GeolCarp_Vol64_No1_3

www.geologicacarpathica.sk

GEOLOGICA CARPATHICA

, FEBRUARY 2013, 64, 1, 3—22 doi: 10.2478/geoca-2013-0001

Introduction

The primary role of provenance studies is to reconstruct the
history of sedimentary rock and to interpret the rock-assem-
blage  of  the  source  area  (Weltje  &  von  Eynatten  2004).  To
this end, the combination of bulk rock and single grain ana-
lytical approaches has been shown to provide comprehensive
insights  into  the  provenance  of  sedimentary  rocks  (e.g.  von
Eynatten 2003; Meinhold et al. 2007; Mikes et al. 2008). Al-
though processes of weathering and erosion, as well as meta-
morphism, commonly alter and remove valuable provenance
information, certain trace element indicators are sufficiently
resilient to survive such destructive processes. Many studies,
both on sedimentary (e.g. Bathia 1985; Bathia & Crook 1986;
McLennan  et  al.  1993),  and  metasedimentary  (e.g.  Slack  &
Höy 2000; Augustsson & Bahlburg 2008) rocks, have shown
that  geochemical  data  can  be  successfully  used  to  study  the
composition and reveal the geotectonic environment of source
rocks,  especially  when  coupled  with  petrography  and  heavy
mineral  assemblages.  Furthermore,  various  studies,  where
analysis is focused on one particular mineral species, are less

Provenance of Paleozoic very low- to low-grade

metasedimentary rocks of South Tisia (Slavonian

Mountains, Radlovac Complex, Croatia)

VANJA BIŠEVAC

, ERWIN KRENN

, FRITZ FINGER

, BORNA LUŽAR-OBERITER

and

DRAŽEN BALEN

Institute of Mineralogy and Petrology, Department of Geology, Faculty of Science, University of Zagreb, Horvatovac 95,

HR-10000 Zagreb, Croatia; vabisevac@geol.pmf.hr

Institute of Geology and Paleontology, Department of Geology, Faculty of Science, University of Zagreb, Horvatovac 102,

HR-10000 Zagreb, Croatia

Division of Mineralogy, Department of Materials Engineering and Physics, University of Salzburg, Hellbrunnerstrasse 34,

5020 Salzburg, Austria

(Manuscript received April 23, 2012; accepted in revised form June 13, 2012)

Abstract: Monazite age dating, detrital heavy mineral content and whole-rock geochemistry provided insight into the
provenance, depositional history and paleogeological setting of the Radlovac Complex very low- to low-grade
metasedimentary rocks (South Tisia, Slavonian Mountains, Croatia). Electron microprobe based Th-U-Pb dating of
detrital monazite indicates a Variscan age of the protolith (330 ± 10 Ma). The detrital heavy mineral assemblages of
representative metasedimentary rocks are dominated by apatite, zircon, tourmaline and rutile accompanied by minor
quantity of epidote/zoisite, monazite and titanite. Judging from the heavy mineral assemblage, felsic igneous rocks
served as the source material. This is consistent with the major and trace element spectrum of studied metasedimentary
rocks characterized by high concentration of Th, high L + MREEs and high ratios of La/Sc, Th/Sc, La/Co, Th/Co and
Th/Cr. The occurrence of magmatic monazite, zircon and xenotime and the absence of metamorphic heavy minerals
suggest that granitoids, migmatites and migmatitic gneisses served as one major source for the metapsammites. Such
rock types are commonly exposed in the Papuk Complex of the older surrounding complexes, while the Psunj Complex
also contains metamorphic rocks. This is in good correlation with the monazite ages presented here which fits better
with ages of Papuk Complex representative rocks than with those of the Psunj Complex known from the literature.
Overall, data show that the Radlovac Complex represents the detritus of the local Variscan crust characterized by
granitoid bodies, migmatites and migmatitic gneisses typical for the Papuk Complex.

Key words: South Tisia, Slavonian Mts, Radlovac Complex, metasedimentary rocks, geochemistry, geochronology,
provenance, heavy minerals, detrital monazite.

affected by the aforementioned processes and are able to re-
veal specific provenance related information (e.g. Hallsworth
et al. 2000; Willner et al. 2001; von Eynatten & Wijbrans
2003; Zack et al. 2004).

From the Radlovac Complex, which occupies the highest

structural  position  of  all  Variscan  complexes  in  the
Slavonian Mountains (Jamičić 1983, 1988; Jamičić & Brkić
1987;  Jamičić  et  al.  1987),  no  provenance  study  has  been
carried  out  although  some  authors  contributed  to  the  origin
of  the  Radlovac  Complex  (e.g.  Brkić  et  al.  1974;  Jamičić
1988).  In  this  study  we  present  results  from  the  Radlovac
Complex which comprises very low- to low-grade metasedi-
mentary  rocks  with  intrusions  of  metabasic  rocks  (Jamičić
1983, 1988; Pamić & Jamičić 1986). We present results from
mineral  and  whole-rock  chemical  analysis  of  16  selected
fresh samples including 8 metapelites and 8 metapsammites.
For  comparison,  additional  7  representative  samples  from
the surrounding igneous-metamorphic complexes were used
for  testing  possible  relations  and  the  provenance  model  of
Jamičić  (1988).  The  analytical  data  include  petrography,
heavy mineral composition analyses, zircon typology, chemi-

BIŠEVAC, KRENN, FINGER, LUŽAR-OBERITER and BALEN

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

cal composition and Th-U-Pb chemical age dating of mona-
zite  and  xenotime  and  whole-rock  geochemistry  including
major, trace and REE element composition. The aim of this
study  is  to  provide  more  detailed  insight  into  the  prove-
nance,  depositional  history  and  paleogeological  setting  of
the  Radlovac  Complex  metasedimentary  rocks  and  to  pro-
vide a good basis for correlation with other similar very low-
to low-grade metamorphic complexes within Tisia.

Geological setting

Tisia is regarded as a microcontinent that broke off from the

southern margin of Variscan Europe during the opening of the
Tethys  (Géczy  1973;  Fülöp  et  al.  1987;  Tari  &  Pamić  1998;
Haas et al. 2000; Pamić et al. 2002; Stampfli et al. 2002; Haas
& Péró 2004; Schmid et al. 2008). Following a complex drift
history, Tisia became incorporated into the Alpine fold belt in
the  Cretaceous  (Csontos  1995;  Márton  2000,  2001).  Tisia  is
built  up  by  three  southward  dipping  Alpine  nappe  systems
(Mecsek, Villány-Bihor and Békés-Codru) (Fig. 1), each com-
prising  igneous  and  metamorphic  basement  rocks  and  post-
Variscan overstep sequences (Haas & Péró 2004; Csontos &
Vörös 2004; Schmid et al. 2008). According to Schmid et al.
(2008)  the  Slavonian  Mountains  belong  to  the  Villány-Bihor
nappe system (Fig. 1) and represent rare basement outcrops of
Tisia (Pamić et al. 1996; Pamić & Jurković 2002).

Following Jamičić (1983, 1988) three tectono-metamorphic

complexes can be defined in the Slavonian Mountains: Psunj
Complex  (PsC),  Papuk  Complex  (PaC)  and  Radlovac  Com-
plex (RC). The RC, which is the target of this research, con-
sists of very low- to low-grade metamorphic sequences largely
composed  of  metapelites  (slates  and  subordinate  phyllites),
metapsammites  (metagreywackes)  and  metaconglomerates
deposited in the shallow marine environment (Jamičić 1988).
According to Pamić & Jamičić (1986) the deepest part of RC
is represented by violet, and grey to silverish white schistose
metagreywackes  which  grade  into  quartz  metaconglomerates
in  some  places  (Fig. 2).  The  middle  parts  are  made  of  violet
and  greyish  finer-grained  schistose  metagreywackes  (Fig. 2)
interlayered with dark greyish slates containing Westphalian
microflora. The highest part of the Radlovac Complex con-
sists mostly red to brownish slates and phyllites (Fig. 2) rarely
interlayered  by  fine-grained  metapsammites.  Based  on  the
structural  and  paleofloristic  data  Jamičić  (1988)  assumed
that the RC was metamorphosed during the late stages of the
Variscan  orogeny  (Late  Paleozoic;  ~ 320—260 Ma),  while
Biševac et al. (2010), using Kübler & Árkai indices accompa-
nied  by  K-Ar  dating  of  illite-muscovite  rich  fractions,  found
evidence  for  Cretaceous  very  low-  to  low-grade  overprint
( ~ 100—80 Ma). The lower and middle parts of the RC are in-
truded  by  metabasic  rocks  which,  according  to  Pamić  &
Jamičić  (1986)  show  clear  signs  of  metamorphic  alteration
with plagioclase metamorphosed into clinozoisite and sericite
accompanied  by  newly  formed  sodic  plagioclase,  while  cli-
nopyroxene  is  moderately  to  strongly  altered  to  fine-grained
aggregate  of  chlorite,  uralite  and  epidote.  Based  on  the  field
relations  the  RC  unconformably  overlies  the  PsC  (Jamičić
1983, 1988) and contains a Westphalian microflora (Brkić et

al. 1974) which documents a Pennsylvanian age of the pro-
tolith.  Since  the  Westphalian  microflora  was  found  in  the
middle pocket of the RC, Pamić & Jamičić (1986) presumed
that the higher parts of the complex belong to the Lower Per-
mian and deeper parts probably to the Upper Devonian. Fur-
thermore,  the  K-Ar  dating  on  clinopyroxene  monomineralic
concentrate from ophitic metagabbro, which intruded the RC
(Pamić  &  Jamičić  1986),  gave  ages  of  416. 0 ± 9.0  and
318.6 ± 12.2 Ma (Pamić et al. 1988; Pamić & Lanphere 1991)
which are partly consistent with paleofloristic determinations.
The  K-Ar  age  determinations  on  two  slates  from  Paleozoic
complexes  yielded  K-Ar  whole-rock  ages  of  203.9 ± 6.9  Ma
and  100.6 ± 3.5 Ma,  which,  according  to  Pamić  et  al.  (1988),
apparently represent partially or completely reset ages, due to
subsequent  heating.  Jamičić  (1988)  proposed  a  model,  based
on  paleofloristic  and  structural  data,  in  which  the  metasedi-
mentary  rocks  of  the  Radlovac  Complex  are  considered  to
represent  the  detritus  of  the  surrounding  igneous  and  meta-
morphic  rocks  of  the  local  pre-Variscan  and  Variscan  crust
(PsC and PaC Complexes, respectively). While RC transgres-
sively overlay the PsC from one side, it is in tectonic contact
with PaC from the other (Fig. 1). The geological evolution of
the  surrounding  rocks  is  also  quite  complex  and  interesting.
The  PsC  is  assumed  to  be  formed  by  a  metamorphic  event
during the Baikalian orogeny (Late Precambrian to Early Pa-
leozoic)  and  overprinted  and  retrogressed  by  younger  meta-
morphic  events  (Jamičić  1988).  It  contains  green  schist  to
amphibolite facies rocks occurring in association with metaba-
sites.  The  K-Ar  ages  on  hornblende  monomineralic  concen-
trate  from  amphibolites  yielded  Variscan  ages  ranging  from
376.4 ± 11.5—352.6 ± 8.5 Ma (Pamić et al. 1988; Pamić 1998).
These  metamorphic  rocks  are  intruded  by  small  bodies  of
I-type  granites  of  Variscan  age  ranging  from  423.7 ± 12.9  to
336.3 ± 8.4 Ma based on the K-Ar dating of muscovite (Pamić
et al. 1988, 1996; Pamić & Lanphere 1991). The PaC endured,
according to Jamičić (1988), metamorphism and migmatitiza-
tion during the Caledonian orogeny (Ordovician to Early De-
vonian;  ~ 490—390 Ma).  It  consists  predominantly  of  S-type
granites  joined  by  migmatites  and  migmatitic  gneisses  of
Variscan age (K-Ar ages of biotite and muscovite fall between
272.2 ± 6.4—336.3 ± 8.4 Ma;  Pamić  et  al.  1988),  which  grade
into amphibolite facies sequences composed of garnetiferous
amphibolites,  paragneisses  and  mica-schists  (Pamić  1986;
Pamić & Lanphere 1991).

Regarding the metamorphic evolution of the Slavonian

Mountains,  there  is  a  general  agreement  about  medium-  to
high-grade pre-Variscan and Variscan metamorphism (Balen
et al. 2006; Horvath et al. 2010). Some authors attributed a
great  role  to  a  late  Variscan  low-grade  metamorphic  event
(Jamičić 1988), while new studies (Biševac et al. 2010, 2011)
show  the  existence  of  Cretaceous  low-T  regional  metamor-
phism in the area.

Analytical methods

Research on representative metasedimentary rock samples

sampled in several quarries and profiles along the roads and
rivers involved thin section and heavy mineral slide analyses

BIŠEVAC, KRENN, FINGER, LUŽAR-OBERITER and BALEN

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

grains were separated manually by hand-picking using bino-
cular lens. Zircon photographs used for zircon typology study
were obtained by TESCAN scanning electron microscope
equipped with back-scatter electron detector and operated at
20 kV at the Department of Geology, Faculty of Science, Uni-
versity of Zagreb. The zircons were carbon coated.

Results

Petrography

Metasedimentary rocks of the Radlovac Complex are well

exposed in several quarries and road-cuts along the Radlovač-
ka River (Fig. 1) in the central part of the complex going from
SW  to  NE  (Fig. 3a)  and  along  the  road  north  of  the  town  of
Velika (Fig. 3b). The most common metasedimentary rocks of
the  RC  are  fine-grained  metapelites  and  moderately  sorted
metapsammites. Here, the term metapelite stands for metased-
imentary  rock  containing  > 70 %  fine-grained  matrix,  while
the  term  metapsammite  is  used  for  metasedimentary  rocks
containing  < 40 % of matrix. Both groups have similar mineral
composition  with  dominant  quartz,  illite-muscovite,  chlorite
and plagioclase, subordinate K-feldspar, paragonite and hema-
tite and rare carbonate minerals (Table 1). Reddish, green and
grey coloured metapelites are characterized by typical micro-
lepidoblastic  texture,  while  characteristic  spaced  cleavage  is
defined by elongated quartz grains (20—50  m), detrital mus-
covite  flakes  and  dominant  fine-grained  micaceous-chlorite
mixture  (Fig. 3c).  Typical  metapsammites  show  schistosity
marked by subparallel muscovite flakes and elongated quartz
grains with apparent grain sizes of 50—300 µm, and compris-
ing  subordinate  plagioclase  embedded  in  clay-  to  silt-sized
matrix  of  recrystallized  quartz,  illite-muscovite  and  chlorite,
and  in  some  samples  paragonite  (Fig. 3d).  Since  the  matrix
content for all samples is relatively high and signs of mineral-

Table 1: Semiquantitative mineral composition of the Radlovac Complex metasedimentary rocks together with heavy mineral data of the
representative metapsammites.

Radlovac Complex metasedimentary rocks

Metapsammites

Metapelites

Sample

R1 R2 R3 R4 R5 R6 R7 R8 R9 R10 R11 R12 R13 R14 R15 R16

Lithology

Msn CMgr Mgr Msn CMgr Mgr Msn Msn Phy Slt Phy Phy Phy Phy Slt Slt

Mineral composition
Quartz

Illite-muscovite

Plagioclase

K-feldspar –

–

Chlorite

Hematite –

–

Paragonite –

–

x –

–

Calcite –

–

Heavy minerals (%)
Zircon 34

Tourmaline

Rutile

Apatite 34

Epidote/Zoisite

–

Monazite +

–

Titanite –

–

Unindentified

Msn — metasandstone
CMgr — conglomeratic metagreywacke
Mgr — metagreywacke
Phy — phyllite
Slt — slate

— dominant; — abundant; — significant; x — poor;

+ — present, but below 0.5 %; – — not present.

ogical  alteration  are  evident,  modal  composition  of  the  sam-
ples  was  not  determined.  Signs  of  alteration  of  feldspars  to
clay minerals occur in all samples (Fig. 3e). Other alterations
include  syndeformational  growth  of  sericite/quartz  strain
fringes in the pressure shadows of detrital quartz (Fig. 3f) and
plagioclase.  This  interesting  feature  indicates  the  percolation
of K-rich fluids (Sutton et al. 1990; Frimmel 1994), a charac-
teristic phenomenon for the green schist facies metasedimen-
tary rocks (Bucher & Frey 1994).

The detrital heavy mineral assemblages of the studied Ra-

dlovac representative metapsammites are dominated by apa-
tite  and  other  minerals  like  zircon,  tourmaline  and  rutile
(Table 1).  Other  heavy  minerals  such  as  epidote/zoisite,
monazite and titanite occur in trace amounts. Apatite occurs
both as fresh and partially altered grains, mostly colourless,
sometimes with a brownish core. Grains are usually irregular
in shape or stubby prisms. Zircons mostly occur as irregular
and fragmented grains, translucent to yellowish or brownish
in  colour.  Euhedral  grains  are  also  commonly  encountered.
Tourmaline grains are dominantly irregular in shape and per-
vasively  display  green-brown  to  yellowish  pleochroic  co-
lours,  although  the  prismatic  crystals  can  be  observed.
Authigenic  tourmaline  is  sporadically  encountered  as  over-
growths. Monazite is discussed in a separate chapter.

Monazite age dating

Monazite was studied in the metapsammite samples R1 and

in the metapelite sample R15 which served as two representa-
tive  samples  from  the  Radlovac  Complex.  Monazite  from
sample  R1  is  ca.  20—50 µm  large  (Fig. 4),  sub-anhedral  and
occurs in the matrix as well as inclusions in coarse muscovite
and quartz. The grain boundaries are irregular and partly re-
sorbed. The chemical Th-U-Pb dates of single monazite anal-
yses  are  listed  in  Table 2.  Analyses  from  both  core  and  rim
domains exclusively provide Variscan ages, which combined

BIŠEVAC, KRENN, FINGER, LUŽAR-OBERITER and BALEN

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

criminated  according  to  their  chemistry.  Type 1  xenotime  is
characterized  by  higher  U  and  Th  (0.66—3.19 wt. %  and
0.2—0.56 wt. %,  respectively)  compared  to  type 2  xenotime
(0.18—0.26 wt. %  and  0.12—0.16 wt. %,  respectively)  (Fig. 9a).
Additionally,  type 1  xenotime  has  lower  Eu

(up to

0.12 wt. %), Dy

(2.63—4.22 wt. %) and Gd

(3.73—

4.71 wt. %) and higher Yb

(2.97—5.46 wt. %) compared to

(0.93—1.11 wt. %), Dy

(4.90—5.06 wt. %) and

(8.71—9.32 wt. %) and Yb

(1.31—1.37 wt. %) char-

acteristic for type 2 xenotime (Table 4; Fig. 9b and c).

Whole-rock geochemistry

The whole-rock element composition of the studied

metasediments is presented in Appendix. Metapsammites
have higher average SiO

and lower Al

, Fe

, MgO,

O and K

O (Appendix) compared to metapelites which

correlates with the dominance of quartz in the metapsammites
and  that  of  clay  minerals  and  hematite  in  metapelites  (Ta-
ble 1).  Metapsammites  can  be  characterized  by  a  felsic  bulk
composition  with  ca.  61—77 wt. %  SiO

10—18 wt. % Al

Table 2: Concentration (wt. %) and age data for monazite and xenotime from samples R1 and R15 calculated after Montel et al. (1996).
Th* values are after Suzuki et al. (1991). Formation temperatures of monazite calculated after Pyle et al. (2001), Heinrich et al. (1997) and
Gratz & Heinrich (1997) are also shown. ** – possible contamination due to the small grain size.

Formation temperature (°C)

Sample

Position Matrix

(wt. %)

Th*

(wt. %)

Age ± 2

(Ma)

X(Xtm) Pyle et al.

(2001)

Heinrich et al.

(1997)

Gratz &

Heinrich (1997)

Monazite
R1 Mzt1-2

rim

Qz–Ms

3.510

1.123

0.095

7.153

298 22

0.09

584

674

675

R1 Mtz1-3

core

Qz–Ms

3.447

0.750

0.090

5.887

345 27

0.07

518

614

579

R1 Mzt2

core

5.085

0.310

0.083

6.092

304 26

0.08

561

653

642

R1 Mzt3

core

Qz–Ms

5.017

0.333

0.076

6.094

281 26

0.07

535

629

603

R1 Mzt4

rim

Qz–Ms

3.739

0.573

0.084

5.602

335 28

0.08

555

647

632

R1 Mzt5

rim

4.741

0.783

0.113

7.288

347 22

0.09

601

689

700

Mzt6

rim Ab–Qz 2.973 0.363 0.054 4.149 291 38 0.07

521

617

584

R1 Mzt7

core

7.950

0.158

0.124

8.465

327 19

0.05

408

515

418

R1 Mzt7

rim

3.219

0.103

0.049

3.554

307 45

0.03

220

344

141

R1 Mzt8

core

5.241

1.173

0.125

9.047

309 25

0.06

463

565

498

Mzt9

core Qz–Ms 6.313 1.559 0.174 11.387 343 20 0.12

669

751

801

R1 Mzt10

rim

3.935

0.518

0.091

5.623

361 28

0.03

222

346

145

R1 Mzt11

core

6.541

2.164

0.192

13.572

318 17

0.07

520

616

582

R1 Mzt12

core

2.695

0.845

0.084

5.446

347 29

0.09

589

679

683

R1 Mzt13

rim

4.257

1.168

0.125

8.061

348 20

0.06

494

592

543

R1 Mzt14

core

5.124

0.662

0.100

7.274

309 22

0.08

573

664

659

Mzt15

rim Qz–Ms 6.076 1.339 0.166 10.440 357 21 0.03

301

418

261

R1 Mzt16

rim

Qz–Ms

4.243

1.202

0.133

8.160

365 19

0.07

518

614

578

R1 Mzt17

rim

4.793

0.673

0.107

6.985

343 23

0.08

569

661

654

R1 Mzt18

core

3.906

0.131

0.062

4.332

321 37

0.05

440

543

464

R1 Mzt18

rim

3.779

0.121

0.062

4.174

332 38

0.06

451

553

480

R1 Mzt19

rim

3.847

0.779

0.091

6.377

320 25

0.13

697

776

841

**R15

Mzt1

small Ab–Qz 0.837 0.031 0.020 0.940 – –

0.02

184

312

**R15 Mzt2

small

0.330

0.081

0.027

0.607

–

0.02

200

–92

**R15 Mzt3

small

0.399

0.027

0.017

0.491

–

0.02

160

290

**R15 Mzt4

small

Qz–Ms

0.120

0.109

0.017

0.489

–

0.01

–73

–289

Xenotime
R1 Xtm1

core

0.172

0.586

0.048

2.103

–

R1 Xtm2

core

0.471

2.403

0.116

8.276

317 27

–

R1 Xtm3

core

Zrn

0.130

0.234

0.053

0.950

–

R1 Xtm4

core

0.482

2.816

0.127

9.616

298 23

–

R1 Xtm5

core

Zrn

0.144

0.213

0.023

0.852

–

R1 Xtm6

core

0.492

2.622

0.115

8.989

288 25

–

R1 Xtm7

core

Zrn

0.108

0.181

0.030

0.724

–

R1 Xtm8

core

Zrn

0.103

0.160

0.023

0.644

–

Fig. 7. Monazite formation temperature according to thermometers
of Gratz & Heinrich (1997), Heinrich et al. (1997) and Pyle et al.
(2001).

PALEOZOIC VERY LOW- TO LOW-GRADE METASEDIMENTARY ROCKS (SOUTH TISIA, CROATIA)

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

Sample

R1 R1 R1 R1 R1 R1 R1 R1 R1 R1 R15 R15

Mzt1-2

Mtz1-3 Mzt2 Mzt3 Mzt7 Mzt7 Mzt9 Mzt15 Mzt18 Mzt18

Mzt1

Mzt3

Position

rim core core core core rim core rim core rim core core

Matrix

Qz–Ms

Qz–Ms Ms Qz–Ms Qz Ms Qz–Ms

Qz–Ms Qz Qz Ms Qz–Ms

Fig. 4-2 Fig. 4-3

Fig. 4-1

SiO

0.25 0.35 0.38 0.41 1.89 0.65 0.42 0.46 0.51 0.53 1.38 0.97

29.24 30.15 28.70 29.14 26.94 28.55 29.08 29.06 29.16 28.86 27.76 29.40

CaO 0.93 0.79 0.87 0.91 0.20 0.11 1.47 1.30 0.52 0.47 2.43 2.61
Y

2.25 1.78 2.04 1.73 0.57 0.38 3.85 0.79 1.04 1.09 0.05 0.16

12.66 11.92 9.65 8.35 11.96 13.86 11.04 13.14 12.51 11.95 13.47 12.91

29.37 29.45 27.97 28.15 29.94 34.00 27.22 29.91 30.77 30.87 31.78 31.49

3.16 3.15 3.15 3.50 3.24 3.63 2.79 2.96 3.41 3.49 3.16 3.20

12.37 12.64 14.01 14.27 10.63 11.29 11.47 11.40 12.43 12.22 11.36 12.33

2.27 2.19 3.42 3.73 2.91 2.75 2.22 1.99 2.59 2.58 1.85 1.90

2.29 1.98 2.27 2.27 1.68 1.23 1.75 1.12 1.94 1.92 0.85 1.15

0.69 0.53 0.45 0.47 0.31 0.12 0.86 0.16 0.46 0.51 0.18 0.15

0.14 0.09 0.08 0.09 0.05 0.01 0.08 0.05 0.06 0.07 0.01 0.04

ThO

3.99 3.92 5.79 5.71 9.05 3.66 7.18 6.91 4.44 4.30 0.38 0.45

1.27 0.85 0.35 0.38 0.18 0.12 1.77 1.52 0.15 0.14 0.09 0.03

PbO

0.10 0.10 0.09 0.08 0.14 0.05 0.19 0.18 0.07 0.07 0.03 0.02

Total 101.00 99.88 99.23 99.17 99.68 100.42 101.45 100.95 100.08 99.07 94.77 96.80

a.p.f.u. based on 4 oxygens

0.01 0.01 0.02 0.02 0.08 0.03 0.02 0.02 0.02 0.02 0.05 0.04

0.97 0.99 0.97 0.98 0.92 0.96 0.96 0.97 0.97 0.98 0.90 0.93

0.04 0.03 0.04 0.04 0.01 0.00 0.06 0.06 0.02 0.02 0.10 0.10

0.05 0.04 0.04 0.04 0.01 0.01 0.08 0.02 0.02 0.02 0.00 0.00

0.18 0.17 0.14 0.12 0.18 0.20 0.16 0.19 0.18 0.18 0.19 0.18

0.42 0.42 0.41 0.41 0.44 0.50 0.39 0.43 0.44 0.45 0.44 0.43

0.05 0.04 0.05 0.05 0.05 0.05 0.04 0.04 0.05 0.05 0.04 0.04

0.17 0.18 0.20 0.20 0.15 0.16 0.16 0.16 0.18 0.17 0.16 0.17

0.03 0.03 0.05 0.05 0.04 0.04 0.03 0.03 0.04 0.04 0.02 0.02

0.03 0.03 0.03 0.03 0.02 0.02 0.02 0.01 0.03 0.03 0.01 0.01

0.01 0.01 0.01 0.01 0.00 0.00 0.01 0.00 0.01 0.01 0.00 0.00

0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00

0.04 0.03 0.05 0.05 0.08 0.03 0.06 0.06 0.04 0.04 0.00 0.00

0.01 0.01 0.00 0.00 0.00 0.00 0.02 0.01 0.00 0.00 0.00 0.00

0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00

Tetr. 0.98 1.01 0.99 1.00 1.00 0.99 0.98 0.99 0.99 1.00 1.01 1.01
A[9] 1.03 0.99 1.02 1.00 1.00 1.02 1.04 1.02 1.01 1.01 1.01 1.01

** — possible contamination due to the small grain size; Tetr. = Si + P; A[9] = REE + Th + U + Pb + Ca + Y

Table 3: Selected electron microprobe analyses (wt. %) of monazite from samples R1 and R15.

Fig. 8. Back-scattered electron (BSE) images of xenotime in metapsammite sample R1. a – Igneous-detrital xenotime showing brighter
and darker domains. b – Hydrothermal xenotime occurring as overgrowth on detrital zircon grain. Mineral abbreviations after Whitney &
Evans (2010). Qz – quartz, Xtm –xenotime, Zrn – zircon, Ms – muscovite, Ilm – ilmenite.

BIŠEVAC, KRENN, FINGER, LUŽAR-OBERITER and BALEN

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

1—6 wt. % Fe

(Appendix) while metapelites contain ca.

49—62 wt. % SiO

, 15—27 wt. % Al

and 6—7 wt. % Fe

(Appendix). However, due to the varying clay fraction in meta-
psammites with up to 40 %, some of them overlap chemically
with metapelites and show relatively high A/CNK (Appendix).

Zr/Sc and Hf/Sc ratios for metapsammites (12—39 and

0.3—1.2,  respectively)  are  somewhat  higher  then  those  for
metapelites (8—16 and 0.2—0.5, respectively) (Appendix). The
discrimination  scheme  of  Roser  &  Korsch  (1988)  based  on
major elements shown in Fig. 10 indicate dominant input from
primary  felsic  sources  for  metapelites,  while  metapsammites
fall into the border of the recycled sources field and primary
felsic  source  field  (Fig. 10).  The  diagrams  shown  in  Fig. 11,
which are based on trace, relatively immobile, elements indi-
cate dominant input of felsic igneous rocks for all samples.

Eu anomalies (Eu/Eu* = 0.6—0.8 for metapsammites;

Eu/Eu* = 0.6—0.7 for metapelites) are present (Appendix).

Table 4: Electron microprobe analyses (wt. %) of xenotime from sample R1.

Sample

R1 Xtm1

R1 Xtm2

R1 Xtm3

R1 Xtm4

R1 Xtm5

R1 Xtm6

R1 Xtm7

R1 Xtm8

Position core core core core core core core core
Matrix

Qz Zrn Qz Zrn Qz Zrn Zrn

Origin

Igneous-

detrital

Igneous-

detrital

Hydrothermal

Igneous-

detrital

Hydrothermal

Igneous-

detrital

Hydrothermal Hydrothermal

SiO

0.02 0.71 0.11 0.77 0.14 0.64 0.10 0.17

0.00 0.00 0.24 0.11 0.23 0.00 0.04 0.08

35.67

35.33

35.52

34.04

35.42

35.23

34.76

34.57

CaO

0.06 0.03 0.08 0.02 0.13 0.02 0.13 0.14

45.34

42.49

42.01

42.14

42.84

43.24

43.76

43.58

0.01 0.09 0.00 0.00 0.05 0.10 0.11 0.10

0.18 0.12 0.14 0.10 0.10 0.00 0.16 0.10

0.21 0.00 0.01 0.21 0.09 0.09 0.16 0.08

0.55 0.21 0.53 0.23 0.52 0.28 0.63 0.68

0.52 0.40 1.48 0.41 1.38 0.24 1.48 1.53

0.00 0.12 0.93 0.00 0.95 0.00 1.11 0.98

4.71 3.88 8.89 3.73 9.11 3.75 8.71 9.32

4.22 2.71 4.90 2.69 4.92 2.63 5.07 5.06

3.30

4.18 2.44 4.31 2.42 4.45 2.28 2.45

O3 2.97 5.01 1.31 5.46 1.33 5.40 1.37 1.34

ThO

0.20 0.54 0.15 0.55 0.16 0.56 0.12 0.12

0.66 2.73 0.26 3.19 0.24 2.97 0.20 0.18

PbO 0.04 0.12 0.06 0.13 0.03 0.10 0.03 0.03
Total

98.66

98.67

99.06

98.13

100.09

99.72

100.26

100.58

a.p.f.u. based on 4 oxygens

0.001 0.024 0.004 0.026 0.005 0.021 0.003 0.006

1.004 1.000 1.004 0.982 0.995 0.994 0.985 0.979

0.000 0.000 0.009 0.004 0.009 0.000 0.002 0.003

0.002 0.001 0.003 0.001 0.004 0.001 0.005 0.005

0.802 0.756 0.746 0.764 0.757 0.767 0.779 0.776

0.000 0.001 0.000 0.000 0.001 0.001 0.001 0.001

0.002 0.001 0.002 0.001 0.001 0.000 0.002 0.001

0.002 0.000 0.000 0.003 0.001 0.001 0.002 0.001

0.007 0.003 0.006 0.003 0.006 0.003 0.007 0.008

0.006 0.005 0.017 0.005 0.016 0.003 0.017 0.018

0.052 0.043 0.098 0.042 0.100 0.041 0.097 0.103

0.000 0.001 0.011 0.000 0.011 0.000 0.013 0.011

0.045 0.029 0.053 0.030 0.053 0.028 0.055 0.055

0.034 0.044 0.026 0.046 0.025 0.047 0.024 0.026

0.030 0.051 0.013 0.057 0.013 0.055 0.014 0.014

0.001 0.004 0.001 0.004 0.001 0.004 0.001 0.001

0.005 0.020 0.002 0.024 0.002 0.022 0.002 0.001

0.000 0.001 0.001 0.001 0.000 0.001 0.000 0.000

Tetr.

1.005 1.024 1.008 1.009 1.001 1.015 0.989 0.987

A[9]

0.990 0.961 0.988 0.985 1.001 0.974 1.020 1.024

Tetr. = Si + P; A[9] = REE + Th + U + Pb + Ca + Y

The values of provenance-indicative element ratios for both
investigated  groups  of  samples,  such  as  Th/Sc,  Th/Co  and
La/Sc (Appendix), are close or slightly above those for Upper
Continental  Crust  (UCC),  and  according  to  Cullers  (2000,
2002)  and  McLennan  et  al.  (1993)  indicate  dominant  felsic
protolith source (Figs. 11 and 12).

The REE signatures of metapsammites and metapelites are

similar and match those from the NASC (North American
Shale Composite) and UCC (Fig. 13). The REE development
of the surrounding older crystalline complexes, namely the
Papuk Complex and the Psunj Complex (Fig. 13) can hardly
be discriminated.

Zircon typology

Zircon grains from representative metapsammites (R1 and

R2) were studied by means of zircon typology (Pupin 1980).

BIŠEVAC, KRENN, FINGER, LUŽAR-OBERITER and BALEN

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

(2003), a direct consequence of variable degrees of substitu-
tion of HREEs, U and Th for Y during magmatic growth, is
consistent with their igneous origin. This is in good correla-
tion with xenotime data of varied origin (igneous, hydrother-
mal  and  diagenetic)  known  from  the  literature  (Kositcin  et
al.  2003  and  references  therein)  (Fig. 9).  Diagenetic  xeno-
time  was  not  detected.  Although,  the  xenotime  grains  were
not suitable for dating due to low Th (especially hydrother-
mal  grains),  the  igneous-detrital  xenotime  seems  to  be
Variscan (Table 2) implying a Variscan igneous source con-
sistent with the detrital monazite ages.

In the case of the hydrothermal xenotime it is possible that

they formed during the Alpine metamorphism.

Monazite grains found in samples R15 are smaller and

have  lower  Th  and  Y  content  indicative  for  low  formation
temperatures (e.g. Read et al. 1987; Rasmussen et al. 2001,
2007; Evans et al. 2002; Rasmussen & Muhling 2007, 2009;
Wan et al. 2007; Wilby et al. 2007), all the more, as the bulk
has  relatively  high  Th  and  Y  contents  (Appendix).  Bearing
in  mind  the  age  dating  and  temperatures  recorded  on  illite
fractions presented in Biševac et al. (2009, 2010), we can as-
sume  that  the  population  of  Th-  and  Y-monazites  found  in
sample R15 are Alpine (Cretaceous).

Heavy mineral assemblage

Heavy mineral analysis is one of the most sensitive and

widely-used  techniques  for  determination  of  the  provenance
of  (meta)sedimentary  rocks  providing  constraints  on  the
mineralogical  nature  of  the  source  terrains  (Morton  &
Hallsworth 1999). The detrital heavy mineral assemblages of
Radlovac  Complex  representative  metapsammites  are  domi-
nated  by  apatite  and  minerals  like  zircon,  tourmaline  and
rutile. Additionally, minor quantity of epidote/zoisite, mona-
zite and titanite can be found. Since the weathering of the par-
ent rocks is a very important factor controlling the diversity of
detrital heavy minerals in weathering profiles and later during
sedimentation,  the  heavy  mineral  assemblage  of  Radlovac
representative  metapsammites  indicate  weathering-limited
erosion.  Under  such  conditions  detritus  is  quickly  removed
without  significant  modification  by  chemical  weathering
(Johnsson et al. 1991), consistent with the presence of detrital
apatite as the most abundant, but least stable mineral in weath-
ering profile (Morton & Hallsworth 1999). Since apatite is a
useful key mineral to detect the influence of acidic groundwa-
ter  percolation  and  tends  to  be  unstable  under  acidic  condi-
tions  (Morton  &  Hallsworth  1999),  its  high  abundance
indicates the lack of acidic condition. The occurrence of other
minerals (zircon, tourmaline and rutile) is not surprising since
they show high stability in weathering profiles, but the presence
of epidote/zoisite and lack of garnet and staurolite belonging to
intermediate  stability  group  (Morton  &  Hallsworth  1999)  as
well as, for example, pyroxenes, calcic amphibole or olivine in-
dicate  that  metamorphic  and/or  basic  igneous  rocks  did  not
serve  as  source  rocks  for  the  Radlovac  Complex  metasedi-
mentary rocks. The presence of detrital igneous monazite and
xenotime further argue for felsic igneous rocks as protolith.

Zircons occur both as irregular fragmented grains and as eu-

hedral grains. The higher degree of roundness for some zircon

grains  than  for  quartz  and  feldspar  grains  in  coarser-grained
samples is probably the result of a minor degree of sedimentary
recycling, since zircons are less prone to crystal growth dur-
ing  low-grade  metamorphism  than  are  quartz  and  feldspar
(Augustsson  &  Bahlburg  2008).  The  euhedral  to  slightly
abraded zircon originated mainly from I-type and subordinately
S-type granites (Fig. 14), also indicating that the protolith ma-
terial  is  characterized  by  shorter  transportation  paths.  The
length/width  ratio  of  zircons  show  that  they  originated  from
magma  characterized  by  slow  to  intermediate  crystallization.
The presence of euhedral zircons in association with prismatic
crystals of tourmaline highlights the significance of the first-
cycle input as well as short transportation.

Geochemistry

The variation of major elements between the two groups of

samples  (metapelites  and  metapsammites)  primarily  reflects
the  effect  of  grain  size.  Since  metapelites  contain  more  clay
fraction  it  is  expected  to  be  richer  in,  for  example,  Al

or Na

O. The bulk chemistry as well as La/Sc, Th/Sc,

La/Co,  Th/Co  and  Th/Cr  values  for  both  metapelites  and
metapsammites  (Appendix),  which  are,  according  to  Cullers
(2000), indicative when evaluating source rocks, point to fel-
sic igneous rocks as protolith for RC metasedimentary rocks.
This is in good correlation with the heavy mineral assemblage
discussed earlier and other discrimination diagrams (Figs. 10,
11 and 12). The diagram in Figure 12 shows that some meta-
psammite  samples  (R2  and  R5)  (Fig. 2)  plot  in  the  passive
margin field (Fig. 12), which can indicate that they comprise
felsic,  old  crustal,  recycled  detritus  (Augustsson  &  Bahlburg
2008). The other metapsammite samples show a trend, which
can be interpreted as due to temporal compositional variations
of the provenance (Fig. 11).

Metapelites have a REE concentration and a Th/Sc, Th/Co

and La/Sc similar to that of UCC (Fig. 11), while the REE con-
centrations  for  metapsammites  are  lower  than  UCC  (Fig. 13)
and Th/Sc, Th/Co and La/Sc values are higher than UCC (Ap-
pendix).  Although,  this  could  imply  that  metapsammites  were
partly affected by sedimentary recycling as discussed earlier, at
least during the initial stages of Radlovac Complex sedimenta-
tion,  we  believe  this  is  the  direct  consequence  of  Sc  content
controlled by grain-size, namely the abundant clay minerals in
metapelites.  Since  Sc  is  often  deposited  in  clay  minerals  to-
gether with iron and aluminium due to their similar ionic radius
(Das et al. 1971), this is in good agreement with higher content
of both Al

and Fe

(Appendix) in metapelites indicating

the  higher  phyllosilicate  content  mostly  related  to  the  fine-
grained  matrix  consisting  predominately  of  illite-muscovite,
chlorite  and  hematite.  Eu  anomalies  (Eu/Eu* = 0.6—0.8  for
metapsammites;  Eu/Eu* = 0.6—0.7  for  metapelites)  are  similar
for both groups and reflect lithospheric or intracrustal fraction-
ation  or  the  breakdown  of  feldspar  during  weathering  and/or
metamorphic processes (see Condie et al. 1995).

Paleogeological settings

Paleogeological settings can be estimated on the basis of

discrimination diagrams using major element and trace ele-

PALEOZOIC VERY LOW- TO LOW-GRADE METASEDIMENTARY ROCKS (SOUTH TISIA, CROATIA)

GEOLOGICA CARPATHICA

GEOLOGICA CARPATHICA, 2013, 64, 1, 3—22

ment  data.  However,  since  the  chemistry  of  the  major  ele-
ments can be modified in conditions of very low- to low-grade
metamorphism due to their mobility, trace elements and lan-
thanides are frequently used for investigating the paleogeolog-
ical  setting  of  low-grade  metasedimentary  rocks.  Elements
such as La, Ce, Nd, Y, Th, Zr, Hf, Nb, Ti, and Sc are consid-
ered as the best indicators (Holland 1978; Bathia 1985; Bathia
& Crook 1986; McLennan et al. 1993; Slack & Hoy 2000) and
were used here to identify the geotectonic setting of the Radlo-
vac  metasedimentary  rocks.  Most  of  the  samples  plot  into
field of continental island arc, very similar to UCC and NASC
(Fig. 12). In this geotectonic environment depositional basins
were  formed  on  a  well-developed  continental  crust  or  thin
continental margin. Sediments deposited along the continental
island arc would be expected to be immature and less recycled
due to smaller individual catchment areas, shorter transporta-
tion  path  and  intermediate-quick  storage  which  is  in  agree-
ment with the chemical “signature” of the samples presented
here.  Comparison  to  data  from  the  presently  exposed  sur-
rounding basement rocks of the Slavonia Mts imply that local
Variscan  crust  could  serve  as  the  protolith  for  the  Radlovac
Complex  metasedimentary  rocks  (Fig. 12).  Granitoid  bodies
of I- and S-type characteristic for the area together with mig-
matites and migmatitic gneisses characteristic for Papuk Com-
plex served as the protolith for all the samples deposited in the
continental  island  arc.  Zircon  typology  studies  of  metapsam-
mites  of  the  Radlovac  Complex  (Fig. 14)  compared  with  zir-
cons  of  representative  samples  of  Papuk  Complex  show  great
similarity and further confirm their genetic connection (Biševac
2009).  Metapsammites  characteristic  for  the  lower  part  of  the
Radlovac Complex (R2 and R5) and granitoid rocks character-
istic for Psunj Complex projected in passive margin field imply-
ing their genetic connection. This is in good agreement with the
model  proposed  by  Jamičić  (1988)  according  to  which  the
Psunj  Complex  rocks  served  as  the  dominant  protolith  during
the initial phases of the Radlovac Complex sedimentation.

Conclusions

1. Monazite, xenotime and the spectrum of heavy earth

minerals  suggest  that  one  major  source  for  the  Radlovac
Complex metasedimentary rocks was felsic, igneous rocks of
Variscan  age.  The  Variscan  age  is  supported  by  chemical
Th-U-Pb monazite age dating. From the high xenotime con-
tents and Y-rich monazite, which suggest formation temper-
atures  of  > 600—800 °C,  we  can  conclude  that  the  Y-rich
monazite grains come from a magmatic source.

2. The chemistry and morphology of type 1 xenotime (igne-

ous-detrital)  is  another  argument  that  the  metasedimentary
rocks  of  the  Radlovac  Complex  were  fed  strongly  by  mag-
matic  igneous  rocks.  Observed  zonation  in  type 1  xenotime
as a direct consequence of variable degrees of substitution of
HREEs, U and Th for Y during magmatic growth, is consis-
tent with their igneous origin. The igneous-detrital xenotime
seems  to  be  Variscan  implying  a  Variscan  igneous  source
consistent with the detrital monazite ages.

3. The detrital heavy mineral assemblages of the Radlovac

Complex representative metapsammites are dominated by

apatite and minerals like zircon, tourmaline and rutile ac-
companied by minor quantities of epidote/zoisite, monazite
and titanite. Such assemblages further argue for felsic igne-
ous rocks as protoliths.

4. The bulk chemistry as well as La/Sc, Th/Sc, La/Co, Th/Co

and Th/Cr values for both metapelites and metapsammites
point to felsic igneous rocks as protoliths for the Radlovac
Complex metasedimentary rocks. This is in good correlation
with the heavy mineral assemblage.

5. Elements such as La, Ce, Nd, Y, Th, Zr, Hf, Nb, Ti, and

Sc were used to identify the geotectonic setting of the Radlo-
vac  metasedimentary  rocks.  Most  of  the  samples  plot  into
the field of continental island arcs, very similar to UCC and
NASC.  In  this  geotectonic  environment  depositional  basins
were  formed  on  a  well-developed  continental  crust  or  thin
continental margin.

6. Comparison to the presently exposed surrounding base-

ment  rocks  of  the  Slavonian  Mts,  data  implies  that  local
Variscan crust could serve as protolith for the Radlovac Com-
plex  metasedimentary  rocks.  The  granitoid  bodies  of  I-  and
S-type  characteristic  for  the  area  together  with  migmatites
and  migmatitic  gneisses  characteristic  for  Papuk  Complex
served as protolith for all samples deposited in the continen-
tal island arc.

7. The provenance study of the RC metasedimentary rocks

based on Th-U-Pb monazite chemical age dating, heavy min-
eral  assemblage  and  whole-rock  geochemistry  leads  to  the
conclusion  that  the  metasedimentary  rocks  of  the  Radlovac
Complex  represent  the  detritus  of  the  local  Variscan  crust,
while Papuk Complex rocks were dominant source material.

8. The identification of the provenance in this study resulted

from combination of several independent analytical tech-
niques supporting the importance of combining different
methods in provenance studies.

Acknowledgments: The authors would like to thank the re-
viewers for their stimulating and constructive comments, as
well  as  the  Editor  for  handling  the  manuscript.  This  study
was  supported  by  the  Croatian  Ministry  of  Science,  Educa-
tion  and  Sports,  Project  No.  119-1191155-1156  and  by  the
Austrian Science Foundation (FWF), Project No. 22408.

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