in mosses has declined the most for lead (77%), followed by vanadium (55%), cadmium 74 (51%), chromium (43%), zinc (34%), nickel (33%), iron (27%), arsenic (21%, since 75 1995), mercury (14%, since 1995) and copper (11%). Between 2005 and 2010, the 76 decline ranged from 6% for copper to 36% for lead; for nitrogen the decline was 5%.

The NERC and CEH trademarks and logos ('the Trademarks') are registered trademarks of NERC in the UK and other countries, and may not be used without the prior written consent of the Trademark owner. As, and Cu. Cluster and Factor analysis with Varimax Rotation was applied to distinguish elements mainly of 20 anthropogenic origin from those predominantly originating from natural sources. Geographical distribution maps 21 of the elements over the sampled territory were constructed using GIS technology. The median values of the 22 elements in moss samples of Albania were high for Al, Cr, Ni, Fe and V and low for Cd, Cu and Zn compared to 23 the many other European countries, but generally were of a similar level as some of the neighbouring countries 24 such as Bulgaria, Croatia, Kosovo, Macedonia and Romania. This study was conducted in the framework of ICP 25Vegetation in order to provide a reliable assessment of air quality throughout Albania and to produce 26 information needed for better identification of contamination sources and improving the potential for assessing 27 environmental and health risks in Albania, associated with toxic metals. 28 29

The NERC and CEH trademarks and logos ('the Trademarks') are registered trademarks of NERC in the UK and other countries, and may not be used without the prior written consent of the Trademark owner.

(2010 -2014 survey). The geographical distribution maps of the elements over the sampled territory were constructed using GIS technology. The concentrations of Cr, Ni, Pb and Zn were higher than the respective median values of Europe, suggesting that the zones with heavy vehicular traffic and industries emission input are important emitters of these elements. Selected zones are highly polluted particularly by Cd, Pb, Hg and Ni. The statistical analyses revealed that a strong correlation exists between the Pb and Cd content in mosses and the degree of pollution in the studied sites were assessed.

The NERC and CEH trademarks and logos ('the Trademarks') are registered trademarks of NERC in the UK and other countries, and may not be used without the prior written consent of the Trademark owner. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 For analysing element input into ecosystems and associated risks due to atmospheric deposition, element concentrations in 51 moss provide complementary and time-integrated data at high spatial resolution every five years since 1990. The paper 52 reviews (1) minimum sample sizes needed for reliable, statistical estimation of mean values at four different spatial scales 53(European and national level as well as landscape-specific level covering Europe and single countries); (2) trends of heavy 54 metal (HM) and nitrogen (N) concentrations in moss in Europe (1990Europe ( -2010; (3) correlations between concentrations of HM in 55 moss and soil specimens collected across Norway (1990Norway ( -2010; and (4) canopy drip-induced site-specific variation of N 56 concentration in moss sampled in seven European countries . While the minimum sample sizes on the European 57 and national level were achieved without exception, for some ecological land classes and elements the coverage with 58 sampling sites should be improved. The decline in emission and subsequent atmospheric deposition of HM across Europe 59 has resulted in decreasing HM concentrations in moss between 1990 and 2010. In contrast, hardly any changes were 60 observed for N in moss between 2005, when N was included into the survey for the first time, and 2010. In Norway, both, the 61 moss and the soil survey data sets were correlated, indicating a decrease of HM concentrations in moss and soil. At the site 62 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 71other manufacturing industries and construction (As, Cd, Cr, Hg, Ni, Pb), electricity and heat production (e.g. Hg, Ni), road 72 transportation (Cu and Sb from brake wear, Pb from petrol, Zn from tires), petroleum refining (Ni, V), and phosphate 73 fertilisers in agricultural areas (Cd) (Harmens et al. 2011 a). N emissions and relateted deposition are due to technical 74 processes and agriculture. Pollutants which were emitted into and transported through the atmosphere finally come down at 75Earth´s surface as wet (rain, snow), occult (fog, mist, rime) or dry (gases, particles) deposition where they accumulate in 76 biota and sediments of terrestrial and subsequently of aquatic ecosystems. 78In Germany, less than 10 % of the HM load of aquatic environments is emitted from industries. More than 80 % of policyclic (Harmens et al. 2015). In contrast to measurements with tec...