doi: 10.1111/j.1365-3121.2006.00710.

Fluid inclusion evidence for deep burial of the Tertiary

accretionary wedge of the Carpathians
Vratislav Hurai,1 Frantisek Marko,2 Antoni K. Tokarski,3 Anna Swierczewska,3 Julia Kotulova4 and
Adrian Biron5
Departments of 1Mineralogy and Petrology; and 2Geology and Paleontology, Comenius University, 842 15 Bratislava, Slovakia; 3Institute of
Geological Sciences, Polish Academy of Science, 31-002 Krakow, Poland; 4Geological Survey of Slovakia, 841 05 Bratislava, Slovakia;
5
Geological Institute, Slovak Academy of Sciences, 974 01 Banska Bystrica, Slovakia

ABSTRACT
Hydrothermal quartz from mineralized joints of the Carpathian
accretionary wedge contains immiscible aqueous, oil-conden-
sate, methane and carbon dioxide-rich fluid inclusions. Distri-
bution patterns of the inclusion trapping PT parameters point to
a crack-seal mechanism during upward and lateral migration of
hot methane-rich fluids from overpressured sediments at the
base of the accretionary wedge. A simple equation is proposed
to calculate depths from densities and trapping pressures of the
buoyant inclusion fluids. In the Carpathian accretionary wedge,
the paleofluid pressures of 52306 MPa correspond to a 5- to
11-km-thick overburden. Prior to exhumation, thickness of the
wedge must have attained 1025 km, of which only c. 50% was
preserved until recently. Anomalously high methane densities
(up to 0.43 g cm)3) recorded in the lowermost nappe sheets are
provisionally interpreted as a result of supralithostatic over-
pressure due to thermal cracking of oil and kerogen to methane
and pyrobitumen at temperatures above 200 C.
Terra Nova, 18, 440446, 2006

Introduction
The non-metamorphosed Tertiary
accretionary wedge of the Carpathian
orogenic system belongs to few thrust-
and-fold belts with economically
important oil and gas deposits. In
such orogenic systems, knowledge on
thermal history and depth of burial is
essential for identication of potential
source rocks, uid migration paths
and location of possible hydrocarbon
traps. Balanced modelling based on
reection seismic proles and struc-
tural data provides a tool for recon-
struction of burial history,
quantication of erosion, shortening
and potential trap-destruction proces-
ses. Controversial quantication of
the balanced proles in the Carpathi-
ans (Behrmann et al., 2000; Posp s il
et al., 2005b; Nemcok et al., 2006)
stems partly in the absence of data
on paleothickness of the accretionary
wedge, because some of the original
nappe units could have been removed
during subduction (Nemcok et al.,
1998) or exhumation.
Correspondence: Prof. Vratislav Hurai,
Department of Mineralogy and Petrology,
Comenius University, Mlynska Dolina,
Bratislava 842 15, Slovakia. Tel.: +42
12 65 31 64 60; fax: +42 12 65 31 62 93;
e-mail: huraiova@fns.uniba.sk
Fluid inclusions are essential source
of information on thermal and pres-
sure history of non-metamorphosed
accretionary complexes. Moreover,
the uid inclusions are most sensitive
geological barometers, from which
also other parameters, such as depths
of burial and geothermal gradients,
can be derived. According to recent
models of rock rheology (e.g. Sibson,
1990; Holbrook, 1999) and leak-o
data from sedimentary basins (Gaa-
renstroom et al., 1993), pore uid
pressure cannot exceed the lithostatic
load plus cohesive (tensile) strength of
the rock without fracturing and reset-
ting the hydrostatic pressure gradient.
Hence, the depth of burial is com-
monly calculated from uid inclusion
trapping pressures assuming either
hydrostatic or lithostatic loads, and
geological constraints. However, in
the case of trapping a buoyant hetero-
geneous uid, the inferred depths are
subject to a large error margin due to
the unknown bulk uid density and
the magnitude of uid overpressure.
A crack-seal mechanism (Ramsay,
1980) and uid buoyancy eect (Sa-
hagian and Proussevitch, 1992) were
employed in this article to quantita-
tively interpret large pressure uctua-
tions of buoyant uids percolating
through open cavities in ysch sedi-
ments of the Tertiary accretionary
wedge and the associated fore-arc
basin of the Outer Western Carpathi-
ans during crystallisation of drusy
quartz. The results show that the
accretionary wedge must have been
substantially thicker than recently
assumed in tectonic models and
balanced cross-sections.
Geological Background
The Carpathian segment of the Euro-
pean Alpine orogenic system consists
of several rootless nappes composed
of Early CretaceousMiocene ysch
sediments detached along single
decollement horizon and thrust north-
ward over shallow-marine Neogene
molasse and the underlying platforms
(e.g. Picha, 1996). A weakly deformed
Eocene-to-Early Miocene fore-arc y-
sch basin (Gedl, 2000; Sotak et al.,
2001; Kazmer et al., 2003) overlies
Variscan crystalline basement and its
Mesozoic cover and nappe units south
of a steep suture-like zone called the
Pieniny klippen belt, which provides
hinterland termination of the accre-
tionary wedge and the boundary
between the outer and inner Carpa-
thians (Fig. 1).
Mineralized joints of the Creta-
ceousOligocene ysch sandstones
contain several generations of brous,
columnar, blocky and drusy calcite
and quartz, having precipitated during
syn-sedimentary folding, thrusting

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Terra Nova, Vol 18, No. 6, 440446 V. Hurai et al. Deep burial of Tertiary accretionary wedge
.............................................................................................................................................................

Fig. 1 Simplied geological map of the study area redrawn from the geological map 1:500 000 (Lexa et al., 2000). Circles with
orange, blue and white sectors denote relative proportions of oil-condensate, carbon dioxide and methane, respectively, in carbonic
uid inclusions. Non-numbered circles denote outcrops, numbered circles are boreholes: 1, Zborov 1 (37145156 m); 2, Hanus ovce
1 (4469 m); 3, Zboj 1 (38964146 m); 4, Lipany 5 (1996 m); numbers in parentheses pertain to depth intervals with the
corresponding uid inclusion composition.

and counter clockwise rotation of the
accretionary wedge (Swierczewska
et al., 2000). Blocky and drusy quartz
studied represent the last generation
formed in central open uid-lled
cavities (Fig. 2a) because of an exten-
sion correlated with a post-Oligocene
collapse and exhumation of the accre-
tionary wedge (Swierczewska et al.,
2000; Tokarski et al., 2006).
Oil-condensate, methane and car-
bon dioxide are the main carbonic
compounds of uid inclusions hosted
in blocky and drusy quartz. Fluid
composition in the quartz diers
strongly from earlier quartz and cal-
cite generations, which contain only
low-to-moderately saline aqueous
solutions. At room temperature, the
oil-condensate inclusions consist of
one to four phases: transparent
oil-condensate liquid, methane-con-
densate vapour bubble, pale green-
to-dark brown heavy liquid oil, and
dark brown-to-opaque solid hydro-
carbons. The oil-condensate phase
uoresce white-to-pale blue under
365 nm UV light (Fig. 2b). Methane
forms mostly monophase liquid inclu-
sions. An additional liquid discernible
in the CH4-rich inclusions corres-
ponds either to oil or to aqueous
solution, and variable phase ratios
indicate trapping a heterogeneous
methanewater mixture (Fig. 2c).
Carbon dioxide-rich inclusions consist
mostly of single liquid phase, and are
thus indistinguishable from the mono-
phase methane inclusions at room
temperature. The presence of carbon
dioxide at room temperature is some-
times indicated by a liquidliquid
vapour phase assemblage diagnostic
of a composite CO2-rich aqueous uid
(Fig. 2d).
Methane with up to 8 mol% of
carbon dioxide is typical of mineral-
ized joints of the Magura nappe and
the underlying Dukla unit, both crop-
ping out in the innermost part of the
accretionary complex. Higher gaseous
hydrocarbons and crude oil accom-
pany the methane in the proximity of
organic-rich Oligocene shales called
Menilite Beds in the Dukla unit. CO2
CH4 mixtures passing in places into
almost pure carbon dioxide liquid are
typical of the Zboj unit underlying
both the Magura nappe and the Du-
kla unit. Oil- and methane-rich con-
densate occurs in the Eocene
Oligocene strata of fore-arc basin,
except for segment uplifted north of
the sub-Tatric fault, where methane
devoid of higher hydrocarbons is the
dominant carbonic species (Fig. 1).
Aqueous solutions accompany the
carbonic compounds in the whole
area. Their salinities range between 0
and 3.2 wt% and most likely reect
mixing of meteoric and marine waters
in the fracture uids.
Temperature and Pressure
In majority of cases, uid inclusions in
quartz are quite reliable indicators of
crystallization PT conditions, because
of retaining their original density dur-
ing tectonic transport to Earths sur-
face. Inclusions of heterogeneous
uids consisting of two or more
immiscible phases with contrasting
densities and compositions are most
useful geothermobarometers (Roed-
der and Bodnar, 1980). The hetero-
geneous uid mixtures are identiable
according to variable phase ratios in
coeval inclusions (Fig. 2c). Methane
(CO2)aqueous mixtures are suit-
able for determination of their trap-
ping PT parameters; because their
composition and density can be easily
inferred from temperatures of phase
transitions on cooling and heating
with assistance from experimental

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Deep burial of Tertiary accretionary wedge V. Hurai et al. Terra Nova, Vol 18, No. 6, 440446
.............................................................................................................................................................

Fig. 2 (a) Photomicrograph of mineralized joints in ysch sandstone, illustrating early fracture lled with columnar calcite
intersected by a later composite fracture lled with columnar calcite at margins and blocky calcite and quartz in the centre. (b)
Primary inclusions of oil-condensate from quartz veins in Middle Oligocene strata of the western part of fore-arc basin, near to
Pucov village. Inset illustrates UV uorescence (365 nm) image of the same inclusions. (c) Pseudosecondary inclusions in quartz
from methane zone of the forearc basin (Middle-Upper Eocene sandstones, Zalesie, Spis ska Magura Mountains), containing
variable proportions of methane and aqueous liquids. Monophase inclusions are composed of methane liquid. Homogenization
temperature of the aqueous inclusion with the smallest bubble marked by arrow corresponds to true trapping temperature. (d)
CO2-bearing aqueous inclusions in quartz from carbon dioxide zone of the accretionary complex. Zboj unit, Upper Eocene-Lower
Oligocene, Zboj-1 borehole, 4164 m. Black bars correspond to 1 mm in (a) and 20 lm in (b)(d).

phase diagrams and equations of state
(e.g. Holloway, 1981; Kleinrahm and
Wagner, 1986; Thiery et al., 1994). In
statistically relevant number of meas-
urements, the minimal homogeniza-
tion temperature (Th) of aqueous
inclusions equals that of trapping,
whereas trapping pressure is dened
by the iso-density line (isochore) of the
coexisting methane inclusion (Vityk
et al., 1996; Evans and Battles, 1999;
Hurai et al., 2002). Total pressure
correction for water dissolved in the
methane and for expansion of the host
quartz is lower than 4 MPa in the
temperature range of 160240 C and
the pressures up to 300 MPa (V. Hu-
rai, in preparation).
In the study area, methane-rich
inclusions show wider scatter of trap-
ping temperatures in the fore-arc
basin and the Magura nappe com-
pared with those in the Dukla and the
underlying Zboj units (Fig. 3). The
temperature scatter, tending to reduc-
tion with depth, is interpreted as
reecting inux of hot uid into colder
sediments. Hence, the minimal uid
inclusion trapping temperature is
likely to approach that of rock,
whereas the maximal temperature
equals that of the incoming uid. This
interpretation is supported by the
d13C values of inclusion methane from
drusy quartz of the fore-arc basin
()31& V-PDB) typical of a thermo-
genic dry gas. The thermogenic
methane with d13C )36& was also
detected in the drusy quartz of the
Dukla unit (Hurai et al., 2002), where
the minimal uid inclusion trapping
temperature of 195 C (i.e. presuma-
ble rock temperature) exceeded the
minimum oil cracking limit of 180 C
(Tissot and Welte, 1984).
Pressures inferred from densities of
methane inclusions (Fig. 3) tend to
increase from 52180 MPa in the fore-
arc basin, to 76200 MPa in the Ma-
gura nappe and to 109370 MPa in
the underlying Dukla unit. Maximum
uid pressures (450 MPa) and tem-
peratures (246 C) have been recorded
in the Zboj unit underlying the Dukla
unit and the Magura nappe. The
strongly uctuating pressures in the
individual tectonic units most likely
reect cyclically changing hydrostatic
and lithostatic regimes caused by a
crack-seal mechanism (Ramsay, 1980;

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Terra Nova, Vol 18, No. 6, 440446
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Fig. 3 Temperatures and pressures derived from coeval methane-rich and aqueous
inclusions in blocky and drusy quartz using the microthermometry data and
equations of state (EOS) for CH4 (Kleinrahm and Wagner, 1986) and CO2CH4
systems (Holloway, 1981; Thiery et al., 1994). Crosses in the upper right diagram
correspond to data from the Middle-Upper Eocene Strihov beds of the Krynica unit
of the Magura nappe transected in the depth of 4469 m in the Hanus ovce-1 borehole.
Holbrook, 1999). The same mechan-
ism is expected also in the Ukrainian
segments of the accretionary wedge,
where a wide range of methane den-
sities has also been documented in
drusy quartz from mineralized joints
(Vityk et al., 1995, 1996; Jarmolowicz-
Szulc and Dudok, 2005).
Depth and Thermal Gradient
Estimates
Taking into consideration uid inclu-
sion composition, textures of fracture
inlling indicative of hydraulic frac-
turing, and the determined trapping
PT parameters, the eect of uid
buoyancy seems to be most plausible
interpretation of the varying fracture
uid pressures in the Carpathian y-
sch. Fluid overpressure exceeding that
of static uid column can be generated
when bubbles in a heterogeneous uid
mixture try to expand when rising
upward, but cannot increase their
volume due to incompressibility of
the surrounding liquid (Sahagian and
Proussevitch, 1992; Osborne and
Swarbrick, 1997). For instance, densi-
ties of the conjugate methane and
aqueous phases calculated from the
equation of state for the binary H2O
CH4 system (Duan et al., 1992)
 2006 Blackwell Publishing Ltd
V. Hurai et al. Deep burial of Tertiary accretionary wedge
change from 0.385 and 0.964 g cm)3,
respectively, at 220 C and 300 MPa
(i.e. presumably lithostatic load in the
Dukla Nappe), to 0.174 and
0.889 g cm)3, respectively, at 205 C
and 50 MPa (i.e. presumably hydro-
static load in the fore-arc basin), thus
corresponding to 9% expansion of the
aqueous liquid and as much as 122%
expansion of the associated methane
bubbles.
Rising gas bubbles transport the
hydrostatic pressure from bottom to
top of the buoyant uid column (Sa-
hagian and Proussevitch, 1992). Assu-
ming an open fracture under a
seawater column, the total uid pres-
sure at the bottom of the fracture is
min
Pfluid Psw 2Pfluid , where Psw is the
load of the seawater column, and
Table 1 Summary of parameters calculated from Eq. (1) and PT data in Fig. 3
Seawater Eroded rock
column (km) column (km)
Fore-arc basin 6.6
3.1 5.4
Magura Nappe 7.4
6.0 5.4
Dukla Unit 11.4
6.1 9.0
Puid is the load of the fracture uid
column. Total uid pressure at the
bottom of cemented and sealed frac-
max
ture corresponds to Pfluid Psw
Prock csr, where Prock stands for
lithostatic load of the rock column,
and csr is cohesive strength of the
fracture inlling (Pa). Assuming the
crack-seal mechanism, the height of
rock column (hrock) can be inferred
from minimal and maximal uid
min
inclusion trapping pressures (Pfluid ,
max
Pfluid in Pa) and the Pascals principle
(P hqg) by solving the equation:
min
Pfluid  hsw sw g
hrock m
2fluid g
P max  csr  hsw sw g
fluid ; 1
rock g
where quid, qrock (2650 kg m)3) and
qsw (1028 kg m)3) are average densi-
ties of fracture uid, rock and sea-
water columns, respectively, g is
acceleration due to gravitation
(9.81 m s)2), and hsw denotes height
of the seawater column (m). The csr
value of 10 MPa typical of a fresh,
non-fractured rock (Lockner, 1995)
was used as maximum limit in our
calculations. Maximal bulk uid den-
sity (quid) and height of the rock
column can be calculated using Eq. (1)
by setting the height of the seawater
column (hsw) to zero. In turn, the
minimal density of methane set as
bulk quid denes maximal height of
the seawater column and minimal
depth of burial.
Simple recalculation of our uid
inclusion data using Eq. (1) results in
a 5- to 11-km-thick column of rocks
removed from the recent erosion level
in the accretionary wedge and in the
fore-arc basin segment north of the
sub-Tatric fault. The corresponding
geothermal paleogradients between 17
and 29 C km)1 (Table 1) are consis-
tent with the estimates based on the
Rock Geothermal Bulk fluid density
temperature gradient at hydrostatic
(C) (C km)1) pressure (g cm)3)
130 20 0.40
24 0.20
155 21 0.53
29 0.24
195 17 0.49
22 0.27
443
Deep burial of Tertiary accretionary wedge V. Hurai et al.
.............................................................................................................................................................
illite/smectite ratios in the country
rocks (Uhl k et al., 2002; Swi-
erczewska, 2005).
Methane zone of the fore-arc basin
overlaps the uplifted segment pene-
trated with N-S-trending normal
faults, having originated probably
during pre-Middle Miocene cross-bed
extension (Sperner et al., 2002). The
extension, likely coeval with that in
the adjacent accretionary wedge, has
probably facilitated incursion of hot
aqueous uids with thermogenic
methane from the overpressured Du-
kla and Zboj units upward into the
Magura nappe and laterally into the
fore-arc basin. According to the uid
inclusion data, vertical throw along
the sub-Tatric fault in the fore-arc
basin corresponds to 2.53 km.
Most recent interpretation of reec-
tion seismic proles (Posp s il et al.,
2005a,b; Nemcok et al., 2006) indi-
cates main thrust detachment horizon
of the accretionary wedge 717 km
below recent erosional surface. Con-
sequently, thickness of the accretion-
ary wedge prior to exhumation must
have attained c. 10 km beneath central
part of the Magura nappe, c. 20 km
close to hinterland termination, and
possibly up to 25 km in the southern
part of the Silesian Nappe (Fig. 4) so
as to account for the high methane
densities recorded in uid inclusions
from outcrop samples. The uid inclu-
sion microthermometry-based recon-
struction in Fig. 4 indicates only c.
50 vol.% of the accretionary wedge
preserved after post-tectonic uplift
and exhumation.
Supralithostatic Fluid Pressure?
Extremely high methane densities of
up to 0.411 g cm)3 (Th )154 C to
liquid) and 0.427 g cm)3 (Th
)164.4 C to liquid) were locally
recorded in drusy quartz from the
Dukla and Zboj units respectively.
Raman spectrometry did not reveal
nitrogen, which could increase the
apparent density above that of the
pure CH4 or CH4CO2 mixtures.
The high methane densities would
correspond to pressures of up to
370 MPa in the Dukla unit, and
450 MPa in the Zboj unit. The anom-
alous densities are unsystematic and
local. For instance, the density of
0.427 g cm)1 was observed in primary
inclusions 3714-m deep in the Zborov-
1 borehole, and the values as low as
0.246 g cm)1 are common in the
neighbourhood of the high-density
methane inclusions in the same quartz
crystal, which does not exhibit signs of
a tectonic deformation, such as frac-
turing and/or undulatory extinction.
The anomalous methane densities can
be explained in terms of crack-seal
model only if geologically unreason-
able depths of burial (1517 km)
and geothermal gradients of 11
Terra Nova, Vol 18, No. 6, 440446
12 C km)1 were admitted. Hence,
we interpret the extremely high
methane densities as reecting an
instantaneous and local supralitho-
static uid overpressure generated
due to thermal cracking of organic-
rich sediments and/or oil at the depths
below 9 km and the temperatures
above 200 C.
Conclusions
Heterogeneously trapped methane-
bearing aqueous uid inclusions per-
mit temperature and pressure to be
calculated directly from microthermo-
metry data only if statistically relevant
number of measurements from coeval
inclusions are available. Formation
depths can then be inferred from the
inclusion uid pressures using an
expanded crack-seal model involving
a uid buoyancy eect. The model
applied to the Tertiary fore-arc basin
and accretionary wedge of the Carpa-
thians indicates up to 11 km of rocks
removed from recent erosion surface.
Distribution of uid temperatures
suggests vertical and lateral uxes of
the hot methane-bearing uids into
colder sediments during an extension
coincidental with the uplift and exhu-
mation. Liberation of thermogenic
methane by cracking of oil and kero-
gen at the temperatures above 200 C
resulted in local supralithostatic uid

Fig. 4 Schematic, non-balanced cross-section of the accretionary wedge across the prole marked in Fig. 1, with the reconstructed
thickness of the removed rocks based on uid inclusion data. The cross-section was constructed using recent geological maps,
balanced cross-sections and geophysical data (Behrmann et al., 2000; Lexa et al., 2000; Oszczypko, 2004; Oszczypko-Clowes and
Oszczypko, 2004; Posp s il et al., 2005a,b; Nemcok et al., 2006). Overburden of the Silesian nappe (Si) has been reconstructed from
uid inclusion data of Jarmolowicz-Szulc and Dudok (2005).

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Terra Nova, Vol 18, No. 6, 440446
.............................................................................................................................................................
overpressure in the lowermost parts of
the accretionary wedge.
Acknowledgements
We thank Jean Dubessy (University Henri
Poincare, Vandoeuvre-les-Nancy, France)
for Raman spectroscopic analyses of
methane and the Director of the Geological
Survey of Slovakia for permission to pub-
lish data obtained within the scope of the
projects 22/95 and 41/97. Fieldwork in
Poland has been nancially supported from
the project 43/20002003 funded to A.S.
and V.H. from the joint project of the Polish
and Slovak Academies of Science. Reviews
of two anonymous referees and editorial
comments of C. Doglioni signicantly im-
proved initial version of the manuscript.
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