ࡱ> 5@xbjbj224XXE/P4p3Z1111111$5R81)%%%13 .-.-.-%81.-%1.- .-N-/0 0\4#+/9143<p3/,8~,8080$.-!K11D( -( Environmental isotope studies in Croatia Ines Krajcar Broni Rudjer Boakovi Institute, Department of Experimental Physics Bijeni ka 54, HR-10000 Zagreb, Croatia In Radiocarbon and Tritium Laboratory of the Rudjer Boakovi Institute in Zagreb, Croatia, isotopes are applied in various types of studies: environmental, geochronological, arhaeological, hydrological, etc. Radiocarbon (14C) and tritium (3H) data measured in the Laboratory are often combined with the stable isotope (2H, 13C, 18O) data. In this paper we would like to present an overview of the most important results of environmental isotope studies performed in our Laboratory. Most of our studies have been performed in the karst area of Dinaric Mountains, and specifically at the Plitvice Lakes National Park system, about 150 km south from Zagreb. Isotope composition (2H, 18O, 3H) of precipitation Monthly samples of precipitation have been collected at two stations in the continental regions of Croatia and Slovenia, namely at Zagreb and Ljubljana, respectively. The stations are included in the GNIP network (Global Network of Isotopes in Precipitation) and have long-term isotopic records, since 1976 and 1981, respectively (IAEA 2005, Krajcar Broni et al. 1998). In the period 2000  2003 the network was extended to six additional meteorological stations along the Adriatic coast (Krajcar Broni et al. 2004, Horvatin i et al. 2005). The largest seasonal variations were observed at both continental stations (~130 ), and they can be attributed to the largest temperature variations at these stations. The differences between minimal and maximal values decrease in a south-east direction. The corelation between 2H and 18O is good for all stations, and both slope and intercept of the regression line decrease in the south-east direction. Annual weighted mean d-excess values vary between 9 in Zagreb and 14 in Dubrovnik. Good corelation between mean monthly air temperature and monthly d18O was obtained for all stations. The highest slope was obtained for the high-altitude station Zavi~an (0.370 /C), followed by ~0.30 /C for the continental stations. The the slope was the smallest for the south-Adriatic stations having the highest mean annual temperatures. Tritium activity in monthly precipitation at all sampling stations for the observation period 2001 2003 shows seasonal variations that are more pronounced at the continental and north-Adriatic stations. The 3H activity in precipitation decreases along the Adriatic coast from north-west to south-east. Since the mean temperature increases in the same direction, the decrease of 3H activity may be due to the influence of increased sea-water evaporation. 14C in the atmosphere Atmospheric co2 has been collected on a monthly basis in Zagreb and Plitvice since 1984 and 2003, respectively. Seasonal variations in D14C have been observed at both locations. The mean annual 14C activities in Zagreb were decreasing after the maximum in 1960-ties and approached the natural pre-bomb activities (Krajcar Broni et al. 1998). During the last 3 years the mean 14C activity D14C remains about 300 . The atmospheric 14C activity in the region for period 1950  1985 was reconstructed by measuring 14C activities of individual tree rings from the spruce tree grown at the Plitvice Lakes area (Kozak et al. 1989). A good agreement with the general atmospheric 14C curve of the Northern Hemisphere was observed. Isotopes (2H, 18O, 3H) in karst springs Stable isotope composition of several karst springs in the Plitvice Lakes area was determined seasonally in period 1983 1985 (Horvatin i et al. 1986) and again in 2003  2004, and it was compared with the stable isotope composition of precipitation. Annual variations in precipitation (~130 ) are much higher than those in karst springs (<10 ). The springs are also characterized by a very constant temperature and chemical compositions, and all these facts suggest a thorough mixing of water in the karst aquifers. Tritium activities in spring waters were also measured on monthly bases for several years, and the mean residence time was determined by applying the exponential model. The MRT is very short, ranging between 1 and 4 years on the average (Krajcar Broni et al. 1986). However, extreme meteorological conditions may change the MRT calculated by the exponential model. After extremely dry summer and fall of 1983, the older water with higher tritium content appeared at the springs and MRT was longer, between 4 and 8 years. After abundant winter precipitation, very low tritium activities (not much different from the winter precipitation) were measured in spring 1984. Isotope composition (13C, 14C) of dissolved inorganic carbon (DIC) Carbon isotope composition (d13C, 14C activity) of dissolved inorganic carbon (DIC) in water in the Plitvice Lakes system was measured in the period 1984  2002 at several locations along the water course of the Korana River. The mean values of d13C for DIC increase from  12.70 in springs to 90 in the surface waters (Fig. 1). The increase in d13C for DIC along the water flow is the combined result of CO2 degassing and carbon isotope exchange between atmospheric CO2 and DIC in the water (Srdo  et al. 1986a). Fig. 1. d13C in DIC in spring and surface waters of the Plitvice Lakes system. Isotope composition of carbonate sediments Various types of secondary carbonates (lake sediments, tufa, speleothem) precipitate from karst waters as the results of the same chemical process, but under different prevailing environmental conditions. d13C and d18O of tufa from Holocene and Pleistocene (as determined by the 14C dating) from the Plitvice Lakes system (having continental climate) and from the Krka River system (having Mediterranean type of climate) are compared in Fig. 2. The range of d13C values is the same for all samples, from 100 to 60 . There is no statistical difference between the d13C values either between the tufa from the same location but different time periods or between the tufa from different locations and the same period. This indicates that conditions for tufa precipitation were similar during each period and for both areas (Horvatin i et al. 2003). The d18O of tufa ranges from 110 to 60 , and two groups are noticeable. The Holocene and Pleistocene data sets from the Plitvice and Krka areas are the same only for the same location, while they are not the same for the same period and different locations, because of different type of climate. The d18O signature of tufa from Krka River is on average 1.70 (old tufa) and 1.80 (Holocene) higher than d18O of tufa from the Plitvice Lakes. The difference may be explained by a different d18O composition in waters from which tufa is formed and/or different mean yearly temperatures. Both of these factors are indicative for the different climate of the regions and both give rise to more negative d18O values at Plitvice Lakes. Mean d13C values for the lake sediments taken from the 12 m long sediment cores from two lakes at the Plitvice Lakes area [(8.60.1)0 and (8.90.2)0 for Lake KozjaPRTzH  ( - K s  ǿDZٗقyٗuqmmmhqUhNh>Eh)&hd|CJh)&hd|CJH*h)&hd|CJaJh)&hd|CJH*aJ hw/]h)& hw/]h,#o hw/]hd| hw/]hw/]hw/]hw/]H* hw/]h5 h)&h(*h,#o h)&hd| h)&hd8h)&hCK5CJ aJ h)&hd85CJ aJ *RT|F H 3 4 h |gd^L$a$gd,#oI$Eƀa$gd^L$ & F 7e^e`a$gdL)$a$gdd8gdd8$a$gdd8xx   % 2 3 4 I J K M O P R S h   , = > [ k `JT\ 帬ykh)&h^LPJmHnHuhNmHnHuh$SmHnHuh)&h,#omHnHuh>Eh,#omHnHuh,#omHnHuh)&h^LmHnHuh)&mHnHuhChd|5H*hChd|5CJaJhChd|5CJH*aJhChd|5 h)&hChd8hqUh,#o* #7WH ZǹǹӰ󞎀wwwwnhmHnHuh,#omHnHuh)&h^LaJmHnHuh)&h^LH*aJmHnHu#h)&h^LOJQJaJmHnHuhE7mHnHuh)&hNaJmHnHuh)&hNmHnHuhNmHnHuh)&h^LH*mHnHuh)&mHnHuh)&h^LmHnHu+ ,Ptx`¶ꭡvlh]UhUQh$Sh)&h7H*h)&h7OJQJhh)&h7@H*h)&h7;@ h)&h7hCh 5hChd|5hChd|5H*h)&hNmHnHuh^LmHnHuh>Eh>EmHnHuh>Eh>EH*mHnHuh>Eh^LmHnHuh)&h^LH*mHnHuh)&h^LmHnHuhNmHnHu(*JNSghiѻqqchChd|5H*mHsHhChd|5CJaJmHsH"hChd|5CJH*aJmHsHhChd|5mHsH h)&h h>Eh h>Eh$S h>Eh>Eh>Eh>EH* h~h~ h~hh$Sh hH*hh7h)&h7OJQJh)&h7H* h)&h7&*$$$))))9*oc $$Ifa$gdC@kd+$$Ifl"+# t644 la $$Ifa$gdKl$a$gdI$ & F 7@0`0a$gdL)$a$gd~$ & F 7e^e`a$gdL)$a$gdL) 4Zp~BPzY [ ?!r!&":""n$r$$$$$$$$$$%&&&& &&(&b&n&p&&'''''''''ùϯϨޝމިި~ނzhChKl h)&hI h#H* h)&h#h)&h#H*h)&h#OJQJ h#h#hChd|5H*hChd|5CJhChd|5CJH*hChd|5 h)&h~h# h>Eh$S h>Ehs?hNhs?h$Sh~0'''' ( ((8(D(H(N(P(R(T(Z(z(|((((r)t)))))))))))8*:*;*g*h*o**********2+3+4+,꿸次ꑍh* h)&hruhy hChd|5hwGhruH*hwGhruOJQJhrujhzU h)&he&hIh)&hI6h)&hIH*h)&hIH*h)&hIOJQJhKl h)&hIhCh$S h)&h#29*:*;*g*5+6UYYYYYu$$If^a$gdz $$Ifa$gd7$a$gd7$a$gde&$ & F 7e^e`a$gdL)$a$gdI>kdX,$$Ifl"+# t644 la ,,,, ,,,,,,,,,,,,"-b-t-v-------....(.H.....߱{{{nd[h)&hIPJh)&hIH*PJh)&hIOJPJQJ h)&hIh>EhIH*h>EhIOJQJ h>EhI h>Eh>E h>Eh@ h>Ehy hy h@h@mHnHuh@h@H*mHnHuh@h@OJQJmHnHu h@hy h@h@h@h@H*h@h@OJQJ#.01111112141b1h1t1~1113V3X3`3b3f3*4,404444R55x6z6~66666668R>RrRtRxRS,S6SpSrSvS:U>UUUUUU····«·¯hCUh)&hIH*h)&hIOJQJhIh)&hH*h)&hOJQJ h)&h hhhh)&hy H*h)&hy OJQJ h)&hy hy hy hy h)&hI9k and Lake Proae, respectively] are similar to the mean d13C for tufa from Plitvice Lakes, (8.31.0)0 , but show much smaller fluctuations. There is also practically no difference in d18O values between tufa (9.60.3)0 and lake sediments: (9.90.3)0 in Lake Proae and (9.30.2)0 in Lake Kozjak. All of these values indicate stable climatic conditions for the region during last 6000-7000 years, which is the 14C age of Holocene tufa and lake sediment in this region (Srdo  et al. 1986b). The d13C of DIC in water and the d13C of lake sediments can be compared. The d13C of DIC in Lake Proae is ~(11)0 , and that of DIC in Lake Kozjak ~(10)0 . The mean annual temperatures are 10.9C and 10.6C, respectively. Thus, the difference dsedim-dDIC is 20 and 1.40 for Lakes Proae and Kozjak, respectively, and it is in accordance with the equilibrium fractionation factor (e~1.50 at 10C). We can conclude therefore that sediment precipitation occurs under carbon isotope equilibrium. Fig. 2 Stable isotope composition of tufa and lake sedimentsFig. 3 d13C and d18O in submerged speleothems, marine overgrowth and recent molluscs Isotope analyses, including d13C, d18O and 14C age, of tufa, lake sediments and speleo-thems in the Dinaric Karst, confirm that these deposits record environmental and climatic information. While speleothem is a good indicator of global climate and palaeoclimatic changes, tufa is a more sensitive indicator of palaeoenvironmental changes. Isotope analyses of several speleothems from three submerged caves (depths of 38.5 m to 17 m) along the Eastern Adriatic coast were applied in an attempt of reconstruction of the late Pleistocene Holocene sea-level rise along the Croatian cost. The marine biogenic overgrowth layer and the youngest and the oldest parts of the speleothems were dated by the 14C method and their d13C and d18O were also measured. The start of overgrowth (i.e., the time of flooding by seawater) was determined to be 10,185 cal BP at -36 m, 9160 cal BP at -34 m, and 7920 cal BP at -23 m (Suri et al. 2005). Our results partially match the sea-level curves reconstructed for adjacent areas, Tyrrhenian Coast and French Mediterranean Coast. The stable isotope composition of the marine overgrowth is in the same range as that of recent molluscs from the Eastern Adriatic Sea (Fig. 3), and can be clearly distinguished from the stable isotope composition of the speleothem layers, which in turn is typical for the terrestrial speleothems in the karst region of Croatia with the prevailing Mediterranean type of climate. References Horvatin i, N., Krajcar Broni, I., Pezdi , J., Srdo , D., Obeli, B. (1986) The distribution of radioactive (3H, 14C) and stable (2H, 18O) isotopes in precipitation, surface and ground-waters during the last decade in Yugoslavia. Nuclear Instrum. Methods B17, 550-553. Horvatin i, N., Krajcar Broni, I., Obeli, B. (2003) Differences in the 14C age, d13C and d18O of Holocene tufa and speleothem in the Dinaric karst. Palaeogeography, Palaeoclimatology, Palaeoecology 193, 139-157. Horvatin i, N., Krajcar Broni, I., Bareai, J., Obeli, B., Vidi , S. (2005) Tritium and stable isotope distribution in the atmosphere at the coastal region of Croatia. In: Isotopic Composition of Precipitation in the Mediterranean Basin in Relation to Air Circulation Patterns and Climate, IAEA-TECDOC (in press). IAEA, 2005,  HYPERLINK "http://isohis.iaea.org/" http://isohis.iaea.org/ Kozk, K., Obeli, B., Horvatin i, N. (1989) Tritium and 14C in tree rings of the last three decades. Radiocarbon 31, 766-770. Krajcar Broni, I., Horvatin i, N., Srdo , D., Obeli, B. (1986) On the initial 14C activity of karst aquifers with short mean residence time. Radiocarbon 28, 436-440. Krajcar Broni, I., Horvatin i, N., Obeli, B. (1998) Two decades of environmental isotope record in Croatia: Reconstruction of the past and prediction of future levels. Radiocarbon 40, 399-416. Krajcar Broni, I., Horvatin i, N., Bareai, J., Obeli, B., Vre a, P., Vidi , S. (2004) Tritium and stable isotope variations in precipitation of Croatia and Slovenia. ESIR VII, Seggauberg, Austria, 27.6.-1.7.2004. In: Berichte des Institutes fuer Erdwissenschaften Karl-Franzens-Universitaet Graz, Bd. 8, Isotope Workshop Volume, 81-83. Srdo , D., Krajcar Broni, I., Horvatin i, N., Obeli, B. (1986a) The increase of 14C activity of dissolved inorganic carbon along the river course. Radiocarbon 28, 515-521. Srdo , D., Obeli, B., Horvatin i, N., Krajcar Broni, I., Mar enko, E., Merkt, S., Wong, H., Sliep evi, A. (1986b) Radiocarbon dating of lake sediments from two karstic lakes in Yugoslavia. Radiocarbon 28, 495-502. Suri, M., Jura i, M., Horvatin i, N., Krajcar Broni, I. (2005) Late Pleistocene - Holocene sea-level rise and the pattern of coastal karst inundation: records from submerged speleothems along the Eastern Adriatic Coast (Croatia). Marine Geology 214, 163-175. 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