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Atmospheric Environment 37 (2003) 671–691 A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe Frank Zimmermann a, *, Herbert Lux b , Willy Maenhaut c ,J . org Matschullat a , Kirsten Plessow a , Friedrich Reuter b , Otto Wienhaus b a Interdisciplinary Environmental Research Centre, Freiberg University of Mining and Technology, Brennhausgasse 14, D-09599 Freiberg, Germany b Institut f . ur Pflanzenchemie und Holzchemie, Technische Universit . at Dresden, Pienner Strae 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 SO 2 , NO x ,O 3 , and fluorine compounds. SO 2 -concentrations declined from about 80 to 120 mgm 3 until 1990 to 5–10 mg SO 2 m 3 air today, while NO x shows little change, and O 3 steadily increases as of 1990. Fluoride deposition decreased with SO 2 . 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 NO 3 -N-concentrations show a slight decline (from 13 to 10–11 kg ha 1 a 1 in throughfall deposition); no trend is visible for NH 4 -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; SO 2 NO x ;O 3 ; 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 150 m a.s.l. at the Elbe river valley to more than 1000 m 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:S1352-2310(02)00829-4
21

A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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Page 1: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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

Page 4: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

(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

Page 5: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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

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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

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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

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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

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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

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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

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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

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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

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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: A review of air pollution and atmospheric deposition dynamics in southern Saxony, Germany, Central Europe

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

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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

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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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