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Particle number size distributions of ambient-state and non-volatile
aerosols in the city offA
Augsburg, Germany
Katja Heinke (1), Wolfram Birmili (1), Alfred Wiedensohler (1), Mike Pitz (2,3), Joseph Cyrys (2,3) and Annette Peters (2)
(1) Leibniz Institute for Tropospheric Research, Permoserstrasse 15, 04318 Leipzig, Germany
(2) GSF – National Research Center for Environment and Health, Institute of Epidemiology , 85758
Neuherberg/Munich, Germany
(3) WZU – Environmental Science Center of the University of Augsburg, 86159 Augsburg, Germany
Email: Heinke@tropos.de
Introduction
Measurements with TDMPS and thermodenuder
Atmospheric
especially anthropogenic aerosols cause adverse health
(ambient state)
TDMPS
3 – 800 nm
Atmospheric
– especially anthropogenic aerosols cause adverse health
effects (e.g. WHO 2004). It is being assumed that especially insoluble (non-
volatile) fine (< 1 μm) particles such as soot have a strongly negative effect of
bi
t
Thermodenuder
(300°C)
the human health.
This
work is concerned with the description and the meteorological analysis of
a preliminary 2 year observation period (2004
2006) of particle number size
ambient
air
APS
a preliminary 2-year observation period (2004 – 2006) of particle number size
distributions in an urban environment of Augsburg. The speciality here was the
measurement and determination of ambient particles and the non-volatile
The combination of a Twin Differential Mobility Particle Sizer (TDMPS) with a thermodenuder
residuals (with thermodenuder).
0,6 – 10 μm
Augsburg
is a centre of environmental epidemiological research (KORA, Holle
et al ; 2005) Data collected at the measurement site will be correlated with
y ()
allows to measure particle number size distributions (3 – 800 nm) at ambient temperatures or
after heating to 300°C. For descriptions of the instruments, see Birmili et al. (1999) and
Wehner et al (2002)
et al.; 2005). Data collected at the measurement site will be correlated with
health endpoints in the near future to identify the most health relevant sub-
fractions of urban aerosols.
Wehner et al. (2002).
General results
Particle number size distributions
16000
18000
20000
with Thermodenuder
spring
0.70
0.75
Summation Method
SF
16000
18000
20000
without Thermodenuder
spring
10
4
10
5
TDMPS
APS
more
1 50
1.75
without
Thermodenuder
01.01.2005
01.01.2006
tion [cm
-3
]
8000
10000
12000
14000
spring
summer
autumn
winter
dN / dlog D
p
[cm
-3
]
0.55
0.60
0.65
spring
shrinking factor S
n-volatile
/ N
ambient
)
8000
10000
12000
14000
pg
summer
autumn
winter
dN / dlog D
p
[cm
-3
]
10
1
10
2
10
3
dN/dlog
less
volatile
volatile
1.00
1.25
1.50
ber concentrat
+
4
10
100
1000
0
2000
4000
6000
d
10
100
1000
0.40
0.45
0.50
spring
summer
autumn
winter
diameter
(N
non
til di
t
Di
4
10
100
1000
0
2000
4000
6000
d
10
-1
10
0
10
D
p
[cm
-3
]
μ
1%
5%
25%
Median
75%
0 25
0.50
0.75
particle numb
particle diameter, D
p
in nm
particle diameter, D
p
in nm
particle diameter, D
p
in nm
The comparison of the number size distributions between ambient (without thermodenuder) and
10
100
1000
10000
10
-3
10
-2
particle diameter, D
p
in nm
75%
95%
99%
307
400
500
600
700
800
900
1000
0.00
0.25
average
Julian Day (3.11.04 - 15.11.06)
3 - 8 nm
8 - 20 nm
20 - 70 nm
70 - 200 nm
200 - 800 nm
800 - 2000 nm
2000 - 10000 nm
non-volatile (with thermodenuder) particles shows high concentrations in autumn and winter.
Furthermore, all particles between 20 – 800 nm seem to contain a non-volatile core. The Aitken
mode decomposed after the thermodenuder in less ( e.g. soot) and more volatile particles. The
The average particle number
size distribution ( 3 nm – 10 μm)
i A b 11/2004 11/2006
The annual cycles show a particle
number concentration peak (< 800
nm) in winter
p
mode decomposed after the thermodenuder in less ( e.g. soot) and more volatile particles. The
summation method is used here to relate ambient and non-volatile particle size distributions.
The diameter ratio is interpreted as a particle “shrinking factor” of particulate matter loss due to
volatilisation The highest soot fraction occurs in autumn and winter at 80 nm
in Augsburg 11/2004 – 11/2006.
nm) in winter.
Diurnal cycles
volatilisation. The highest soot fraction occurs in autumn and winter at 80 nm.
The effect of the local sources (e.g.
traffic) can be seen best in particle
without Thermodenuder
y
10000
12000
on [cm
-3
]
Monday - Thursday
Saturday
Sunday
10000
12000
on [cm
-3
]
Monday - Thursday
Saturday
Sunday
N 20 – 70 nm without thermodenuder
N 8 – 20 nm with thermodenuder
traffic) can be seen best in particle
number concentrations between 20
– 70 nm without thermodenuder
The colour plots show a diurnal variation of
particle number size distribution without and with
10
100
800
in nm
without Thermodenuder
2.315E4
3.727E4
6E4
0
2
4
6
8 10 12 14 16 18 20 22 24
0
2000
4000
6000
8000
particle number concentratio
0
2
4
6
8
10 12 14 16 18 20 22 24
0
2000
4000
6000
8000
particle number concentratio
and between 8 – 20 nm with
thermodenuder.
The
shrinking
factor SF shows that the soot
thermodenuder. The Aitken mode split-up after the
heating in two peaks: at 80 nm (soot particles) and
at 20 nm. The size distributions show the highest
3
10
800
Diameter, D
p
with Thermodenuder
log
D
p
, cm
-3
2152
3464
5563
8955
1.442E4
0
2
4
6
8 10 12 14 16 18 20 22 24
hour of day
0
2
4
6
8
10 12 14 16 18 20 22 24
hour of day
30 nm shrinking factor SF
80 nm shrinking factor SF
0 64
0.68
0.72
SF
0.64
0.68
0.72
Monday - Thursday
Saturday
Sunday
or SF
fraction
(non-volatile)
has
a
maximum at 80 nm and a minimum
at 30 nm during the rush hour
at 20 nm. The size distributions show the highest
particle concentrations between 06:00 and 09:00
in the morning caused by vehicles (rush hour).
0
2
4
6
8
10 12 14 16 18 20 22 24
3
10
Particle D
100
d
N
/ dl
321.2
517.0
832.4
1337
0 40
0.44
0.48
0.52
0.56
0.60
0.64
Monday - Thursday
Saturday
Sunday
diameter shrinking factor
(N
non-volatile
/ N
ambient
)
0 40
0.44
0.48
0.52
0.56
0.60
diameter shrinking facto
(N
non-volatile
/ N
ambient
)
Back trajectory cluster analysis
at 30 nm during the rush hour.
0 2 4 6 8 10 12 14 16 18 20 22 24
hour of day
Comparison between particle concentration and other parameters
0 2 4 6 8 10 12 14 16 18 20 22 24
0.40
hour of day
0 2 4 6 8 10 12 14 16 18 20 22 24
0.40
hour of day
Back trajectory cluster analysis
with Thermodenuder
Comparison between particle concentration and other parameters
0
330
30
360
(a)
(b)
70
-60
-30
0
30
70
1
180
200
S
ster
16
18
20
22
with Thermodenuder
in μm
3
/cm
-3
spring
summer
R
2
= 0.8252
30
35
40
latile residuals
-³]
autumn
summer
winter
30
300
60
330
60
60
2
3
4
5
6
7
80
100
120
140
160
NO
W
SW
ectories in the clus
6
8
10
12
14
me (8-800 nm)
summer
autumn
winter
R
2
= 0.9066
15
20
25
centration of non-vol
8 - 800 nm [μm³/ cm
spring
Linear (spring)
Linear (summer)
90
240
120
270
3-8 nm
50
50
0
20
40
60
80
N
NO
W
NO
number of traje
0
500 1000 1500 2000 2500 3000 3500
0
2
4
6
particle volum
R
2
= 0.7335
R
2
= 0.7707
0
5
10
0.00
5.00
10.00
15.00
20.00
25.00
volume con
Linear (winter)
Linear (autumn)
150
180
210
38
8-20 nm
20-70 nm
70-200 nm
200-800 nm
800-2000 nm
2000-10000 nm
(c)
(d)
-60
-30
0
30
40
40
1
2
3
4
5
6
7
Cluster #
14000
16000
1
2
3
14000
16000
1
2
3
Particle
number
concentrations
mixed layer height in m
Particle volume and number The volume of non-volatile
Black Carbon [μg/m³]
6000
8000
10000
12000
/ dlog D
p
[cm
-3
]
3
4
5
6
7
6000
8000
10000
12000
N / dlog D
p
[cm
-3
]
3
4
5
6
7
depend on local wind direction. The
map characterize the measurement
site in Augsburg (red point).
concentrations depend on mixing
layer
height.
The
highest
concentrations occurred during winter
particle residuals correlate with
the optical Black Carbon (PM
2.5
)
measurements (R
2
= 0.9).
4
10
100
1000
0
2000
4000
dN
particle diameter, D
p
in nm
4
10
100
1000
0
2000
4000
dN
particle diameter, D
p
in nm
Ak ld
t
References
site in Augsburg (red point).
concentrations occurred during winter
and with low mixing layer heights.
measurements (R
0.9).
(e)
(f)
p
2500
3000
3500
4000
instable
NN in m
p,
p
0 65
0.70
0.75
0.80
ctor SF
ent
)
1
2
3
4
5
We acknowledge broad support by Prof. Jörg Matschullat (TU
Bergakademie Freiberg IOZ Germany)
Acknowledgements
Birmili W, Stratmann F, Wiedensohler A (1999) Design of a DMA-based Size Spectrometer for a large
Particle Size Range and Stable Operation,
Journal of Aerosol Science
, 30, pp. 549 – 553.
References
500
1000
1500
2000
2500
stable
height about
1
2
3
4
5
6
0.50
0.55
0.60
0.65
ameter shrinking fa
(N
non-volatile
/ N
ambie
6
7
Bergakademie Freiberg, IOZ, Germany).
Back trajectories were calculated on the NOAA ARL READY
Website
using
the
HYSPLIT
(Hybrid
Single-Particle
Lagrangian Integrated Trajectory) Model (Reference: Draxler,
R R and Rolph G D
2003 NOAA Air Resources
Particle Size Range and Stable Operation,
Journal of Aerosol Science
, 30, pp. 549
553.
Holle R, Happich M, Löwel H, Wichmann HE (2005) KORA – A Research Platform for Population Based
Health Research,
Gesundheitswesen, G7, Sonderheft 1
, S. 19 – 25.
Wehner B Philippin S Wiedensohler A (2002) Technical Note
Design and Calibration of a
Th
bktjti h thtth t hi
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
0
500
virtual potential temperature in °C
7
10
100
1000
0.40
0.45
dia
particle diameter, D
p
in nm
R. R. and Rolph, G. D., 2003, NOAA Air Resources
Laboratory, Silver Spring, MD, USA).
Wehner B, Philippin S, Wiedensohler A (2002) Technical Note – Design and Calibration of a
Thermodenuder with an Improved Heating Unit to Measure the size-dependent volatile Fraction of Aerosol
Particles,
Journal of Aerosol Science
, 33, pp. 1087 – 1093.
WHO (2004) Health Effects of Air Pollution Results from the WHO Project “Systematic Review of Health
The back trajectories show that the atmospheric
stratification is more important than pure geographical
air masses. Low mixing layer heights cause high particle
LibiItittf T hiR hPhi D t tA lG
Aspects of Air Pollution in Europe”,
World Health Organisation
, No. E83080, Geneva.
gy
g
gp
number concentrations.
Leibniz Institute for Tropospheric Research – Physics Department, Aerosol Group