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The levantine amber belt
Journal of African Earth Sciences, Vol. 14, No. 2, pp. 295-300, 1992. Printed in Great Britain
0899-5362/92 $5.00+0.00 © 1992 Peglamon ltrsss Ltd
The Levantine amber belt A. NissEr,m^uMand A. HoRowrl2* Weizmann Institute of Science, Rehovot 76100, Israel *Palynological Laboratory, Institute of Archaeology, Tel Aviv University, Tel Aviv 69978, Israel (First receined 4 March, 91; revised form received 5 July, 1991) Abstract - Amber, a fossil resin, is found in Early Cretaceous sandstones and fine clastics in Lebanon, Jordan, and Israel. The term "Levantine amber belt" is coined for this amber-containing sediment belt. The amber occurs as small nodules of various colors and frequently contains inclusions of macro- and microorganisms. The Lebanese amber contains Lepidoptera and the amber from southern Israel is rich in fungai remains. The source of the amber, based on geochemical and palynological evidence, is assumed to be from a conifer belonging to the Araucariaceae. The resins were produced by trees growing in a tropical near shore environment. The amber was transported into small swamps and was preserved there together with lignite. Later reworking of those deposits resulted in redeposition of the amber in oxidized sandstones.
GEOGRAPHIC DISTRIBUTION
INTRODUCTION
The earliest k n o w n report of Levantine a m b e r A m b e r is a fossilized tree-derived resin which is f o u n d in t h e geological record from t h e Late is from the L e b a n o n (Fraas, 1878). More recent inC a r b o n i f e r o u s t h r o u g h t h e p r e s e n t d a y formation w a s provided by Schlee a n d Dietrich (Langenheim, 1964; 1990). Amber usually occurs (1970). The a m b e r w a s f o u n d n e a r Jezzin (Fig. I) in as discrete n o d u l e s or l u m p s ranging in size from Early Cretaceous s a n d s t o n e s belonging to the a few m m to m a s s e s as large as 20 kg. The s t u d y "Gres de Base" u n i t of probably B a r r e m n i a n age. of a m b e r h a s a very long history, being one of t h e The amber, which is f o u n d t h r o u g h o u t a 300 m earliest g e m s u s e d by m a n k i n d (Frondel, 1968). thick section of the s a n d s t o n e s , o c c u r s a s multiThe s t u d y of a m b e r s ranges from detailed geo- colored small pieces, with t h e d o m i n a n t colors chemical analysis (Grimalt et al., 1988) to s t u d y of being yellow, orange, red, b r o w n a n d black, u s u a l t h e insect a n d other inclusions (Larsson, 1978). ly with a cloudy a p p e a r a n c e d u e to n u m e r o u s Attention w a s given, primarily by scientists from inclusions. Schlee a n d Dietrich (I 970) differentiat h e USSR a n d e a s t e r n Europe, to the sedimento- ted, on the basis of lithological associations, betlogy of a m b e r a n d its e n v i r o n m e n t of deposition. w e e n " p a r a u t h o c h t h o n o u s " a m b e r associated with Naturally e n o u g h , m o s t of this w o r k c o n c e n t r a t e d lignite horizons, a n d "placer" deposits of secondary on a m b e r from t h e Baltic area, w h i c h probably or in. r e p r e s e n t s t h e largest a c c u m u t a t i o n of a m b e r in In J o r d a n , a m b e r was f o u n d in s a n d s t o n e s a n d the world (Trofimov, 1978; Masicka, 1972). silts belonging to t h e K u r n u b group, of Early Many o c c u r r e n c e s of a m b e r c a n be referred to as Cretaceous age, in Wadi Zerka (Fig. l) between t h e a m b e r belts, since t h e y u s u a l l y occur in time- King Talal reservoir a n d t h e Zerka bridge (Bandel equivalent horizons which c a n be quite wide- a n d Abdallah, 1981; Bandel a n d Vavra, 1981). The s p r e a d geographically. Thus, Baltic a m b e r is f o u n d a m b e r occurs as small, reddish or yellowish drop in E o c e n e - O l i g o c e n e s e d i m e n t s from e a s t e r n s h a p e or spherical pieces w h i c h occasionally c a n E n g l a n d to t h e e a s t e r n Baltic coast. A n o t h e r s u c h reach a diameter of u p to 9 cm. The a m b e r is f o u n d example is amber, of Oligocene-Miocene age, which in clay- a n d silt-rich horizons, associated with is f o u n d from Chiapas, Mexico to the Dominican pieces of fossil wood a n d o t h e r plant r e m a i n s with Republic, a distance of several h u n d r e d kilo- a n o c c a s i o n a l l y well d e v e l o p e d root s y s t e m . meters. Frequently t h e rock is rich in pyrite a n d coaly The p r e s e n t s t u d y describes a n Early Cretaceous organic m a t t e r (Bandel a n d Abdallah, 1981). a m b e r belt, the oldest k n o w n belt, which ranges Amber h a s b e e n f o u n d in Israel a n d vicinity in from S o u t h e m Lebanon to s o u t h e r n Israel, a dis- four localities (Fig. I): in surface e x p o s u r e s (1) on t h e tance of a b o u t 200 km. s o u t h e r n slopes of Mt. Hermon, b e t w e e n MaJdal S h a m s a n d Newe Ativ; (2) in the e a s t e m escarpm e n t s of the Naftali Mountains, overlooking Qiryat 295
296
A. NISSENBAUMand A. HOROWlTZ
riched in carbon. The s a m e is t r u e for the stable c a r b o n and hydrogen isotope distribution. Although the factors which control the stable isotope composition of a m b e r s are not known, t h e similarity of the isotopic v a l u e s m a y indicate t h a t t h e Levantine a m b e r s were formed from the s a m e type of tree. If the d e u t e r i u m c o n t e n t of the a m b e r s c a n be considered a s a reflection of t h e d e u t e r i u m c o n t e n t of the e n v i r o n m e n t a l w a t e r a n d of t e m p e r a t u r e , t h e n the Levantine resins were all formed in a similar e n v i r o n m e n t a n d climate. The infra-red s p e c t r a of Levantine a m b e r from Qiryat S h e m o n a , Israel (Fig. 2a) is typical of m a n y other a m b e r s (Beck et al., 1964; L a n g e n h e i m a n d Beck, 1965; L a n g e n h e i m a n d Beck, 1968) a n d r e s e m b l e s the J o r d a n i a n a n d L e b a n e s e a m b e r s MAN d e s c r i b e d b y B a n d e l a n d Vavra (1981) a n d b y R o t t l a n d e r a n d Mischer (1970). The d o m i n a n t p e a k s are t h o s e of c a r b o n - h y d r o g e n b o n d stretching (2 9 3 0 c m -~] a n d b o n d b e n d i n g (1 4 6 0 a n d 1 3 8 0 c m I) a n d t h e 1 7 2 0 c m ~ so called carbonyl band. However, the 887, 1 6 4 0 a n d 3 0 7 0 c m -~ p e a k s of exocyclic d o u b l e b o n d s are m i s s i n g in t h e older Levantine a m b e r a s c o m p a r e d with t h e y o u n ger Baltic a m b e r (Fig. 2b). Also, a s observed b y Grimalt et aL, (1988) the s t r u c t u r e of the s p e c t r a b e t w e e n 1 2 5 0 a n d 6 1 0 c m ~ is m o r e f e a t u r e l e s s in the Levantine amber. Thus, the Levantine a m b e r r e p r e s e n t s higher degree of diagenetic c h a n g e of the organic m a t t e r a s c o m p a r e d with y o u n g e r 0 5pKm, a m b e r s a n d resins, a n d this is m o s t l y e x p r e s s e d in t h e h y d r o g e n a t i o n of u n s a t u r a t e d c o m p o n e n t s . Data on t h e m o l e c u t a r c o m p o s i t i o n of the orgaFig. I. Location m a p of a m b e r o c c u r r e n c e s in Lebanon, nic c o m p o n e n t s of Levantine a m b e r is available J o r d a n a n d Israel. only on s a m p l e from Mt. H e r m o n (Simoneit e t aL. 1986; Grimalt et al., 1988). The cyclic terpenoid S h e m o n a (Flexer, 1969); a n d in b o r e h o l e s in s o u t h e m Israel: (3) in the Kokhav 2 borehole a n d (4) t h e c o n t e n t of the a m b e r w a s low, b u t s k e l e t o n s of B a r b o o r I borehole (Fig. 1, a n d N i s s e n b a u m , 1975). v a r i o u s mono-, sesqui- a n d in particular, diterpeThe a m b e r o c c u r s a s n o d u l e s a n d droplets, disse- noids c o u t d b e identified. The extract of the a m b e r m i n a t e d in t h e rock matrix. The n o d u l e s range in w a s p r e d o m i n a n t l y c o m p o s e d of a c o m p l e x mlxcolor from pale yellow to orange-red a n d brown. ture of s a t u r a t e d a n d aromatic h y d r o c a r b o n s , The size r a n g e s from a few millimeters to a few w h e r e t r a n s f o r m e d t e r p e n o i d p r o d u c t s were a b u n centimeters. In all t h e localities the a m b e r is f o u n d dant. A m o n g them, alkylbenzenes, tetra-, octain Early C r e t a c e o u s s a n d s t o n e s of Hauterivian- a n d p e r h y d r o n a p h t a t e n e s , tetradeca- a n d tetraValanglnian age. Similar to the L e b a n e s e occur- h y d r o p y c e n e s . Although the p r e c u r s o r s of t h o s e rence, t h e a m b e r is f o u n d either as discrete no- diagenetic p r o d u c t s c a n not a l w a y s b e pinpointed, d u l e s in oxidized s a n d s t o n e s or, m o r e commonly, s o m e of the c o m p o u n d s c a n be correlated to abienin fine silty s h a l e s rich in organic matter, pyrite tane, pimarane or s a n d o p l m a r a n e s t r u c t u r e s which a n d c a r b o n i z e d plant r e m a i n s which are often are the m a i n c o m p o n e n t s of m o d e m r e s i n s . Occasionally s o m e of t h e original s t r u c t u r e s s u c h replaced b y pyrite. as k a u r a n e a n d p h y l l o c l a d a n e derivatives c a n still be recognized. In c o m p a r i s o n with y o u n g e r resins CHEMICAL PROPERTIES a n d a m b e r s , the Mt. H e r m o n a m b e r s h o w s diaT h e c h e m i c a l a n d i s o t o p i c c o m p o s i t i o n of genetic alteration w h i c h is e x p r e s s e d b y low conLevantine a m b e r is given in Table 1, together with tent of functionatized g r o u p s , a m a r k e d d e c r e a s e d a t a for o t h e r a m b e r a n d resin occurrences. The in olefinic b o n d s , particularly in exocyclic posic a r b o n a n d h y d r o g e n c o n t e n t of Levantine a m b e r s tions, and i n c r e a s e in aromaticity. T h u s , t h e is c o m p a r a b l e in all o c c u r r e n c e s a n d differ from m a t u r a t i o n s e q u e n c e of a m b e r s involves primarily other r e s i n s a n d a m b e r s b y being s o m e w h a t en- olefin polymerization
A
~i! ¸~ •
~ ki~ ¸ ~i ~,
~
~i~'~
'~
~
~
~,
~!,~!~ ;~!~~,i;ii,~'
298
A. Niss~,a3^UMand A. HoRowrrz Table I. Chemical a n d isotopic * composition of Levantine a m b e r and comparison with other ambers and resLns. (~)~3C data vs. PDB s t a n d a r d a D data vs. SMOW standard). Location Mt. Hermon Q. Shemona, Israel Barboor, Israel Kokhav, Israel W. Zerka, J o r d a n Lebanon Baltic Sea Coast Chiapas, Mexico Burma Manitoba, Canada Dominican Republic Kauri Resin Pine Resin, Israel Copal Resin, Phillipines
Age E. Cretaceous E. Cretaceous E. Cretaceous E. Cretaceous E. Cretaceous E. Cretaceous Eo-Oligocene Oligocene Miocene U. Cretaceous Oligocene Holocene Recent Recent
%C 81.90 81.20 80.90 81.20 83.78 82.20 79.30 76.45
%H 10.20 10.10 10.10 10.20 10.66 10.61 10.20 11.85
71.46 79.48 74.60
9.15 10.97 10.50
74.30
10.60
~ 13C %0 -20.4 -20.1 - 19.5 -20.1 -21.5 -24.6 -25.1
~D %0
-205
-243 -272
- 18.9
-23.8
-25.7 -24.1
- 188 -236
*Stable isotope data from DeNiro and Nissenbaum (unpublished)
h u m i d environment with low reliefwhlch resulted in the formation of m a r s h e s , lagoons a n d swamps probably not far from the seashore. This reconThe exact straUgraphic horizon in which the strucUon agrees with the conclusions of Sneh early Cretaceous Levantine a m b e r is found is (1974) and Karcz (1965) that the K u m u b Group difficult to define due to the n a t u r e of the sedi- was deposited mainly in near-shore (marine and m e n t s which contains it. In the Kokhav 2 ocur- continental] areas. Recently, Weissbrod etal., (1990) rence it is found in horizons of Hauterivian - discussed the Early Cretaceous in s o u t h e r n Israel Valanglnian age, while in most other occurrences, and showed t h a t during the Albian-ApUan, several a n d especially in the placer deposits, it is found in shallow marine ingresslons c a n be recognized in B a r r e m n i a n or y o u n g e r strata. The autochtho- the continental sandstone section, indicating their n o u s a m b e r in s o u t h r e n Israel m a y have been deposition in n e a r shore areas. According to formed during the freshwater to brackish event re- Masaad (1976)the Early Cretaceous sandstones of presented b y ostracode zone L-2* of Rosenfeld and Lebanon were deposited in a fluvio-deltaic enviRaab (1980). If so, the a m b e r was formed in the r o n m e n t with small depressions, which persisted Hautrevian-Barremnian periods, represented by for some time a s stagnant swamps, where organic the base of the Heletz formation. Reworking of the m a t t e r was accumulated. The m a s r s h e s into which the a m b e r was transa m b e r source beds resulted in the occurrence of ported from the s u r r o u n d i n g area were highly a m b e r in s l ~ h t l y younger sections of the sandreducing d u e to the high organic load, resulting in stone sequence. The environment of deposition of the amber is preservation of the amber. The life time of those dictated by its own nature. It is produced on land water bodies was very probably quite short and and due to its brittleness, large pieces c a n n o t be rapid burial by aeolian d u n e s or by coastal s a n d s t r a n s p o r t e d over a long distance. The pollen as a result of rising sea level helped in preserving assemblages of the s a n d s t o n e s u r r o u n d i n g the the amber. Rosenfeld a n d Raab (1980) described authigenic a m b e r in the Mt. Hermon and Kokhav ostracode zone L-2* in the Early Cretaceous, which 2 o c c u r r e n c e s (this r e p o r t a n d Ting a n d probably correlates in time with a n a m b e r forming Nissenbaum, 1986) indicate a local m a r s h vege- period, to have been deposited in fresh water to taUon s u r r o u n d e d by a dense forest composed brackish, lacustrine, lagoonal a n d deltaic environment, u n d e r a tropical climate. This interpretation primarily of Araucarian conifers. Paleoenvironmental reconstruction based on the agrees with the paleoenvironment as reconstructsedimentology of the surrounding sediments indi- ed from the palynological data on the Levantine cates that the a m b e r originated In a tropical. amber. STRATIGRJkPHY
The Lzvantine amber belt
BOTANICAL SOURCE
299 PAI.EOBIOI,OGY
Amber is considered to be one of the best, if not Due to difficulties in dissolving the amber, no studies were m a d e on the pollen trappd in the the best, m e d i u m for preservation of non-skeletal a m b e r matrix itself. There is some information, organisms (Nissenbaum, in press). The inclusions, however, on the pollen in the s u r r o u n d i n g c o u n t r y as t h e y are oRen referred to, are exceptionally wen rock. The organic rich silty s a n d s t o n e s from Mt. preserved, including the soR parts. The organisms Hermon (Fig. 1) contain a considerable n u m b e r of are trapped in the resin as it flows down the tree palynomorphs of which the most c o m m o n are t r u n k to become completely embedded. The most pterydophyte spores: Cyath~_~i_tes australls - 32 %, frequently found organisms are various types of Cingulatisportes sp. - 20 %, Cicatricoslsporites sp. insects, although larger organisms s u c h as frogs - 5 %, Matonlsporltes phlebopteroides - 3 %, have also b e e n reported (Poinar a n d Cannatella, Gleicheniidltes senonicus - 3 %. G y m n o s p e r m 1987). palynomorphs are also quite common: AracuariaInsects have b e e n reported from Lebanese a m b e r cites _n_~_~_starlis-12 %, Eucommildites troedsonii- 8 by Schlee a n d Dietrich (1970) a n d by Whalley %, Ephedr/p/tes sp. - 5 %, Tsugapollenites dampieri (1977). The insects described so far belong to -2%. Orthoptera, Homoptera, Coleoptera, Diptera, a n d A n g i o s p e r m s p a l y n o m o r p h s are quite rare: Lepidoptera. According to Schlee a n d Dietrich Trlpollenites sp. - 3 %, Clavatipollenites hughessii- (1970) the insect f a u n a is characteristic of the 2 %. In addition to the pollen, the sample was very tropical north coast of Gondwanaland. rich in cuticle remains, particularly of AraucariaTing a n d N i s s e n b a u m (1986) described well ceae, Ting a n d Nissenbaum (1986) described from preserved fungi in the a m b e r from the Kokhav 2 the s a n d s t o n e s in the Kokhav 2 borehole, a pollen borehole (Fig. 3) The lack of septate h y p h a e places a s s e m b l a g e c o n t a i n i n g Cicatricosisporltes sp., the fungi in the Phycomycetes group. Absence of C n g u l a t i s p o r i t e s sp., C y c a t h i d i t e s sp., a n d forms representing the full llfe cycle precluded Eucomiidites sp. The pollen assemblage from strict comparison with m o d e m species, b u t a tenKokhav 2 is t h u s very similar to t h a t from Mt. tative reconstitution of the developmental sequence Hermon, although a few additional plants are allowed t h e i d e n t i f i c a t i o n of f o u r s p e c i e s : found in Kokhav 2. Phycomlcetes eucarpii, Peronosporites p y t l u s and The J o r d a n i a n a m b e r was not investigated for its Blastocladltes Israeli. Ting a n d Nissenbaum (I 986) pollen c o n t e n t . B a n d e l a n d Abdallah (1981) proposed t h a t the fungi were trapped in the a m b e r reported fern-like imprints in the a m b e r bearing while the resin was flowing down the tree trunk, rocks, b u t the m o s t c o m m o n remains are from since the fungal bodies oRen show strong alignAgathis-like c o n i f e r b e l o n g i n g to t h e m e n t with flow lines. Araucariaceae. WAVENUMBER (cm-I) Attempts have b e e n m a d e to deduce the botaI000 2000 5000 4OOO nical source of the Levantine a m b e r by using IR l | spectra, whole sample m a s s spectroscopy and thin ® layer c h r o m a t o g r a p h y (Rotflander and Mischer, 1970; Bandel a n d Vavra, 1981). While those studies indicated the fairly close relationships between the Lebanese and J o r d a n i a n ambers they did not point, inter alia, to the botanical source of the amber. A detailed molecular s t u d y ofMt. Hermon a m b e r by GC-MS a n d CP/MAS~3C NMR (Grlmalt et al., 1988) showed t h a t the chemical composition of the plant derived molecules h a s been greatly modified by diagenetic processes, so that relating the data to extant resin-forming trees is difficult. The findings, however, were fairly similar to the analysis of Baltic r e s i n by Mills et al., (1984), who s u p p o r t e d Araucarian source for Baltic amber. Thus, the botanical a n d geochemical information suggests that the Levantine a m b e r was produced by a conifer, belonging to the Araucariaceae. Fig. 3. Infra-red spectra of (A) Levantine (Mt. Hennon} and (B} Baltic ambers.
A. NISSENBAUMand A. HoRowrrz
300
The fungi in the amber form fairly dense mycorrmlzae but microscopic observations do not s h o w a n y c o m e c t i o n to t h e o r g a n i c d e b r i s in t h e sandstone matrix. The sharp demarcation indicates, therefore, that the amber nodules are detrital.
Acknow~ts-
The a u t h o r s wish to t h a n k Dr A. S e r b a n (WlS) for the IR analyses.
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Masicka, H. 1972. Presence d ' a m b r e c o m m e Indice d ' u n e ancienne ligne de rivage. Mar. Geology 1 3 , 3 4 7 354. Massaad, M. 1976. Origin a n d e n v i r o n m e n t of deposition of Lebanon b a s a l s a n d s t o n e s . Eclogae Geol. Helv. 8 9 / 1 , 85-91. Mills, J. S., White, R. and Gough, L. J. 1984. The chemical composition of BaIUc amber. Chem. GeoL 47, 15-39. Mroueh, M. A. a n d S m i m o v a , S. B. 1986. S u r l a position stratigraphique d u Ores de Base d u Sud-Liban. Syrian J. o f Geology I 0 , 58-63. Nissenbaum, A. 1975. Lower Cretaceous a m b e r from Israel. Naturwlssenschaflen 7, 341-342. Poinar, G. O., Jr. a n d Cannatella, D. C. 1987. An Upper Eocene frog from the Dominican Republic and its implication for Caribbean biogeography. Sclence 237, 1 2 1 5 - I 216. Rosenfeld, A. a n d Raab, M. 1980. Lower Cretaceous ostracodes from Israel. GSI Current Research I, 6265. Rottlander, R. a n d Mischer, G. 1970. C h e m i s c h e untersuchungen an Libanesischen Unterkreide b e m s t e l n . N. Jb. Geol. Palaeont. Mh. 8, 452-464. Schlee, D., a n d Dietrich. H. - G. 1970. Insektenfuhrender bernstein a u s der unterkreide des Libanon. N. Jb. Geol. Palaeont. Mh. 1,1970. Simoneit, B. R. T., Grimalt, J. O., Wang, T. G., Cox, R. E., Hatcher, P. G. a n d N i s s e n b a u m , A- 1986. Cyclic terpenoids of c o n t e m p o r a r y resinous plant detritus a n d of fossil w o o d s , a m b e r s a n d coals. Org. Geochemistry I 0 , 877-889. Sneh, A. 1974. StraUgraphy of the Lower Cretaceous s y s t e m of n o r t h e m israel, with special e m p h a s i s on depositlonal environments a n d economic significance. Unpublished M.Sc. Thesis, Renesselaer Polytechnic Institute, Troy, New York. "ring, W. S. a n d N i s s e n b a u m , A. 1986. F~ungi in Lower Cretaceous amber f r o m Israel, Special Publication by the Chinese Petroleum Corp., Taiwan: 1-27 p. Trofimov, V. S. 1978. A m b e r concentrates in the shore a r e a s zones of recent a n d ancient seas a n d oceans. Littu Min. Res. 13, 307-313. Weissbrod, T., Gvirtzman, G. a n d Levy, Z. 1990. Early Cretaceous m a r i n e ingressions in the Negev: new findings. Abs. Geol. S o c Israel. Ann. Meeting, Elat: 91. Whalley, P. 1977. Lower Cretaceous lepidoptera, Nature 288, 526.
0899-5362/92 $5.00+0.00 © 1992 Peglamon ltrsss Ltd
The Levantine amber belt A. NissEr,m^uMand A. HoRowrl2* Weizmann Institute of Science, Rehovot 76100, Israel *Palynological Laboratory, Institute of Archaeology, Tel Aviv University, Tel Aviv 69978, Israel (First receined 4 March, 91; revised form received 5 July, 1991) Abstract - Amber, a fossil resin, is found in Early Cretaceous sandstones and fine clastics in Lebanon, Jordan, and Israel. The term "Levantine amber belt" is coined for this amber-containing sediment belt. The amber occurs as small nodules of various colors and frequently contains inclusions of macro- and microorganisms. The Lebanese amber contains Lepidoptera and the amber from southern Israel is rich in fungai remains. The source of the amber, based on geochemical and palynological evidence, is assumed to be from a conifer belonging to the Araucariaceae. The resins were produced by trees growing in a tropical near shore environment. The amber was transported into small swamps and was preserved there together with lignite. Later reworking of those deposits resulted in redeposition of the amber in oxidized sandstones.
GEOGRAPHIC DISTRIBUTION
INTRODUCTION
The earliest k n o w n report of Levantine a m b e r A m b e r is a fossilized tree-derived resin which is f o u n d in t h e geological record from t h e Late is from the L e b a n o n (Fraas, 1878). More recent inC a r b o n i f e r o u s t h r o u g h t h e p r e s e n t d a y formation w a s provided by Schlee a n d Dietrich (Langenheim, 1964; 1990). Amber usually occurs (1970). The a m b e r w a s f o u n d n e a r Jezzin (Fig. I) in as discrete n o d u l e s or l u m p s ranging in size from Early Cretaceous s a n d s t o n e s belonging to the a few m m to m a s s e s as large as 20 kg. The s t u d y "Gres de Base" u n i t of probably B a r r e m n i a n age. of a m b e r h a s a very long history, being one of t h e The amber, which is f o u n d t h r o u g h o u t a 300 m earliest g e m s u s e d by m a n k i n d (Frondel, 1968). thick section of the s a n d s t o n e s , o c c u r s a s multiThe s t u d y of a m b e r s ranges from detailed geo- colored small pieces, with t h e d o m i n a n t colors chemical analysis (Grimalt et al., 1988) to s t u d y of being yellow, orange, red, b r o w n a n d black, u s u a l t h e insect a n d other inclusions (Larsson, 1978). ly with a cloudy a p p e a r a n c e d u e to n u m e r o u s Attention w a s given, primarily by scientists from inclusions. Schlee a n d Dietrich (I 970) differentiat h e USSR a n d e a s t e r n Europe, to the sedimento- ted, on the basis of lithological associations, betlogy of a m b e r a n d its e n v i r o n m e n t of deposition. w e e n " p a r a u t h o c h t h o n o u s " a m b e r associated with Naturally e n o u g h , m o s t of this w o r k c o n c e n t r a t e d lignite horizons, a n d "placer" deposits of secondary on a m b e r from t h e Baltic area, w h i c h probably or in. r e p r e s e n t s t h e largest a c c u m u t a t i o n of a m b e r in In J o r d a n , a m b e r was f o u n d in s a n d s t o n e s a n d the world (Trofimov, 1978; Masicka, 1972). silts belonging to t h e K u r n u b group, of Early Many o c c u r r e n c e s of a m b e r c a n be referred to as Cretaceous age, in Wadi Zerka (Fig. l) between t h e a m b e r belts, since t h e y u s u a l l y occur in time- King Talal reservoir a n d t h e Zerka bridge (Bandel equivalent horizons which c a n be quite wide- a n d Abdallah, 1981; Bandel a n d Vavra, 1981). The s p r e a d geographically. Thus, Baltic a m b e r is f o u n d a m b e r occurs as small, reddish or yellowish drop in E o c e n e - O l i g o c e n e s e d i m e n t s from e a s t e r n s h a p e or spherical pieces w h i c h occasionally c a n E n g l a n d to t h e e a s t e r n Baltic coast. A n o t h e r s u c h reach a diameter of u p to 9 cm. The a m b e r is f o u n d example is amber, of Oligocene-Miocene age, which in clay- a n d silt-rich horizons, associated with is f o u n d from Chiapas, Mexico to the Dominican pieces of fossil wood a n d o t h e r plant r e m a i n s with Republic, a distance of several h u n d r e d kilo- a n o c c a s i o n a l l y well d e v e l o p e d root s y s t e m . meters. Frequently t h e rock is rich in pyrite a n d coaly The p r e s e n t s t u d y describes a n Early Cretaceous organic m a t t e r (Bandel a n d Abdallah, 1981). a m b e r belt, the oldest k n o w n belt, which ranges Amber h a s b e e n f o u n d in Israel a n d vicinity in from S o u t h e m Lebanon to s o u t h e r n Israel, a dis- four localities (Fig. I): in surface e x p o s u r e s (1) on t h e tance of a b o u t 200 km. s o u t h e r n slopes of Mt. Hermon, b e t w e e n MaJdal S h a m s a n d Newe Ativ; (2) in the e a s t e m escarpm e n t s of the Naftali Mountains, overlooking Qiryat 295
296
A. NISSENBAUMand A. HOROWlTZ
riched in carbon. The s a m e is t r u e for the stable c a r b o n and hydrogen isotope distribution. Although the factors which control the stable isotope composition of a m b e r s are not known, t h e similarity of the isotopic v a l u e s m a y indicate t h a t t h e Levantine a m b e r s were formed from the s a m e type of tree. If the d e u t e r i u m c o n t e n t of the a m b e r s c a n be considered a s a reflection of t h e d e u t e r i u m c o n t e n t of the e n v i r o n m e n t a l w a t e r a n d of t e m p e r a t u r e , t h e n the Levantine resins were all formed in a similar e n v i r o n m e n t a n d climate. The infra-red s p e c t r a of Levantine a m b e r from Qiryat S h e m o n a , Israel (Fig. 2a) is typical of m a n y other a m b e r s (Beck et al., 1964; L a n g e n h e i m a n d Beck, 1965; L a n g e n h e i m a n d Beck, 1968) a n d r e s e m b l e s the J o r d a n i a n a n d L e b a n e s e a m b e r s MAN d e s c r i b e d b y B a n d e l a n d Vavra (1981) a n d b y R o t t l a n d e r a n d Mischer (1970). The d o m i n a n t p e a k s are t h o s e of c a r b o n - h y d r o g e n b o n d stretching (2 9 3 0 c m -~] a n d b o n d b e n d i n g (1 4 6 0 a n d 1 3 8 0 c m I) a n d t h e 1 7 2 0 c m ~ so called carbonyl band. However, the 887, 1 6 4 0 a n d 3 0 7 0 c m -~ p e a k s of exocyclic d o u b l e b o n d s are m i s s i n g in t h e older Levantine a m b e r a s c o m p a r e d with t h e y o u n ger Baltic a m b e r (Fig. 2b). Also, a s observed b y Grimalt et aL, (1988) the s t r u c t u r e of the s p e c t r a b e t w e e n 1 2 5 0 a n d 6 1 0 c m ~ is m o r e f e a t u r e l e s s in the Levantine amber. Thus, the Levantine a m b e r r e p r e s e n t s higher degree of diagenetic c h a n g e of the organic m a t t e r a s c o m p a r e d with y o u n g e r 0 5pKm, a m b e r s a n d resins, a n d this is m o s t l y e x p r e s s e d in t h e h y d r o g e n a t i o n of u n s a t u r a t e d c o m p o n e n t s . Data on t h e m o l e c u t a r c o m p o s i t i o n of the orgaFig. I. Location m a p of a m b e r o c c u r r e n c e s in Lebanon, nic c o m p o n e n t s of Levantine a m b e r is available J o r d a n a n d Israel. only on s a m p l e from Mt. H e r m o n (Simoneit e t aL. 1986; Grimalt et al., 1988). The cyclic terpenoid S h e m o n a (Flexer, 1969); a n d in b o r e h o l e s in s o u t h e m Israel: (3) in the Kokhav 2 borehole a n d (4) t h e c o n t e n t of the a m b e r w a s low, b u t s k e l e t o n s of B a r b o o r I borehole (Fig. 1, a n d N i s s e n b a u m , 1975). v a r i o u s mono-, sesqui- a n d in particular, diterpeThe a m b e r o c c u r s a s n o d u l e s a n d droplets, disse- noids c o u t d b e identified. The extract of the a m b e r m i n a t e d in t h e rock matrix. The n o d u l e s range in w a s p r e d o m i n a n t l y c o m p o s e d of a c o m p l e x mlxcolor from pale yellow to orange-red a n d brown. ture of s a t u r a t e d a n d aromatic h y d r o c a r b o n s , The size r a n g e s from a few millimeters to a few w h e r e t r a n s f o r m e d t e r p e n o i d p r o d u c t s were a b u n centimeters. In all t h e localities the a m b e r is f o u n d dant. A m o n g them, alkylbenzenes, tetra-, octain Early C r e t a c e o u s s a n d s t o n e s of Hauterivian- a n d p e r h y d r o n a p h t a t e n e s , tetradeca- a n d tetraValanglnian age. Similar to the L e b a n e s e occur- h y d r o p y c e n e s . Although the p r e c u r s o r s of t h o s e rence, t h e a m b e r is f o u n d either as discrete no- diagenetic p r o d u c t s c a n not a l w a y s b e pinpointed, d u l e s in oxidized s a n d s t o n e s or, m o r e commonly, s o m e of the c o m p o u n d s c a n be correlated to abienin fine silty s h a l e s rich in organic matter, pyrite tane, pimarane or s a n d o p l m a r a n e s t r u c t u r e s which a n d c a r b o n i z e d plant r e m a i n s which are often are the m a i n c o m p o n e n t s of m o d e m r e s i n s . Occasionally s o m e of t h e original s t r u c t u r e s s u c h replaced b y pyrite. as k a u r a n e a n d p h y l l o c l a d a n e derivatives c a n still be recognized. In c o m p a r i s o n with y o u n g e r resins CHEMICAL PROPERTIES a n d a m b e r s , the Mt. H e r m o n a m b e r s h o w s diaT h e c h e m i c a l a n d i s o t o p i c c o m p o s i t i o n of genetic alteration w h i c h is e x p r e s s e d b y low conLevantine a m b e r is given in Table 1, together with tent of functionatized g r o u p s , a m a r k e d d e c r e a s e d a t a for o t h e r a m b e r a n d resin occurrences. The in olefinic b o n d s , particularly in exocyclic posic a r b o n a n d h y d r o g e n c o n t e n t of Levantine a m b e r s tions, and i n c r e a s e in aromaticity. T h u s , t h e is c o m p a r a b l e in all o c c u r r e n c e s a n d differ from m a t u r a t i o n s e q u e n c e of a m b e r s involves primarily other r e s i n s a n d a m b e r s b y being s o m e w h a t en- olefin polymerization
A
~i! ¸~ •
~ ki~ ¸ ~i ~,
~
~i~'~
'~
~
~
~,
~!,~!~ ;~!~~,i;ii,~'
298
A. Niss~,a3^UMand A. HoRowrrz Table I. Chemical a n d isotopic * composition of Levantine a m b e r and comparison with other ambers and resLns. (~)~3C data vs. PDB s t a n d a r d a D data vs. SMOW standard). Location Mt. Hermon Q. Shemona, Israel Barboor, Israel Kokhav, Israel W. Zerka, J o r d a n Lebanon Baltic Sea Coast Chiapas, Mexico Burma Manitoba, Canada Dominican Republic Kauri Resin Pine Resin, Israel Copal Resin, Phillipines
Age E. Cretaceous E. Cretaceous E. Cretaceous E. Cretaceous E. Cretaceous E. Cretaceous Eo-Oligocene Oligocene Miocene U. Cretaceous Oligocene Holocene Recent Recent
%C 81.90 81.20 80.90 81.20 83.78 82.20 79.30 76.45
%H 10.20 10.10 10.10 10.20 10.66 10.61 10.20 11.85
71.46 79.48 74.60
9.15 10.97 10.50
74.30
10.60
~ 13C %0 -20.4 -20.1 - 19.5 -20.1 -21.5 -24.6 -25.1
~D %0
-205
-243 -272
- 18.9
-23.8
-25.7 -24.1
- 188 -236
*Stable isotope data from DeNiro and Nissenbaum (unpublished)
h u m i d environment with low reliefwhlch resulted in the formation of m a r s h e s , lagoons a n d swamps probably not far from the seashore. This reconThe exact straUgraphic horizon in which the strucUon agrees with the conclusions of Sneh early Cretaceous Levantine a m b e r is found is (1974) and Karcz (1965) that the K u m u b Group difficult to define due to the n a t u r e of the sedi- was deposited mainly in near-shore (marine and m e n t s which contains it. In the Kokhav 2 ocur- continental] areas. Recently, Weissbrod etal., (1990) rence it is found in horizons of Hauterivian - discussed the Early Cretaceous in s o u t h e r n Israel Valanglnian age, while in most other occurrences, and showed t h a t during the Albian-ApUan, several a n d especially in the placer deposits, it is found in shallow marine ingresslons c a n be recognized in B a r r e m n i a n or y o u n g e r strata. The autochtho- the continental sandstone section, indicating their n o u s a m b e r in s o u t h r e n Israel m a y have been deposition in n e a r shore areas. According to formed during the freshwater to brackish event re- Masaad (1976)the Early Cretaceous sandstones of presented b y ostracode zone L-2* of Rosenfeld and Lebanon were deposited in a fluvio-deltaic enviRaab (1980). If so, the a m b e r was formed in the r o n m e n t with small depressions, which persisted Hautrevian-Barremnian periods, represented by for some time a s stagnant swamps, where organic the base of the Heletz formation. Reworking of the m a t t e r was accumulated. The m a s r s h e s into which the a m b e r was transa m b e r source beds resulted in the occurrence of ported from the s u r r o u n d i n g area were highly a m b e r in s l ~ h t l y younger sections of the sandreducing d u e to the high organic load, resulting in stone sequence. The environment of deposition of the amber is preservation of the amber. The life time of those dictated by its own nature. It is produced on land water bodies was very probably quite short and and due to its brittleness, large pieces c a n n o t be rapid burial by aeolian d u n e s or by coastal s a n d s t r a n s p o r t e d over a long distance. The pollen as a result of rising sea level helped in preserving assemblages of the s a n d s t o n e s u r r o u n d i n g the the amber. Rosenfeld a n d Raab (1980) described authigenic a m b e r in the Mt. Hermon and Kokhav ostracode zone L-2* in the Early Cretaceous, which 2 o c c u r r e n c e s (this r e p o r t a n d Ting a n d probably correlates in time with a n a m b e r forming Nissenbaum, 1986) indicate a local m a r s h vege- period, to have been deposited in fresh water to taUon s u r r o u n d e d by a dense forest composed brackish, lacustrine, lagoonal a n d deltaic environment, u n d e r a tropical climate. This interpretation primarily of Araucarian conifers. Paleoenvironmental reconstruction based on the agrees with the paleoenvironment as reconstructsedimentology of the surrounding sediments indi- ed from the palynological data on the Levantine cates that the a m b e r originated In a tropical. amber. STRATIGRJkPHY
The Lzvantine amber belt
BOTANICAL SOURCE
299 PAI.EOBIOI,OGY
Amber is considered to be one of the best, if not Due to difficulties in dissolving the amber, no studies were m a d e on the pollen trappd in the the best, m e d i u m for preservation of non-skeletal a m b e r matrix itself. There is some information, organisms (Nissenbaum, in press). The inclusions, however, on the pollen in the s u r r o u n d i n g c o u n t r y as t h e y are oRen referred to, are exceptionally wen rock. The organic rich silty s a n d s t o n e s from Mt. preserved, including the soR parts. The organisms Hermon (Fig. 1) contain a considerable n u m b e r of are trapped in the resin as it flows down the tree palynomorphs of which the most c o m m o n are t r u n k to become completely embedded. The most pterydophyte spores: Cyath~_~i_tes australls - 32 %, frequently found organisms are various types of Cingulatisportes sp. - 20 %, Cicatricoslsporites sp. insects, although larger organisms s u c h as frogs - 5 %, Matonlsporltes phlebopteroides - 3 %, have also b e e n reported (Poinar a n d Cannatella, Gleicheniidltes senonicus - 3 %. G y m n o s p e r m 1987). palynomorphs are also quite common: AracuariaInsects have b e e n reported from Lebanese a m b e r cites _n_~_~_starlis-12 %, Eucommildites troedsonii- 8 by Schlee a n d Dietrich (1970) a n d by Whalley %, Ephedr/p/tes sp. - 5 %, Tsugapollenites dampieri (1977). The insects described so far belong to -2%. Orthoptera, Homoptera, Coleoptera, Diptera, a n d A n g i o s p e r m s p a l y n o m o r p h s are quite rare: Lepidoptera. According to Schlee a n d Dietrich Trlpollenites sp. - 3 %, Clavatipollenites hughessii- (1970) the insect f a u n a is characteristic of the 2 %. In addition to the pollen, the sample was very tropical north coast of Gondwanaland. rich in cuticle remains, particularly of AraucariaTing a n d N i s s e n b a u m (1986) described well ceae, Ting a n d Nissenbaum (1986) described from preserved fungi in the a m b e r from the Kokhav 2 the s a n d s t o n e s in the Kokhav 2 borehole, a pollen borehole (Fig. 3) The lack of septate h y p h a e places a s s e m b l a g e c o n t a i n i n g Cicatricosisporltes sp., the fungi in the Phycomycetes group. Absence of C n g u l a t i s p o r i t e s sp., C y c a t h i d i t e s sp., a n d forms representing the full llfe cycle precluded Eucomiidites sp. The pollen assemblage from strict comparison with m o d e m species, b u t a tenKokhav 2 is t h u s very similar to t h a t from Mt. tative reconstitution of the developmental sequence Hermon, although a few additional plants are allowed t h e i d e n t i f i c a t i o n of f o u r s p e c i e s : found in Kokhav 2. Phycomlcetes eucarpii, Peronosporites p y t l u s and The J o r d a n i a n a m b e r was not investigated for its Blastocladltes Israeli. Ting a n d Nissenbaum (I 986) pollen c o n t e n t . B a n d e l a n d Abdallah (1981) proposed t h a t the fungi were trapped in the a m b e r reported fern-like imprints in the a m b e r bearing while the resin was flowing down the tree trunk, rocks, b u t the m o s t c o m m o n remains are from since the fungal bodies oRen show strong alignAgathis-like c o n i f e r b e l o n g i n g to t h e m e n t with flow lines. Araucariaceae. WAVENUMBER (cm-I) Attempts have b e e n m a d e to deduce the botaI000 2000 5000 4OOO nical source of the Levantine a m b e r by using IR l | spectra, whole sample m a s s spectroscopy and thin ® layer c h r o m a t o g r a p h y (Rotflander and Mischer, 1970; Bandel a n d Vavra, 1981). While those studies indicated the fairly close relationships between the Lebanese and J o r d a n i a n ambers they did not point, inter alia, to the botanical source of the amber. A detailed molecular s t u d y ofMt. Hermon a m b e r by GC-MS a n d CP/MAS~3C NMR (Grlmalt et al., 1988) showed t h a t the chemical composition of the plant derived molecules h a s been greatly modified by diagenetic processes, so that relating the data to extant resin-forming trees is difficult. The findings, however, were fairly similar to the analysis of Baltic r e s i n by Mills et al., (1984), who s u p p o r t e d Araucarian source for Baltic amber. Thus, the botanical a n d geochemical information suggests that the Levantine a m b e r was produced by a conifer, belonging to the Araucariaceae. Fig. 3. Infra-red spectra of (A) Levantine (Mt. Hennon} and (B} Baltic ambers.
A. NISSENBAUMand A. HoRowrrz
300
The fungi in the amber form fairly dense mycorrmlzae but microscopic observations do not s h o w a n y c o m e c t i o n to t h e o r g a n i c d e b r i s in t h e sandstone matrix. The sharp demarcation indicates, therefore, that the amber nodules are detrital.
Acknow~ts-
The a u t h o r s wish to t h a n k Dr A. S e r b a n (WlS) for the IR analyses.
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