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Atmospheric Environment 37 (2003) 671–691
A review of air pollution and atmospheric deposition dynamicsin southern Saxony, Germany, Central Europe
Frank Zimmermanna,*, Herbert Luxb, Willy Maenhautc, J .org Matschullata,Kirsten Plessowa, Friedrich Reuterb, Otto Wienhausb
a Interdisciplinary Environmental Research Centre, Freiberg University of Mining and Technology, Brennhausgasse 14,
D-09599 Freiberg, Germanyb Institut f .ur Pflanzenchemie und Holzchemie, Technische Universit .at Dresden, Pienner Stra�e 21, D–01 735 Tharandt, Germany
c Instituut voor Nucleaire Wetenschapen, Universiteit Gent, Proeftuinstraat 86, B–9000 Gent, Belgium
Received 29 May 2002; received in revised form 23 September 2002; accepted 4 October 2002
Abstract
This is the first comprehensive compilation of air pollution history in the Erzgebirge region. It presents selected data
sets from more than 20 years of continuous research, chosen after rigorous quality control. Gases and particulates, and
wet deposition are discussed in sequence. The gases include SO2, NOx, O3, and fluorine compounds. SO2-concentrations
declined from about 80 to 120 mgm3 until 1990 to 5–10 mg SO2m3 air today, while NOx shows little change, and O3
steadily increases as of 1990. Fluoride deposition decreased with SO2. Particle deposition is differentiated by sampling
methods and grain sizes, and their chemical composition. The total amount of aerosols has decreased in the past 12
years, and many trace constituents now show 10% of their previous concentrations. Precipitation is represented by wet
only, throughfall, fog and cloud water deposition, including major and minor chemical compounds. As with the gases,
S-compounds decreased considerably. While NO3-N-concentrations show a slight decline (from 13 to 10–11 kg ha�1 a�1
in throughfall deposition); no trend is visible for NH4-N. As of the mid-1990s, continuously lower base cation inputs
are being measured, and pH-values are on steady increase (now 4.8). The final synopsis rounds up the experience gained
from those valuable data sets and can be used for many regions worldwide.
r 2003 Elsevier Science Ltd. All rights reserved.
Keywords: Aerosol; Dry deposition; Bulk deposition; Atmospheric deposition trends; Time series; SO2 NOx; O3; Erzgebirge; Black
triangle
1. Introduction and regional air pollution history
Southern Saxony presents a highly diverse landscape
bordering the Czech Republic. The region features
undulating hills and mountains, with altitudes from a
little over 150m a.s.l. at the Elbe river valley to more
than 1000m at the Erzgebirge crest. Extensive forests,
agricultural land, and industries, often still related to the
great mining history of the area, make for a unique
checkerboard of diverse land-use patterns. Until re-
cently, southern Saxony was part of a larger region
including SW Poland (Silesia) and Northern Czech
Republic (Northern Bohemia), with the ugly nickname
‘‘Black Triangle’’. Fortunately, the last few years have
seen major improvements in air quality status and
although considerable work is still needed, people can
now refer to the region as a green triangle—acknowl-
edging the density of forests and rich semi-natural
landscapes.
One of the first local references on air pollution-
related environmental damage dates back to the late
17th century (Lehmann, 1699). In his chronicle ‘‘Histor-
ical scene of the peculiarities in the Meissen upper
AE International – Europe
*Corresponding author.
E-mail addresses: [email protected]
(F. Zimmermann), [email protected]
(J. Matschullat).
1352-2310/03/$ - see front matter r 2003 Elsevier Science Ltd. All rights reserved.
PII: S 1 3 5 2 - 2 3 1 0 ( 0 2 ) 0 0 8 2 9 - 4
Page 2
Erzgebirge’’, Lehmann described the environmental
impact of the Annaberg silver smelters. Many more
local examples exist and even back to Agricola (1557),
old depictions are available that demonstrate the
abundance and impact of late medieval ore dressing
and smelting facilities in the area. Later, a rapid
industrialisation led to rising emissions in the mid-19th
century. In those days, even more intense environmental
damage occurred. The newly established industrial
enterprises were almost exclusively built in river valleys
because of their high water demand. Thus, a whole chain
of dispersed industrial centres emerged causing atmo-
spheric pollution. Other emission centres grew in the
hard coal mining districts of Zwickau and Lugau-.Olsnitz as well as in the area around Chemnitz (Fig. 1).
The predominant spruce forest, itself a heritage from
earlier mining and smelting history, became most
seriously impaired by the industrial emissions. Environ-
mental damage could no longer be neglected and led to
the establishment of a special branch of forestry research
in the mid-19th century. A first survey by Schr .oter
(1907), entitled ‘‘The smoke-emitting sources in the
kingdom of Saxony and their influence on forestry’’ is
one witness for this period.
This type of air pollution, characterised by local
pollution sources, primarily situated in the valleys,
persisted almost unchanged over centuries (16th–19th
century), characteristic for the northern slope of the
Erzgebirge. Regional air pollution occurred only at the
transition from the northern slope to the hilly Erzge-
birge foreland in Saxony. There, zones of larger
pollution dispersal were found juxtaposed or even
partly superimposed. This gave rise to discussions
among forestry professionals, especially concerning
the question whether there was a connection between
the hoarfrost breakage calamities in the Erzgebirge
and the increasing number of condensation cores in
the air due to industrial waste gases from the NW-
Bohemian basin (D .obele, 1935; Heger, 1935, 1940;
Lampadius, 1941; Singer, 1916). ‘‘Modern’’ air pollution
became apparent after the second World War
with the installation of numerous coal power plants
and related industries both in the Bohemian basin and in
Saxony. In the 1950s, the relation between increasing
spruce decline phenomena and air pollution became
more and more apparent (Materna, 1956, 1962; Pelz,
1962).
Even though the Erzgebirge shares many meteorolo-
gical and climatic characteristics with other Central
European mountainous areas, the dispersion of emis-
sions in southern Saxony depends on local meteorolo-
gical particularities. In contrast to the northern slope,
extensive air pollution caused by specific local climatic
conditions occurred along the southern slope of the
Erzgebirge and its ridges (Flemming, 1964). Wind and
turbulence are the dominant meteorological factors in
Chemnitz
Dresden
Leipzig
Zittau Mountain
Eastern Erzgebirge
Central Erzgebirge
Western Erzgebirge
Elbe Sandstone Mountains
Northern Bohemia
Silesia
Fig. 1. Geographical position of the monitoring stations in the Erzgebirge (parts of Europe as an inset with Saxony in white).
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691672
Page 3
air pollution transfer. Comparatively stable air stratifi-
cation occurs under SE winds—this leads to a focussed
concentration of pollutants at a scale-height above
500m a.s.l. This stratification is reduced immediately
across the southern Erzgebirge escarpment due to
dynamic and thermal influences that allow for a large-
scale dispersal of industrial waste gases and dusts from
the NW-Bohemian basin. Temperature inversion is
another common phenomenon. The inversion layer is
lowest in winter and may be stable over several days.
This leads to intense smog phenomena in the Bohemian
basin. At the same time, the higher reaches of the
Erzgebirge are almost free of pollutants and display a
very high air quality. Sometimes, this ‘‘Bohemian fog’’
crosses the Erzgebirge ridge and it flows down the
Saxonian Erzgebirge, resulting in SO2-deposition peaks.
Thermal destabilisation of the atmospheric layers often
occurs on ridges and passes that then serve as pollutant
pathways in northerly direction. This destabilisation
occurs more often in summer. In spring and fall, the two
effects mix and thermal effects prevail in the mornings of
radiation-rich days. Local differences are more pro-
nounced in winter as compared to summer conditions
(Zimmermann et al., 1997).
1.1. Monitoring networks
1.1.1. Atmospheric gases
The extensive spruce decline phenomena in the areas
around Deutscheinsiedel and Markersbach (boundary
between the Elbe Sandstone Mountains and the eastern
Erzgebirge) initiated the establishment of a gas monitor-
ing network in the mid-1960s, using SO2-aspirators
(TCM method, modified after Herrmann, 1965). This
network was a joint effort by the Institute of Phyto-
chemistry and Wood Chemistry (Dresden University of
Technology, TUD), the Bezirkshygieneinspektionen
Chemnitz and Dresden (BHI), and the Meteorological
Service of the former GDR (MD). In the 1970s, SO2-
concentration records (half-hour values) were started by
MD and BHI, using the coulometric instruments CM 4
and CM 5 (Junkalor, Dessau).
After German re-unification, a more comprehensive
air pollution monitoring network was build-up in
Saxony (Table 1; Fig. 1), organised under the auspices
of the Regional Office for Environment and Geology
(LfUG). Today, forest ecosystem monitoring stations
exist at Carlsfeld and Fichtelberg in the western
Erzgebirge, eastern Erzgebirge at Schwartenberg
Table 1
Atmospheric gas and deposition monitoring stations in the Erzgebirge. Elevations in m above sea level
Station Owner Elevation Site characteristics Components Start yr End yr
Altenberg SLAF 750m Spruce forest Bulk, throughfall 2000
Annaberg LfUG 545m Urban, traffic SO2, NOx, O3 1988
Aue LfUG 348m Urban, traffic SO2, NOx, O3 1989
Bad Schandau SLAF 260m Beech forest, remote Bulk, throughfall 1998
B.arenstein LfUG 705m Urban SO2 1981 2001
Carlsfeld LfUG 896m Forest, remote SO2, O3 1991
Wet only, dust 1991
Cunnersdorf SLAF 440m Spruce forest Bulk, throughfall 1993
Fichtelberg LfUG 1214m Mountain, remote SO2, O3 1970
Klingenthal SLAF 840m Spruce forest Bulk, throughfall 1993
Lehnm .uhle UBA 525m Forest, remote SO2, NOx, O3 1993
Wet only 1993
L .uckendorf UBA 490m Forest, remote SO2, NOx, O3 1992
Marienberg LfUG Urban, background Wet only 1985
Mittelndorf LfUG 323m Rural SO2, NOx, O3 1995
Wet only, dust 1995
Oberb.arenburg TUD 735m Forest, remote SO2, NOx, O3 1992 1999
TUD, TUBAF Spruce forest Wet only, bulk, throughfall, fog, dust, aerosols 1984
Olbernhau LfUG 448m Urban, background SO2, NOx, O3 1991 2000
SLAF 720m Spruce forest Bulk, throughfall 1994
Schwartenberg LfUG 787m Mountain, remote SO2, NOx, O3 1998
Tharandt forest TUD 385m Forest, remote SO2, NOx, O3 1993
TUD, TUBAF Forest, remote Wet only, bulk, throughfall, dust, aerosols 1985
Zinnwald LfUG 877m Mountain, remote SO2, NOx, O3 1971
Wet only, dust 1985
LfUG: Regional Office for Environment and Geology; SLAF: Saxonian Regional Office for Forestry; TUBAF: Freiberg University of
Mining and Technology; TUD: Technical University of Dresden; UBA: German Environmental Protection Agency.
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 673
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(Central Erzgebirge), and at Zinnwald. The central
Erzgebirge lacks a representative monitoring station.
The station at B.arenstein continued to operate until late
2001, although with a slightly different programme. In
addition, data from Olbernhau and Annaberg are
available (monitoring within the town boundaries). This
governmental network is supplemented by the station at
Oberb.arenburg (OBB), eastern Erzgebirge, initiated by
TUD and today jointly operated with the Interdisci-
plinary Environmental Research Centre of Freiberg
University of Mining and Technology (TUBAF). It was
based on measuring equipment (Horiba APSA 350E,
Horiba APOA 350E, Ecophysics CLD 700), comparable
with the governmental network. The Lehnm .uhle station,
operated by the Environmental Protection Agency
(UBA), complements this arrangement. Other stations,
monitoring forested areas in southern Saxony are
Mittelndorf (LfUG) in the ‘‘Elbe sandstone mountains’’;
L .uckendorf (UBA) in the Zittau Mountains; and
Tharandt Forest (TUD); see Table 1 and Fig. 1.
1.1.2. Atmospheric deposition
The relevance of atmospheric deposition for under-
standing potential air pollution effects led to the parallel
establishment of a related monitoring network. In the
1970s and early 1980s, element inputs were measured at
single sites, and only at irregular intervals in the
Erzgebirge. Noteworthy are the works of Pankert and
Panning (1975), and unpublished data in the Eastern
Erzgebirge and by Flemming and Gei�ler (1985) in
Neunzehnhain in the central Erzgebirge. In the early
1980s, ‘‘forest decline’’ and ‘‘acid precipitation’’ led to
the design of monitoring stations for atmospheric
deposition at many places in Europe, including the
former GDR. This included the network of the
Meteorological Service (1973) and monitoring stations
of the Forestry College in Eberswalde (lowlands) and
the Institute of Phytochemistry in Tharandt (highlands).
The MD monitoring network started in 1985 with
bulk samplers (custom made). From 1989 onwards, wet-
only samplers were used exclusively (ANTAS, Institute
of Energetics, Leipzig), and as of 1998/1999 wet only
samplers by Eigenbrodt. In the Erzgebirge, the measure-
ments began at Marienberg in the central Erzgebirge
and at Zinnwald in the eastern Erzgebirge. The network
was extended in the early 1990s by the station at
Carlsfeld, western Erzgebirge, and later by one near
Mittelndorf. Likewise, wet-only samplers (Eigenbrodt)
were used by UBA at L .uckendorf since 1992, and at
Lehnm .uhle as of 1993. Starting 1984/1985, monitoring
stations to assess atmospheric deposition on forest
ecosystems were exclusively operated by the TUD, in
the upper eastern Erzgebirge (OBB), and in the
Tharandt Forest. Starting 1990, yet another station
was established in Carlsfeld. The equipment consisted of
automatically operated wet-only samplers (ANTAS,
Institute of Energetics, Leipzig) and bulk samplers
(custom-made) for total deposition.
Within the framework of the EU-Level II programme,
the network was considerably extended by the Regional
Office for Forestry in Graupa (SLAF). This was
supplemented by one station each in the western
Erzgebirge near Klingenthal, in the eastern Erzgebirge
near Olbernhau and in the transitional area to the Elbe
sandstone mountains near Cunnersdorf. Since 2000, a
new site was established near Altenberg, eastern
Erzgebirge. These data sets are supplemented by series
started in 1983, focussing on the input of heavy metals
and fluorides. Again, TUD initiated monitoring efforts
located along the southern border of Saxony, from the
Central Erzgebirge up to the Zittau Mountains (Table 1,
Fig. 1). This work was soon complemented by detailed
dry (low volume samples, Derenda, Berlin) and total
deposition (custom made bulk samplers) research with a
very broad array of elements (Matschullat et al., 1995;
Matschullat and Bozau, 1996; Matschullat and Kritzer,
1997).
2. Gaseous atmospheric compounds
The three major gaseous pollutants are sulphur
dioxide (SO2), nitrogen oxides (NOx: NO, NO2) and
ozone (O3).
2.1. Sulphur dioxide
In the Erzgebirge, SO2 is the prominent atmospheric
pollutant in respect to its emission history, its ambient
concentration, and its effects on ecosystems. The gas has
an atmospheric lifetime of several days. With an average
wind speed of 4m s�1, the gas will be transported over
some hundred kilometres prior to deposition or oxida-
tion to sulphate. Most of the anthropogenic sulphur is
released in the atmosphere by fossil fuel combustion.
The large power plants in Southern Saxony and North-
ern Bohemia are exclusively based on the combustion of
lignite with partly high sulphur content from pyrite
(FeS2). The average sulphur content of Saxonian lignite
is 1,7% (Leipzig basin; Just et al., 1986) and 0.5–1%
(Lusatia; LAUBAG, pers. comm.), and in the Bohemian
basin from 0.5 to 5.75% (Sulovsky, pers. comm.). Until
1990, most regional power plants worked without
desulphurisation and dust removal. Following the Ger-
man re-unification, many factories and power plants
were shut down or modernised. This lead to emission
reductions of about 92% in Saxony (baseline 1989;
Fig. 2).
2.1.1. Air concentrations—historical data
The first regional data on atmospheric SO2-concen-
trations were presented by D.assler and Stein (1968,
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691674
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1972) and by Auermann and Kneuer (1977). Table 2
shows the annual SO2 mean concentrations by
Auermann and Kneuer from 1968 to 1972. For
comparison, the five-year mean value (1966–1971) by
D.assler and Stein (1972) for the area around R .ubenau
(Central Erzgebirge) is 60 and 90mgm�3 for Rehefeld
(Eastern Erzgebirge). These early measurements
point to a shift from the initial impact area around
Deutscheinsiedel (mainly due to the chemical works
Zalusi near Litvinov) in a westward direction to a
new area around Reitzenhain, J .ohstadt. This shift is a
result of distant emission sources that temporally
coincide with the construction of new power plants
(e.g. Tusimice with a 200m high smokestack). Starting
1970, following the start-up of the industrial unit
VRESOVA near Karlovy Vary, a distinct SO2-concen-
tration increase occurred around Oberwiesenthal, Fich-
telberg (Table 2).
These results were confirmed by measurements from
the 1960s and 1970s. Major centres of air pollution
occurred around Deutscheinsiedel/Deutschneudorf in
the Einsiedler saddle, and on the Czech side, Nova Ves v
horach and Mnisek, as well as in an area of the Central
Erzgebirge starting from B.arenstein and Veiperty in the
Czech Republic, via J .ohstadt, Satzung, Hirtstein,
Reitzenhain, K .uhnhaide to R .ubenau, with annual
means exceeding 120mg SO2m�3. The area of Kahleberg
in the Eastern Erzgebirge was slightly less polluted, with
annual means around 80 mgm�3. A first air pollution
map of the area was delivered by Liebold and Drechsler
(1991; Fig. 3).
Oberb.arenburg registered the input of noxious sub-
stances, and discontinuously measured SO2-concentra-
tions from November 1986 to October 1987. In this
period, the mean SO2-concentration was 55 mgm�3
(Zinnwald: 80 mgm�3). The half-hour maxima reached
950 mgm�3 in November 1986. Table 3 shows the OBB
monthly means in comparison with data from Zinnwald
(restricted to data recorded simultaneously at both
stations). At OBB, located leeward from the eastern
slope of mount Kahleberg, the SO2-concentrations were
considerably lower than at Zinnwald, most pronounced
when diurnal values exceeded 100 mgm�3 at Zinnwald.
During periods of a low air mass exchange, however,
higher SO2-concentrations were measured at OBB. The
results of the SO2-monitoring network, established after
1990 are summarised in Table 4.
Table 2
Annual SO2-means (mgm�3) for various Erzgebirge sites from
1968 to 1972 (Auermann and Kneuer, 1977)
Location 1968 1969 1970 1971 1972 1968–1972
Western Erzgebirge
Oberwiesenthal 11 60 60 80 53
Central Erzgebirge
J .ohstadt 43 85 103 98 82
Pockau 58 70 132 128 90 96
Reitzenhain 42 92 135 87 89
Eastern Erzgebirge
C.ammerswalde 75 70 57 67
Deutscheinsiedel 58 63 94 98 62 81
Sayda 78 60 100 88 80 83
0
500
1000
1500
2000
2500
1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999year
SO
2-em
issi
on
[kt
a-1
]
Fig. 2. SO2-emissions in Saxony from 1986 to 1999 (LfUG, 1997b, 2000).
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 675
Page 6
Until 1996, there was no significant SO2-decrease in
the upper Erzgebirge as compared to other areas of
Saxony. At these higher altitudes, episodes of very
high pollutant concentrations still occurred, mainly
due to SO2-emissions from the N-Bohemian industrial
region. The Central Erzgebirge, followed by its
eastern part, was most severely affected by air pollution
whereas the Auersberg region in the Western Erzgebirge
received comparatively low pollution levels. Extremely
high SO2-concentrations of several 100 mgm�3 have
been observed in the Erzgebirge, when the res-
pective measurement was made downwind from an
emission trail of a power station, typically extending
a few kilometres. Concentration maxima are de-
pendent on wind dynamics and thus, considerable
horizontal concentration gradients may occur (Beyrich
et al., 1998).
From 1996 to 2000, the SO2-concentrations declined
drastically, following the modernising of the N-Bohe-
mian power plants (Table 4). In the last few years,
annual SO2-means reached levels between 5 and
10mgm�3. A similar trend was observed for peak
concentrations. The 98th-percentile of SO2 reached
70 mgm�3 in the year 2000 (LfUG, 2001).
2.1.2. Mobile measurements
From 1983 to 1996, a mobile SO2-monitoring network
operated in southern Saxony (Reuter and Wienhaus,
1995). Measurements were made at 40 selected locations
in the central and eastern parts of the Erzgebirge, in the
Elbe sandstone mountains, and the Zittau Mountains.
Short interval measurements took place discontinuously
during the growing season from May to September,
weekly and randomly regarding wind direction and
weather situation. Forest/crop field boundaries and,
partly, forest sites (remote from settlements) were
selected as locations of the measuring points. The
DESAGA gas sampler served as a direct measuring
instrument. SO2 is absorbed, using sodium tetra-
chloromercurate (II) (TCM), and colorimetrically de-
termined using pararosaniline. Based on mean values,
results from the mobile equipment (Table 5) were
only partly (Eastern Erzgebirge) comparable with those
from stationary measurements (Table 4), due to the
discontinuous character of the mobile records. These
mobile measurements underlined the relevance of
distinct source areas as derived through a differentiated
analysis of wind directions (Wienhaus et al., 1994;
Table 6):
1. The highest SO2-concentrations in the Central
and Eastern Erzgebirge and the adjoining Elbe
sandstone mountains occurred with SE winds. The
influx from the N-Bohemian lignite mining centre
was obvious.
2. SW winds are of relevance for the same area. Its
mountainous relief led to an air pollution impact,
specific for the industrial emissions from N-Bohemia.
SO2-concentration (mg m-3) 0.055 0.065 0.085 0.090 0.100 0.120
Fig. 3. Annual average SO2 concentrations (mgm�3) in Southern Saxony (Liebold and Drechsler, 1991; data from the 1980s).
Table 3
Monthly SO2-means (mgm�3), at Oberb.arenburg, OBB, and
Zinnwald, ZW (1986/1987)
OBB ZW
November 1986 88 101
December 1986 71 69
April 1987 48 101
May 1987 37 78
August 1987 46 52
September 1987 53 118
October 1987 47 45
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691676
Page 7
3. NE winds influenced the Zittau Mountains, and
transported emissions from power stations of eastern
Saxony and Silesia in Poland.
4. With the prevailing westerlies, low SO2-concentra-
tions were recorded at all sites. Their mean values
were below 20 mg SO2m�3.
Air pollutants from N-Bohemia played an important
role until 1996. Their impact depended on the occur-
rence of heavily loaded air masses from SE, on inverted
atmospheric conditions, on season and on relief
(mountain incisions). One of these events was measured
in 1992 by the mobile Lidar system ARGOS (Advance
Remote Gaseous Oxides Sensor) of GKSS research
centre Geesthacht (Goers, 1994; Reuter and Wienhaus,
1995; Fig. 4). The SO2 concentration profile, measured
in a southerly air flow from Schwartenberg to Einsiedler
saddle (Erzgebirge ridge) revealed SO2-loaded air masses
that move in a relatively thin layer of 200–300m across
the Erzgebirge crest. This may explain the temporarily
low SO2-concentrations measured on the mountains,
while at the same time very high concentrations were
measured at lower locations and in the vicinity of cuts
and hollows.
2.2. Nitrogen oxides
Nitrogen oxides (NOx), consisting of nitric oxide
(NO) and nitrogen dioxide (NO2), are mostly emitted as
nitric oxide (> 90% of total) via anthropogenic
combustion processes. NOx-emissions are high in and
around cities und much lower in rural and remote areas
like the Erzgebirge. Table 7 shows mean seasonal NO2-
data for different locations in Southern Saxony from
Table 5
SO2 concentrations (mgm�3) in Southern Saxony from mobile measurements 1993–1996
1993 1994 1995 1996
N Mean Max N Mean Max N Mean Max N Mean Max
Central Erzgebirge 82 44 238 107 80 1322 118 35 234 119 28 209
Schwartenberg 64 73 321 70 40 204 49 70 380 62 26 123
Eastern Erzgebirge 84 36 494 92 47 426 61 40 212 81 26 328
Elbe sandstone mts., western Elbe river 117 36 207 164 47 540 144 32 540 138 25 130
Elbe sandstone mts., eastern Elbe river 204 30 155 209 35 205 160 24 241 197 16 64
Zittau mountains 76 36 161 107 30 239 96 30 606 80 14 82
Table 4
Annual SO2-means (mgm�3) in the Erzgebirge from 1991–1995, and 1996–2000
Western Erzgebirge Central Erzgebirge Eastern Erzgebirge
Year Carlsfeld Fichtelberg B.arenstein Annaberg Olbernhau Zinnwald Oberb.arenburg Lehnm .uhle Tharandt forest
1991 34 44 107 123 95 61 51a n.d. n.d.
1992 15 24 70 80 73 37 59 n.d. n.d.
1993 24 28 86 78 78 38 50 n.d. n.d.
1994 21 31 66 68 67 43 38 32 36
1995 13 31 55 51 42 36 35 36 26
1991–1995 21 32 77 80 71 43 49 n.d. n.d.
1996 n.d. 37 73 59 54 37 30 35 37
1997 11 20 31 21 28 29 25 18 24
1998 6 10 13 10 15 18 15 11 10
1999 4 7 7 6 9 7 7 7 8
2000 4 6 8 7 n.d. 8 n.d. 6 8
1996–2000 6 16 26 21 26 20 n.d. 15 17
aAltenberg; n.d.: no data.
Table 6
Total SO2-means in each respective year, compared with the
individual SO2-means from selected wind direction sectors (all
data in mgm�3)
Year Total SE SW NW NE
1993 38 61 30 20 31
1994 45 80 38 17 38
1995 34 48 40 16 21
1996 22 30 21 11 16
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 677
Page 8
1992 to 2001. No long-term trend was visible in the
10-year period. Seasonal changes occured, with higher
concentrations during winter and considerably lower
ones during the vegetation period. In winter, heating
power stations act as additional emission sources, also
generating SO2-maxima. The NOx-concentrations in
forest areas of Southern Saxony were not phytotoxic.
The threshold in the growing season is given with
60mgm�3 (WHO, 1987), or with an annual mean of
30mgm�3 (Ashmore and Wilson, 1994). Thus, NOx
may be interpreted as a ‘‘leaf fertiliser’’. With the
prevailing low concentrations (NO 1–2 mgm�3, NO2
10–15mgm�3), the risk for forest ecosystems is very
limited. The ecotoxicological relevance is more relevant
in the character of nitric oxides as precursor substances
for O3-formation in the atmosphere.
2.3. Ozone
Different from SO2 and NOx, high O3-concentrations
were not only detected close to sources, but also in rural
and remote areas (Table 8). Since 1988, the forest areas
of Southern Saxony are exposed to increasing levels of
photooxidants, supporting O3-formation over the sum-
mer months (mean values in summers 1981–1987 at
Fichtelberg ca. 57mgm�3, from 1988 above 80mgm�3;
unpublished data LfUG). Depending on meteorological
conditions (radiation, general weather situation), fluc-
tuations occur within individual years. Despite the
relatively weak solar radiation and the cool summer of
1996, higher monthly O3-values were measured than in
1994 and 1995, which were both distinguished by record
high temperatures and long periods of strong solar
Table 7
Mean seasonal NO2-concentrations (mgm�3) at forest monitoring stations of Southern Saxony. Data from 1992 to 2001
Periode Zinnwald Schwartenberg Oberb.arenburg Lehnm .uhle Tharandt forest
Winter 17 16 15 15 13
Summer 11 10 11 7 9
Table 8
Mean summer O3-concentrations (mgm�3) in the Erzgebirge. Data from remote stations
Station 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 2001
Carlsfeld — — 64 62 77 80 76 86 85 88 85 82
Fichtelberg 92 81 69 84 — 83 86 94 95 99 96 94
Schwartenberg — — — — — — — — 80 88 85 82
Zinnwald — — — — — 79 75 90 83 91 88 83
Oberb.arenburg — — 62 55 83 77 73 90 84 — — —
Lehnm .uhle — — — — 70 74 72 72 68 73 74 —
Fig. 4. SO2 zenith scan by LIDAR (adapted from Goers, 1994). The profile was measured at location Schwartenberg (No. 10 in
Fig. 1).
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691678
Page 9
radiation. So far, the highest O3-concentrations oc-
curred in the summer of 1999 with a slight decrease in
subsequent years. The critical O3-level for forests of
50mgm�3 during the growing season (April–September;
7-h-value; UN-ECE (1988)-Critical Level has been
exceeded at all stations for several years (Table 8).
While the measured O3-concentrations are insufficient to
cause direct damage on the relatively ozone-resistant
spruce, more sensitive tree species such as beech, birch,
oak, and pine, may receive acute damage during
radiation-rich high-summer periods. This risk is under-
pinned by the new Critical Level of Fuhrer and
Achermann (1994): AOT40-value of 10 ppmh >40ppb
ozone. At Oberb.arenburg, the AOT40 accounted for
18.7 ppmh in 1994, 17.9 ppmh in 1995, 12.4 ppmh in
1996, 21.2 ppmh in 1997, and 18.5 ppmh in 1998. Ozone
thus presents the highest damaging potential of all gases
for the Erzgebirge forest ecosystems.
2.4. HF and fluorine
In the N-Bohemian industrial area, the SO2:HF ratio
was 50:1. With emissions of e.g., 500,000 t SO2 per year
(1996) about 10,000 t HF were emitted annually.
Consequently, the high SO2-loads of the past, in winds
blowing from southerly directions, were accompanied by
high F�-levels. The classical noxious substance ‘‘fluor-
ine’’ embodies a damage-enhancing factor and most
probably fluoride contributed to the forest damage of
Southern Saxony (Wienhaus et al., 1992; Reuter et al.,
1997). This became evident in the winter of 1995/1996
where major calamities with financial losses of ca.
50Mio. Euro occurred in the upper Erzgebirge (Zim-
mermann et al., 1997). Declining SO2-concentrations led
to declining F�-inputs over the past few years (Table 9).
From 1997 onwards, the concentrations no longer
reached phytotoxic levels. It can be concluded from
the decrease of SO2-emissions until today (2002), that
this fact holds true for the following years.
As shown above, F�-inputs played a major role in
explaining forest decline phenomena in the Erzgebirge.
Phytotoxic concentrations were reached both in the gas
phase and the particulate phase, due to high F�-
concentrations in regional lignite. Their contribution
to the extreme forest damage encountered in the winter
of 1995/1996 could be shown by needle analysis (Fig. 5).
Analogous to the SO2-decline, recent air chemistry
results demonstrate a distinct decrease of HF. Both air
and needle concentrations are now below phytotoxic
values.
3. Particulate atmospheric compounds
Over the past years, atmospheric emissions in Central
Europe decreased considerably (e.g. Matschullat et al.,
1995, 2000; UBA, 1998). The most prominent examples
are the declines of sulphur from point sources and of
lead (Pb) from leaded fuels. While S-emissions declined
simultaneously in Western and Central Europe and
parts of North America (e.g. Dillon et al., 1988; UBA,
1998), the decrease of Pb-deposition was first observed
in North America due to the earlier introduction of
unleaded fuel (e.g. Eldred and Cahill, 1994; Mielke,
1997) and became apparent in Europe only after a
10-year delay (Schulte and Blum, 1997). Trends of other
aerosol components are just as important, however, and
sites with unusually high pollutant loading deserve
special attention.
3.1. Aerosol concentration (low volume samplers)
To assess the atmospheric aerosol concentration in
the area, two aerosol samplers were deployed from 1992
to 1994 at the stations Zinnwald (ZI) and the Malter
reservoir (MA) (Kritzer, 1995; Matschullat et al., 1995;
Matschullat and Bozau, 1996; Matschullat and Kritzer,
1997). Comparable bulk deposition results between the
stations Oberb.arenburg (OBB) and Zinnwald triggered
the decision to combine forces of the two projects. The
results have already been discussed in detail in this
journal (Matschullat et al., 2000). A multi-element
survey was carried out by Proton-induced X-ray
spectrometry (PIXE), Instrumental Neutron Activation
Analysis (INAA), and Graphite-Furnace Atomic Ab-
sorption Spectrometry (GF-AAS) for samples from
1992–1994 and 1996–1997 (Al, As, Ba, Br, Ca, Cl, Cr,
Cu, Fe, Ga, Ge, I, In, K, Mg, Mn, Na, Ni, P, Pb, S, Se,
Si, Sr, Ti, V, Zn). The results support the efficiency of
emission control in Central Europe. The concentrations
of many anthropogenic constituents in both bulk
deposition and in aerosols today have declined con-
siderably. In the formerly highly polluted Eastern
Erzgebirge, particle deposition can now be addressed
Table 9
HF air concentration (mgm�3) in Deutschneudorf and Zinnwald in 1997 and 1998. Data from LfUG, 1997c, 1999
Site 02/1997 11/1997 12/1997 01/1998 02/1998 03/1998
Deutschneudorf 0.09 0.06 0.07 0.05 0.04 —
Zinnwald 0.29 0.08 0.05 0.07 0.06 0.01
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 679
Page 10
as comparable to rural areas without major local or
regional influences.
3.2. Dust analysis (Bergerhoff method)
Dust sedimentation measurements were performed
since 1983 (Reuter et al., 1995). Locations remote from
settlements and along forest-field boundaries were
chosen. Measurements took place from May to October
(growing season) with monthly sampling intervals.
Tables 10 and 11 present selected results for fluoride
and calcium. As of 1991, fluoride inputs strongly
declined, but reached the old level once again in 1994.
A completely different situation can be observed
regarding calcium deposition. Calcium inputs vary
between 3.5 and 6.9 kg ha�1 a�1 without spatial differ-
entiation. The highest means were obtained from the
Central and Eastern Erzgebirge, the Elbe sandstone
mountains and the Zittau Mountains. A steady decline
could be observed over the past years. While fluoride
deposition will continue to decrease, calcium input is
now influenced by the irregular liming activities to
combat further forest soil acidification.
4. Precipitation and fog water
A differentiation is made between occult (fog and
cloud water) and wet (rain and snow) deposition. Wet
deposition is particularly effective for atmospheric self-
cleaning. It includes rainout: within-cloud scavenging
where aerosol-type air pollutants are incorporated in
cloud droplets that can be transported over long
distances—up to 1000 km—and finally precipitate as
rain, and washout: below-cloud scavenging of dust and
gases often close to an emitter. Under moderate climate
conditions, rainfall occurs to about 10% of the total
time. Between precipitation events, gases and dusts are
deposited only in dry form on surfaces. This deposition
is slower than by rain, depending on particle size and
shape (turbulence-enhancing) and on surface conditions.
Deposition is highest on conifers and open water
surfaces. As air contaminants are efficiently withheld
by the interception of canopy, forests are highly
susceptible to atmospheric pollutants (acids, trace
metals), and excess amounts or disproportional nutrient
input (N, S, Ca). Rainwater chemistry changes, after
passing a canopy, result from four different processes
(Dambrine et al., 1998): (1) relative evaporative con-
centration of precipitation by the canopy; (2) older dry
deposition washed off during the precipitation event; (3)
leaching of organic and mineral compounds from leaf or
needle surfaces, and (4) absorption of organic and
mineral elements. The most important canopy transfor-
mations are direct assimilation of nutrients like N by the
foliage or the phyllosphere microflora, H+ buffering,
and leaching of basic cation, e.g. K+.
Throughfall deposition thus represents the sum total
of wet deposition, dry deposition of aerosols, cloud
droplet deposition on leaf surfaces, and canopy interac-
tion. The relative proportions of these processes vary
largely with location. At lower sites it may rain for only
0 10 20 30 40 50 60
Fluoride content in mg kg-1 d.m. d.m. = dry matter
Deutscheinsiedel
Rübenau
Satzung
Reitzenhain
Zschirnstein
Holzhau
Kahleberg
Zittau Mountains
growing season winter 95/96
Fig. 5. Fluoride contents in spruce needles 1995/1996 (needle age class 1995).
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691680
Page 11
7% of the time, so that dry deposition of S and N may
make a significant contribution. Here, droplet deposi-
tion plays a minor role. Since wind speeds also increase
with altitude, the efficiency of droplet impact on
vegetation surfaces also increases. At higher elevation
sites, the additional input by droplet deposition leads to
an increase in water and element input. This is clearly
visible with the throughfall data in Fig. 6, while the wet
deposition does not change with altitude. The through-
fall deposition indicates a strong increase in S-deposition
with elevation, leading to roughly a doubling of
throughfall S-deposition at the upper site compared to
the lowest. In contrast, wet deposition of SO4-S does not
increase significantly with elevation.
A minor concentration enhancement was observed at
the ridge site, mainly caused by the seeder–feeder effect
(Fowler et al., 1989). The high elevation forests receive
more precipitation than the forests at low elevation sites.
For the time period 1985–2000, an interception loss of
47% was calculated for the lower site, while only 20%
were measured at the upper site. However, this cannot
be attributed only to the greater evaporation at the
lower site. The rapid increase of fog events at the
altitude of the inversion layer (700m a.s.l.; Goldberg
et al., 1998) contribute to the increase in water input on
forest ecosystems. Throughfall measurements at OBB
and at P .obelbach (Bozau, 1995; Matschullat and Bozau,
1996) in May 1992–April 1994 showed significant
differences in the chemical composition of throughfall
precipitation (Fig. 7). While both sites are located at
similar altitudes (735m a.s.l. vs. 690–760m a.s.l.), the
P .obelbach site was more influenced by the so-called
‘‘Bohemian fog’’, leading to higher SO4-S and F�-
inputs.
4.1. Wet-only deposition
The ion concentration of rainwater is an air pollution
indicator. Therefore, changes in the precipitation
chemistry indicate a change in emission pattern. A
detailed presentation of the results of measurement by
the MD monitoring network for the periods 1985–1989
and 1990–1994 was given by M .oller and Lux (1992) and
by LfUG (1994, 1995). Table 12 shows the results of
measurement obtained from monitoring stations in the
Erzgebirge (kg ha�1 y�1). Additional results from wet-
only samplers at OBB and Tharandt Forest for 1984–
1989 and 1990–1994 were published by Lux (1993,
1995). Again, the strong decrease of basic cations, and
some of the anions is visible after 1990 (largely due to
the implementation of modern filter technology in
Saxonian power plants). The additional decrease of
Table 10
Fluoride input in kg ha�1 a�1 (open field) in the Erzgebirge
Location Until 1990 1991 1992 1993 1994 1995 1996 1997 1998
J .ohstadta Central Erzgebirge 2.5 — — 1.96 2.0 1.25 1.12 0.95 0.66
Satzung, Central Erzgebirge 2.1 0.47 1.97 1.89 2.6 1.85 1.79 1.20 0.88
Heidersdorf, Eastern Erzgebirge near Schwartenberg 2.0 0.78 1.47 1.07 1.8 1.48 1.34 0.95 0.77
Liebenau, Eastern Erzgebirge 1.5 0.66 0.73 1.52 2.8 1.56 2.1 0.99 0.95
aMeasuring point at B.arenstein up to 1990.
Table 11
Calcium input in kg ha�1 a�1 (open field) in the Erzgebirge
Standort Until 1990 1991 1992 1993 1994 1995 1996
J .ohstadta, Central Erzgebirge 16.9 — — 3.95 4.95 6.16 7.9
Satzung, Central Erzgebirge 13.6 4.98 3.76 6.35 4.43 6.9 6.2
Heidersdorf, Eastern Erzgebirge near Schwartenberg 18.8 5.56 5.05 4.26 3.46 5.48 5.7
Liebenau, Eastern Erzgebirge 14.2 6.34 6.48 5.65 6.86 6.35 4.7
aMeasuring point at B.arenstein up to 1990.
0
100
200
300
400
500
600
700
0 200 400 600 800 1000
elevation (m a.s.l.)
SO
42--
dep
osi
tio
n (
mo
l ha
-1)
wet deposition
throughfall
Fig. 6. SO42�-deposition (mol ha�1) in the year 2000 at four
different elevations in the E-Erzgebirge.
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 681
Page 12
S-emission from power plants in the Bohemian basin
occurred after 1995 (Tables 12 and 13).
Within the scope of the SANA project (SANitation of
the Atmosphere above the new German states/Sanierung
der Atmosph .are .uber den Neuen Bundesl .andern), a wet-
only sampler (ANTAS) was installed for daily
sampling at Oberb.arenburg. Table 13 presents results
for 1992–1995 (Br .uggemann and Rolle, 1998), 1996–
1998 (Zimmermann et al., 1998) and the year 2000
(Zimmermann, unpubl.).
4.2. Throughfall deposition
Results from direct canopy throughfall measurements
show a very high variability, both in respect to
precipitation amounts and to the chemical composition
of the water droplets. This variability requires the
parallel use of different samplers. At each of the SLAF,
TUD, and TUBAF monitoring sites, 15 inexpensive
bulk deposition samplers were placed. While throughfall
deposition is relatively easy to measure, the related data
interpretation is a lot more complex due to the many
processes that co-occur in the canopy. The longest data
series were generated from sites operated by TUD at
Oberb.arenburg and in the Tharandt Forest (Table 14).
Results for the periods 1984–1989 and 1990–1994 have
been published by Lux (1993, 1995). All data are
differentiated by the respective stand age. In 1993,
SLAF commenced its measurements at monitoring sites
that are integrated in the Level II EU-Programme
(SLAF, 1999; Table 15).
4.2.1. Spatial variability
An E–W gradient of SO42�-deposition became appar-
ent, related to the position of emission sources in the
Eger graben, the orographic setting, and the meteor-
ological conditions (dominating SW-winds). Both the
stations Klingenthal (near Vogtland) and Carlsfeld
(Western Erzgebirge) register significantly lower SO4-S,
N, F�, and acid input as compared to forests in the
Central, and Eastern Erzgebirge. The higher precipita-
tion amounts in the Western Erzgebirge slightly cover
this effect. But even these western regions receive acid
and N-inputs that exceed the critical loads. The highest
inputs were measured in the Central Erzgebirge,
enhanced during fog-rich periods at higher altitudes.
The monitoring site Olbernhau is a hotspot, where dry
SO2-S-deposition and SO4-S-fog deposition led to a
throughfall input of 77 kg ha�1 a�1 during the hydro-
logical year 1996. In the same period, 40–50 kg SO4-
S ha�1 were measured on sites in the Eastern Erzgebirge
(Zimmermann et al., 1998). Further east (Elbe sandstone
mountains), lower annual precipitation amounts and
longer longitudinal distances to emission sources yield
even lower inputs as compared with the Central
Erzgebirge, but higher than those encountered in the
Western Erzgebirge.
The described East–West gradient is further differ-
entiated by topography and altitude. Lower precipita-
tion at lower altitudes and longer distances to the
emission sources in the Bohemian basin, as well as the
negligible input via fog and cloud water led to lower
inputs. This is primarily true for SO4-S and F�, and
Fig. 7. Throughfall deposition (kg ha�1 a�1) on two Norway Spruce stands in the Eastern Erzgebirge between 05/1992 and 04/1994.
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691682
Page 13
Table 12
Wet only deposition at several stations in the Erzgebirge (kg ha�1 yr�1)
Marienberg Zinnwald Carlsfeld
1985–1989 1990–1994 1995–1999 1985–1989 1990–1994 1995–1999 1992–1994 1995–1999
pH 4.36 4.26 4.46 4.29 4.28 4.50 4.35 4.54
Na 6.2 2 3.5 6.9 2.7 3.3 2.4 3.5
K 3 0.9 0.8 3 0.7 0.9 0.7 0.6
Mg 2.6 0.8 0.6 2.5 0.8 0.6 0.7 0.5
Ca 18 5.6 2.9 18 4.7 3.0 2.7 2.0
NH4�N 12 6.7 8.5 10 5.6 7.7 5.9 8.4
NO3�N 8.5 5.1 6.0 7.8 5.1 5.2 5.3 6.4
SO4�S 35 14.3 10.4 32 16 10.3 10.5 8.9
Cl 14.5 4.9 5.8 12.5 5.6 5.3 4.4 4.4
Table 13
Wet only deposition at Oberb.arenburg from 1992 to 2000 (kg ha�1 yr�1)
Oberb.arenburg
1992 1993 1994 1995 1996 1997 1998 2000
Precipitation (mm) 1088 1087 983 1306 946 962 1176 996
pH 4.5 4.3 4.3 4.3 4.4 4.6 4.6 4.8
Conductivity (mS cm–1) 37 37 34 30 24 23 21 17
Na 6.5 4.6 3.2 3.5 2.6 3.7 2.7 3.8
K 2.3 1.6 1.35 0.8 1.6 0.5 0.5 0.7
Mg 0.7 0.6 0.6 0.7 1.0 1.0 0.6 0.6
Ca 5.3 3.6 2.7 2.3 3.9 2.8 3.1 2.6
NH4�N 8.7 6.8 5.6 7.5 7.3 6.9 6.5 6.0
NO3�N 5.9 6 5.1 6.5 5.7 5.2 5.6 4.9
SO4�S 15 13.7 11.5 13.9 8.1 7.4 7.7 5.8
Cl 5.4 4.9 5.9 6.8 3.0 5.0 4.4 5.8
Table 14
Throughfall deposition mean values (kg ha�1 a�1) for different periods at OBB, Tharandt forest and Carlsfeld. Stand age based on the
year 2002
Years P(mm) SO4�S Cl NO3�N F NH4�N K Na Ca Mg H
(a) Oberb .arenburg, spruce pole wood (47 yr)
84–89 817 104.5 23.8 15.8 3.6 16.4 31.6 12 65.3 8.4 2.49
90–94 749 65 13 13.1 2.2 9.6 25.8 8 25.4 4.1 1.56
95–98 848 37.2 12.2 11.4 1.3 9.1 25.3 7.85 16.1 5.5 1.04
99–01 728 21 11.7 11 0.46 10.6 19.1 6.3 10.4 2.2 0.4
(b) Oberb .arenburg, spruce mature timber (97 yr)
92–94 846 65.5 18.5 20.2 2.1 13.4 20.7 12.3 26 6 1.69
95–97 847 39.9 17.4 17.7 1.5 14.6 18.2 11.1 19.8 7.6 1.12
(c) Tharandt forest, spruce mature timber (112 yr)
84–89 428 149.9 23.7 20.4 4.1 21.6 25.3 11 104.9 10.9 2.08
90–94 398 59.5 12.8 12.3 1.4 13.2 18.2 6.3 26.3 3.9 1.37
95–98 482 29.1 11.4 10.0 0.8 14.6 17.3 6.7 12 2.7 0.65
99–01 413 12.1 9.5 10.1 0.36 13.4 13.7 4.4 5.7 1.4 0.12
(d) Carlsfeld, spruce pole wood (48 yr)
92–94 876 44.5 11.6 8.3 0.56 8.1 21.5 6.5 14.8 2.6 1.11
95–97 1065 24.3 10.6 7.7 0.36 7.9 19.8 7.3 9.6 2.5 0.85
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 683
Page 14
becomes apparent with data from the Tharandt forest,
gathered after the emission reduction measures within
Saxony came into effect. The N-inputs deliver an even
more differentiated picture. Local agricultural sources
led to higher NH4-N-inputs in the lower-lying areas
while the high altitudes show low NH4-N. As a
consequence of traffic related NOx-emissions and their
enrichment beneath the inversion layers (Zimmermann
and Wienhaus, 2000), the lower altitudes receive higher
NO3-N inputs (when evaluating throughfall deposition
data it needs to be emphasised that only the lower input
level of total N is represented because of the non-
quantifiable amount of plant uptake).
Fog and cloud water deposition have to be taken into
account as a third type of atmospheric deposition at
higher altitudes. While an increase of SO4, F�, and acid
inputs via ‘‘Bohemian fog’’ is characteristic on the
Erzgebirge ridge (Bridges et al., 2002), cloud water is of
high relevance for the input of NO3, Na+, and Cl� at
higher altitudes. Fog water measurements from OBB
support this hypothesis, jointly with increased through-
fall deposition of these ions from old spruce stands that
more efficiently comb out fog than younger spruce
stands.
4.2.2. Time-related variability
Analogous to the emission development, three major
time sections can be differentiated with throughfall
deposition data: prior to 1990 with high air pollution,
the years from 1990 to 1996 parallel to emission
reduction measures in Saxony, and as of 1997 with a
similar emission reduction programme for the large
Bohemian power plants.
Sulphate-sulphur: About 100 kg SO4-S ha�1 a�1 were
deposited prior to 1990 at higher altitudes of the
Erzgebirge, and about 150 kg SO4-S ha�1 a�1 at lower
altitudes. In the following years, this load decreased to
60–65 kg SO4-S ha�1 a�1. Following the event period of
1995/1996, partly with loads of 80 kg SO4-S ha�1,
emission reduction measures in Northern Bohemia
decreased to ca. 35–30 kg ha�1 a�1 in 1997/1998. In
2001, about 20 kg ha�1 a�1 were measured at higher
altitudes, and at lower altitudes loads of 10–
12 kg ha�1 a�1. This reduction of 80–90% (based on
the mid-1980s) can be seen as a major success story of
environmental management. A similar reduction is
visible with fluoride and acid inputs.
Nitrogen: Based on the data from the mid-1980s, both
NO3-N and NH4-N deposition showed a certain decline
(shut-down of outdated industrial units, reduction in
agricultural production). In the 1990s, a minor decrease
of NO3-N is measurable despite a strong growth in
automobile numbers. At the same time, NH4-N input
stagnates both on high and lower altitudes at 10–
15 kgNH4-Nha�1 a�1. Thus N-input remains a serious
threat for the stability of spruce ecosystems in the
Erzgebirge.
Base cations: The input of base cations in throughfall
deposition results from two different sources, total
deposition (wet + dry + interception), and internal
leaching. The latter is the dominating mechanism for
K+. The leaching efficiency depends on ambient SO2-
concentrations (Slovik et al., 1996) and on precipitation,
because K+ is highly mobile and present as an
electrolyte within the plant. The SO2-decrease conse-
quently led to a reduction of K+ input. Observed
variations were simply related to precipitation varia-
bility. Different from K+, both Ca2+ and Mg2+ are
bound to plant tissue and are being exchanged via ion
exchange processes against protons. Lower pH-values
thus lead to higher leaching rates. Thus, the drastic
reduction of Ca2+ and Mg2+ deposition is not only
related to a reduction in dust emissions but to the
increase of pH-values in precipitation. During 1996 and
1997, widespread liming of forest soils with ground
dolomite momentarily led to higher Ca2+ and Mg2+
deposition. Sodium is not easily leached. The reduction
of Na+ and Cl� inputs as of 1990 is probably related to
a shift from salt rich coal to salt poor varieties in
regional power plants.
Table 15
Annual element fluxes at the Saxonian SLAF level II survey sites (kg ha�1 yr�1)
Klingenthal Olbernhau Cunnersdorf
840m a.s.l., Norway spruce 720m a.s.l., Norway spruce 440m a.s.l., Norway spruce
1994 1995 1996 1997 1995 1996 1997 1994 1995 1996 1997
H+ 1.51 1.6 2.48 0.89 2.07 4.05 1.77 1.77 1.51 1.67 0.77
K 17.3 24 19 14.8 34.4 31.2 14.7 14.6 18.7 16.2 11.0
Ca 9.9 12.2 10.2 13.0 17.4 18.9 12.6 11.1 11.6 10.3 8.7
Mg 1.4 2.5 1.5 3.5 3.7 4.5 3.3 1.9 2.9 2.1 1.9
NTotal 20.3 23.8 22.4 18.9 28.0 46.7 35.4 27.6 26.3 31.4 25.2
SO4�S 35 39.4 37.0 24.4 66.7 77.1 33.3 46.1 44.2 41.9 24.9
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691684
Page 15
Regional variability with time: In Germany, a dense
network of monitoring stations for atmospheric gases
and depositions exists since the early 1980s. To
demonstrate major differences in air pollution between
eastern and western parts of Germany, throughfall
deposition data of SO4-S, Ca, NO3-N, and NH4-N at
OBB are compared with those from Idar-Oberstein
(Fig. 8). Idar-Oberstein is situated in the Hunsr .uck
forest (Rhineland-Palatinate), about 500 km west of the
Erzgebirge, close to the French border. Like Ober-
b.arenburg, the Idar-Oberstein site features a high
elevation forest (660m a.s.l.) dominated by spruce (130
years old). The striking feature at Oberb.arenburg are the
S and Ca2+ reductions of 80% and 85%, respectively,
since 1984. In W-Europe, air pollution prevention
measures were carried out earlier than in former E-
Europe. Moreover, the use of lignite was not that
common in the West. Therefore, significantly lower
deposition rates were measured in 1984 at Idar-
Oberstein. Deposition rates of 33 kg ha�1 a�1 for S,
and 16 kg ha�1 a�1 for Ca2+, respectively, were about
3–4-times lower than at OBB. These atmospheric inputs
were still high enough; however, to cause severe tree
damages in W-Europe. From 1984 to 2000, the S and
Ca2+-deposition rates decreased by 50–40% at Idar-
Oberstein. Current values at OBB and Idar-Oberstein
are in the same order of magnitude. Sulphur deposition
(21 kg ha�1 a�1) at OBB still exceeds that at Idar-
Oberstein (16 kg ha�1 a�1). This difference may be due
to a local household consumption of lignite, primarily in
the winter season.
Nitrogen deposition rates display a different story.
Compared to S and Ca2+, the deposition varied in a
narrow range only. From 1984 to 1994, the total N-
deposition declined from 32 to 21 kg ha�1 a�1 at OBB,
while Idar-Oberstein shows no changes. As of 1995,
both sites display similarly constant values for NO3-N
and a continuous increase for NH4-N. A decade after
German re-unification, atmospheric deposition rates
become uniform, too.
4.3. Fog and cloud water
The relevance of fog and cloud water for the
hydrological budget of forest ecosystems has been
known for a long time. In particular at sites above
600m a.s.l., part of the precipitation input and thus also
of the element input originates from fog and cloud
scavenging. The ecotoxicological relevance of occult
deposition results from the drastically elevated element
concentrations in fog droplets. The concentration of
pollutants like SO2 and NOx in fog and cloud water may
exceed that in rain water by two orders of magnitude.
Under extreme conditions, the formation of strong
acids like H2SO4 und HNO3 may lead to pH-values
below 2.0 (Sigg et al., 1987). While such low pH-values
have not been observed in German forests, evaporation
of intercepted fog water leads to more acidic solutions
on the leaf surfaces of plants (Frevert and Klemm,
1984).
4.3.1. Erzgebirge
First measurements of the elemental composition of
fog water began in the 1950s in the Eastern Erzgebirge
(Mrose, 1961) and were resumed in the 1980s (Zier,
1991). More detailed studies of the chemical composi-
tion of fog and cloud water and their additional water
input in the Eastern Erzgebirge followed in the late
1990s (Zimmermann and Zimmermann, 1999, 2001,
2002). Time series from weather stations in the
Erzgebirge show a significant dependence between the
number of days with fog, and altitude. The average
annual number of days with fog occurrence varies
between 50 at elevations of 500m a.s.l. and up to 300 at
the Fichtelberg (1214m a.s.l.). In the Eastern Erzge-
birge, the annual number of fog days amounts to 200 at
900m a.s.l. (Zinnwald). The input of fog and cloud
water in spruce stands reaches 20mm in the
Tharandt forest, 100mm at higher altitudes, and
200mm at the Erzgebirge crest (Flemming, 1993a, b).
Wind exposed sites at the ridge may well receive up to
500mmyr�1. Model calculations for the Fichtelberg
area yielded an additional 1000mmyr�1 (Zimmermann
and Zimmermann, 2002). Mean volume-weighted ionic
Idar-Oberstein / Hunsrück
0
20
40
60
80
100
120
1984-1989 1990-1994 1995-1998 1999-2000
kg*h
a-1*a
-1
SO4-S
Ca
NO3-N
NH4-N
Oberbärenburg / Erzgebirge
0
20
40
60
80
100
120
1984-1989 1990-1994 1995-1998 1999-2001
kg*h
a-1*a
-1
SO4-S
Ca
NO3-N
NH4-N
Fig. 8. Throughfall deposition (kg ha�1 a�1) between 1984 and
2001 for a forest site in Rhineland-Palatinate* (Idar-Oberstein,
660m a.s.l.) and in Saxony (OBB, 735m a.s.l.). *source:
Forstliche Landesversuchsanstalt Rheinland-Pfalz.
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 685
Page 16
concentrations of fog and cloud water samples are
presented in Table 16 (Zimmermann and Zimmermann,
2001).
At both experimental sites, ZW and OBB, ionic
concentrations were up to 25 times higher in fog and
cloud water than in wet deposition. The median pH-
value in fog was 4.0 (minimum pH 3.3). The chemical
composition of fog differs between sites. The ridge is
strongly influenced by the so-called ‘‘Bohemian Fog’’.
Dominant species in the fog water were SO42� and NH4
+.
Compared to rain, relatively high F�-concentrations
were observed (41 meq l�1, OBB rain/snow 1.1meq F� l�1
in the year 2000). In contrast, fog water composition at
the upper sites were dominated by NO32� (988meq l�1),
and high concentrations of Na+ and Cl�. This may be
caused by the dominant front fog at this site and
enrichment of traffic emissions in the inversion layer.
For the ridge sites in the Eastern Erzgebirge, a mean
additional water input by fog deposition of 165mm was
calculated with a deposition model (Pahl, 1996). For a
40 year old spruce stand, 60mm of additional water
input through fog deposition were calculated by a
canopy water balance model. One hundred millimetres
were calculated for a 100 years old spruce stand at the
same site. Obviously, fog deposition depends on stand
height and slope exposition. Table 17 summarises the
S- and N-input via wet, fog and throughfall deposition
in the hydrological year 2000 at OBB for the 40 years old
spruce stand (Zimmermann and Zimmermann, 2001). In
the year 2000, the mean value of SO2-concentration at
OBB was 8mgm�3. With an estimated deposition
velocity Vd of 0.8 cm s�1 for the younger spruce stand,
a dry deposition of 10 kg SO2-S ha�1 yr�1 can be
calculated. The calculated sum of wet, fog and dry
S-deposition agreed quite well with the measured
S-deposition by throughfall. For N, the calculation led
to an overestimation, which might be due to direct
absorption and biological uptake of N-compounds in
the canopy.
4.3.2. Comparative data
Only few long-term data sets for fog water composi-
tion in Germany are available. At Mt. Brocken (Harz
mountains, 1142m a.s.l.), routine sampling of cloud
water has been executed since 1991 (M .oller et al., 1996;
Acker et al., 1998). Only recently, a fog study was
conducted at the research site Waldstein (Fichtelgebirge,
786m a.s.l.; Wrzesinsky and Klemm, 2000). Table 18
lists the results of these studies for the years 1995–1997.
At all sites, the mean ionic concentrations are in the
same order of magnitude or fit in the range of maximum
and minimum values, respectively. Fog water composi-
tion was dominated by SO42�, NO3
2� and NH4+. These
ions contribute to about 70–90% to the total ionic
charge. Some differences are obvious between the sites.
Sulphate and NH4+-concentrations are somewhat higher
for the Erzgebirge and Waldstein than for the Brocken
site (Tables 16 and 18). This may be due to the fact that
these sampling sites are more often influenced by air
masses from Eastern and Central Europe with higher
SO2 content. Mt. Brocken cloud water chemistry shows
a considerable variation. While the data sets from 1995
and 1996 (Acker et al., 1998) correspond well, a 2-and
6-fold lower ionic concentrations was measured in 1997
(Plessow et al., 2001). The data from 1997 represent only
a short period of time of Mt. Brocken cloud water
chemistry, whereas the samples of 1995 and 1996 were
collected from April until October. Thus, the results
underline the large variations which occur in fog and
cloud water compositions depending on liquid water
content, formation of fog water, surface interactions and
air mass origin.
5. Synopsis
Based on the experience of the past decades it
becomes obvious that a complex problem such as air
pollution and atmospheric deposition requires a broad
systems approach in order to (a) properly understand
the underlying processes, (b) deliver a sound interpreta-
tion of data and observed phenomena, and (c) to work
at finding sustainable solutions for the encountered
problems. The following paragraphs sum up the
experience.
Table 16
Mean volume-weighted ionic concentrations [meq l�1] of fog
and cloud water at the sites Zinnwald (877m a.s.l.) and OBB
(735m a.s.l.). Values rounded for clarity
Site Zinnwald Zinnwald Oberb.arenburg
Time
period
December 1997–
May 1998
October 1998–
April 1999
October 1999–
May 2000
pH 4.0 4.0 3.8
SO42� 560 570 440
NO3� 180 200 990
NH4+ 560 630 640
Na+ 52 26 388
Cl� 48 27 393
Table 17
Deposition of S and N-compounds at OBB for the hydrological
year 2000 (kg ha�1 yr�1)
Wet Fog Throughfall
P (mm) 1085 45 878
SO4�S 5.9 3.2 19.1
NO3�N 5.0 6.3 11.0
NH4�N 6.9 4.1 11.4
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691686
Page 17
5.1. Gases
5.1.1. Sulphur dioxide
Until 1990, SO2-concentrations in forested areas of
the Erzgebirge were between 80 and 120 mgm�3. This
concentration declined to 30–40 mgm�3 in the mid-
1990s. Further emission reductions led to a continuing
reduction over the last 5 yr. Today, the annual average
mean concentration is 5–10 mg SO2m�3 air. These
concentrations do not show phytotoxic effects. Even
short-time concentration peaks of several-hundred
micrograms of SO2 do not exceed the detoxification
capacity of an SO2-sensitive tree species like spruce
(Slovik et al., 1992).
5.1.2. Nitrogen oxides
During the 1990s, NO2-concentrations revealed little
change at higher altitudes of the Erzgebirge. The annual
means were 10–15 mg NO2m�3 air. The phytotoxic
potential of NO2 is smaller than that of SO2 und O3.
No direct risk for forest ecosystems should be expected
from the encountered concentrations. A more important
aspect is the contribution of nitrogen oxides as O3-
precursor gases and their role as N-fertiliser in the N-
limited Erzgebirge forests. In more remote areas, NO
can be detected in small concentrations only. Average
concentrations are 1–2 mgm�3. Under inversion condi-
tions and with long-distance transport from the North-
ern Bohemian basin, elevated concentrations may be
encountered (Zimmermann and Wienhaus, 2000). The
prevailing low concentrations and the low deposition
velocity leads to a very limited risk for forest ecosystems.
5.1.3. Ozone
Different from the situation in the 1990s at lower
altitudes, O3-concentrations continuously increased at
higher Erzgebirge elevations. While lower and middle
altitudes show annual average concentrations of 50–
60mg O3m�3, averages of 70–80 mg O3m
�3 are typical
for the higher altitudes. A slight decrease is noticeable in
the last 2 yr (2000–2001). Emission reduction of the
precursors NOx and VOC led to a decrease of O3 peak
concentrations, and short-time peaks hardly exceed the
threshold of 180 mgm�3. At the same time, the frequency
of elevated concentrations (100–120 mgm�3) increased,
however, and the number of O3-destroying situations
(via NO) has decreased. Therefore, the changes are not
reflected in the average concentrations. Thus phytotoxic
thresholds, like AOT40, are being exceeded at all
stations and in each year. Ozone thus presents the
highest damaging potential of all gases for the Erzge-
birge forest ecosystems.
5.1.4. Hydrogen fluoride and fluoride dusts
As shown above, F�-inputs played a major role in
explaining forest decline phenomena in the Erzgebirge.
Phytotoxic concentrations were reached both in the gas
phase and the particulate phase, due to high F�-
concentrations in regional lignite. Their contribution
to the extreme forest damage encountered in the winter
of 1995/1996 could be shown by needle analysis.
Analogous to the SO2-decline, recent air chemistry
results demonstrate a distinct decrease of HF. Both air
and needle concentrations are now below phytotoxic
values.
5.2. Aerosol concentrations and deposition
In general, the bulk of air pollutants is being washed
from the atmosphere as wet deposition or deposited on
vegetation surfaces as dry or interception deposition.
Thus, the measurement of both open field and canopy
throughfall deposition reveal valuable data to assess the
development of atmospheric pollution.
5.2.1. Sulphate
Parallel to the SO2-decrease in air, SO4-S-inputs have
diminished both in open field and throughfall deposi-
tion. Extremely high SO4-S inputs of 30–35 kg ha�1 a�1
were measured in the field during 1985–1989. In the
1980s, the total input in pure spruce stands of ca.
100 kg ha�1 (80–120 kg ha�1) of SO4-S was caused by the
filter effect of the forests. In the mid-1990s, about 10 kg
SO4-S ha�1 a�1 were imported via wet deposition,
and 40–50 kg ha�1 a�1 via throughfall. Today, open
field deposition yields 5–7 kg ha�1 a�1 and through-
fall deposition ca. 20 kg ha�1 a�1 at higher altitudes,
10–12 kg ha�1 a�1 at lower altitudes. Higher fog density
and frequencies as well as wind speeds lead to increasing
loads with altitude.
5.2.2. Protons
The decreasing trend in S-deposition is accompanied
by a significant increase of pH-values in precipitation.
Table 18
Fog and cloud water chemistry (meq l�1) at different mountainsites in Germany
Brocken Waldstein
Time period 1995* 1996* 1997** 1997***
N 1340 2049 60 56
pH 3.8 4.0 4.3 4.3
SO42� 320 304 125 497
NO3� 364 347 122 481
NH4+ 468 454 198 669
Na+ 117 121 23 65
Cl� 110 118 18 54
*Acker et al. (1998); **Plessow et al. (2001); ***Wrzesinsky and
Klemm (2000).
F. Zimmermann et al. / Atmospheric Environment 37 (2003) 671–691 687
Page 18
The first determinations in the 1980s delivered
average open field values of pH 4.3, and in throughfall
pH 3.5. Today, open field precipitation shows pH-values
of 4.8 and in throughfall 4.4 (higher altitudes) and
4.6 (lower altitudes), a noteworthy reduction in H+-
deposition.
5.2.3. Nitrogen
Minor changes are being observed for N-inputs.
While a slight decline can be seen for NO3-N in
throughfall deposition from 13 kg ha�1 a�1 in the early
1990s to 10–11 kg ha�1 a�1 at the end of the decade
(open field 5–6 kg ha�1 a�1), no such trend is visible for
NH4-N. The respective values are 6–8 kg in open field an
11–15 kg ha�1 a�1 in throughfall deposition.
5.2.4. Base cations
Corresponding to the drastic reduction of dust
emissions after 1990 and the increased pH-values in
precipitation, continuously lower base cation inputs are
being measured in throughfall deposition.
5.2.5. Acid input and eutrophication
Despite the good news above, the total acidic input,
related to sulphur and nitrogen deposition still remains
above the critical loads, tolerable for a sustainable
development of the ecosystem (LfUG, 2001). This is
similarly true for the eutrophying N-loads. Particularly
threatened are nutrient poor forest soils at higher
altitudes of the Erzgebirge.
Acknowledgements
It goes without saying that such a review—although
backed with many of our own data—could not be
compiled and discussed without the numerous direct and
indirect contributions of many colleagues that have or
still do dedicate themselves to research in this area of
Central Europe. We highly appreciate their comments
and support and wish to thank every one of them. Two
anonymous referees and the editor of this journal have
spent a great deal of their time critically reviewing the
first version of this paper. We are grateful for their very
constructive criticism that has significantly improved the
clarity of this paper. And last but not least, we wish to
acknowledge the continuous financial support of several
donor agencies that enable us to pursue our contribution
for further improvements in air quality status in Europe.
Current funding of BMBF under AFO 2000 is gratefully
acknowledged. A special Thank you is extended to
Dr. Harald Kohlstock from Freiberg University for his
substantial support in upgrading the technical infra-
structure at Oberb.arenburg.
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