soot particles are particularly sur-
face-reactive and may carry carcinogenic compounds (e.g.
PAHs; Highwood and Kinnersley, 2006). The debate already
open on ‘‘whether additional (to PM10 and PM2.5) metrics
on the ambient air particle concentration should be moni-
tored to improve human health protection’’ has prompted
several studies focused on characterising aerosol physical
properties. The PM Working Group of the European Com-
mission recognised that more studies are necessary on
other metrics of the aerosol concentration in order to con-
sider a possible regulation of metrics complementary to
PM10 and PM2.5 (Second Position Paper on PM, 2004). Re-
cently, much of the attention has been paid to ultrafine par-
ticles in cities.
Ultrafine particles typically account for 80–90% of the
total number concentration (e.g. Wehner and Wiedensoh-
ler, 2003; Rodrı́guez et al., 2007). In urban air, new ultrafine
particles have two main origins:
(1) Primary vehicle exhaust emissions. Primary particles
emitted by vehicle exhausts tend to exhibit a size distribu-
tion with a ‘‘nucleation mode (<30 nm)’’ and a ‘‘soot mode
(50–80 nm)’’ (Burtscher, 2005; Rose et al., 2006). The ‘‘nu-
cleation mode’’ is mainly attributed to binary H2O–H2SO4
nucleation, nucleation of some organic compounds and
subsequent particle growth (up to w30 nm) by condensa-
tion processes during the dilution and cooling of vehicle
exhaust (Harris and Maricq, 2001; Casati et al., 2007).
Low ambient air temperature, low dilution conditions or
high relative humidity increase the formation and growth
rates of nucleation particles during the dilution and cooling
of vehicle exhaust (Olivares et al., 2007; Casati et al., 2007).
The ‘‘soot mode’’ is mainly made up of elemental carbon,
absorbed organic material and some other trace elements
formed in the engine and directly emitted in the aerosol
phase (Burtscher, 2005; Harris and Maricq, 2001). Soot
emissions have classically been higher in diesel than in gas-
oline vehicles.
(2) In situ new particle formation in ambient air. This may
occur by nucleation of photo-oxidized species under high
solar radiation conditions (Boy and Kulmala, 2002; Rodrı́-
guez et al., 2005; Hamed et al., 2007). Although it is known
that these processes also occur in urban air (e.g. Wehner
and Wiedensohler, 2003; Kulmala et al., 2004, 2005; Qian
et al., 2007), they have not yet been investigated in depth
owing to the fact that most of these studies on nucleation
in ambient air have been performed in rural and remote
areas.
Processes affecting PM1, PM2.5 and PM2.5–10 concen-
trations are significantly different from those affecting the
ultrafine particle number concentration. Accumulation
mode particles (0.1–1 mm) are the most important contrib-
utors to PM1 and PM2.5, even if they account for a marginal
fraction of the number concentration (10–15%). Although
some primary emissions may contribute (e.g. soot due to
heavy duty diesel engines or mineral dust), most of the ac-
cumulation mode mass is due to gas to particle conversion
processes onto pre-existing particles and to ultrafine parti-
cle growth (Cabada et al., 2004). In contrast, coarse parti-
cles (>1 mm) are mainly made up of mineral dust,
abrasion products from tyre and brake wear, and sea salt
at coastal sites. Ultrafine, accumulation and coarse particles
also differ in life time. Coarse particles are relatively rapidly
removed through sedimentation, whereas ultrafine parti-
cles rapidly grow through condensation and coagulation.
In contrast, accumulation mode particles exhibit a long res-
idence time (from days to a few weeks) and consequently,
they may significantly contribute to the urban and regional
aerosol background.
There is a growing interest in studying the processes
affecting the relationship between metrics representative
of the particle concentration in urban air. The relation-
ship between PM10 and number concentration has been
studied in several cities (Ketzel et al., 2004; Mönkkönen
et al., 2004; Harrison and Jones, 2005). Ruuskanen et al.
(2001) performed a comparative study on PM2.5 filter
blackness and concentrations of PM2.5, ultrafine and
accumulation mode particles in cities in Germany, Fin-
land and The Netherlands. Rodrı́guez et al. (2007) studied
the relationship between number size distribution and
PM2.5 composition in Milan, Barcelona and London.
More recently, Puustinen et al. (2007) investigated the
spatial variations of PM10, PM2.5, soot and number con-
centration in Amsterdam, Athens, Birmingham and Hel-
sinki. The relationship between number concentration
and other aerosol concentration metrics may be complex
for several reasons. For example, long range transport of
(aged) aerosol may exhibit a much higher influence on
PM10 and on PM2.5 than in number concentration (Ket-
zel et al., 2004). On the other hand, processes contribut-
ing to the decrease in PM10 and/or PM2.5 (e.g.
meteorology) may enhance the new particle formation
rates owing to the fact that reductions in PMx may
decrease the surface area acting as a condensation sink
for the aerosol gaseous precursors (Burtscher, 2005;
Hamed et al., 2007). In a recent study, Hoek et al.
(2008) observed that in urban areas the number concen-
tration exhibits a much higher spatial variability than
PM2.5, soot and sulphate-aerosol.
The purpose of this study is to investigate the influ-
ence of sea breeze circulation and of road traffic emis-
sions on the relationship between the particle number,
black carbon, PM1, PM2.5 and PM2.5–10 concentrations
in a coastal city. Studies performed in urban areas of East-
ern Spain showed that sea breeze exerts a major influ-
ence on PM10 and PM2.5 concentrations (Viana et al.,
2005). The results of this study show how the great
changes in the daylight–night meteorological conditions
(including inland entries of clean air during daylight)
exert a marked influence on the relationship between
number concentration and other aerosol concentration
metrics.
 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534
2. Methodology
2.1. Study city
This study was performed in Santa Cruz de Tenerife (Ca-
nary Islands; 28 280 N, 16 150 W; Fig. 1). This is a 221,500
inhabitant city (distributed over 150 km2) located at the
bottom of the southern slope of the Anaga ridge and the
eastern slope of the SW to NE ridge crossing the Island.
Fig. 1. (A)Topographic map of Tenerife for every 100 m. Santa Cruz de Ten-
erife city: (B) Vertical contour highlighting the direction of the breeze blow-
ing (grey rectangles represent buildings), (C) picture of the city, and (D)
regular daily evolution of wind speed and direction during the measurement
campaign (mode of wind direction and mean of wind speed). Different parts
of the city are indicated: Santa Cruz Observatory (SCO), Tome Cano (TC),
Gladiolos (GL) and the Crude Oil Refinery (COR).
6525
This topographic setting protects the city from the Trade
winds (NNE) that blow over the ocean (see details on the
meteorology in Guerra et al., 2004). The main sources of an-
thropogenic aerosols in the city are: (1) road traffic (the two
main city roads are highlighted in Fig. 1A), (2) a crude oil re-
finery (COR) located on the SE shore of the city (see COR in
Fig. 1C), and (3) ship emissions in the harbour. Natural
Saharan dust and sea salt may significantly contribute to
the daily aerosol load (>100 mgPM10 m3 during dust
events; Viana et al., 2002).
2.2. Measurements
Measurements of PM were performed simultaneously
(mid-March to mid-April 2006) at three sites in the city
of Santa Cruz de Tenerife (Fig. 1C): (1) Santa Cruz Observa-
tory (SCO), (2) Tome Cano (TC) and (3) Gladiolos (GL).
(A) Santa Cruz Observatory (SCO; Fig. 1C) is a coastal urban
background site located on the roof of an 8-floor build-
ing at 52 m above sea level, at about 45 m above
ground. Measurements of meteorological parameters
(wind speed and direction, temperature, relative
humidity, pressure and global radiation), trace gases
(CO, SO2 and O3) and particles at SCO are performed
by the staff of Izaña GAW Observatory in the frame-
work of the GURME (GAW) program. The site is on
the NE edge of the city, close to the shore and on the
western side of ‘‘Anaga Avenue’’ (a 4-lane road running
along the shore). The main data set used in this study
was collected at this site, where the following mea-
surements were performed:
B PMx mass concentrations. One-minute concentrations of
PM1, PM2.5 and PM10 have been obtained at this site
since 2002 by multiplying the aerosol volume concen-
trations (monitored with an ‘‘Optical Particle Counter –
OPC’’ – GRIMMÔ) by experimentally determined ‘‘vol-
ume-to-mass conversion factors’’. These factors were
determined by cross correlating the aerosol (PM10 and
PM2.5) mass (determined by 24-h filter sampling with
high volume samplers) versus the volume (<10 mm
and <2.5 mm) determined by the OPC measurements.
These PM ‘gravimetric’ versus ‘OPC-volume’ measure-
ments showed a good degree of agreement: slope 1.65
r2 ¼ 0.94 for PM10 and 1.31 r2 ¼ 0.75 for PM2.5. These
values were obtained with 53 PM10 and 51 PM2.5
samples collected from January to September 2006.
B The mass concentrations of black carbon (BC; the com-
ponent of soot responsible for light absorption) less
than 10 mm were monitored by placing a PM10 impac-
tor in the inlet of a ‘‘Multi Angle Absorption Photome-
ter – MAAP’’ (ThermoÔ Carusso 5052). These
measurements were performed from 17th March to
10th April 2006.
B The number concentration of particles coarser than
3 nm (N3) was continuously monitored with an ‘‘Ultra-
fine Condensation Particle Counter – UCPC’’ (TSIÔ -
model 3025A). These measurements were performed
from 17th March to 10th April 2006.
6526 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534
(B) Gladiolos and Tome Cano are city centre sites located to
the NW of the industrial area of the city (crude oil refin-
ery) and to the NW of the motorway (which links the
city to the northern side of the island; Fig. 1C). At these
sites measurements of PM10, PM2.5, gaseous pollut-
ants (CO, NOx, SO2 and O3) and meteorology (wind
speed and direction, temperature, relative humidity
and pressure) are continuously performed by following
standard procedures in air quality networks. Measure-
ments of PM10 and PM2.5 were performed with beta
and TEOM instruments, respectively. PM2.5 was not
monitored at the Tome Cano site.
Finally, measurements of road traffic intensity (number
of vehicles h1) were also performed in several parts of the
city by city council staff. In this article we will only show the
road traffic intensity at the coastal Anaga Avenue (where
the SCO site is located).
3. Results and discussion
During the intensive field measurement campaign,
mean concentrations of 24 mg m3 of PM10, 14 mg m3 of
PM2.5, 9 mg m3 of PM1, 1.9 mg m3 of BC and 26 305
cm3 of N3 were recorded at the urban background SCO
site (Santa Cruz Observatory), 46 mg m3 of PM10 at TC
(Tome Cano) and 43 mg m3 of PM10 and 13 mg m3 of
PM2.5 at GL (Gladiolos) were recorded at the city centre
sites. These mean PMx concentrations are slightly lower
than the annual mean PMx concentrations typically
recorded in this city because Saharan dust events (the
main cause of high PMx concentrations in this city; Viana
et al., 2002) did not occur during our campaign. These
mean PMx concentrations are within the range of those
typically observed in mid European cities (Harrison and
Jones, 2005; Puustinen et al., 2007; Rodrı́guez et al.,
2007; Ruuskanen et al., 2001).
3.1. Mean daily evolution of aerosols
The urban scale transport of air pollutants in Santa Cruz
de Tenerife is mainly driven by breeze circulation (Fig. 1B
and C). This breeze is characterised by inland (westward)
airflows during daylight (3–4 m s1) and a slight seaward
(eastward) airflow at night (w1 m s1). Inland breeze blow-
ing started at 08:00 and was characterised by an abrupt
shift in wind direction. Fig. 2 displays the regular daily evo-
lution of the road traffic intensity and the particle and some
gaseous pollutant concentrations at the SCO coastal
(Fig. 2A–F), TC and GL city centre (Fig. 2G–I) sites.
At the SCO coastal site, particle (PMx, BC and N3) and CO
concentrations exhibited a maximum during the morning
rush hours of working days, and a subsequent decrease
(09:0019:00) associated with the easterly entry of marine
air (Fig. 2A–F). At night, a smooth increase in the PMx con-
centrations, associated with slight westerly winds bringing
air masses from the city centre, was observed at SCO.
At the TC and GL city centre sites, after the maximum in
the NO and PMx concentrations recorded during the
morning rush hours, a decrease in the PMx concentrations
such as that described above at SCO (09:00–19:00) was not
observed (Fig. 2G–I). However, PM10 and PM2.5 at TC and
GL showed an increasing trend until 21:00 (local time).
This contrasting behaviour between the PMx concentra-
tions at the coastal (SCO) and city centre (TC and GL) sites
is a consequence of the easterly inland breeze blowing dur-
ing daylight, which prompts the entry of ‘‘clean’’ marine air
masses along the coast and favours the inland transport of
the pollutants (emitted in the eastern part of the city) to the
city centre. This is one of the reasons because PM10 con-
centrations are much lower at SCO coastal than at TC and
GL city centre sites. In fact, this daylight breeze results in
the inland transport of the (refinery) SO2 plumes, giving
rise to higher SO2 concentrations during daylight than at
night at the TC and GL city centre sites (Fig. 2G–I).
At the SCO coastal site, N3 and BC concentrations also
exhibited well defined daily cycles (Fig. 2A–C). During
working days, N3 and BC presented a maximum during
the morning rush hours. The morning maximum in the
‘‘vehicles h1/wind speed’’ ratio indicates that the morning
maximum in the particle concentration is favoured by the
coupled effects of an increase in the road traffic intensity
and low wind speed in the morning (owing to the fact
that the inland breeze has not yet started blowing). Observe
that the daily evolution of N3 and BC during weekdays is
different from that recorded at weekends because of the
change in road traffic patterns. This daily evolution in num-
ber concentration is similar to that typically observed in
other cities (e.g.Wehner and Wiedensohler, 2003; Charron
and Harrison, 2003; Rodrı́guez et al., 2007). In Helsinki and
Liepzig, a similar daily evolution in the ‘‘black carbon mass’’
and ‘‘soot number’’ concentrations has been observed,
respectively (Pakkanen et al., 2000; Rose et al., 2006).
3.2. Processes affecting urban coastal aerosol concentrations
The relationship between road traffic intensity,
meteorology and particle concentration at SCO (coastal
urban background site) was examined using Principal
Component Analysis (PCA) followed by a varimax rota-
tion. This analysis was performed at several times of
the day: morning (07:00–09:00), central daylight
(11:00–17:00) and night (00:00–05:00). Three principal
components, accounting for 81, 66 and 72% of the total
variance for the three daytime periods selected, were
found (Table 1):
B principal component 1 is positively correlated with PMx
and BC and negatively correlated with wind speed.
The fact that this component does not exhibit a signifi-
cant correlation with road traffic intensity (number of
vehicles h1) indicates that fresh road traffic emissions
do not exhibit a major influence on PMx variance. The
significant negative factor loading of wind speed indi-
cates that this component accounts for the influence
on the aerosol mass (BC and PMx), of the dilution and
the air mass renovation prompted by wind blowing
over the study city. The negative association of the N3/
BC ratio in this component will be discussed later.
 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534 6527

Monday-Friday Saturdays Sundays

2·vehicles/h / wind speed, s/m

50·103 1500
A B C
10·BC, ng/m3
N3, cm-3

1000

2·CO, µg/m3
vehicles / h
25·103
500

SCO SCO SCO

0 0

30
D SCO E SCO F SCO
µg/m3

15 PM10
PM2.5
PM1
PM2.5-10
0
0 4 9 14 19 0 4 9 14 19 0 4 9 14 19

60
G H I PM10 -TC
PM10 -GL
µg/m3

30 2xPM2.5 -GL
NO -GL
SO2 -GL
TC & GL TC & GL TC & GL
0
0 4 9 14 19 0 4 9 14 19 0 4 9 14 19
GMT

Fig. 2. Mean daily cycles. Hourly averaged concentrations of CO and the particle N3, BC and PMx concentrations at the Santa Cruz Observatory (SCO) ‘‘coastal
urban background site’’ (A–C) and of PM10, PM2.5 and gaseous pollutants at the Tome Cano (TC) and Gladiolos (GL) city centre sites (G–I) during weekdays, Sat-
urdays and Sundays.

B principal component 2 is positively correlated with road
traffic intensity, BC and N3. This component represents
the influence of fresh vehicle exhaust emissions on the
particle concentration.
B principal component 3 is present during daylight (i.e.
morning rush hours 07:00–09:00 and central daylight
period 11:00–17:00). The positive correlation of the
N3/BC ratio and solar radiation intensity suggests that
nucleation of photo-oxidized vapours contributes to in-
creasing the above ratio by enhancing new particle for-
mation in ambient air. Further details are provided
below.
3.3. Influence of wind speed
The results of the PCA shown above indicate that wind
speed exerts: (1) a major influence on PMx, (2) a moderate
influence on BC and (3) a relatively low influence on N3. In
fact, wind speed exhibited Pearson’s correlation coefficients
(r) of 0.50, 0.44, 0.41, 0.33 and 0.0 with PM2.5–10,
PM2.5, PM1, BC and N3, respectively (values calculated using
3092 10-min observations). These results are corroborated
when analysing the particle concentration versus wind
speed plots shown in Fig. 3. The fact that high N3 concentra-
tions (>45  103 cm3) may still be recorded under high
wind speed conditions (>5 m s1) may be accounted for by
new particle formation processes. At a roadside site in Lon-
don, Charron and Harrison (2003) found that increases in
wind speed produced much higher decreases in the concen-
tration of accumulation mode particles (0.1–1 mm) than in
the concentration of nucleation mode particles (<30 nm).
They argued that this was caused by the fact that ‘‘clean
atmospheres’’ (favoured by high wind speeds) tend to favour
new particle formation owing to the low aerosol surface area
(mostly occurring in the accumulation mode) available for
condensation of the aerosol gaseous precursors. They con-
cluded that the lack of correlation between wind speed
and number concentration is a feature of new particle for-
mation. Similar results were found by Rodrı́guez et al.
(2005) at a rural site influenced by nearby town emissions
in Northern Italy. The analysis of the N3/BC ratios shown
below supports this involvement of the new particle forma-
tion processes during periods of high wind speed (typically
associated with inland breeze blowing).
3.4. Quantification of the impact of road traffic emissions
The impact of fresh road traffic emissions on the particle
concentration was quantified at several times of the day.
Fig. 4A1–F1 presents the mean BC, N3 and PMx concentra-
tions measured for each 100 vehicles h1 bin during the
morning (07:00–09:00), the central part of daylight
(11:00–17:00) and at night (00:00–05:00). The use of 100
vehicles h1 bins smoothes the variability in the concentra-
tions due to other influencing parameters (mainly meteo-
rology). The concentrations of BC and N3 tend to increase
when increasing road traffic intensity (Fig. 4A1 and B1).
6528 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534

Table 1
Factor loading of the Principal Components Analysis performed with data from selected periods

Morning rush hours (07:00–09:00) Central daylight (11:00–17:00) Night (00:00–05:00)

PC 1 PC 2 PC 3 PC 1 PC 2 PC 3 PC 1 PC 2
Vehicles h1 0.11 0.89 0.14 0.29 0.51 0.04 0.01 0.85
BC 0.56 0.70 0.33 0.39 0.82 0.22 0.75 0.59
N3 0.17 0.90 0.07 0.32 0.81 0.28 0.30 0.80
N3/BC 0.50 0.05 0.61 0.23 0.18 0.77 0.77 0.04
PM1 0.95 0.06 0.07 0.86 0.27 0.08 0.86 0.36
PM2.5 0.96 0.04 0.08 0.89 0.21 0.05 0.86 0.37
PM2.5–10 0.88 0.16 0.08 0.52 0.16 0.55 0.85 0.46
Wind speed 0.42 0.15 0.81 0.63 0.07 0.12 0.49 0.09
Radiation 0.24 0.03 0.73 0.08 0.20 0.72
Explained variance 38% 24% 19% 29% 20% 17% 46% 26%

This behaviour is not observed for PM2.5 and PM1 (Fig. 4C1
and D1). During the morning, the PM2.5–10 concentrations
also tend to increase when road traffic intensity increases,
this being most probably due to road dust re-suspension
(Fig. 4E1).
The much lower ‘‘direct influence’’ of the road traffic
emissions in PM2.5 and PM1 (Fig. 4C1 and D1) than in N3
and BC (Fig. 4A1 and B1) may be accounted for by the com-
ing into force of the European Standards EURO 1–4 (pro-
gressively since 1992) for vehicle exhaust emissions.
Because these standards are established in terms of ‘‘parti-
cle mass’’ (g km1), they have decreased the emissions of
accumulation (0.1–1 mm) and coarse (>1 mm) mode parti-
cles, which are the main contributors to PMx. In contrast,
N3 and BC tend to increase when the road traffic intensity
increases. This is due to the fact that vehicle exhaust mostly
emits ultrafine and soot particles and these are the main
contributors to N3 and BC (Burtscher, 2005; Harris and
Maricq, 2001; Rose et al., 2006).
Although BC concentrations tend to increase when road
traffic intensity increases, different BC concentrations are
observed for a given number of vehicles h1 bin at different
times of the day (Fig. 4A1). For example, a road traffic inten-
sity within the range of 1100–1200 vehicles h1 is associ-
ated with 3.7 mgBC m3 during the 07:00–09:00 period
and with 1.5 mgBC m3 during the 11:00–17:00 period.
The lower BC concentrations during the 11:00–17:00 pe-
riod are a consequence of the higher wind speeds during
that period of daylight (because of the inland breeze blow-
ing). For this reason we have normalized the road traffic in-
tensity data by dividing them by wind speed (Fig. 4A3).
Observe how BC concentrations tend to increase in
a more regular way (monotonic growth) when increasing
the vehicles h1/wind speed ratio than when increasing
the vehicles h1 ratio (Fig. 4A1 and A3). The results show
how increases in 200 vehicles h1 m1 s1 are associated
with BC increases of about 0.50  0.29 mgBC m3 (on aver-
age) at any time of the day.
This analysis of particle concentration versus vehi-
cles h1/wind speed was also applied to the PMx and N3 con-
centrations (Fig. 4A3–F3). The most important results are:
(1) N3 also exhibits an increasing trend with the vehi-
cles h1/wind speed ratio of about 3250  2395 cm3
every 200 vehicles h1 m.s1 during the 07:00–09:00
period and of about 6523  1437 cm3 every 200 vehi-
cles h1 m.s1 in the 11:00–17:00 period. These higher
values in the 11:00–17:00 period in comparison with
the 07:00–09:00 period suggest an enhancement in
the particle formation processes at noon and during
the afternoon. This interpretation is supported by the
results shown in the following section.
(2) PM2.5 and PM1 do not exhibit a strong association with
the vehicles h1/wind speed ratio (as that described for
BC and N3).
(3) PM2.5–10 exhibits a clearly increasing trend of about
1.20  0.90 mgPM2.5–10 m3 every 200 vehicles h1
m.s1 during the morning rush hours (07:00–09:00),
most probably due to road dust re-suspension. The
weaker association observed during the 11:00–17:00
period (Fig. 4E3) is probably due to the influence of
sea salt transported inland during daylight.
3.5. The number–to–black carbon ratios
The relationship between N3 and BC concentrations at
the SCO site has been used to identify periods of enhance-
ment in the new particle formation rates, which would lead
to an increase in the N3/BC ratio. At SCO, N3 and BC
exhibited a significant correlation because of the vehicle
exhaust emissions: r ¼ þ0.70 during the whole measure-
ments campaign (based on 3092 10-min averages data).
When plotting the N3 versus BC data, it can clearly be ob-
served that all points are comprised between two well
defined borders with slopes (S) Smin ¼ 4.8  106 parti-
cles ngBC1 and Smax ¼ 47  106 particles ngBC1, repre-
senting the minimum and maximum N3/BC ratios
observed in ambient air at the SCO site, respectively
(Fig. 5). The fact that the N3 versus BC data are comprised
between these two slopes is observed at any time of the
day. For the periods 00:00–05:00, 07:00–09:00 and
11:00–17:00, Smin and Smax exhibit values of 4.5, 4.9 and
8.1 106 particles ngBC1 and 48, 43 and 57 parti-
cles ngBC1, respectively (plots not shown for the sake of
brevity). The fact that the slope Smin is much higher during
the central part of daylight, indicates that: (1) the slope Smin
is strongly related to the minimum contribution of the ve-
hicle exhaust emissions to the particle number
 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534 6529

A 12
y = 1.87x-0.38
ratio exhibits a daily evolution with a maximum during
daylight. Previous studies have shown that enhancements
R2 = 0.120 in the new particle formation rates during the dilution
BC, µg/m3

and cooling of the vehicle exhaust are favoured by low am-

6 bient air temperature (e.g. Olivares et al., 2007) and/or low
wind speed leading to less dilution (Casati et al., 2007).
However, these two reasons are not plausible at SCO, where
the highest N3/BC ratios are observed during the period of
0 highest temperature and wind speed 11:00–17:00 (Fig. 6).
At SCO the N3/BC ratio reaches the highest values during
B 20
the noon and afternoon period when:
y = 5.68x-0.59
PM2.5-10, µg/m3

R2 = 0.524

10
(1) solar radiation intensity reaches the highest values. In
fact, in the PCA discussed above, it was shown how
Principal Component 3 is correlated with the N3/BC ra-
tio and the solar radiation (PC 3 in Table 1),
0
(2) PM1 and PM2.5 concentrations (where most of the
C 40
y = 14.9x-0.21
aerosol surface area is comprised) are minima (Figs. 2
R2 = 0.323
and 6). The fact that the N3/BC ratio exhibited a much
PM2.5, µg/m3

higher anti-correlation with PM1 and PM2.5 than

with PM2.5–10 during the 11:00–17:00 period (plot
20
not shown), suggests a more active role of the accumu-
lation mode particles (which typically accounts for
most of the aerosol surface area) as condensation sink
for the aerosol gaseous precursors,
0

D 90 (3) it is positively correlated with wind speed for wind

speed values between 0 and 4 m s1 (Figs. 3E and 4F3).
N3·103, cm-3

45 These features suggest that, in addition to the new particle

formation during the dilution and cooling of the vehicle ex-
haust, there is a non-negligible contribution to N3 concentra-
tions due to new particle formation in ambient air. In fact, the
0 features described above fit very well with those of the new
E 40 particle formation in ambient air described by Boy and Kul-
mala (2002), Rodrı́guez et al. (2005) and Hamed et al.
N3/BC, ·106, /ng

(2007). The behaviour observed at the SCO site indicates

20
0 gaseous precursors formed by photo-oxidation processes.
0 2 4 6 8 10
wind speed, m/s
Fig. 3. Concentration of particles (A–D) and N3/BC ratio (E) versus wind
speed at the SCO site. Red dots and line in plots D and E represent the
mean N3 and N3/BC values for each 1 m s1 bin.
concentration (minimum amount of particles emitted and
formed during the dilution and cooling of exhaust per
nanogram of BC emitted by the vehicle exhaust), and (2)
there is an enhancement in the new particle formation
rates during daylight resulting in a higher N3/BC ratio
(4.9  106 particles ngBC1 during the 07:00–09:00 period
and 8.1 106 particles ngBC1 during the 11:00–17:00 pe-
riod on average; Fig. 6). Observe in Fig. 6 how the N3/BC
that the decrease in PM1 and PM2.5 concentrations, promp-
ted by the increase in wind speed (due to the inland breeze
blowing), results in a decrease in the aerosol surface area con-
centrations. This would favour nucleation, rather than con-
densation onto pre-existing particles, for those aerosol
Observe in Fig. 6 how the daily variation of the N3/BC ratio
is much better modulated by the daily evolution of the in-
verse of PM1 (which typically comprises most of the aerosol
surface) than by the daily evolution of PM2.5–101. An exam-
ple of one of these events (8th April 2006) is shown in Fig. 7:
observe the correlated increases in the N3/BC ratio and in so-
lar radiation intensity from 10:00 to 16:00. This contribution
to N3 due to nucleation in ambient air during the central part
of the daylight accounts for: (1) the faster decrease in the BC
than in the N3 concentrations after the morning rush hours
(Fig. 2 A), and (2) the higher increase in N3 concentrations
for every 200 vehicles h1 m.s1 bin during the 11:00–
17:00 period than during the 07:00–09:00 period (described
above; 3250 cm3 during the 07:00–09:00 and about
6523 cm3 during the 11:00–17:00 periods).
6530 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534

8
7-9h
11-17h
A1 A2 A3
BC, µg/m3
0-5h
4

0
60
103·N3, m-3

30

B1 B2 B3
0
15
PM1, µg/m3

10

5
C1 C2 C3
0
20
PM2.5, µg/m3

10

D1 D2 D3
0
20
E1 E2 E3
PM2.5-10, µg/m3

10

0
N3/BC, 106/ng

20

10

F1 F2 F3
0
0

400

800

1200

1600

2000

2400

0 2 4 6 8
0

400

800

1200

1600

2000

vehicles·h-1 wind speed, m/s vehicles·h-1/ wind speed, s/m

Fig. 4. Particle concentration and N3/BC ratio averaged for each ‘‘100 vehicles h1’’ bin (A1–F1), for each ‘‘1 m s1’’ bin (A2–F2) and for each ‘‘200 vehicles h1’’
bin (A3–F3).

3.6. Day-to-day particle events
Fig. 8 shows the hourly BC, N3 and PMx concentrations
at the SCO site and the road traffic intensity during a period
of the measurement campaign. Fig. 9 shows the median of
the BC, N3 and PMx concentrations for each wind direction
for the 07:00–09:00, 11:00–17:00 and 00:00–05:00 periods
during all the measurement campaigns. These data (Figs. 8
and 9) clearly illustrate how N3, BC and PMx are influenced
in different ways by breeze circulation, vehicle exhaust
emissions and ageing processes given that:
1. high BC and N3 concentrations are recorded during the
morning rush hours due to fresh vehicle exhaust emis-
sions (07:00–09:00; Figs. 8A,B and 9A,B), the highest be-
ing BC and N3 concentrations registered when wind
blows from the city centre (Southwest; Fig. 9A1) or
from the coastal Anaga Avenue (East; Fig. 8A1);
2. high N3 concentrations (associated with high N3/BC ra-
tios) during the central part of daylight (11:00–17:00)
are associated with easterly winds (inland breeze;
Fig. 9B2) due to the above described new particle forma-
tion in ambient air (Figs. 6 and 9A2,B2). Examples of
 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534
100·103
Smax
N3, cm-3
50·103
0 70·103
0 6
BC, µg/m3
Fig. 5. Hourly averaged values of the particle number N3 versus particle
black carbon (BC) concentrations at the SCO site.
these events occurred during the periods 22–24 and 28–
31 March 2006, when N3/BC ratios of 15–25  106 parti-
cles ngBC1 and <10  106 particles ngBC1 were
recorded during daylight and at night, respectively
(Fig. 8; N3/BC ratios not shown); and
3. the highest PM1 and PM2.5 and the lowest N3 and BC
concentrations are recorded at night when the wind
blows from the city centre, bringing aged particulate
pollutants to the shore owing to the seaward airflow as-
sociated with nocturnal breeze circulation (Fig. 9C3 and
D3). See examples of these PM1 and PM2.5 nocturnal
events associated with the outflows from the city centre
during the periods 23–26 March and 30 March–2 April
2006 (Fig. 8).
BC and N3 tend to exhibit patterns correlated with
those of the road traffic intensity, evidencing the high in-
fluence of ‘‘fresh emissions’’ (Fig. 8). In contrast, PM1 and
PM2.5 tend to exhibit high concentrations at night, when
road traffic emissions are not significant. The nocturnal
conditions (e.g. decrease in the boundary layer depth
N3 / BC, 106/ng
50·PM2.5-10-1, m3/µg
125·PM1-1, m3/µg
wind speed, m/s
1000
global radiation, w/m2
500
0 0
0 4 8 12
time of day
Fig. 6. Daily mean cycle (hourly averaged values) of the global radiation,
wind speed, the N3/BC ratio, and the inverse of the PM1 (PM11) and
PM2.5–10 (PM2.5–101) concentrations.
6531
70·103
A 1000
10·BC, ng/m3
Radiation, w/m2
35·103
500
Smin
0 0
12
B 30
N3/BC, 106/ng
N3, cm-3
35·103
15
0 0
0 6 12 18
time of day
Fig. 7. 10-min averaged values of the solar radiation, N3/BC ratio, black car-
bon (BC) and number N3 concentrations at the SCO site during 8th April
2006.
resulting in an increase of the concentrations of aerosols
and its gaseous precursors, or decrease in temperature
decreasing the equilibrium vapour pressure and conse-
quently favouring condensation) favour particle growth
by coagulation and condensation processes and this con-
tributes to the increase in the particle mass in the accu-
mulation mode and consequently to the increase in PM1
and PM2.5 concentrations. Observe in Fig. 10A how
PM2.5 experiences low spatial variations across the city
(slope and intercept of about 1.0). In contrast, PM10 ex-
periences a much higher spatial variability across the
city because of the local contribution of coarse particles
in the city centre (w20 mg m3): see the high value of
the intercept (18–21 mg m3) of the scatter plots ‘‘PM10:
GL versus SCO (Fig. 10B) and TC versus SCO (Fig. 10C)’’
and ‘‘PM2.5–10: GL versus SCO (Fig. 10D)’’. This supports
the idea that PM2.5 is mostly representative of the urban
background (accumulation mode aged aerosols formed
by condensation/reaction of gases onto pre-existing par-
ticles) whereas PM2.5–10 is mostly affected by local
30 (street) emissions.
4. Summary and conclusions
20 In a coastal urban environment the daily cycles of breeze
circulation (inland during daylight and seaward at night)
and the road traffic emissions exert a great, but differenti-
ated, influence on the particle black carbon (BC), number
10 (N3, >3 nm) and PMx (PM1, PM2.5 and PM2.5–10) concen-
trations. BC and N3 concentrations are greatly influenced
by fresh vehicle exhaust emissions and exhibit an increas-
ing trend when the ‘‘road traffic intensity (vehicles h1)/
wind speed’’ ratio increases. In contrast, PMx (specially
16 20
PM1 and PM2.5) reaches the highest values at night due
to the seaward transport of aged particulate pollutants to
the shore, and the lowest values during daylight due to
the inland entry of clean marine air. Although N3 and BC
concentrations exhibit a significant correlation throughout
6532 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534

SCO

2000 A 10

BC, µg/m3
1000 5

0 0
80·103
B
vehicles / h

2000

N3, cm-3
40·103
1000

0 0
60

µg/m3
2000 C
30 PM10
1000 PM2.5
PM1
0 0 PM2.5-10
21 22 23 24 25 26 27 28 29 30 31 1 2 3
March April

Fig. 8. Hourly mean values of road traffic intensity at the coastal Anaga Avenue (vehicles h1) and of the particle BC, N3 and PMx concentrations at the SCO site
from March 21st to April 3rd 2006.

the whole day, the N3/BC ratio experiences a daily evolu-
tion correlated with that of the solar irradiance and wind
speed, in such a way that high N3 concentrations associated
with high N3/BC ratios and high solar irradiance conditions
are recorded during the ‘‘daylight inland breeze’’ period
due to an enhancement of some ‘‘new particle formation’’
processes. The analysis performed indicates that this en-
hancement in the new particle formation processes is
strongly related to the nucleation of photo-oxidized va-
pours under the relatively low PMx (and consequently
low aerosol surface area) concentrations prompted by the
inland entry of clean marine air due to the daylight breeze
blowing. The statistical tools used in this study corroborate
the association between ‘‘BC and N3 with road traffic inten-
sity (fresh emissions)’’, ‘‘PMx and wind speed1’’ and ‘‘N3/
BC ratio and solar radiation (enhancement in the new par-
ticle formation due to photo-oxidation processes)’’.
Although it is known that new particle formation due to
photo-oxidation of aerosol gaseous precursors may occur
in the urban atmosphere (e.g. Wehner and Wiedensohler,
2003; Kulmala et al., 2004; Qian et al., 2007), most studies
on urban ultrafine particles are currently focused mainly
on ‘‘primary vehicle exhaust emissions’’. The results obtained
here indicate that this contribution due to photo-chemically

N BC N3 x103 PM1 PM2.5 PM2.5-10

12 70 20 40 20
A1 B1 C1 D1 E1
6 35 10 20 10
7-9h
morning

A2 12
B2 70
C2 20
D2 40
E2 20

6 35 10 20 10

11-17h
central
daylight

A3 12
B3 70
C3 20
D3 40
E3 20
6 35 10 20 10
0-5h
night

Fig. 9. Hourly mean concentrations of the particle BC, N3 and PMx for each wind direction at several times of the day at the SCO site.
 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534
GL vs. SCO GL vs. SCO
40 100
A PM2.5
B PM10
µg/m3
20 50
y=1.0x + 1.0 y=0.9x + 20.7
r2= 0.88 r2= 0.82
0 0
0 20 40 0 50 100
PMx SCO, µg/m
Fig. 10. Daily mean concentrations of PM2.5, PM2.5–10 and PM10 at city centre sites (GL and TC) versus at SCO coastal urban background.
induced nucleation may significantly contribute to the urban
ultrafine particle concentration.
The results of this study show how the strong changes in
daylight to night meteorological conditions (which in-
cludes inland entries of clean air during daylight) exert
a great/major influence on the ‘complex’ relationship be-
tween the number concentration and other aerosol con-
centration metrics. This, and other processes, not yet well
characterised, may contribute to the large spatial variability
in the particle number concentration as described by Hoek
et al. (2008).
According to Kulmala et al. (2004), new particle forma-
tion rates in a coastal environment as high as those in indus-
trial plumes are frequently recorded. This could, in part, be
due to the fact that some of the factors which may favour nu-
cleation are present in the coastal environment: (i) enough
high relative humidity to favour binary H2O–H2SO4 nucle-
ation (Easter and Peter, 1994; Olivares et al., 2007), (ii) rela-
tively clean air conditions (low aerosol surface area
concentration) due to the marine air entries) and (iii) the
mixing of two air parcels with different temperature and dif-
ferent relative humidities (Nilsson and Kulmala, 1998).
Acknowledgements
This study was financed by the Ministry for the Environ-
ment of Spain (Dirección General de Calidad Ambiental;
Project B026/2007/3-10.1: ‘‘Evaluación integral del impacto
de las emisiones de partı́culas de los automóviles en la cal-
idad del aire urbano’’). The Council of Santa Cruz de Tener-
ife and the Departments of ‘‘Environmental Health’’ and of
the ‘‘Environment’’ of the Canary Islands Government also
contributed to this study. Measurements at SCO are per-
formed within the framework of the GURME (GAW) pro-
gram. Part of this study was performed into the
framework of the project- GRACCIE (CONSOLIDER
INGENIO; Ministry of Education and Culture of Spain).
References
Boy, M., Kulmala, M., 2002. Nucleation events in the continental boundary
layer: influence of physical and meteorological parameters. Atmo-
spheric Chemistry and Physics 2, 1–16.
Burtscher, H., 2005. Physical characterization of particulate emissions
from diesel engines: a review. Journal of Aerosol Science 36, 896–932.
Cabada, J.C., Rees, S., Takahama, S., Khlystov, S.A., Pandis, S.N., Davidson, C.
I., Robinson, A.L., 2004. Mass size distributions and size resolved
chemical composition of fine particulate matter at the Pittsburgh
supersite. Atmospheric Environment 38, 3127–3141.
6533
TC vs. SCO GL vs. SCO
100 50
C PM10
D PM2.5-10
50 25
y=1.2x + 17.7 y=0.78x + 21.3
r2= 0.89 r2= 0.54
0 0
0 50 100 0 25 50
3
Casati, R., Scheer, V., Vogt, R., Benter, T., 2007. Measurement of nucleation
and soot mode particle emission from a diesel passenger car in real
world and laboratory in situ dilution. Atmospheric Environment 41,
2125–2135.
Charron, A., Harrison, R.M., 2003. Primary particle formation from vehicle
emissions during exhaust dilution in the roadside atmosphere. Atmo-
spheric Environment 37, 4109–4119.
Dockery, D., Pope, A., 1996. Epidemiology of acute health effects: sum-
mary of time-series studies. In: Wilson, R., Spengler, J.D. (Eds.), Parti-
cles in Our Air: Concentration and Health Effects. Harvard University
Press, Cambridge, MA, USA, pp. 123–147.
Easter, R.C., Peters, L.K., 1994. Binary homogeneous nucleation: tempera-
ture and relative humidity fluctuations, nonlinearity and aspects of
new particle production in the atmosphere. Journal of Applied
Meteorology 33, 775–784.
Guerra, J.C., Rodrı́guez, S., Arencibia, M.T., Garcı́a, M.D., 2004. Study on the
formation and transport of ozone in relation to the air quality man-
agement and vegetation protection in Tenerife (Canary Islands). Che-
mosphere 56, 1157–1167.
Hamed, A., Joutsensaari, J., Mikkonen, S., Sogacheva, L., Dal Maso, M.,
Kulmala, M., Cavalli, F., Fuzzi, S., Facchini, M.C., Decesari, S.,
Mircea, M., Lehtinen, K.E.J., Laaksonen, A., 2007. Nucleation and
growth of new particles in Po Valley, Italy. Atmospheric Chemistry
Physics 7, 355–376.
Harris, J.S., Maricq, M.M., 2001. Signature size distributions for diesel and
gasoline engine exhaust particulate matter. Journal of Aerosol Science
32, 749–764.
Harrison, R.M., Jones, A.M., 2005. Multisite study of particle number con-
centrations in urban air. Environmental Science and Technology 39,
6063–6070.
Highwood, E.J., Kinnersley, R.P., 2006. When smoke gets in your eyes:
the multiple impact of atmospheric black carbon on climate, air
quality and health. Environment International 32, 560–566. Review
article.
Hoek, G., Kos, G., Harrison, R., de Hartog, J., Meliefste, K., ten Brink, H.,
Katsouyanni, K., Karakatsani, A., Lianou, M., Kotronarou, A.,
Kavouras, I., Pekkanen, J., Vallius, M., Kulmala, M., Puustinen, A.,
Thomas, S., Meddings, C., Ayres, J., van Wijnen, J., Hameri, K., 2008. In-
door–outdoor relationships of particle number and mass in four Eu-
ropean cities. Atmospheric Environment 42, 156–169.
Ketzel, M., WåhlinKristensson, A., Swietlicki, E., Berkowicz, R., Nielsen,
O.J., Palmgren, F., 2004. Particle size distribution and particle mass
measurements at urban, near-city and rural level in the Copenhagen
area and Southern Sweden. Atmospheric Chemistry and Physics 4,
281–292.
Kulmala, M., Petäjä, T., Mönkkönen, P., Koponen, I.K., Dal Maso, M.,
Aalto, P.P., Lehtinen, K.E.J., Kerminen, V.M., 2005. On the growth of
nucleation mode particles: source rates of condensable vapor in pol-
luted and clean environments. Atmospheric Chemistry and Physics 5,
409–416.
Kulmala, M., Vehkamaki, H., Petäjä, T., Dal Maso, M., Lauria, A.,
Kerminen, V.M., Birmili, W., McMurry, P.H., 2004. Formation and
growth rates of ultrafine atmospheric particles: a review of observa-
tions. Journal of Aerosol Science 35, 143–176.
Mönkkönen, P., Umac, R., Srinivasan, D., Koponen, I.K., Lehtinen, K.E.J.,
Hämeri, K., Suresh, R., Sharma, V.P., Kulmala, M., 2004. Relationship
and variations of aerosol number and PM10 mass concentrations in
a highly polluted urban environmentdNew Delhi, India. Atmospheric
Environment 38, 425–433.
Nilsson, E.D., Kulmala, M., 1998. The potential for atmospheric mixing
processes to enhance the binary nucleation rate. Journal of Geophys-
ical Research 103, 1381–1389.
6534 S. Rodrı́guez et al. / Atmospheric Environment 42 (2008) 6523–6534
Olivares, G., Johansson, C., Ström, J., Hansson, H.C., 2007. The role of am-
bient temperature for particle number concentrations in a street can-
yon. Atmospheric Environment 41, 2145–2155.
Pakkanen, T.A., Kerminen, V.M., Ojanen, C.H., Hillamo, R.E., Aarnio, P.,
Koskentalo, T., 2000. Atmospheric black carbon in Helsinki. Atmo-
spheric Environment 34, 1497–1506.
Peters, A., Wichmann, H.E., Tuch, T., Heinrich, J., Heyder, J., 1997. Respira-
tory effects are associated with the number of ultrafine particles.
American Journal of Respiratory and Critical Care Medicine 155,
1376–1383.
Puustinen, A., Hämeri, K., Pekkanen, J., Kulmala, M., de Hartog, J.,
Meliefste, K., ten Brink, H., Kos, G., Katsouyanni, K., Karakatsani, A.,
Kotronarou, A., Kavouras, I., Meddings, G., Thomas, S., Harrison, R.,
Ayres, J.G., van der Zee, S., Hoek, G., 2007. Spatial variation of particle
number and mass over four European cities. Atmospheric Environ-
ment 41, 6622–6636.
Qian, S., Sakurai, H., McMurry, P.H., 2007. Characteristics of regional nu-
cleation events in Urban East St. Louis. Atmospheric Environment
41, 4119–4127.
Rodrı́guez, S., Van Dingenen, R., Putaud, J.P., Martins-Dos Santos, S.,
Roselli, D., 2005. Nucleation and growth of new particles in the rural
atmosphere of Northern ItalydRelationship to air quality monitoring.
Atmospheric Environment 39, 6734–6746.
Rodrı́guez, S., Van Dingenen, R., Putaud, J.P., Dell’Acqua, A., Pey, J.,
Querol, X., Alastuey, A., Chenery, S., Kin-Fai, H., Harrison, R.M.,
Tardivo, R., Scarnato, B., Gianelle, V., 2007. A study on the relationship
between mass concentrations, chemistry and number size distribu-
tion of urban fine aerosols in Milan, Barcelona & London. Atmospheric
Chemistry and Physics 7, 2217–2232.
Rose, D., Wehner, B., Ketzel, M., Engler, C., Voigtländer, J., Tuch, T.,
Wiedensohler, A., 2006. Atmospheric number size distributions of
soot particles and estimation of emission factors. Atmospheric Chem-
istry and Physics 6, 1021–1031.
Ruuskanen, R., Tuch, Th., Ten Brink, H., Peters, A., Khlystov, A., Mirme, A.,
Kos, G.P.A., Brunekreef, B., Wichmann, H.E., Buzorius, G., Vallius, M.,
Kreyling, W.G., Pekkanem, J., 2001. Concentrations of ultrafine, fine
and PM2.5 particles in three European cities. Atmospheric Environ-
ment 35, 3729–3738.
Second Position Paper on Particulate Matter, 2004. CAFE working group
on particulate matter (accessed 20.12.04).
Viana, M., Querol, X., Alastuey, A., Cuevas, E., Rodrı́guez, S., 2002. Influ-
ence of African dust on the levels of atmospheric particulates in the
Canary Islands air quality network. Atmospheric Environment 36,
5861–5875.
Viana, M., Pérez, C., Querol, X., Alastuey, A., Nickovic, S., Baldasano, J.M.,
2005. Spatial and temporal variability of PM levels and composition
in a complex summer atmospheric scenario in Barcelona (NE Spain).
Atmospheric Environment 39, 5343–5361.
Wehner, B., Wiedensohler, A., 2003. Long term measurements of submi-
crometer urban aerosols: statistical analysis for correlations with me-
teorological conditions and trace gases. Atmospheric Chemistry and
Physics 3, 867–879.