Geological Quarterly, 2013, 57 (4): 649-664 DOI : http://dx.doi .org/10.7306/gq .1119 Conventional and high-resolution heavy mineral analyses applied to flysch deposits: comparative provenance studies of the Ropianka (Upper Cretaceous-Paleocene) and Menilite (Oligocene) formations (Skole Nappe, Polish Carpathians) Dorota SALATA1* and Alfred UCHMAN1 1 Institute of Geological Sciences, Jagiellonian University, Oleandry 2a, 30-063 Krakow, Poland Salata D. and Uchman A. (2013) Conventional and high-resolution heavy mineral analyses applied to flysch deposits: com- parative provenance studies of the Ropianka (Upper Cretaceous-Paleocene) and Menilite (Oligocene) formations (Skole Nappe, Polish Carpathians). Geological Quarterly, 57 (4): 649-664, doi: 10.7306/gq.1119 Conventional and high-resolution analyses of heavy minerals from the gravity flow-deposited sandstones of the Campanian-Maastrichtian interval of the Ropianka (Upper Cretaceous-Paleocene) and Menilite (Oligocene) formations of the Polish Carpathians display similar compositions in terms of mineral species. Zircon, tourmaline, rutile, garnet, staurolite and kyanite belong to the main constituents in both formations. Apatite is common in the Ropianka Fm., while the Menilite Fm. almost lacks this mineral. Furthermore, individual hornblende grains were found in the Ropianka Fm., while andalusite is present only in the Menilite Fm. The Ropianka Fm. is relatively richer in zircon, tourmaline, garnet and apatite, while the Menilite Fm. contains more staurolite and kyanite. Zircon and tourmaline colour and morphological varieties are similar in both formations. The similarities of the heavy mineral assemblages studied suggest origin of these minerals from lithologically similar rocks. Negative correlations between the zircon + tourmaline + rutile (ZTR) values and the content of garnet and staurolite in the Ropianka Fm. may indicate, to a large extent, first-cycle delivery of garnet and staurolite to the for- mation. Negative, but low, correlation valid only for ZTR and garnet and positive correlations for ZTR and staurolite and kyan- ite in the Menilite Fm. suggest delivery of these minerals from sedimentary rocks or/and palimpsest sediments. The data obtained on mineral relationships and their morphology suggest mixed first-cycle and recycled provenance of the heavy min- erals studied. Additionally, the first-cycle material input seems to be larger during the Ropianka Fm. sedimentation, while during the deposition of Menilite Fm. the contribution of material delivered from erosion of recycled sediments appears more prominent. The heavy mineral evidence suggests a change at the northern margin of the Skole Basin from an immature pas- sive margin with a high relief during sedimentation of the Campanian-Maastrichtian part of the Ropianka Fm. to a mature passive margin with a low relief during sedimentation of the Menilite Fm. Key words: heavy minerals, high-resolution, sedimentary provenance, flysch, Outer Carpathians, Skole Nappe. INTRODUCTION Lithological reconstructions of source areas and prove- nance studies of clastic deposits are a field of interest for re- searchers dealing with non-existing source massifs. Exotic rock studies, composition of sandstones and heavy mineral analy- ses are usually used as tools in such research. Lithologically diverse suites of exotic rock pebbles are rela- tively frequent in strata of the Ropianka Formation and in some types of younger deposits such as Babica Clay (e.g., Wdowiarz, 1949; Bukowy, 1957; Kotlarczyk and Śliwowa, 1963; Bromo- wicz, 1974, 1986; Skulich, 1986; Rajchel, 1990; Rajchel and Myszkowska, 1998). By contrast, deposits of the Menilite For- * Corresponding author, e-mail: dorota.salata@uj.edu.pl Received: May 22, 2013; accepted: July 12, 2013; first published online: September 19, 2013 mation are poor in exotic pebbles (e.g., Kotlarczyk and Śliwowa, 1963; Ślączka and Unrug, 1966; Kotlarczyk, 1976). In such cases palaeogeographic stud ies and lithological reconstruction of source area based on exotic rocks is possible only for a nar- row time-span, hindering comparative studies. The sandy frac- tion is abundant throughout the succession representing the entire Late Cretaceous-Oligocene time-span in the Skole Ba- sin. However, the composition of flysch sandstones is very mo- notonous (e.g., Kamieński et al., 1967; Bromowicz, 1974) and generally very similar in many facies. By contrast, heavy miner- als provide much information. Therefore, heavy mineral analy- sis is an excellent tool for comparative studies and provenance interpretation. The choice of the Ropianka and Menilite forma- tions allows comparison of initial and late stages of the history of the source area supplying western parts of the northern margin of the Skole Basin. Previous heavy mineral studies of Upper Cretaceous and Oligocene strata of the Skole Basin were concentrated in the eastern and most southeastern part of the Skole Nappe (e.g., Jaskólski, 1931; Tokarski, 1947; Szczurowska, 1970, 1971, 1973; Wdowiarz et al., 1974; Żytko, 1975). Analyses were 650 Dorota Salata and Alfred Uchman made mostly in rocks drilled in deep boreholes. In the area cur- rently researched, heavy mineral assemblages have been briefly described only in the Węgierka Marl (Geroch et al., 1979) in the upper part of the Ropianka Formation (Kotlarczyk, 1978). These studies were limited to ba sic op ti cal de scrip tions of heavy minerals and provided basic information about mineral content or only on the relative proportions of minerals. Palaeo- geographic interpretations or lithological reconstructions of source massif(s) were usually not made or treated only briefly, while comparative study of heavy minerals from the Ropianka and Menilite formations was not conducted. Heavy mineral analysis is a use-ul tool in identification of sediment provenance. However, due to commonly known fac- tors influencing heavy mineral assemblages, such as trans- portation processes, including hydraulic selection, diagenetic changes and mixi ng of source material (e.g., Morton and Hallsworth, 1999; Mange and Wright, 2007a), heavy mineral data are difficult to interpret. This is especially true for multi-cy- cle or mixed-source sedimentary rocks to which flysch strata often belong. The most commonly used method in heavy mineral stud ies is a conventional analysis based on the distribution of mineral species regardless of mineral variety. In contrast, high-resolu- tion heavy mineral analysis (HRHMa) categorises the main mineral species accounting their colour varieties, internal zon- ing, inclusions and degree of roundness (Mange-Rajetzky, 1995; Lihou and Mange-Rajetzky, 1996; Mange and Wright, 2007b; Nie et al., 2012). The HRHMA method is especially use- ful for ultrastable minerals such as zircon and tourmaline since they, due to their high re sis tance, re main in multi-cycled depos- its. The presence and proportions of highly rounded grains to euhedral ones yields information about source rock types, while comparison of mineral varieties in a pro-ile enables more spe- cific comparative provenance studies. Conventional and HRHMA methods have been used in the current comparative study of heavy mineral assemblages from flysch sandstones of the Campanian-Maastrichtian part of the Ropianka Formation (Upper Cretaceous-Paleocene) and the prevailingly Kliva and Boryslav sandstone types of the Menilite Formation (Oligocene) from the northern margins of the Skole Nappe (Polish Flysch Carpathians). The results of conventional heavy mineral analyses of the Menilite Formation, already pub- lished by Salata and Uchman (2012), have currently been sup- plemented with HRHMA analyses and compared with new heavy mineral data from the Ropianka Formation. Such a com- bination allows refined comparative studies providing more specific data regarding the origins of heavy minerals from these formations. The data obtained provide a basis for further, more detailed, provenance research based on single-grain analyses (e.g., Eynatten and Dunkl, 2012; Nie et al., 2012). GEOLOGICAL BACKGROUND The Skole Nappe is situated on the north-east bend of the Carpathian orogenic arc (Fig. 1). It is formed of Lower Creta- ceous-Lower Miocene deep-sea, mostly flysch strata that ac- cumulated in the Skole Basin, which was at least about 150 km wide (Gągała et al., 2012), being a trough bordered by the Euro- pean Plattorm in the north and by the Subsilesian ridge and slope in the south. The sedimentary fill of the basin has been folded and thrusted northwards during the Miocene. The Upper Cretaceous-Paleocene strata are distinguished as the Ropianka Formation (Kotlarczyk, 1978 and references therein) and called also the Inoceramian Beds in the older literature. They are overlain by the upper Paleocene-Eocene deep-sea mudstone-dominated strata of the Variegated Shale Formation and the Eocene mudstones, sandstones and marls of the Hi- eroglyphic Formation (Rajchel, 1990). The Oligocene part is composed of the Menilite and Krosno formations (Fig. 2; Kotlarczyk, 1966; Kotlarczyk and Leśniak, 1990). The Ropianka Formation was studied in the area of Husów and its vicinity (Fig. 3), where Wdowiarz (1949) distinguished lower, middle and upper levels in the Ropianka Formation (his Inoceramian Beds), which are altogether 500 m thick. Kotla- rczyk (1978) subdivided the Ropianka Formation into the Cisowa Member (Turonian-Lower Campanian), Wiar Member (Lower Campanian-Lower Maastrichtian), Leszczyny Member (Lower Maastrichtian-Lower Paleocene) and Wola Korze- niecka Member (Paleocene). The de pos its stud ied be long to the Wiar and Leszczyny members. The sections studied repre- sent a proximal part of the depositional system, probably chan- nel facies of a submarine fan, as in the case of sandstone-domi- nated sections (Manasterz, Husów - Patria, Husów - Biedro- niówka, Nieważka), or more distal parts of the depositional sys- tem, such as lobes, interlobes or fan fringes (Husów - Gaj, Husów Bąkowiec, Husów - Bagnisty Stream, Rzeki - Gąszcz Stream, Tarnawka - leśniczówka A, B, Tarnawka 1-5, Tarnawka Quarry). These strata were deposited by turbidity currents or other density-flow currents. The outcrops belong to the Marginal Thrust Sheet, Husów Thrust Sheet and the Hadle Kańczudzkie-Chmielnik Thrust Sheet (Figs. 3-6). The Husów - Gaj section is dated to the Gansserina gansseri Zone (Upper Campanian-Lower Maastrichtian) (Gasiński and Uchman, 2009), while the Bąkowiec section belongs to the Abatho- mphalus mayaroensis Zone of the Upper Maastrichtian (Gat siński and Uchman, 2011). The Tarnawka 2 section represents the same zone as the latter (A. Gasiński and A. Uchman, pers. comm., 2013). The Menilite Formation is characterized by dark, mostly black or brown shales, which accumulated on the deep-sea, pe- riodically anoxic flysch basin floor (Kotlarczyk and Uchman, 2012 and references therein). The shales contain horizons of chert, marl, limestone and diatomite, and lithosome of sandt stone (Kotlarczyk and Leśniak, 1990; Kotlarczyk et al., 2006). The material studied derives mainly from the Boryslav and Kliva sand stones, which were de pos ited from gravi ty flows, mainly in chan nel zones. The sections studied are related to the Rzeszów and Łańcut channel zones (Kotlarczyk and Leśniak, 1990; Fig. 1). Their description and conventional heavy mineral characteristics are provided by Salata and Uchman (2012). SANDSTONE COMPOSITION Quartz is a dominant constituent of the Ropianka Formation sand stones, in the presently studi ed area, SE of Rzeszów. They contain feldspars, lithic fragments and subordinate amounts of mica, glauconite and organic debris. The sand- stones rep re sent mainly sublitharenite, subordinately sub- arkose types. They are mostly fine- to medium-grained and well- to moderately-sorted (Bromowicz, 1974). Among lithic frag ments, sed i men tary rocks rep re sented mainly by lime- stones and siliceous rocks prevail. Additionally, igneous rocks such as fine-grained granitoids and, less frequent, dacites as well as meta morphic mica-schists and gneisses are also pres- ent (e.g., Bromowicz, 1974, 1986 and references therein). Peb- bles of sedimentary rock are more abundant in the lower part of the Ropianka Formation while fragments or clasts of igneous and meta morphic rocks appear more frequently in its higher part (Bromowicz, 1974). According to Bromowicz (1986), the Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 651 Fig. 1. General geological map showing location of the sections studied of the Menilite Formation (based on Kotlarczyk and Leśniak, 1990; modified by Kotlarczyk and Uchman, 2012; Salata and Uchman, 2012) A more detailed map of the Husów area showi ng the location of the Ropianka Formation sections studied is included (Fig. 3) con tri bu tion of ig ne ous and meta morphic rocks in the source cordillera was dis-inctly smaller than the contribution of sedi- mentary rocks. The Kliva Sandstone and lithologically similar Boryslav Sandstone (Oligocene) are mostly fine- to medium-grained and well- to moderately-sorted, although conglomeratic sandstones are also present. They are quartz-dom i nated; quartz is accom- panied by feldspar and muscovite, and glauconite is often pres- ent. Among exotic clasts, coal clasts, chert and siltstone are common. The sandstones are poorly cemented, mostly mas- sive, occasionally laminated (Żgiet, 1963; Kotlarczyk, 1966, 1976; Ślączka and Unrug, 1966). REMARKS ON PALAEOGEOGRAPHY The region stud ied, south-east of Rzeszów and south of Łańcut, refers to the northern marginal parts of the Skole Basin. To the north, the basin was surrounded by land or a shallow sea transitional to epicontinental basins (e.g., Książkiewicz, 1962; Bromowicz, 1974 and references therein). The palaeotransport directions indicate that the basin, for most of its development, was supplied mainly from its northwestern margin (e.g., Książkiewicz, 1962; Kotlarczyk, 1966, 1976; Ślączka and Unrug, 1966; Bromowicz, 1974; Kotlarczyk and Leśniak, 1990). Therefore, the area studied represents a region located close to the southern margin of the source area. During accumulation of the Ropianka Formation in the area studied, sedimentation fluctuated from low energy deposition represented by shaly flysch, through sandy and normal flysch up to the appearance of submarine slides (Bromowicz, 1974). The fluctuations were re I ated to activ ity along the northwestern source area termed Northern Cordil lera(s) or Marginal Cordil- lera (e.g., Książkiewicz, 1962; Bromowicz, 1974, 1986). How- ever, sea level changes and autocyclicity of the depositional system (probably deep-sea fans) should be also taken in the ac count. The sediments of the Boryslav and Kliva sandstones were deposI ted mostly from gravity flows in channel zones extend- ing south-east of Rzeszów and Łańcut, but similar deposits oc- cur also outside the main channel zones (Kotlarczyk and Leśniak, 1990). According to Kotlarczyk and Leśniak (1990) 652 Dorota Salata and Alfred Uchman Fig. 2. Stratig raphy of the Skole Nappe (based on Gasiński and Uchman, 2009 and references therein) with indication of the time-span intervals stud ied of the Ropianka and Menilite formations (grey rectan - gles) TRShMb - Trójca Red Shale Member, VSh - Vari egated Shale, ChSMb - Chmielnik Striped Sandstone Member and Kotlarczyk (1991), the channel zones were pro i onga-ion of canyons and rivers (Jucha, 1985). According to Kotlarczyk and Śliwowa (1963) and Kotlarczyk (1976), during sedimenta- tion of the lower part of the Menilite Formation, the clastic ma- terial was transported by rivers from nearby land where gentle slopes, beaches and coastal sandy dunes prevailed, in con- trast to the Campanian-Eocene interval, when, judging by the diversity and dimensions of exotic rock blocks (e.g., Bukowy, 1957; Kotlarczyk and Śliwowa, 1963; Skulich, 1986; Rajchel, 1990; Rajchel and Myszkowska, 1998), the source area in- cluded high cliffs. required mechanical crushing. Otherwise, only gentle disinte- gration was needed for further preparations of the prevail i ng part of samples. This ensured that original grain shape would be preserved. The clastic material was cleaned with water to re- move clays and sieved to obtain the 0.063-0.25 mm fraction, which was used for heavy mineral separa tion. Heavy minerals were separated using sodium polytungstate with 2.9 g/cm3 den- sity. Optical analyses were carried out on grain mounts in Can- ada balsam. 200 to 300 transparent, non-micaceous grains were counted accordi ng to the ribbon method and shown as number percentages (Galehouse, 1971). This conventional method was followed by the high resolution heavy mineral anal- ysis (HRHMA) applied to zircon and tourmaline populations. The sum of at least 75 grains of each species were counted. Colourl ess, pink to purple and zonal colourl ess and zonal pink varieties of zircon and brown, green, blue, pink and patchy and zonal tourmaline colour varieties were established as the chief categories. In each colour variety those minerals were categor- ised in terms of round i ng to three main groups rep resenti ng rounded, subrounded and an gu lar (in clud ing euhedral and pieces of euhedral) grains. The roundness degree was esti- mated accord i ng to the visual scale of Powers (1953). The group of euhedral zircon was additionally subdivided into zir- cons formi ng short or long prisms. Thirty six samples from the Ropianka Formation were studied using conventional and HRHMA methods and 36 samples of the Menilite Formation by means of the HRHMA method. The counti ng has not revealed significant differences in frequencies of zircon and tourmaline varieties between samples taken in outcrops stratigraphically and geographically located close to each other. Taking this into consideration and to overcome misleading differences resulting from sorti ng processes, the HRHMA data are shown as mean percent values of mineral varieties calculated for samples rep- resenting outcrops stratigraphically and geographically located near to each other. The calcu i ated standard deviations of min- eral contents between samples (s) were: s < 5 for con tent ranges of 10-90%; s < 2 for content ranges of 1-5% and s < 0.3 for the range lower than 1%. The HRHMA data of the Ropianka Formation shown in suitable figures were grouped as follow: Gaj (sample from Husów - Gaj); Patria area (samples from Husów - Patria and Bąkowiec); Husów (samples from Husów - Biedroniówka, Husów - Centrum, Husów - Dół); Tarnawka L. (sam ples from Tarnawka - leśniczówka A and B); Rzeki area (sam ples from Husów: the Bagnisty Stream and Rzeki: the Gąszcz Stream); Nieważka (sample from Nieważka); Tarnawka (samples from Tarnawka Quarry and Tarnawka 1-5); Manasterz (samples from Manasterz). Sample group i ng shown in figures showi ng the HRHMA data of the Menilite For- ma tion corresponds to profiles sampled by Salata and Uchman (2012). To avoid mis lead ing differences emerg i ng from the hy- draulic behaviour of minerals, heavy mineral assemblages oc- curring only in fine- to medium-grained deposits were taken into account for current comparative studies. Therefore, the miner- als from very-fine grained sandstones of the Hermanowa 1 sec- tion of the Menilite Formation (Salata and Uchman, 2012)were excluded from the current comparative studies. METHODOLOGY RESULTS The sampled rocks of both formations are represented mostly by weakly or even almost unconsol idated fine- to me- dium-grained sandstones and sands (Figs. 4-6; see also Salata and Uchman, 2012). Sandstones sampled in the Husów - Gaj and Husów - Bąkowiec sections were well-cemented and CONVENTIONAL HEAVY MINERAL STUDY Heavy mineral assemblages of the Campanian-Maastri- chtian part of the Ropianka and Menilite (Oligocene) formations in terms of mineral species are very simi l ar. Zircon, tourmal ine, Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 653 Fig. 3. Geological map of the Husów area (based on Wdowiarz, 1949; description of lithostratigraphic units modified according to Salata, 2013c) with indication of the sections studied of the Ropianka Formation 654 Dorota Salata and Alfred Uchman Fig. 4. Sampled profiles of the Ropianka Formation in the Husów Thrust Sheet Grain-size scale: cl - clay, vf - very fine sand, m - medium sand, vc - very coarse sand rutile, garnet, kyanite and staurolite are typical minerals of both forma- tions, while other mineral species are subordinate (Fig. 7). However, there are some differences in mineral fre- quencies. The Ropianka Formation displays relat ively higher amounts of zircon, garnet and apafite while the Menilite Formation contains compara- tively more kyan ite and staurolite and almost lacks apatite (Fig. 7). Besides, individual grains of hornblende were found only in the Ropianka Formation, while the Menilite Formation contains lo cally pres ent an da lu site, which was not found in the Ropianka Formation. The zircon-tourmaline-rutile index value (zircon + tourmaline + rutile = ZTR; Hubert, 1962) vari es across a broad range of 27-95% (mean value 63%) and 29-55% (mean value 43%) in the Ropianka and Menilite forma- tions, respectively. The Ropianka For- mation, in reiation to the Menilite For- mation, shows higher amounts of the ZTR, result ing mainly from elevated zircon frequencies (Figs. 8 and 9). To check if any corre i ation exi sts between ultrastable minerals, ex- pressed as the content of ZTR and garnet, staurolite and kyanite (the three main constituents outside zir- con, tourmaline and rutile) the Pear- son’s correlation coefficient (r) was applied. This index not only shows the strength of a linear relationship of a rank of values but also shows its di- rection. A positive correlation (r-val- ues from 0 to 1) informs that an in - crease in one variable is accompa- nied by an increase in the second one. A neg a tive cor re la tion (r-val ues from 0 to -1) indicates an increase in one variable accompanied by a de- crease in the second one. The clos- est to 1(-1) a value of the corre iation coefficient, the better is the reiaiion- ship between variables considered. A strong negative correlation be- tween the ZTR value and garnet con- tent (r = -0.90) and a moderate nega- tive correlation between ZTR and staurolite content (r = -0. 54) is pres- ent in the Ropianka Formation. This means that with decreasing ZTR, the content of garnet and staurolite in- creases (Fig. 9A, B). No correlation ex ists be tween the ZTR value and kyanite con tent in this formaiion (r = -0.18; Fig. 9C). In the Menilite For- mation, a weak (negative) correlation concerns only ZTR and garnet (r = -0.37). In the case of staurolite and kyanite from the Menilite Formation, Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 655 Fig. 5. Sampled profiles of the Ropianka Formation in the Marginal Thrust Sheet (section Husów - Gaj) and the Husów Thrust Sheet For explanations see Figure 4 656 Dorota Salata and Alfred Uchman Fig. 6. Sampled profiles of the Ropianka Formation in the Hadle Kanczudzkie-Chmielnik Thrust Sheet For explanations see Figure 4 Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 657 Fig. 7. Frequencies of heavy minerals in the Ropianka Formation compared to frequencies of minerals from selected samples of the Menilite Formation (data dealing with minerals of the Menilite Formation taken from Salata and Uchman, 2012) the relationship is reversed: the higher ZTR value the higher the amounts of these minerals, which is reflected in relatively strong and weak positive correlations of r = 0.89 and r = 0.28 respec- tively (Fig. 9B, C). Although there are some differences regarding mineral con- tents between the formations in question, the mineral habits are the same. Highly rounded, subrounded and euhedral grains are present in all heavy mineral species. Rounded and subrounded grains prevail in the zircon, tourma I ine (Figs. 10 and 11), and rutile populations. Garnet and staurolite, in both formations, most often occur as irregular, angular fragments, which may be pieces of rounded as well as euhedral grains. However, the presence of whole rounded and euhedral garnet was also de- tected. The same concerns the remain I ng minerals. In almost all mineral species features of dissolution processes, visible mainly as facets, hacksaw terminat ions or etch pits on grain surfaces, are present. The dissolution microtextures are adt vanced to various degrees, rang I ng from light to incipient in skeletal crystals. Nevertheless, mineral fragments with smooth fracture surfaces, and euhedral crystals, not significantly af- fected by dissol ut ion processes, are also present (see also Salata and Uchman, 2012). 658 Dorota Salata and Alfred Uchman Tur Menilite Formation Fig. 8. Mutual proportions of zircon, tourmaline and rutile shown in the tourmaline-rutile-zircon tri an gle HIGH-RESOLUTION HEAVY MINERAL ANALYSES Zircon varieties are almost iden-ical in both forma-ions studied (Fig. 10): rounded colourless varieties clearly prevail comprisi ng from 60 to 90% of the zircon popuia-ion. Subro- unded colourless zircon frequencies mostly vary in the range of 10-20% in both formations, rarely reaching 5-10% in the Ropianka Forma-ion and 20-30% in the Menilite Formation. Euhedral colourless zircon constitutes less than 5%, occasion- ally reachi ng ranges of 10-20% and 5-10% in the Ropianka and Menilite formations, respectively. Both elongated and short prisms of colourless zircon are present, al though elongated prisms are more frequent than short ones. Euhedral, long zir- con prisms are more frequent in the Ropianka Formation than in the Menilite Formation, reaching the range of 10-20% in the T arnawka - leśniczówka and Patria area profiles. Pink to purple zircon, without visible zonation, is represented by rounded grains (1-5%), while subrounded and euhedral grains are rare (<1% in individual samples). Zircon with oscillatory zonation is present mostly as rounded or subrounded colourl ess grains and comprises usually 1-5% or <1%, excep-ionally 10-20%, while euhedral zonal as well as pinki sh zonal zircon is very scarce in both formations (<1% or occasionally 1-5%; Fig. 10). Tourmaline varieties, like zircon, display typological simi- larity in both Ropianka and Menilite formations (Fig. 11). The most numerous group in both format ions comprises rounded (up to 80%) or subrounded (up to 50%), brown i sh, visually not zonal tourmaline. Greenish, rounded tourmaline comprises mostly 5-10% (occasionally 1-5% or 10-20%), while sub- rounded grains occur in amounts usually from 5 to 10% or 1-5%, reach i ng the range of 10-20% only in the Menilite For- ma-ion. Zonal and “patchy” (1-5% and <1%), blue and pink (both <1%) tourmal ine is scarce and rep resented mainly by rounded or subrounded grains. Euhedral tourmaline is not com- mon and is present dom i nantly as the brown variety (up to 20%), while other colour varieties of euhedral tourmaline usu- ally do not reach 1% in both formations (Fig. 11). ZTR [%] Fig. 9. Correlation between A - garnet (Grt), B - staurolite (St) and C - kyanite (Ky) and zircon + tourmaline + rutile (ZTR) values for the Menilite (Boryslav and Kliva sand- stones) and the Ropianka formations; r- Pearson's corre- lation coefficient DISCUSSION The compositional sim I iari ties of the heavy mineral assem- blages stud ied as well as the resemblance of the zircon and tourmaline varieties suggest that both the formations studied were supplied from lithologically sim iiar source area(s). Addn tionally, the occurrence of rounded along with subrounded and euhedral zircon and tourmaline varieties in both formations sug- gests that these sediments have a mixed polycyclic and first-cy- Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 659 00 rounded colourless subrounded colourless euhedral, short prismatic colourless euhedral, long prismatic colourless rounded pink t. rounded zonal Colourless Pink to purple Zonal colourless Zonal pink R SR A R SR A R SR A R SR A L S MENILITE FORMATION Siedliska 1 (n =1) 69.0 18.3 2.8 2.8 1.4 1.4 4.2 Hermanowa Ż. (n = 2) 66.2 19.5 5.2 2.6 3.9 2.6 Hermanowa 2 (n = 5) 75.6 10.1 6.9 2.8 2.8 0.9 0.9 Hucisko Jaw. (n = 2) 76.2 14.3 0.8 2.4 3.2 0.8 2.4 Siedliska 2 (n = 3) 45.3 28.8 5.3 2.4 0.6 11.2 6.5 Straszydle (n = 2) 67.0 12.5 0.5 2.6 0.3 0.7 Widaczów 1, 2 (n =9) 83.4 10.2 0.6 0.6 4.5 0.6 Tarnawka (n =12) 72.8 17.1 2.1 2.4 3.4 0.9 0.3 0.9 ROPIANKA FORMATION Gaj (n = 1) 78.4 9.5 1.4 5.4 4.1 1.4 Patria area (n = 3) 75.1 6.0 10.2 4.2 2.6 0.4 0.4 1.1 Husów (n = 5) 77.6 11.6 3.5 2.6 1.7 2.1 0.7 0.2 Tarnawka L. (n = 3) 61.7 14.1 10.2 4.9 1.9 5.8 1.5 Rzeki area (n = 6) 68.3 14.3 7.7 5.8 1.7 0.6 1.4 0.3 Nieważka (n = 1) 69.5 13.6 4.2 6.8 4.2 0.8 0.8 Manasterz (n = 4) 77.2 6.5 4.9 2.0 4.1 3.7 0.8 0.8 Tarnawka (n =13) 72.5 11.9 6.0 4.1 1.7 1.4 1.8 0.3 0.1 0.1 Fig. 10. Representative images of the most typical zircon varieties and frequencies of them in the Ropianka and Menilite for ma tions Numbers in the table denote mean percent values; n - number of samples studied; R - rounded grains; SR - subrounded grains; A - angui ar grains (euhedral crystals and fragments); scale bars are 0.1 mm long; see “Methodology” section for further explanation 660 Dorota Salata and Alfred Uchman rounded brown subrounded brown angular, euhedral brown rounded green rounded blue angular blue rounded pink rounded zonal Brown Green Blue Pink Patchy and zonal I Ft | | SR A R | SR A I R I SR | I A | I R I SR | A I R I I SR | A Location MENILITE FORMATION Siedliska 1 (n =1) 32.0 20.0 12.0 16.0 12.0 4.0 4.0 Hermanowa Ż. (n = 2) 22.0 45.0 10.0 3.7 11.0 3.7 0.9 3.7 Hermanowa 2 (n = 5) 51.0 26.5 2.0 8.2 6.5 0.8 0.4 0.4 0.4 2.4 1.2 Hucisko Jaw. (n = 2) 60.9 19.6 9.4 4.3 0.7 1.4 0.7 2.2 0.7 Siedliska 2 (n = 3) 31.6 41.2 11.0 6.6 7.4 1.5 0.7 Straszydle (n = 2) 65.0 25.1 0.7 7.1 4.1 0.5 0.5 Widaczów 1, 2 (n = 9) I 57.4 | 29.3 0.8 7.0 1.7 0.8 0.8 2.1 Tamawka (n =12) 63.6 22.2 1.5 6.9 2.5 1.8 0.7 0.4 0.4 ROPIANKA FORMATION Gaj (n = 1) 71.7 13.3 5.0 5.0 3.3 1.7 Patria area (n = 3) 62.6 13.2 1.7 9.8 6.3 2.3 0.6 0.6 2.3 0.6 Husów (n = 5) 48.5 24.4 7.1 8.8 5.5 1.1 0.3 0.3 0.3 0.5 1.9 1.4 Tamawka L. (n = 3) 32.0 23.8 16.8 5.3 12.7 5.3 0.8 0.4 0.8 0.8 0.4 0.8 Rzeki area (n = 6) 41.1 34.3 5.9 5.3 8.6 0.3 1.2 0.3 0.3 0.9 1.5 0.3 Nieważka (n =1) 41.9 31.4 10.5 7.0 4.7 1.2 2.3 1.2 Manasterz (n = 4) 56.9 24.5 6.7 4.7 2.8 0.8 0.4 2.8 0.4 Tamawka (n =13) 49.7 23.9 5.6 8.4 7.8 0.8 0.3 0.2 0.1 0.4 0.4 0.8 0.8 0.2 [%] 80-70 <70-60 <60-50 <50 i---40 <40-30 <30-20 <20- 10 ■ <10-5 <5 -1 <1 0 Fig. 11. Representative images of the most typical tourmaline varieties and frequencies of these in the Ropianka and Menilite formations Other explanations and abbreviations as for Figure 10; scale bars are 0.1 mm long cle provenance. However, since rounded grains prevail in these mineral populations, they seem to derive mainly from sedimen- tary rocks. Such a conclusion may be also drawn from the ZTR value, rang l ng widely from low to high values. However, the ZTR value alone may be misleading as it is largely controlled by the source rock composition. High ZTR values do not necessar- ily indicate delivery of multi-cycle sedimentary material since erosion of low-grade metasedimentary rocks, where zircon, tourmaline and rutile dominate as accessory minerals, may give the same index value (e.g., Garzanti and Ando, 2007). How- Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 661 NW SE Fig. 12. Schematic models (not to scale) of development of the northern margin of the studied part of the Skole Basin during sedimentation of the Ropianka and Menilite formations ever, the ZTR index is commonly used as an indicator of a de- gree of modification or maturity of heavy mineral assemblages. It is striking that the ZTR values versus garnet and staurolite and kyanite content correlation trends are always negative in the Ropianka Formation, while in the Menilite Formation only ZTR/garnet relationship is negative (Fig. 9). The negative correlations of ZTR values with garnet amounts, mean i ng that the lower the ZTR value the higher amount of garnet, may reflect first-cycle delivery of some part of garnet population to both formations. However, the correlation coefficient value closer to -1 for the ZTR-garnet pair in the Ropianka Formation (Fig. 9A) suggests a larger input of garnet coming directly from crystalline rocks during sedimentation of this formation than duri ng Menilite Formation deposition. The ZTR and staurolite relationship in the Ropianka Formation dis- plays the same negative trend as for ZTR-garnet, although the correiation is not as high as in the garnet case. This suggests that also staurolite in the Ropianka Formation may, to some ex- tent, orig i nate directly from its parent rocks. The same refers to kyanite, albeit the correlation of this mineral with ZTR, and thus the probabil i ty of its ori gin directly from parent rocks, is uncer- tain. The same negafive trends of reiafionship beiween ZTR and garnet, staurolite and, to lesser extent, kyanite suggest that these minerals were delivered during the same sedimentary ep isode and origi nate from the same source rocks. In case of the Menilite Formation the negative correlation vis ible only for the ZTR and garnet implies that garnet repre- sents first-cycle delivery. However, the correlation is worse than in the Ropianka Formation. The positive correlation trends con- cern the ZTR and staurolite and kyani te conient (Fig. 9B, C), which may indicate that staurolite and kyani te derive from sedi- mentary rocks or palimpsest sediments sensu McManus (1975), as the re lationships should rather be reversed for first-cycle input. The same concerns the low corre lation of gar- net with the ZTR value. Accord ing to McManus’s palimpsest definition, the garnet, staurolite and kyanite populations studied would accumu I ate at first on the basin shore or slope, mix with ZTR constituents delivered from sedimentary rocks and then would be redeposi ted to the basin together. Zircon, tourmal ine, rutile, staurolite and kyanite display comparable resistance to weathering (e.g., Morton and Hallsworth, 1999 and references therein), which may explain the similar trend in their relationship to the ZTR values. The primary heavy mineral signal of the source area, and thus the proposed view concernI ng mineral provenance based on the mineral relationships, may be easily obscured by changes in cli mate con di tions con trol ling weath er ing of the eroded material prior to its final deposition in the Skole Basin. The Carpathian flysch bas I ns remained in a temperate climatic zone (e.g., Kiessling et al., 2003) during the Late Cretaceous and Oligocene, although during the Cretaceous the climate was warm and humid, while during the Oligocene it was cool and hu- mid (e.g., Zachos et al., 2001; Friedrich et al., 2005; Melinte, 2005; Sotak, 2010; Kędzierski and Leszczyński, 2013 and ref- erences therein). Such a climatic change should reduce chemi- cal weather ing of primary heavy mineral suites as chemi cal weatheri ng should be more intensive in a warm and humid cli- mate. The content of garnet, kyanite and staurolite does not sig- nifi cantly differ between the formations studi ed, but those min- erals display different relationships with the ultrastable ZTR suite. Moreover, apatite, despite a warm and humid envi rant ment strongly in flu enc ing its weath er ing (e.g., Turner and Mor- 662 Dorota Salata and Alfred Uchman ton, 2007 and references therein), is present in the Ropianka Formation. However, there is a visi ble decrease in the apatite content and lack of hornblende in the Menilite Formation in comparison to the Ropianka Formation. The lackofamphibole is not surprising, since it is very unstable during burial diagenesis (e.g., Morton and Hallsworth, 1999, 2007; Turner and Morton, 2007 and references therein) but the significant decrease of apatite in the Menilite Formation is striki ng. More- over, the remained apat ite grains are mostly highly corroded, though only slightly corroded grains are infrequently present (Salata and Uchman, 2012). Such a coexistence of vari ously etched apatite indicates that the incipient corrosion of part of the apatite grains took place before its final deposition in the Skole Basin. The lack of apatite in the Menilite Formation has previ- ously been attributed to a prolonged storage in the Skole Basin fore land prior to deposition in the basin (Salata and Uchman, 2012). Apatite is stable during burial diagenesis but it is sensi- tive to storage conditions in coversands in a subaerial environ- ment (Morton and Hallsworth, 1999; Turnerand Morton, 2007 and references therein). Therefore, if apatite was present in the source rocks, its lack in the Menilite Formation may be caused by weatheri ng dun ng a long storage period. The impoveri shment in apat ite and hornblende caused by weathering during storage periods may result in a misleading interpretation of lithological change in a source area over time, though such a scenario should also be taken into account. Ac- cord I ng to this, initially (dun ng the Ropianka Formation sedi- mentation) rocks rich in garnet, apatite and stable minerals (zir- con, tourmaline, rutile) would be eroded and then (during the Menilite Formation sedimentation) rocks containing staurolite, kyani te and stable minerals became available. The change in source area petrography is also supported by the presence of andalusite only in the Menilite Formation. The assemblages composed of garnet, staurolite, kyanite and andalusite are characteristic of metamorphic bodies. Therefore, the remark on a change in source rocks petrography refers mainly to meta- morphic rocks. Recent data on the chem ical composit ion of garnet from the Ropianka and Menilite formations indicate its crystallisation mainly in metamorphic rocks of eclogite to am- phibo i ite facies and in igneous rocks (Salata, 2013a, c), which supports the metamorphic ori gin of garnet in both format ions deposits and the existence of metamorphic bodies in the source area. Judging by the similarities in composition of garnet from the Ropianka and Menilite formations and garnet occur- ring in crystal i ine rocks of the Bohemian Massif, as well as in detrital garnet delivered from the massif (e.g., Biernacka, 2012; Salata, 2013a, b and references therein) the metamorphic bod- ies may have similar lithology to those of the Bohemian Massif. The diversity of euhedral tourmaline and zircon varieties suggests petrographic variability of crystalline source rocks. Brown tourmaline, typical of the schorl-dravite series, is not highly diagnostic since it may crystal i ise in igneous as well as metamorphic rocks. However, euhedral blue and pinkvarieties (although very scarce), suggesting elbaitic tourmaline composi- tion, imply the presence of granites and pegmatites in the source area. The occurrence of igneous rocks is additionally in- dicated by the presence of elongated euhedral zircon, which is characteristic of rapidly cooled, porphyritic, shallow, sub-volca- nic bodies of granite and gabbro, while euhedral short prismatic zircon crystals suggest, in turn, provenance from deeply situ- ated, slowly cooled igneous intrusions (e.g., Corfu et al., 2003). The fact that sharp euhedral zircon and blue and pink euhedral tourmaline are a minor component in the heavy mineral popula- tions studied may indicate that igneous bodies in the source re- gion were not large compared to the contribution from sedimen- tary or metasedimentary rocks. To verify the hypothesis based on heavy mineral analyses the data obtained should be compared with the types of pebbles occurring in the formations studied. Rock fragments occurring in sandstones of the Ropianka Formation in the area of investi- gation are dom i nated by sed i mentary rocks among which Ju- rassic limestones of the Stramberk-type prevail but quartz sandstones and coal clasts are also present (Wdowiarz, 1949). The group of crystal line rocks is represented by igneous and metamorphic fragments compris i ng up to 32 and 9%, respec- tively (see Bromowicz, 1974). Igneous rocks are mainly gran- ites while metamorphic rocks are represented by gneisses (Wdowiarz, 1949), metaquartzites and phyllites (Bromowicz, 1974, 1986 and references therein). According to Bromowicz (1974, 1986), judging by the frequency of pebbles, the contribu- tion of crystalline rocks in the source area was smaller than that of sedi mentary rocks. Such an inference may be also drawn from heavy mineral stud ies presented in this paper. In the re- gion south-east of the area stud ied (near Bircza), Ropianka Formation sandstones, beside the kinds of pebbles noted above, contain also porphyritic andesite and dacite clasts (Nowak, 1963). The Kliva Sandstone of the Menilite Formation, in contrast to the Ropianka Formation, does not contain such numerous and diverse clasts of exotic rocks, be ing dom t nated by sand. Among the pebbles mostly sedi mentary rocks, coal fragments and coal-beari ng shales have been described (Kotlarczyk and Śliwowa, 1963; Ślączka and Unrug, 1966; Kotlarczyk, 1976). Some information about crystalline pebbles come from the Widaczów area (Wdowiarz, 1949; D. Salata, A. Uchman, K. Du- dek, pers. comm., 2013) and from the middle part of the Menilite Formation at Borek Nowy (Kotlarczyk, 1985), which implies that crystal line rocks may have been exposed not only during the Ropianka Formation sedimentation but also during the Menilite Formation sedimentation. However, specific lithological variet- ies and frequencies of crystalline rock pebbles in the Widaczów area remain currently unspecified. The heavy mineral correlation trends juxtaposed with the small contribution of pebbles in the Menilite Formation and their larger contribution in the Ropianka Formation may reflect evolu- tion of the source area. The area may have evolved from an ini- tially elevated, rap î dly eroded landscape (an immature passive margin), during sedimentation of the Campanian-Maastrichtian part of the Ropianka Formation (Upper Cretaceous-Paleocene), to a more subdued (mature passive margin) landscape, slowly eroded during accumulation of the Kliva and Boryslav sandstone types of the Menilite Formation (Oligocene) (Fig. 12). This infer- ence may explain the del ivery of a large part of the garnet and staurolite directly from their source rocks and thus the negative correlation trend of these minerals with the ZTR value in the part of the Ropianka Formation studied. During sedimentation of the Menilite Formation, a mature margin of the basin foreland devel- oped as topograph ically less diverse areas with low ret ief, which favoured longer storage periods prior to deposition in the basin. In consequence, palimpsest sediments could develop, which could be redepos rted later to deeper parts of the basin, result ng in the positive correlation of kyanite and staurolite with the ZTR value. The longer storage period may also explain the lack of ap- atite in the Menilite Formation. This model of local foreland evolu- tion based on heavy mineral analyses is in agreement with the views by Kotlarczyk and Śliwowa (1963) and Kotlarczyk (1976), who suggested sandy beaches and coastal dunes at the margin of the Skole Basin during sedimentation of the Kliva Sandstone. Conventional and high-resolution heavy mineral analyses applied to flysch deposits. 663 CONCLUSIONS Heavy mineral assemblages of the Ropianka and Menilite formations display comparable compositions in terms of min- eral species and their varieties, which suggests provenance of minerals from lithologically similar rocks during sedimentation of both formations. Heavy mineral assemblages display different frequencies of some mineral species be tween the format ions. The Campa - nian-Maastrichtian part stud i ed of the Ropianka Formation re- veals higher amounts of zircon, garnet and apatite and traces of hornblende, while the Menilite Formation has a relatively higher content of staurolite and kyanite and coniains andaiusite, but lacks ap a tite and am phi bole. Negative correlation trends of the ZTR and garnet and staurolite conient in both formations suggest that part of the garnet and staurolite population represent first-cycle delivery. Additionally, better correlation of ZTR and garnetcontentforthe Ropianka Formation, compared to the Menilite Formation, sug- gests that direct delivery of first-cycle garnet was greater during the Ropianka Formation sedimentation. Positive correlation trends between the ZTR value and staurolite and kyani te con- tent in the Menilite Formation suggest that these minerals could origin, to large degree, from sedi meniary rocks or pa limpsest sediments. Zircon and tourmaline varieties and their frequen- cies are very simi l ar in both format ions, suggesti ng that diver- sity of their host rocks in the source area did not change signifi- cantly in time. All these conclusions may reflect differences in first-cyt cle/re-cycled minerals ratio in clastic input during sedimentation of the formations stud I ed. The data suggest that first-cycle ma- terial and direct delivery were greater durl ng the Ropianka For- mation sedimentation, while during deposition of the Menilite Formation the contribution of material delivered from erosion of sedimentary rocks or redeposition of palimpsest sediments was prom i nent. Mineral frequencies and ratios in the intervals studied of the Ropianka and Menilite formations, when compared with litera- ture data concerning exotic rock pebbles, reflect evolution of the source area from an initially elevated (immature passive mar- gin) landscape, during sedimentation of the Ropianka Forma- tion, to more subdued (mature passive margin) landscape dur- ing accumulation of the Menilite Formation. Integrated conventional and high-resolution analyses ap- plied to comparat ive study of depleted heavy mineral assem- blages, enable to determination of the provenance of minerals in mixed first-cycle and re-cycled clastic mate rial, which is a necessary basis for further research. Acknowledgements. The manuscript benefited from sug- gestions and comments of J. Rajchel (AGH University of Sci- ence and Technology), J. Biernacka (University of Poznań) and an anonymous reviewer, to whom we are kindly grateful. 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