Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 279

Diagenesis and Reservoir-Quality Evolution of Deep-Water Turbidites: Links to Basin Setting, Depositional Facies, and Sequence Stratigraphy
HOWRI MANSURBEG

ACTA UNIVERSITATIS UPSALIENSIS UPPSALA 2007

ISSN 1651-6214 ISBN 978-91-554-6817-0 urn:nbn:se:uu:diva-7634

Dissertation at Uppsala University to be publicly examined in Axel Hamberg-salen, Geocentrum, Friday, March 23, 2007 at 10:00 for the Degree of Doctor of Philosophy. The examination will be conducted in English Abstract Mansurbeg, H. 2007. Diagenesis and Reservoir-Quality Evolution of Deep-Water Turbidites: Links to Basin Setting, Depositional Facies, and Sequence Stratigraphy. Acta Universitatis Upsaliensis. Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 279. 59 pp. Uppsala. ISBN 978-91-554-6817-0 A study of the distribution of diagenetic alterations and their impact on reservoir-quality evolution in four deep-water turbidite successions (Cretaceous to Eocene) from basins in active (foreland) and passive margins revealed the impact of tectonic setting, depositional facies, and changes in the relative sea level. Diagenetic modications encountered in the turbiditic sandstones from the passive margin basins include dissolution and kaolinitization (kaolin has 18 OV SMOW = +13.3 to +15.2 ; DV SMOW = -96.6 to -79.6 ) of framework silicates, formation of grain coating chloritic and illitic clays, cementation by carbonates and quartz, as well as the mechanical and chemical compaction of detrital quartz. Kaolinitization, which is most extensive in the lowstand systems tracts, is attributed to meteoric-water ux during major fall in the relative sea level. Preservation of porosity and permeability in sandstones from the passive margin basins (up to 30% and 1 Darcy, respectively) is attributed to the presence of abundant rigid quartz and feldspar grains and to dissolution of carbonate cement as well as mica and feldspars. Diagenetic modications in turbidites from the foreland basins include carbonate cementation and mechanical compaction of the abundant ductile rock fragments, which were derived from fold-thrust belts. These diagenetic alterations resulted in nearly total elimination of depositional porosity and permeability. The wide range of 13 CV PDB values of these cements (about -18 to +22 ) in passive margin basins is attributed to input of dissolved carbon from various processes of organic matter alterations, including microbial methanogenesis and thermal decarboxylation of kerogen. The narrower range of 13 CV PDB values of these cements (about -2 to +7 ) in the foreland basins suggests the importance of carbon derivation from the dissolution of carbonate grains. The generally wide range of 18 O values (about -17 to -1 ) of the carbonate cements reect the impact of oxygen isotopic composition of the various uid involved (including marine depositional waters, uxed meteoric waters, evolved formation waters) and the wide ranges of precipitation temperatures. Results of this study are anticipated to have important implication for hydrocarbon exploration in deep-water turbidites from passive and active margin basins and for pre-drilling assessment of the spatial and temporal distribution of reservoir quality in such deposits. Keywords: Diagenesis, turbidites, reservoir quality, passive and active margins, basin setting, depositional facies, sequence stratigraphy Howri Mansurbeg, Department of Electronic Publishing, Uppsala University, Villavgen 16, SE-752 36 Uppsala, Sweden c Howri Mansurbeg 2007 ISSN 1651-6214 ISBN 978-91-554-6817-0 urn:nbn:se:uu:diva-7634 (http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-7634)

The important thing in science is not so much to obtain new facts as to discover new ways of thinking about them. William Lawrence Bragg Dedicated to Mansurbeg and Shorish families

List of Papers

This thesis is based on the following papers, which are referred to in the text by their Roman numerals. I Mansurbeg, H., Mohamed A.K. El-ghali, Morad, S., Plink-Bjrklund, P. (2006) The impact of meteoric water on the diagenetic alterations in deep-water, marine siliciclastic turbidites. Journal of Geochemical Exploration, 89:254-258 Mansurbeg, H., Morad, S., Marl, R., El-ghali1, M.A.K., Nystuen, J.P., Caja, M.A., Amorosi, A., Garcia, D. (2007) Diagenesis and reservoir quality evolution of palaeocene deep-water, marine sandstones, the Shetland-Faroes Basin, British Continental Shelf. Marine and Petroleum Geology, In review. Mansurbeg, H., De Ros, L. F., and Morad, S. (2007) Diagenesis of the Urucutuca Formation (Lowe Cretaceous), Espirito Santo Basin, eastern Brazil: Impact on the reservoir quality and heterogeneity evolution pathways in turbiditic sandstones. Sedimentary Geology, To be submitted Mansurbeg, H., Morad, S., Plink-Bjrklund, P. and El-Ghali, M.A.K. (2007) Diagenetic alterations related to falling stage and lowstand systems tracts of shelf, slope and basin oor sandstones (Eocene Central Basin, Spitsbergen). IAS Special Publication, accepted. Mansurberg, H., Caja, M.A., Marl, R., Garcia, D., Morad, S., Remacha, E., Amorosi, A. (2007) The diagenetic evolution and porosity destruction of hybrid turbiditic arenites of foreland basin: Evidence from the Eocene Hecho Group, Pyrenees, Spain. Sedimentary Geology, To be submitted. Marl, R., Mansurbeg, H., Garcia, D., Caja, M.A., Remacha, E., Morad, S., Amorosi, A., Nystuen, J-P. (2007) Dolomite-rich condensed sections in overbank deposits of turbidite channels, the Eocene Hecho Group, south-central Pyrenees, Spain. IAS Special Publication, accepted.

II

III

IV

VI

Reprints were made with permission from the publishers.

Contents

2 3 4 5 6 7 8

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1.1 Aims of Study . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1.2 Sequence Stratigraphy of Turbidite Deposits . . . . . . . . . . . . . . 1.3 Depositional Facies of Turbidite Deposits . . . . . . . . . . . . . . . . 1.4 Theory and Approach of Linking Diagenesis to Sequence Stratigraphy of Deep-Water Turbiditic Sandstones . . . . . . . . . . 1.5 Sedimentary Successions Selected for Study . . . . . . . . . . . . . . Methodology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Important Eogenetic Alterations in the Deep-Water Turbiditic Deposits . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Most Common Mesogenetic Alterations in the Deep-Water Turbiditic Deposits . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Porosity and Permeability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Predictive Models of Diagensis and Reservoir-Quality Evolution in Deep-Water Turbiditic Sandstones . . . . . . . . . . . . . . . . . . . . . . . . . Computer Modelling of Impact of Fluid Flow on Geochemical and Mineralogical Modications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Summary Of The Papers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.1 The Impact of Meteoric Water on The Diagenetic Alterations in Deep-Water, Marine Siliciclastic Turbidites . . . . . . . . . . . . . 8.2 Diagenesis and Reservoir Quality Evolution of Palaeocene Deep-Water, Marine Sandstones, the Shetland-Faroes Basin, British Continental Shelf . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.3 Diagenesis of the Urucutuca Formation (Lowe Cretaceous), Espirito Santo Basin, Eastern Brazil: Impact on the Reservoir Quality and Heterogeneity Evolution Pathways in Turbiditic Sandstones . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.4 Diagenetic Alterations Related to Falling Stage and Lowstand Systems Tracts of Shelf, Slope and Basin Floor Sandstones (Eocene Central Basin, Spitsbergen) . . . . . . . . . . . . . . . . . . . . 8.5 The Diagenetic Evolution and Porosity Destruction of Hybrid Turbiditic Arenites of Foreland Basin: Evidence from the Eocene Hecho Group, Pyrenees, Spain . . . . . . . . . . . . . . . . . . 8.6 Dolomite-Rich Condensed Sections in Overbank Deposits of Turbidite Channels, The Eocene Hecho Group, South-Central Pyrenees, Spain . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

9 11 11 13
14 15 19

21 25 29 31 35 39
39

39

40

41

42

42

9 Concluding Remarks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10 Summary in Swedish . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

45 47

1. Introduction

The diagenetic evolution of siliciclastic deposits is complex and controlled by several inter-related parameters (Fig. 1.1), including detrital composition, pore-water chemistry, depositional facies, paleo-climatic conditions, rate of deposition, and burial-thermal history of the basin (Stonecipher et al., 1984; Morad et al., 2000). The detrital composition of sandstones is strongly controlled by the tectonic setting of the basin, such as location in passive versus active margin settings. Changes in the relative sea level, which occur due to eustacy and/or the tectonic uplift/subsidence, control important aspects of sediment diagenesis (Fig. 1.2), such as pore-water chemistry, amounts and types of intrabasinal grains (e.g. mud intraclasts), grain size and sorting, and sedimentation rates, (i.e. residence time of sediment at near sea oor conditions). Recent studies have, thus, demonstrated that the diagenetic evolution of paralic and shallow-marine, siliciclastic deposits can be better understood and predicted when linked to the sequence stratigraphic framework (Morad et al., 2000; Ketzer et al., 2002, 2003a, b, 2005; Salem et al., 2005; Al-Ramadan et al., 2005; El-ghali et al., 2006). Conversely, linking the distribution of diagenetic alterations to sequence stratigraphy of deep-water turbiditic sediments is difcult, and thus not well explored in the literature. This is probably because of difculties in deriving well-constrained sequence stratigraphic models for deep-water deposits, which owes in turn to the equivocal, direct impact of major changes in the relative sea level on these deposits. Instead, changes in the relative sea level have an indirect impact on the sequence stratigraphic framework and on related distribution of diagenetic alterations of turbiditic deposits. Rapid fall in the relative sea level is accompanied by erosion of the exposed shelf sediments may lead to the incorporation of intra-basinal, siliceous and/or carbonate bioclasts. Additionally, large proportions of coarse-grained sand are by-passed across the shelf through incised valleys and delivered to the slope and basin oor. Conversely, rapid rise in the relative sea level results in the deposition of ne-grained, hemi-pelagic sediments, whereas the coarser grained sediments are trapped further landward on the shelf. Rapid rise in the relative sea level may also result in the derivation of mud intraclasts of various sizes by erosion of mud deposits on the slope and basin oor by means of turbidity currents. Diagenetic regimes used in this summery, which are sensu Morad et al., (2000), include: (1) eodiagenesis (<70C; depth < 2 km), during which porewater chemistry is controlled by surface waters (i.e. depositional and/or me-

Figure 1.1: Flow chart of the interrelationship of the main parameters that control diagenetic evolution of siliciclastic deposits (Stonecipher et al., 1984)
A
Highstand Systems Tract (HST) Maximum Flooding Surface (MFS)
Sequen ce Bou ndar y

Transgressive surface Slope fan PREVIOUS SEDIMENTARY SEQUENCE Basin floor fan

Transgressive Systems Tract (TST) Lowstand Systems Tract (LST)

B
Time

Slope fan late LST

Figure 1.2: (A) idealized sequence stratigraphic model showing the systems tracts and key stratigraphic surfaces in shallow- and deep-water marine turbiditic siliciclastic deposits. (B) conceptual model of a relative sea level cycle through time, which is divided into falling limb and rising limb separated by the lowstand systems tract (modied after Emery and Myers, 1996; Moore, 2001).

10

TST

fan oor ) in fl Bas rly LST (ea

HST

teoric waters); and (2) mesodiagenesis (>70C; depth > 2 km), which is mediated by evolved formation water and elevated temperature (Morad et al., 2000).

1.1

Aims of Study

The aims of this thesis are to unravel: (i) parameters controlling the diagenetic evolution of deep-water turbiditic sandstones based on integrating the petrological and geochemical data into tectonic setting (passive versus active margin basin settings), depositional facies and sequence stratigraphy, and (ii) the impact of diagenetic alterations on the temporal and spatial distribution of reservoir quality and heterogeneity.

1.2 Sequence Stratigraphy of Turbidite Deposits

Sequence stratigraphy, which is the study of genetically related facies within a framework of chronostratigraphically signicant surfaces, provides a powerful tool for unravelling and predicting the stratigraphy and architecture of deep-marine clastic systems (e.g. Pickering et al., 1995; Emery and Myers, 1996; Richards and Bowman, 1998; Posamentier and Allen, 1999; Stow and Mayall, 2000). However, sequence stratigraphy in deep-water turbiditic deposits is difcult to constrain because it merely indirectly reects the complex interplay between a range of interdependent parameters on the continental shelf, including changes in the relative sea level, tectonic setting of the basin and sediment supply (Emery and Myers, 1996). Consequently, a wide variability of facies distribution and organization of architectural elements should be expected in the deep-water depositional environments (Reading and Richards, 1994). Thus, no single global model can provide accurate description and prediction for turbidite systems (Normark et al., 1983; Mutti et al., 2000). In contrast to shallow marine and paralic deposits, the identication of key sequence-stratigraphic surfaces in deep-water sediments, which is merely based on analyses of seismic proles and identication of stratal stacking patterns, is fraught with difculties (Bouma and Stones, 2000). Sedimentation in the deep water is commonly suggested to be indirectly controlled by changes in the relative sea level on the shelf. Rapid fall in the relative sea level (during early LST) is bringing the shoreline close to, or below the shelf break, providing a mechanism for transfer of sediment into basin oors and formation of basin oor fans (Fig. 1.2). During deposition of the late LST (Fig. 1.2) relative sea level is stabilized and rise slowly results in bypassing sediments onto the slope areas forming slope fans. The slope fan deposits are characterized by channel-levee complexes at the apex and front of canyon mouths (Emery and Myers, 1996).
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Deposition of the late LST is followed by a rapid rise in the relative sea level, which results in the formation of transgressive surface (TS; Fig. 1.2); the TS separates the LST from the overlying transgressive systems tract (TST; Fig. 1.2). In a vertical section through submarine fan deposits, packages of turbiditic sandstone would be interpreted as LST deposits and major units of mudstone would be considered as TST deposits. A widespread marine ooding surface on the shelf, which represents furthest landward migration of the relative seal level is called maximum ooding surface (MFS; Fig. 1.2). The MFS, which separates the underlying TST deposits from the overlying highstand systems tract (HST; Fig. 1.2) is probably recognizable in deep-water deposits because it may display evidence of stratigraphic condensation (low sedimentation rates), such as burrowed surfaces, hardground, mineralization, and fossil accumulations (Posamentier and Allen, 1999). The central assumption of sequence stratigraphic models in the deep-water turbiditic sandstones is that sedimentation within deep-water systems increases during relative sea-level lowstand, while during transgression and sea-level highstand sedimentation diminishes or temporarily halts (e.g. Shanmugam et al., 1985; Posamentier and Vail, 1988). However, an increasing number of authors have suggested that submarine fans can be deposited during rise in the relative sea level, such as the Amazon Fan (Flood et al., 1995) and Navy Fan (Piper and Normark, 1983). Deposition of deep-water sand during rising sea level is apparently favored by narrow shelves, incised submarine canyons, shelf-parallel currents and tectonic activity at the basin margin and hinterland (e.g. Reading and Richards 1994; Stow and Mayall 2000; Shanmugam, 2000). When submarine canyons are connected with a shelf-edge delta or directly connect with the river mouth, sediment may be transported straight into the basin (e.g. Burgess and Hovius, 1998). Another controversial aspect regarding the sequence stratigraphy of the deep-water turbiditic sediments is the placement of sequence boundary (SB). In the original sequence stratigraphical model devised in the late 1970s (Vail et al., 1977; Mitchum, 1977), the SB is placed at the base of the early LST in deep-water sediments corresponds to the correlative conformity, which forms at the start of the relative sea level fall. More recent sequence stratigraphic models (e.g. Hunt and Tucker, 1992) suggest that the sequence boundary should be placed at the lowest position reached by relative sea level. Hunt and Tucker (1992) argued that the correlative conformity can be traced to the top of the prograding submarine fan complex, and thus suggested that the SB over the falling stage systems tract (FSST; also known as forced regressive systems tract FRWST) does not match Mitchums (1977) original denition of SB or its time equivalent marine correlative conformity in the deep-water sediments that was tied to the onset of a sea level fall.

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Figure 1.3: Field photos showing: (A) sand-rich channel complex that belongs to the Spanish lowstand systems tract of Eocene, the Pyrenees, (B) ne-grained levee sandstones, (C) laterally extensive carbonate-cemented sediments belonging to the transgressive systems tracts, which have presumably formed below marine ooding surfaces.

1.3

Depositional Facies of Turbidite Deposits

Turbidites are sediments transported beyond the shelf edge into deep water by gravity ow and deposited on the continental slope and the basin oor. The main depositional elements of deep-water turbiditic sandstones are basin oor fans, slope fans, channel complexes and ne-grained levees (Figs 1.2 and 1.3A, B and C). Basin oor and slope fans are the basinward portion of the lowstand systems tract. Channel turbidite deposits are usually composed of coarse-grained to conglomeratic sandstones, which have sharp erosional bases and ning up successions (Fig. 1.3A). Levee-overbank deposits, which form reservoirs lateral to the main channel (Figs 1.3B and C), show no channel lags. Channel turbidite deposits are characterized by high sand/mud ratio than the ne-grained, levee-overbank deposits.
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1.4 Theory and Approach of Linking Diagenesis to Sequence Stratigraphy of Deep-Water Turbiditic Sandstones
The primary reservoir properties of sandstones are strongly controlled by several parameters, which are related to provenance, depositional facies, rates of sediment supply and changes in the relative sea-level. These parameters include detrital mineralogical composition, grain size, sorting, spatial distribution of architectural elements and meso-scale heterogeneities and sand/mud ratio (Figs 1.3A, B and C). Variable extents of reservoir-quality modication occur by diagenetic alterations, which are strongly controlled by parameters like the detrital composition of the sand, pore-water chemistry, texture, and organic-matter content. These parameters are, in turn, linked to rates of changes in relative sea level, rates of sediment supply, and hence to the sequence stratigraphic framework (Fig. 1.2). The interplay between rate of sediment supply and rate of changes in the relative sea level is the main factor controlling transgression and regression events, i.e. creation and destruction of accommodation, on continental shelves. Changes in the relative sea level are controlled, in turn, by basin-oor subsidence/uplift and/or by changes in the eustatic sea-level (Posamentier and Allen, 1993). Basin oor subsidence/uplift and rates of sediment supply are controlled by tectonic setting of the basin. The rates of creation and destruction of accommodation versus rates of sediment supply control the spatial and temporal distribution of depositional facies and the sequence stratigraphic framework of sedimentary successions, including the formation of various systems tracts and key sequence stratigraphic surfaces. Changes in the relative sea level and rates of sediment supply are accompanied by changes in pore-water composition (meteoric, brackish and marine) and residence time of the sediments under certain geological conditions, and hence in the pattern of diagenetic alterations of shelf and, probably, of deepwater turbiditic sediments (Morad et al., 2000; Mansurbeg et al., 2006). The residence time of sediment under certain geochemical conditions such as below the seaoor and below exposed shelf (i.e. below sequence boundaries) control magnitude of these diagenetic alterations, which include dissolution and alteration of framework silicates and carbonate cementation. Major fall in the relative sea level (i.e. regression) results in less accommodation and, perhaps, even subaerial exposure of the shelf, which is accompanied by: (i) incursion of under-saturated meteoric waters into exposed sediments and deep-water turbiditic sandstones, which induces grain dissolution and kaolinitization (Carvalho et al., 1995; Morad et al., 2000; Mansurbeg et al., 2006) and cementation by blocky to poikilotopic calcite in the lowstand and forced regressive wedge (or falling stage) systems tracts (Al-Ramadan et al., 2005), and (ii) erosion of exposed older shelf sediment by advancing rivers and, thus, the formation of incised valleys. The intra-basinal sand grains (e.g.
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mud intraclasts, glaucony and carbonate bioclasts), derived from shelf erosion are by-passed, together with extra-basinal sediments (mainly quartz, feldspar and rock fragments derived from outside the depositional basin), to the continental slope and basin oor via the incised valleys, resulting in the deposition of submarine fans (falling stage or lowstand systems tract). Deposition is restricted though to lobes, which cover part of the submarine fan whilst other parts of the fan receive mainly pelagic sediments. Conversely, transgression events on the shelf result in: (i) domination of marine pore-water composition, which results in the formation of dolomite and grain-coating minerals (berthierine and micro-quartz), and (ii) low sedimentation rates and starvation in offshore as well as basin slope and oor settings owing to sediments entrapment in landward depositional settings. Sedimentation on the basin oor will be dominated by pelagic and hemipelgic sediments (transgressive and highstand systems tracts). Low sedimentation rates in the outer shelf and slope areas favor the formation of abundant evolved glaucony (Amorosi, 1997 and Ketzer at al., 2003a) and extensive cementation by microcrystalline carbonates (Al-Ramadan et al., 2005), which is enhanced by diffusive ux of dissolved Ca and carbon into the pore water from the overlying seawater (Morad et al., 2000). Thus, sedimentary events on the shelf are anticipated to have indirect but profound impact not only on the sequence stratigraphic framework but also on the detrital composition and diagenetic evolution of deep-water marine deposits. Detrital composition of the sand determines its chemical and physical properties, and hence the pattern of diagenetic alterations at near surface conditions and during progressive burial and increase in temperature (Primmer et al., 1997; Morad et al., 2000). Hence, regression-transgression events have important control on the proportion of extra-basinal (mainly quartz, feldspar, mica and rock fragments derived from the hinterland) and intra-basinal (mainly carbonate grains, mud intraclasts, and glaucony derived within the basin) sand grains (Fig. 1.4).

1.5

Sedimentary Successions Selected for Study

For comparison purposes, two basins located along passive margins (Shetland-Faeroe, Esprito Santo Basin, Eastern Brazil) and two basins along active margins (Ainsa-Jaca and Spitsbergen) were selected for study (Fig. 1.5). The Shetland-Faeroe Basin (ca 125 km wide and 600 km long) is located between the West Shetland platform in the east and the Faeroe Islands in the west. The area is ve times that of the prospective part of the North Sea Basin, but mainly because of extreme water depths (ca 2.5 km), it has been only slightly explored. Sequence stratigraphic studies recognize a complex basin margin, with marked basinward and landward shifts in sedimentation determining the location of sand-rich depositional systems (Mitchell et al., 1993). Ebdon et al., (1995) recognized a major sequence
15

boundary at the base of the Late Paleogene and subdivided the succession into several stratigraphic sequences, based mainly on maximum ooding surfaces, which can be correlated with their equivalents to the North Sea Basin. The reservoirs are comprised of submarine-fan sandstones deposited as early lowstand systems tracts. The Esprito Santo Basin covers an area of 25,000 km2 in eastern Brazil passive margin with only 3220 km2 of it is onshore. The basin basement is composed of Precambrian migmatites, granulites, gneisses and granites, structured as a homoclinal of faulted blocks tilted towards east. Neocomian rift phase lacustrine shales of the basal Cricar Formation are the main source rocks of the basin (Estrella, 1984; Carvalho, 1989). The main reservoirs are the turbidites of the Urucutuca Formation, which contain close to 60 million barrels of recoverable oil (Carvalho, 1989). In the onshore portion of the basin, deposition of these turbidites occurred dominantly within submarine canyons incised in the border of the platform during relative sea-level falls that punctuated the overall transgressive setting of the late Cretaceous and early Tertiary. Some of the turbidite successions can be connected with global, eustatic sea-level curves. Thus, deposition may have resulted from increased sediment supply related to tectonic reactivation in the source area and basin margin, and/or to climatically-controlled denudation rates in the source area (Bruhn, 1993).
extrabasinal clasts

lithic-, arkose-, and quartzarenites

re ssi o

hybrid arenites

g re s re n sio

re g

calcarenites

glauconitic, and/or phosphatic arenires

intrabasinal carbonate clasts

intrabasinal non-carbonate clasts

Figure 1.4: Triangle showing possible changes in the proportion of extra-basinal and intra-basinal, framework grain composition of sandstones due to changes in the relative sea level (modied from Zuffa 1980).

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180 60 140 80
Central Spitsbergen Basin, Svalbard
O

140 100 180

Shetland-Faroe Basin
ARCTIC

100 60

O O

20 0O 20

O O O O O

80 60 40O 20
AFRICA
O O

60
NORTH AMERICA ATLANTIC OCEAN EUROPE ASIA

40
The Eocene Hecho Group in the south central Pyrenees
CARIBBEAN

PACIFIC OCEAN

20

0
SOUTH AMERICA ATLANTIC OCEAN PACIFIC OCEAN 0 INDIAN OCEAN 2.000 Miles 2.000 Kilometers

Equator

PACIFIC OCEAN
OCEANIA

0O 20 40 60 80
O O O O

20

OCEANIA

40
Espirito Santo Basin, Brazil
0

60 80O 160 0
O

ANTARCTICA

120

80

40

O O

40

80

120

160

Figure 1.5: Location map of the studied basins.

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The Ainsa-Jaca Basin is located in the south central Pyrenees (Spain). The Pyrenees, extending in northern Spain and south of France are an Alpine chain formed as a fold and thrust belt during late Cretaceous to Miocene, at the collisional boundary between the Iberian and the Eurasian plates, as a result of a roughly N-S crustal contraction, comprise 10-12 million years of deposition of deep-marine clastics with a cumulative thickness of 4 km and provide an ideal natural laboratory for studying slope-basin depositional systems. The Ainsa basin contains about 20-25 deep-water sand bodies, typically 10s m thick but packaged essentially as seven coarse clastic depositional complexes, each in the order of at least 100-300 m thick. The Spitsbergen Basin is located on Svalbard and bounded to the west by the West Spitsbergen fold- and thrust belt, which die out towards the eastern part. This basin was a foreland basin during the initial period of active thrusting, but became a piggy-back basin (Blythe and Kleinspehn, 1998) on account of foreland propagation of thrusting. The Lomfjorden and Billefjorden fault zones east of the Central Basin probably represent late stage reactivation of deep-watered reverse faults (Braathen et al., 1999). The slope and basin oor fans of Eocene age were the target of this study. The basin is rare in the sense that a linkage of coastal-plain, shelf, slope and basin-oor facies tracts can be walked out along large-scale shelf-margin clinoforms. The clinoforms are successive time lines in the stratigraphy, generated as the basin margin accreted southeastwards. Each clinoform surface represents a morphologic prole from the coastal plain to the marine shelf and down into the deeper water slope and basin-oor environments of the depositional system.

18

2. Methodology

The studied successions occur as outcrops and in the subsurface. Sandstone core samples that represent various depositional facies, systems tracts and key sequence stratigraphic surfaces were collected. Thin sections were prepared for all samples subsequent to vacuum impregnation with blue epoxy. Modal analyses of the sandstone samples were preformed by counting 300 points in each thin section. Scanning electron microscope (SEM) was used to study crystal habits and paragenetic relationships among diagenetic minerals in representative samples. Polished thin sections representing sandstones from the various depositional facies and systems tracts encountered were coated with a thin layer of carbon for the purpose of electron microprobe (EMP) analyses. Cameca SX50 instrument equipped with three spectrometers and a backscattered electron detector (BSE) was used to determine the chemical compositions and paragenetic relationships of different cement types. Operating conditions during analysis were an accelerating voltage of 20 kV, a measured beam current of 10 nA for carbonates and 12 nA for silicates, and a spot size of 1-5 m. The standard and count times used were wollastonite (Ca, 10 s), MgO (Mg, 10 s), strontianite (Sr, 10 s), MnTiO3 (Mn, 10 s), and hematite (Fe, 10 s). Analytical precision was better than 0.1% for all elements. Stable carbon and oxygen isotope analyses were carried out on carbonatecemented sandstones representative of the various depositional environments and systems tracts in order to determine the geochemical conditions, pore waters composition and/or temperature of precipitation. Calcite-cemented samples were reacted with 100% phosphoric acid at 25C for one hour, and Fedolomite/ankerite and siderite-cemented samples were reacted at 50C for one day and six days, respectively (e.g. Al-Aasm et al., 1990). The CO2 gas released was collected and analyzed using a Delta plus mass spectrometer. Samples containing calcite, dolomite and siderite were subjected to sequential chemical separation treatment (Al-Aasm et al., 1990). The phosphoric acid fractionation factors used were 1.01025 for calcite at 25C (Friedman and ONeil, 1977), 1.01060 for dolomite at 50C and 1.010454 for siderite at 50C (Rosenbaum and Sheppard, 1986). Precision of all analyses was better than 0.05 for both 13 C and 18 O. Oxygen and carbon isotope data are presented in the notation relative to the V-PDB and V-SMOW standards. The 87 Sr/86 Sr isotope ratios in carbonate cements were analyzed (papers III and VI) using an automated Finnigan 261 mass spectrometer equipped with 9 faraday collectors. Some of calcite-cemented samples from different systems

19

tracts were washed with distilled water and then reacted with dilute acetic acid in order to avoid silicate leaching. Correction for isotope fractionation during the analyses was made by normalization to 86 Sr/88 Sr = 0.1194. The mean standard error of mass spectrometer performance was 0.00003 for standard NBS-987. A JEOL JEM 2010 200KV analytical transmission electron microscope (TEM) was used for a detailed characterization of the < 2 micron clay mineral fractions. Sulfur isotope ratios in pyrite-cemented sandstones were analyzed to unravel the source of sulfur (paper II). X-ray diffraction (XRD) analyses were preformed on the ne fraction (< 20 m) from representative sandstone samples using a Siemens D5000 diffractometer (paper II). A high sensitivity cathode CL microscope was used to study zonation in various carbonate cements (paper V). Microthermometric analyses of the uid inclusions were preformed in the Shetland-Faroes Basin sandstones samples (paper II) using Linkham TH600 stage calibrated for the temperature range between -100 and 400C. The temperatures were measured using the procedure described in Shepherd et al. (1985). He-porosity and permeability measurements were performed on core plugs (paper V). The oxygen and hydrogen isotopes of kaolin from 11 samples were analyzed, and the results are reported in relative to the Vienna Standard Mean Ocean Water (V-SMOW) standard. Samples were subjected to removal of organics by exposing them to NaOOH solution adjusted to a pH of 9.5 while placed in boiling water bath for 15 minutes, followed by centrifugation at 800 rpm for 5 min. The remaining mud was centrifuged at 750 rpm for 3.3 minutes to separate the clay fraction. Samples containing carbonates were exposed to the same procedure above after being subjected to carbonate removal by simmering in a buffer solution of acetic acid for at least eight hours. Conventional petrographic methods and the use of whole rock chemistry provide basic information needed to discriminate between detrital inputs and diagenetic alterations. Applying these methods to the deep marine turbidites helps recognizing condensed surfaces in otherwise monotonous successions, and hence aiding the sequence stratigraphic interpretation.

20

3. Important Eogenetic Alterations in the Deep-Water Turbiditic Deposits

This study shows that the types, extent and distribution pattern of eogenetic alterations in the deep-water turbiditic sandstones vary considerably between basins located at passive versus active margin settings. Turbiditic sandstones obtained from active (foreland) basins show mainly: (i) mechanical compaction of ductile sedimentary and low-grade metamorphic rock fragments, which resulted in nearly complete elimination of depositional porosity and permeability, and (ii) formation of minor amounts of calcite, siderite, non-ferroan dolomite cements and pyrite. Carbonate cementation is most extensive below marine ooding surfaces, particularly in the presence of detrital carbonates. Eogenetic alterations in turbiditic sandstones from the passive margin settings include: (i) mechanical compaction, which is manifested by grain rearrangement, bending of micas, and formation of pseudomatrix owing to ductile deformation of mud intraclasts, (ii) kaolinitization and dissolution of the framework silicate grains (feldspars, mica and mud intraclasts), particularly in the channel sand and basin oor sand fans (Figs 3.1 and 3.2), (iii) cementation by blocky to poikilotopic calcite, which occurs as continuously cemented, thin or several meters thick sandstone layers or as scattered concretions (paper II: calcite cement occurs mainly below marine ooding and maximum ooding surfaces), and (iv) formation of smectitic grain-coating clays. Kaolinitization is most abundant in the FSST and LST sandstones and below the SB (papers II) in basins located in passive continental margins. The loosely expanded texture of the kaolinitized silicate grains in the studied sandstones suggests formation during near-surface eodiagenesis (Figs 3.1A, B and C). Kaolinitization is attributed to the ux of meteoric water into the deep-water turbiditic sandstones during major fall in the relative seal level (Fig. 3.3; Mansurbeg et al., 2006; Prochnow et al., 2006). However, other mechanisms of meteoric water ux into deep-water sand, such as hyperpycnal ow and increase in hydraulic head owing to basin margin uplift, cannot be ruled out. Stable oxygen and hydrogen isotopes of the kaolin ( 18 OV SMOW = +13.3 to +15.2 ; DV SMOW = -96.6 to 79.6 ) fall close to the kaolinite meteoric water line, supporting a meteoric origin (Fig. 3.4; Morad et al., 2003; paper III). Deviation of the stable isotopic values from this line is attributed to partial conversion of kaolinite into dickite during mesodiagenesis.

21

Figure 3.1: (A) Backscattered image showing kaolinitized mica. Mica has expanded into adjacent pores, which resulted in porosity deterioration. (B) optical micrograph (unpolarized light) showing kaolinitization of pseudomatrix. (C) SEM image displaying morphological features of grain-replacing, kaolinite that has been transformed partly into thicker dickite.
Passive margin

Faroe-Shetland Basin

Hecho group Active margin

Figure 3.2: Optical micrographs (A and B; plane polarized) showing variable and successive degrees of alteration and dissolution of detrital biotite and the formation of large secondary porosity (the Shetland-Faroe Basin, passive margin). C and D (shown for comparision) are optical micrographs under plane polarized and cross nicols, respectively, showing that calcite cementation and intergranular pressure dissolution have resulted in complete destruction of reservoir quality (no signs of dissolution) in Ainsa-Jaca Basin, active margin.

22

Figure 3.3: Schematic model of prograding deltaic-slope facies on passive continental margin showing that major sea-level fall may extend the inuence of meteoric water circulation (arrows) into deep-water sandstones (Modied after Bethke, 1989 and Einsele, 2000)

The occurrence of abundant carbonate cement below marine ooding and maximum ooding surfaces is attributed to the long residence time of sediments below the ooding surfaces that enhance the diffusion of dissolved carbon and Ca2+ from the overlaying seawater and/or to abundant intrabasinal carbonates. (Kantorowicz et al., 1987; Taylor et al., 1995; Morad et al., 2000; Ketzer et al., 2003b; Al-Ramadan et al., 2005). Glaucony is a common feature and, in some cases, relatively abundant in turbiditic sandstones from sandstones obtained from basins located in passive margin settings. The greenish colour and presence of internal micro-cracks within the glaucony pellets suggest formation within the basin, yet probably in the outer shelf and on the slope and has been slumped into the basin oor. The formation of glaucony in these depositional environments occurs immediately below the seaoor and was presumably enhanced by low sedimentation rates. Conversely, glaucony is completely absent in turbiditic sandstones obtained from active basin settings, being attributed to the high sedimentation rates encountered in these basins. High sedimentation rates preclude glaucony formation because of the rapid establishment of iron reduction geochemical zone below the seaoor by rapid burial of the sediments (Ketzer et al., 2003a).

23

kaolin from Urucutuca meteoric line weathering kaolinite (Savin and Epstein, 1970) Cretaceous of Canada (Longstaffe, 1989) kaolin from Brent (Glassman et al., 1989) kaolinite from Brent (McAulay et al., 1994) Dickite from Brent (McAulay et al., 1994)

0 -20

DW O M S

-40 -60 -80 -100 -120 -140 +5 +10 +15 +20

18OW O M S

+25

+30

+35

Figure 3.4: Cross plot of DV SMOW and 18 OV SMOW values of diagenetic kaolin from different sandstones and weathering kaolin. Kaolin from the Urucutuca sandstones (Brazil) are situated close to the meteoric water line.

24

4. Most Common Mesogenetic Alterations in the Deep-Water Turbiditic Deposits

The distribution pattern of mesogenetic alterations is inuenced to considerable extent by the distribution of eogenetic alterations in the sandstones, which were in turn strongly linked to the passive versus active margin basin setting. The most common mesogenetic alterations in the deep-water turbiditic sandstones from the passive margin basins include: (i) clay mineral transformation, such as conversion of kaolinite into dickite and chloritization and illitization of kaolinite and of grain coating smectite; dickite, has not been illitized owing to its more stable crystal structure than kaolinite (Morad et al.,1994), (ii) cementation by quartz overgrowths of sandstones with clean quartz surfaces; the dissolved silica needed was derived from concomitant intergranular pressure dissolution of quartz grains in sandstones that are enriched in grain-coating illitic clays and mica, (iii) cementation by Fe-dolomite and ankerite, (iv) albitization of detrital plagioclase and, to smaller extent, K-feldspar grains. Typical diagenetic alterations in turbiditic sandstones from the active margin basins include albitization of detrital plagioclase and, less commonly, K-feldspar grains and the precipitation of calcite and Fe-dolomite cement. SEM studies indicate that the grain-coatings chloritic clays have impeded the precipitation of quartz overgrowths, and hence promoted the preservation of reservoir quality in deeply-buried sandstones (Ehrenberg, 1993; Aase et al., 1996; Lima and De Ros, 2003 and Salem et al., 2005; paper II). Various occurrence habits of quartz cements (overgrowths, outgrowths, discrete crystals, poikilotopic and rare micro-quartz) in sandstones from the different depositional facies and systems tracts of the passive margin basins indicate various origins (Worden and Morad, 2000). Variations in the amounts of quartz cement are also attributed to facies-controlled variations in the distribution of illitic clay coatings and presence of mica, which exerted decisive control on the intergranular pressure dissolution of quartz grains (Oelker et al., 1996). Pressure dissolution acted as the most obvious source of dissolved silica needed for quartz cementation. Conversely, sandstones that are poor in clay coatings have been subjected to considerable degree of cementation by quartz overgrowths (cf. Bloch et al., 2002). Quartz overgrowths and intergranular pressure dissolution are known to be signicant at temperature of about 90-130C and burial depths > 3 km (McBride, 1989; Walderhaug, 1996). Fluid inclu-

25

sion thermometry indicates that quartz cementation occurred at temperatures of 90-110C (paper II). Dickite occurs as blocky crystals (5-15 m across) with book-like and vermicular stacking patterns containing etched of thin kaolinite remnants. Kaolin is engulfed by, and hence predates, quartz overgrowths. Conversion of kaolinite to dickite is known to occur with increase in burial depth and temperature (paper II) through small-scale dissolution and re-precipitation (Ehrenberg, 1993; Morad et al., 1994), which is evidenced by: (i) the association of dickite and etched kaolinite, and (ii) preservation of vermicular and booklet stacking pattern of kaolinite in dickite (paper II and IV). Kaolinite to dickite conversion was presumably enhanced by ux of acidic waters, which maintained low aK +/aH + ratio, such as waters derived upon maturation of kerogen (Morad et al., 1994). Albite in the turbiditic sandstones from the passive margin basins (paper II) occurs as numerous small, lath-like crystals (1-15 m across) that are parallel aligned to each other and to remnants of severely etched plagioclase and, less commonly, K-feldspar grains, and are hence considered as albitized feldspar (e.g. Morad, 1986 and Saigal et al., 1988, Morad et al., 1990). Partly albitized plagioclase grains have preserved their original twining pattern, whereas partly albitized K-feldspar contain irregular patches of albite and of remnants of the detrital host feldspar. Albitized feldspars, particularly plagioclase, contain variable amounts of intragranular pores, are untwined, vacuolated and display patchy extinction patterns. Thus, these feldspars display petrographic features similar to diagenetically albitized feldspars described by Morad (1986), Morad et al. (1990) and Saigal et al., (1988). Albitization of plagioclase acted as a source of Al3+ and Ca2+ , which were incorporated in mesogenetic clay minerals (dickite, illite and chlorite) and carbonate cements, respectively. Albitization of K-feldspar has acted as a source of potassium needed for the formation of illite (up to 8%; Morad et al., 1990; Bjrlykke and Aagaard, 1992). Albitized feldspar grains in arenites from the active margin basins are apparently of both diagenetic and detrital origins. Distinguishing diagenetically albitized feldspar from those formed in the source area is a serious problem (paper V). Nevertheless, the lack of well-developed, smooth-surfaced, parallel-aligned, tiny albite crystals and of intragranular porosity in the feldspar, and/or the presence of sericite and epidote can be used as evidence of albitization in the source area, such as during hydrothermal albitization of granitic rocks (Varlamoff, 1972). Stable oxygen and carbon isotope analyses (Fig. 4.1) show that the carbonate cements were precipitated at diverse geochemical conditions and/or temperatures. The cross plot of 13 C versus 18 O values of carbonate cements in the studied successions reveals the lack of correlation when carbonate cements are considered for each basin as well as for the whole carbonate cement (Fig. 4.1). This lack of correlation between 13 C versus 18 O values is attributed to
26

25 20 15 10

5 0 -5 -10 -15 -20 -20

Faeroe-Shetland Basin Spitsbergen Basin Esprito Santo Basin Hecho group yellow marker beds of Hecho group

CB P D

13

-18

-16

-14

-12

-10

-8

-6

-4

-2

OB D P

18

Figure 4.1: Cross plot of 13 C versus 18 O values of carbonate cements in the studied successions reveals the lack of correlation when carbonate cements are considered for each basin as well as for the whole carbonate cement. This lack of correlation is attributed to wide variations both in the sources (e.g. marine versus meteoric) of dissolved carbon as well as in the biochemical (e.g., bacterial sulphate reduction and methanogenesis, such as in the Esprito Santo Basin, Brazil), thermo-chemical (thermal decarboxylation) processes of organic matter degradation, and dissolution of carbonate grains.

wide variations both in the sources (e.g. marine versus meteoric) of dissolved carbon as well as in the biochemical (e.g., bacterial sulphate reduction and methanogenesis, such as in the Esprito Santo Basin, Brazil), thermo-chemical (thermal decarboxylation) processes of organic matter degradation and dissolution of carbonate grains. This postulation is supported by the wide range of the 13 C values (Fig. 4.1), For each carbonate cement type, there is specic temperature-dependent, oxygen isotope fractionation equation between the mineral and pore waters, which is used to determine either the precipitation temperature and/or isotopic composition of the pore water (Fig. 4.2). Assuming that the 18 OV SMOW values of pore waters varied between marine and evolved marine composition (-1.2 to +2 ), the 18 O values of the carbonate cements suggest precipitation at wide range of temperatures (Fig. 4.2). The overall low 18 O values may, in some cases, be related to the ux of meteoric waters, which have lower 18 O values than marine pore waters.

27

100

calcite concretions

-8

150
siderite

-13

-11 -9

-7-5

-12

-4

Temperature C

50

100

0 -10 0 10

50 -10 150
poikilotopic Calcite

0
Fe-dolomite /ankerite

10

150

-14 -10

-11 -9

-7
-5

-16

Temperature C

100

-6

100

50

50
-10 0 10
-10 0

10

18

OSMOW

18

OSMOW

Figure 4.2: Curves of oxygen-isotopes fractionation between calcite, siderite and dolomite/ankerite and water as a function of temperature. The shaded elds illustrate the possible ranges of precipitation temperatures of carbonate cements in the studied turbidites if waters involved were of marine origin ( 18 OV SMOW = -1.2 permil ; Shackleton and Kennett, 1975) and moderately evolved brine ( 18 OV SMOW = +2.0 )

28

5. Porosity and Permeability

In contrast to arenites from active margin basins, fairly high porosity (12-23%) and permeability (0.6-1241 mD) values are commonly encountered in passive margin turbiditic sandstones, being attributed mainly to variation in detrital composition of the sand between these basin settings. Turbiditic sandstones from passive margin are rich in quartz, and thus chemically and mechanically stable, and have better potential to form good reservoirs even upon deep burial (paper II and III). However, some of the passive margin sandstones are rich in feldspar too, and are thus mechanically stable but chemically fairly unstable. Prolonged percolation of undersaturated meteoric water promotes feldspar dissolution and kaolinitization. Arenites from the active margin basins are rich in lithic fragments (low-grade metamorphic and/or carbonate rock fragments), and are thus mechanically unstable causing rapid loss in porosity and permeability during burial due to mechanical compaction (Bloch, 1994; papers IV and V). Porosity in deep-water turbiditic sandstones from passive margin settings (papers II and III) contain variable amounts of intergranular, intragranular and moldic pores, and micropores (< 10 m) to macropores. Intragranular and moldic pores are commonly formed by partial to completely dissolution of detrital feldspar, mud intraclasts and mica (papers II and III). Dissolution of these chemically labile grains has created secondary macropores that are, in many cases, well connected to the overall pore system in the sandstone. Secondary porosity in sandstones from the passive margin basins has also been formed by the dissolution of calcite cement (papers II and III). Signicant amounts of microporosity, which induces high water saturation in the reservoir sandstones, occur within kaolin crystals that have replaced feldspar, mud intraclasts and mica. The dissolution of framework grain and cement is more signicant in permeable, coarser-grained, channel complexes than in the nergrained, less permeable crevasse splay sandstones (paper III). Helium porosity and permeability (paper III) is higher in the coarse-grained to conglomeratic, channel complex sandstones (12-23%; av. 17% and 1.41241; av. 190 mD, respectively) than in the ner-grained crevasse splay sandstones (6-15%; 0.6-53 mD; av. 12 mD), resulting in considerable degree of reservoir heterogeneity. In some of the sandstones, reservoir heterogeneity may occur within the same depositional facies owing to variations in the diagenetic evolution pathways that are, in turn, related mainly to variations in the detrital composition.

29

35

channel complex sandstones fine-grained levee sandstones slope and basin-floor-fan sandstones

30

25

Porosity (%)

20

15

10 10 100 1000

Log Permeability (mD)

Figure 5.1: Cross plot of porosity versus log permeability for channel complex, negrained levee, slope and basin oor fan sandstones from passive margin settings. The lack of correlation is presumably owing to the presence of abundant microporosity as well as intragranular and moldic pores that are poorly connected with the overall pore system in the sandstones, which has enhanced porosity without signicant contribution to permeability.

The cross plot of porosity versus permeability values of sandstones from the passive margin reveals no correlation (Fig. 5.1), which is attributed to the presence of considerable amounts of microporosity in the clay minerals, in intragranular pores and moldic pores that are isolated from the overall pore systems. Hence, such pores contribute to the total porosity values but little, if any, to the permeability values. Conversely, sandstones that are characterized by high porosity and permeability values (Fig. 5.1) include those which are rich in quartz grains and characterized by the presence of considerable amounts of intergranular pores to which moldic pores are well connected.

30

6. Predictive Models of Diagensis and Reservoir-Quality Evolution in Deep-Water Turbiditic Sandstones

Integrating the detrital composition of the sand, sequence stratigraphy, and depositional facies is of profound importance in deciphering the spatial and temporal distribution of diagenetic alterations and their impact on reservoirquality evolution pathways. The quartz-feldspar dominated framework grains of turbiditic sandstones from the passive margins are derived predominantly from uplifted granitic and gneissic basement rocks, whereas framework grains of sandstones from the active margin settings are derived from predominantly sedimentary (carbonates and mudstones) and low-grade metamorphic rocks of fold-thrust belts (Fig. 6.1). Sand composition and its impact on reservoirquality evolution pathways are, thus, a function of tectonic setting of the basin. Thus, highly immature, ductile-grains rich, turbiditic sandstones are deposited in active margin settings. Apart from few, extensively carbonate-cemented sandstones, such as those below marine ooding surfaces, compaction is more important than cementation in porosity destruction due to the presence of abundant ductile grains (Fig. 6.2). The inuence of meteoric waters on diagenesis of turbiditic sandstones is limited in such basinal settings, probably because: (i) porosity and permeability are deteriorated early after deposition and precluding circulation of such waters, and (ii) buffering of the acidic meteoric waters by interaction with the abundant carbonate rock fragments. Conversely, the deposition of quartz-feldspar rich sands, which results in mechanically stable and chemically relatively unstable sandstones, is favoured in passive margin conditions owing to the low relief, and hence low erosion rates, intense, prolonged chemical weathering in the source area, long transport distances, and the dominantly granitic-gneissic source rocks (Fig. 6.1). Limited mechanical compaction of turbiditic sandstones from passive margin settings would, thus, lead to porosity preservation to depths as great as 3 km, particularly when the sandstones are rich in grain-coating clays, which retarded cementation by quartz overgrowths (Pittman and Larese, 1991). Conversely, sandstones that are poor in mica and grain-coating clays have lost their porosity and permeability owing to extensive cementation by quartz overgrowths. Considerable amounts of intragranular and moldic porosity were formed in turbiditic sandstones from passive margin basins by the dissolution

31

Quartz

Feldspar
!CTIVEMARGIN

Lithics !CTIVEMARGIN

"

Quartz grain Calcite cement

Low-grade metamorphic rock fragment Quartz cement

Porosity

Mud intraclast Siderite Dolomite

Feldspar

Kaolinitized mica

$ETRITAL CARBONATEGRAIN

Figure 6.1: Schematic model showing the spatial and temporal distribution of diagenetic alterations and variations in the diagenetic evolution pathways in turbiditic sandstones deposited in active and passive margins, respectively. The block diagrams A and B are modied after Bouma and Stone (2000)

32

Mesodiagenesis
'LAUCONY

70C

Eodiagenesis

Passive margin turbidites

Active margin turbidites

0 10
30
0 %

25

20
10

In te rg ra nu la rp or os ity

20

(% )

20

10

50

75

90 100 100
0

25

50

75

Original porosity destroyed by cementation (%)

Figure 6.2: Cross plot of intergranular cement volume versus total intergranular volume (cf. Houseknecht, 1987, modied by Ehrenberg, 1993) of the studied turbiditic sandstones showing that the intergranular porosity has been reduced mainly by compaction rather than by cementation. In contrast to passive margin turbidites, active margin turbidites have almost no porosity.

of framework feldspar, mud intraclasts and mica grains. Grain dissolution in sandstones from passive margin basins was presumably enhanced by the slow rates of primary porosity and permeability loss owing to limited mechanical compaction of ductile framework grains in sandstones, which hence ensured efcient uid ow,. Opposite to what was thought earlier (Bjrlykke, 1983; Bethke, 1989), we provide evidence showing that the diagenesis and reservoir-quality evolution of deep-water, turbiditic sandstones are not merely mediated by marine pore waters, but by meteoric waters too. Meteoric-water incursion into deep-water, passive margins turbiditic sandstones is enigmatic, but is suggested here to occur during shallow burial as response to considerable fall in the relative sea level (Fig. 3.3). Meteoric-water percolation has induced pervasive dissolution and kaolinitization of the framework silicates, and hence in concomitant formation of considerable volume of secondary micro- and macropores, particularly in LST and FSST sandstones. The macropores are, in many cases, fairly well connected to the overall pore system, and have thus contributed to permeability enhancement of the sandstones (papers II and III).

Original porosity destroyed by mechanical compaction and intergranular pressure solution (%)

0
40

10

Cement (%) 20 30

40

Intergranular volume (%)

30

33

7. Computer Modelling of Impact of Fluid Flow on Geochemical and Mineralogical Modications

Computer modelling of the geochemical and mineralogical changes in turbiditic sandstones from passive-margin settings induced by uid-sediment interactions under the initial (i.e., initial mineralogical and organic matter composition of the sediment) and boundary conditions (timing, T, driving mechanism, chemistry of the uid involved) performed. Such computer modelling will give quick insight into how diagenetic processes progress and what are the parameters that control the nal diagenetic products in turbiditic sandstones from passive and active margins and potential development of predictive models of mineral-water interaction pathways (Figs 7.1A and 7.1B). Preliminary simulations, which were conducted using a reaction transport code (DIAPHORE) (Le Gallo et al., 1998), integrate the mineralogy, diagenetic histories and geodynamic contexts of passive versus active margins. Turbiditic sandstones from the ShetlandFaroes Basin and from the Hecho group differ in detrital mineralogy by being quartz-feldspar dominated and hybrid arenites (dominated by carbonate and low-grade metamorphic grain), respectively. Compositional differences are accounted for by selecting representative modal sandstone compositions from representative basins. Meteoric recharge, which is anticipated to occur upon rapid fall in the relative sea level on the shelf, is allowed to occur for the sedimentary pile of the passive margin (ShetlandFaroes) Basin. The geodynamic context controls also the possibilities of tilting of the sedimentary pile upon deposition and subsequent burial. Tilting controls the steepness of the temperature gradients that may occur along a given genetic unit, such as from proximal to distal settings. Assuming that preferential, basinward uid ow pathways existed within these units upon meteoric recharge of the continental shelf (at lowstand), we have tentatively simulated the coupled uid and rock compositional evolutions. We have, so far, explored simple1D geometries where the moving uid is conned to a single, mineralogically homogeneous, sandstone interval. Even in this simple case, the combination of downow increase in temperature and elemental transport drives complex patterns of uid rock interaction, and hence substantial mineralogical changes. For the Shetland-Faroe Basin case, where the temperature gradients is expected to be the lowest, competition be-

35

A
Flow against a temperature gradient 1C km-1 with marine + mudstone-derived waters
60C

after 2 ky

90C porosity

80 75 70 65 60

60C

after 20 ky

90C porosity
solids vol% calcite siderite chlorite illite plagio albite K-felds kaol quartz

inlet

20km

40km 1 10-2 10-4 10-6 10-8

inlet

20km

40km

solutes
mol. kg-1

C Cl Na Ca K Si Fe Al H+

Flow against a temperature gradient 2C km-1 with marine + shale-derived waters

50C

after 10 ky

100C

80 75 70 65 60

50C

after 30 ky

100C
solids vol% calcite siderite chlorite illite plagio albite K-felds kaol quartz

inlet

10km

20km 1 10-2 10-4 10-6 10-8

inlet

10km

20km

solutes
mol. kg-1

C Cl Na Ca K Si Fe Al H+

Figure 7.1: (A) and (B) Simulated evolution of the mineralogy (upper boxes) and the uid chemistry (lower boxes) for a model siliciclastic reservoir from passive margin (e.g. Shetland-Faroes Basin) upon downwards migration of pore waters against a smooth (1C km1 ) temperature gradient. The input water (left side) is seawater equilibrated at low T (60C) with the reservoir mineralogy, with some additional carbonate (representing shale-derived water)

36

tween Ca transport and kinetically controlled, T dependent, plagioclase dissolution drives albitization (+ minor kaolin and calcite), whereas K-feldspar is essentially stable (Figs 7.1A and 7.1B), which is in agreement with petrographical observations (paper II). For the avctive margin (ex. Hecho group) case, basinward owing uids, which are expected to experience much steeper temperature gradients, modelling predicts that albitization of the K-feldspar should develop as a consequence of the temperature dependent Na+ /K+ activity ratio in equilibrium with diagenetic albite and detrital K-feldspars.

37

8. Summary Of The Papers

Paper I 8.1 The Impact of Meteoric Water on The Diagenetic Alterations in Deep-Water, Marine Siliciclastic Turbidites
Meteoric-water ux and formation of kaolinite owing to the dissolution of detrital silicates are common features of continental and paralic sandstones. In deep-water marine sandstones, meteoric-water ux is commonly considered unlikely to occur. However, the study of deep-water, marine sandstones of the ShetlandFaroe Basin on the British continental shelf revealed widespread and extensive dissolution and kaolinitization of mica and feldspar grains, which are attributed to meteoric-water ux during a sea-level lowstand. We suggest that this apparently enigmatic meteoric-water ux mechanism is likely to have occurred by hyperpycnal ow. Hyperpycnal ow occurs when river efuent directly transfers into sediment gravity ow, and enters seawater as a mixture of sediment and fresh water. The likelihood for hyperpycnal ows increases at times when rivers and distributary channels reach the shelf edge, and their ows are delivered directly onto the deepwater slope.

Paper II 8.2 Diagenesis and Reservoir Quality Evolution of Palaeocene Deep-Water, Marine Sandstones, the Shetland-Faroes Basin, British Continental Shelf
Mineralogic, petrographic, and geochemical analyses of siliciclastic, lowstand, transgressive and highstand systems tract turbiditic sediments (Middle-Upper Palaeocene) recovered from six wells in the West of Shetland-Faroes Basin (British continental shelf) are used to decipher and discuss the diagenetic alterations and related reservoir-quality evolution. The Middle-Upper Palaeocene sandstones (subarkoses to arkoses) are cemented by carbonates, quartz and clay minerals. Carbonate cements (intergranular and grain replacive calcite, siderite, ferroan dolomite and ankerite) are of eogenetic and mesogenetic origins. The eogenetic alterations have been
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mediated by marine, meteoric and mixed marine/meteoric pore waters and resulted mainly in the precipitation of calcite ( 18 OV PDB = -10.9 and -3.8 ), trace amounts of non-ferroan dolomite, siderite ( 18 OV PDB = -14.4 to -0.6 ), as well as smectite and kaolinite in the LST and HST turbiditic sandstone below the sequence boundary. Minor eogenetic siderite has precipitated between expanded and kaolinitized micas, primarily biotite. The mesogenetic alterations are interpreted to have been mediated by evolved marine pore waters and resulted in the precipitation of calcite ( 18 OV PDB = -12.9 to -7.8 ) and Fe-dolomite/ankerite ( 18 OV PDB = -12.1 to -6.3 ) at temperatures of 50-140C and 60-140C, respectively. Quartz overgrowths and outgrowth, which post- and pre-date the mesogenetic carbonate cements is common in the LST and TST of distal turbiditic sandstone. Discrete quartz cement, which is closely associated with illite and chlorite, is the nal diagenetic phase. The clay minerals include intergranular and grain replacive eogenetic kaolinite, smectite and mesogenetic illite and chlorite. Kaolinite has been subjected to mesogenetic replacement by dickite, and the K-feldspar and plagioclase grains have been albitized. Dissolution of calcite cement and of framework grain (feldspar, volcanic fragments and mud intraclasts) has resulted in a considerable enhancement of reservoir quality.

Paper III 8.3 Diagenesis of the Urucutuca Formation (Lowe Cretaceous), Espirito Santo Basin, Eastern Brazil: Impact on the Reservoir Quality and Heterogeneity Evolution Pathways in Turbiditic Sandstones
Turbidite sandstones deposited in passive continental margins are currently among the main targets of hydrocarbon exploration. However, the impact of diagenesis on reservoir quality of such sandstones is relatively poorly explored in the literature. Recent studies of turbidite sandstones of different basin have provided evidence showing that the diagenesis and reservoir quality evolution of such sandstones are not merely controlled by marine pore waters but commonly by meteoric waters. Meteoric-water incursion in the Lower Cretaceous, canyon-lling turbiditic sandstones of the Esprito Santo Basin, eastern Brazil, which occurred during shallow burial and as response to a considerable fall in the relative sea-level, induced pervasive dissolution and kaolinitization ( 18 OV SMOW = +13.3 to +15.2 ; DV SMOW = -96.6 to 79.6 ) of the framework silicate grains. Intragranular dissolution macropores, which form by dissolution of feldspar, mud intraclasts and mica grains, are fairly wellconnected to the intergranular pore system, and have thus enhanced permeability of the sandstones. The circulation of meteoric uids probably occurred

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through contacts with Lower Cretaceous sandstones along the margins of the canyons. Eogenetic alterations include cementation by siderite (av. 18 OV PDB = 7.2 ; 13 CV PDB = +9.3 ) and pyrite. Progressive sediment burial (present depths = 1530-2027 m) resulted in the formation of poikilotopic calcite (av. 18 OV PDB = -7.7 ; 13 CV PDB = +3.9 ), ferroan dolomite/ankerite (av. 18 OV PDB = -7.9 ; 13 CV PDB = +2.9 ), partial dickitization of kaolinite and precipitation of minor amounts of quartz overgrowths. Despite the presence of various cement types, mechanical compaction was more important than cementation in reducing depositional porosity in the Urucutuca sandstones.

Paper IV 8.4 Diagenetic Alterations Related to Falling Stage and Lowstand Systems Tracts of Shelf, Slope and Basin Floor Sandstones (Eocene Central Basin, Spitsbergen)
Diagenetic alterations and detrital composition of shelf, slope and basin oor litharenitic to sublitharenitic sandstones from the Eocene Central Basin of Spitsbergen display fairly systematic variations among the falling stage (FSST) and lowstand systems tracts (LST). The diagenetic processes in both systems tracts include mechanical and chemical (pressure dissolution of quartz grains) compaction, kaolinitization of detrital silicates such as mica and feldspar, cementation by carbonates and quartz overgrowths, and illitization of kaolinite. Apart from few, extensively carbonate-cemented sandstones, such as those below marine ooding surfaces, compaction is more important in porosity destruction than cementation due to the abundance of ductile grains. Kaolinitization of detrital silicates is more common in the FSST than in the LST sandstones due to greater meteoric-water ux during sea level fall. However, the mechanisms of meteoric water ux into the FSST slope deposits and basin-oor fan sandstones are enigmatic, but could have been as a consequence of hydraulic head creation along the basin margin during a major fall in the relative sea level. Cementation by carbonates such as calcite and dolomite occurred in both FSST and LST sandstones, being most extensive in sandstones immediately below marine and maximum ooding surfaces, which is attributed to the presence of detrital carbonate grains below these surfaces. The Eocene central basin of Spitsbergen is a potential analogue for the study of other deep-water reservoirs in similar basinal settings in which reservoir quality assessment is of considerable importance. This study shows that constructing a conceptual model for the distribution of diagenetic alterations, and

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thus reservoir-quality evolution in deep-marine turbiditic sandstones is possible by integrating diagenesis and sequence stratigraphy.

Paper V 8.5 The Diagenetic Evolution and Porosity Destruction of Hybrid Turbiditic Arenites of Foreland Basin: Evidence from the Eocene Hecho Group, Pyrenees, Spain
Hybrid turbiditic arenites of the Eocene Hecho Group (south-central Pyrenees, Spain) have been deposited in a foreland basin. The arenites show wide variation in detrital composition, which reect variations in provenance terrains and changes in the relative sea level. The diagenetic evolution pathways of the arenites are closely linked to the variation in detrital composition, particularly the proportion and types of extrabasinal non carbonates (NCE), extrabasinal carbonates (CE), and intrabasinal carbonate (CI) grains. Arenites that are enriched in carbonate grains (CE and CI) are extensively cemented by carbonates (calcite and dolomite) and display intergranular pressure dissolution of the carbonate grains, arenites enriched in ductile low-grade metamorphic rocks (NCE) reveal extensive mechanical compaction, whereas arenites enriched quartz and feldspar display intergranular dissolution of quartz grains, cementation by quartz overgrowths, and albitization of detrital feldspars. Illitic and chloritic clays have presumably been formed by progressive illitization and chloritization of grain-coating smectite.

Paper VI 8.6 Dolomite-Rich Condensed Sections in Overbank Deposits of Turbidite Channels, The Eocene Hecho Group, South-Central Pyrenees, Spain
High-resolution correlation of monotonous, thin-bedded turbidites is desirable but commonly difcult. Correlation within the Eocene turbidites of the Hecho Group, south-central Pyrenees is facilitated by the occurrence of decimetrethick, yellowish beds of micritic limestones and marlstones. These yellow beds (YB) occur in the overbank deposits of major turbidite channel complexes (referred here to as the lower muddy stage). The YB occur at top of sandy deposits within the lowstand wedge of a third-order depositional sequence, as single or multiple beds related to high-frequency, fourth-order depositional cycles. The upper muddy stage, which comprises the rest of the lowstand systems tract contain no YB.
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The YB are interpreted as condensed sections where surfaces of burrowed and abundant planktonic and benthic microfossil assemblages were temporarily sustained by oxygen and nutrients delivered by turbidite currents. The YB are, thus, reliable markers of the early lowstand wedge prograding complex, being coeval with initiation of delta restoration. Whole-rock and XRD analyses indicate that most YB contain detrital clay fraction and consistent excess of Fe, Mn, and P contents, which are ascribed to condensation driving redox relocations (hardground). The YB are also richer in dolomite and calcite than the adjacent claystones, which is attributed to colonization by biogenic algae. Dolomite crystals vary in shape, zonation pattern and chemical composition from early zones are nearly stoichiometric to later more ferroan. The 18 OV PDB values (-10.4 to -6.2 ) of Fe-dolomite, which broadly correlate with 18 OV PDB values (-8.1 to -5.6 ) of calcite suggest formation at elevated temperature. Likewise, dolomite has more radiogenic 87 Sr/86 Sr (0.707926 and 0.707876) than ambient seawater, suggesting partial derivation of Sr from detrital aluminosilicates. These laterally extensive dolomitic YB can act as outstanding potential seals in the overbank deposits for major channel complexes.

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9. Concluding Remarks

The petrological and geochemical studies of the deep-water turbiditic sandstones from four basins along passive and active (foreland) margins have revealed that:
Diagenetic alterations, particularly compaction and, to lesser extent, cementation, have had a profound impact on reservoir-quality evolution pathways Diagenetic and reservoir-quality evolution pathways are closely linked to basinal setting (passive versus active margins), depositional facies, sequence stratigraphy, and burial depth reached by the sandstones. Turbiditic sandstones from active margins are strongly enriched in ductile grains (e.g. low-grade metamorphic rock fragments), which resulted in rapid and near complete elimination of porosity and permeability by mechanical compaction. In contrast to arenites from active margin settings, sandstones from the passive margin basins are enriched in quartz and feldspar, and have thus better retained the depositional porosity and permeability. Additionally, the reservoir quality of these sandstones display reservoir-quality enhancement owing to partial to complete dissolution of framework grains, primarily feldspars, mud intraclasts and micas. In contrast to what was suggested earlier in the literature, diagenetic alterations in deep-marine turbiditic sandstones, particularly those deposited in passive margin basins, are not mediated merely by marine pore waters, but in some cases even by extensive percolation of meteoric waters. Meteoric water percolation is most evidenced (kaolinitization and dissolution of framework silicates) in lowstand systems tract sandstones and is suggested to have occurred during major fall in the relative sea level and consequently shelf exposure. Carbonate cementation is most common, particularly, in the vicinity of marine ooding surfaces, which is attributed, at least partly, to low sedimentation rates (i.e. long residence time of the sediment below the seaoor) and presence of considerable amounts of detrital carbonates. Detrital carbonate grains have acted as nucleation sites for carbonate cementation. The wide ranges and lack of correlation between oxygen and carbon values suggest carbonate cementation at various geochemical conditions and/or temperatures. 45

 Near total lack of glaucony in turbiditic sandstones from the active margin basins, in contrast its common presence or, in some cases, even considerable amounts in turbiditic sandstones from passive margin basins, is attributed to the high rates of sedimentation rates on the shelf and continental slope. Lack of correlation between porosity and permeability and the greater degree of permeability than porosity reduction in the sandstone reservoirs are attributed to the presence of abundant micro-porosity and intragranular and moldic pores that are poorly connected to the overall pore system. Channel complex sandstones are characterized by better reservoir quality than the ner-grained, crevasse splay sandstones.

In summary, this study shows that different strategies should be adopted during hydrocarbon exploration in deep-water turbidites in passive versus active margin basins.

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10. Summary in Swedish

Diagenes och utveckling av reservoarkvalitet hos turbiditiska sandstenar frn djuphavet: Kopplingar till bassngtyp, avsttningsfacies och sekvensstratigra. Sammanfattning
Fr att kunna urskilja diagenetiska frndringar i turbiditiska sandstenar frn djuphavet och deras pverkan p utvecklingen av reservoarkvalitet i tid och rum, har petrologiska och geokemiska studier utfrts p fyra successioner (Krita till Eocen), frn bassnger lokaliserade dels vid aktiva grnser (Foreland), dels vid passiva grnser. Studien visar p den stora betydelsen av tektonisk omgivning, avsttningsfacies, samt frndringar i relativ havsyteniv, parametrar vilka i sin tur kontrollerade kornsammansttning, sedimentationshastighet, sammansttning av porvatten hos de turbiditiska sandstenarna. De allra viktigaste diagenetiska omvandlingar i turbiditsandstenar associerade med passiva marginalbassnger inkluderar upplsning och kaolinitisering av sandkorn (kaolin uppvisar 18 OV SMOW = +13.3 till +15.2 ; DV SMOW = -96.6 till 79.6 ), bildning av klorit hinnor runt kornen, utfllning av karbonater och kvarts som cement, samt mekanisk kompaktering och tryckupplsning av detritisk kvarts. Kaolitiseringen r mest omfattande i bassngbottendeltat och hos strmkanalsandstenarna, vilka hr till the lowstand systems tract. Dessa sandstenar har bibehllit hgre porositet (up till 30%) och permeabilitet (up till 1 Darcy) tack vare den mekaniska stabilitieten hos de detritiska kvarts-fltspatkornen, och av en delvis till fullstndig upplsning av cementmineralen samt av glimmer och fltspat. Fretrdesvis diagenetiska modikationer av turbiditiska sandstenar frn foreland bassngar omfattar cementering av karbonater samt mekanisk kompaktering av de rikligt frekommande duktila sedimentra och lggradigt metamorfa bergartsfragmenten, vilka har sitt ursprung i fold-thrust blten. Dessa diagenetiska omvandlingar resulterade i en total eliminering av ursprunglig porositet och permeabilitet. Den stora variationen i 13 CV PDB vrden hos karbonatcementen frn passiva grnser (ca -18 till +22 ) tyder p att upplst CO2 hrrr frn varierande nedbrytnings processer av organiskt material, t ex bakteriell metanogenes och termal dekarboxylering av kerogen. Mindre variationer i 13 CV PDB vrden (ca -2 till +7 ) hos karbonatcementen frn foreland bassngen tyder p att upplsning av karbonatkornen var
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en viktig CO2 klla. Strre variationer i 18 OV PDB vrden (ca -17 till -1 ) hos karbonatcementen i allmnhet hnfrs till variationer i syreisotopsammansttningen hos vattnet (inkl marint, meteoriskt och formationsvatten) samt i bildningstemperaturen. Denna studie frvntas komma att f stor betydelse vid letning efter olje och gas i djupvatten turbiditsediment i passiva kontra aktiva grnser, srskilt nr det gller utvrderingen av reservoarkvaliteten innan borrningsarbeten pbrjas.

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Acknowledgments

I would like to express my deepest gratitude, appreciation and respect to my supervisor Professor Sadoon Morad, for his guidance, encouragement constructive criticism and comments during all stages of my work. I am greatly indebted to his help regarding matters of academic and non academic concerns. I thank him for contributing to my development as a person and how to become a critical thinker and, potentially, a researcher. I would also like to thank his wife Liisa and his kids for the warm reception and friendship. My thesis has greatly beneted from guidance and support provided by Professor Hemin Koyi, head of Solid-Earth Geology. His unreserved encouragement and help has greatly eased the completion of this thesis. Thank you for teaching me how to present scientic results through your and Dr. Morads excellent course Scientic Writing and Presentation. I am lucky and proud to have a chance to work with some very well established scientists in the eld of diagenesis, among whom are Dr. Luiz Fernando De Ros (Federal University of Rio Grande do Sul, Porto Alegre, Brazil) and Dr. Marcelo Ketzer (Pontical Catholic University of Rio Grande do Sul Environmental Institute). I highly appreciate the strong support and inspiration they have provided me during the entire period of this work. I would like to extend my thanks to my co-authors of the papers Drs. Rafaela Marl (Universidad Complutense de Madrid-Spain), Alessandro Amorosi (University of Bologna-Italy), Daniel Garicia (Centre SPIN -France), Mohamed El-ghali (Al-Fateh University-Libya), Miguel Caja (Universidad Complutense de Madrid-Spain), Edward Remacha (Universitat Autnoma de Barcelona, Barcelona-Spain), Piret Plink-Bjrklund (The Colorado School of Mines Department of Geology and Geological Engineering), Johan Petter Nystuen (University of Oslo), for their valuable contribution and thoughtful discussions on diagenesis and sequence stratigraphy. I wish also to thank the supervisors of my M.Sc. thesis Dr. Niek Molenaar (Denmark Technical University) and Dr. Anders Ahlberg (Lund University) for introducing me the wonderful world of diagenesis. I also thank staff members of the Department of Earth Sciences, Uppsala University for creating such a friendly working environment. Drs. Ala Aldahan, rjan Amcoff, Hans Harryson, Hans Annersten, Per Nysten, Peter Lazor, Hkan Sjstrm, Tore Eriksson, Christopher Talbot, and Per Nysten, for various kinds of help. Special thanks go to Kersti Glersen for many administrative help. I also thank Dr. J.D. Martn-Martn for help with the XRD
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of clay minerals. I am very grateful to Anna, Taher, Johan, and Leif for all the help with printing and technical issues. Sincere thanks go to my former and present colleagues and dear friends at the department Dr. Mohamed Elghali, Dr. Khalid Al-Ramadan, Osama Hlal, Masoumeh Kordi, Faramarz Nilfouroushan, Zurab Chemia, Hesam Kazemeini, Alireza Malemir, Erik Ogenhall, Soa Winell, Zuzana Konopkova, Kristina Zarins, Sara Carlsson, Farag El-Khutari, Ashour Abouessa, Muftah Khalifa, Lijam Hagos Zemichael, Tuna Eken, Mattias Lindman. Masoumeh and Zurab have provided invaluable assistance in editing this thesis, without their friendship and care I would have faced much more complexities. In Uppsala there are many great friends whom helped me to solve daily life problems, in particular my dear friend Mahir and his wonderful wife Sayran, they have helped me and my family in many critical moments and they have always been there for us when we needed assistance. Dr. Ron Steel (University of Texas, Austin), Christian Carlsson and Anna Pontn (Gteborg university) are specially acknowledged for providing invaluable assistance in the eld. I have many wonderful friends and relatives outside the academia, who helped me, supported me and had the condence that I will accomplish this thesis work. In particular I would like to thank Dr. John Fournier from Chicago (for stimulating discussions about science and history), Dr. Saleem Qadir and his wife Dr. Yasameen Shakir for their continuous support and interest in my research work. I would like to take this opportunity to tell my dear parents, brothers and sisters, my beloved kids, nephews and nieces that I owe you everything. You stayed by my side and showered me with love, kindness and care, which made feel that I am extremely lucky to have been blessed with such a family. Many thanks go to my mother in law and brothers and sisters in law and my cousins whom always provided me with a safe haven when I was in need of rest. I want to express my heartfelt thanks to my wife Zakaw and tell her that she made my life very exciting and happy. I would not have reached my destination without your love and affection. Thank you for always being there for me no matter what new difculty appeared, and for never stop believing that I would eventually nish my Ph.D. studies successfully. There are simply too many people to mention and thank by name. But I would like to mention several of you, who have spent considerable time in encouraging me and never lost interest in what I was doing: Pishtiwan, Zhuka, Firas, Sarwar, Sakar, Hevy, Qazi, Bayar, Hiwa, Vian, Nian (and your wonderful parents),Sura, Sardar, Walid, Shamal, Dila (Rahman), Ara, Sardar, Nyan, Meha, Shilan, Shwan, Shawnm, Zhala, Shaho, Awni, Zyad, Zirak, Dara, Zozek, Handren, Mursal, Rasul, Mustafa, Nasrin, Kubra, Farida, Nushin, Parvin, Sharmin, Sirwa, Firishta, Yasin, Afshin, Masud, Nasir, Simko, Sarbaz, Rojgar, Dara, Mercedes, Jos Luis Prez.

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Acta Universitatis Upsaliensis

Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 279 Editor: The Dean of the Faculty of Science and Technology A doctoral dissertation from the Faculty of Science and Technology, Uppsala University, is usually a summary of a number of papers. A few copies of the complete dissertation are kept at major Swedish research libraries, while the summary alone is distributed internationally through the series Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology. (Prior to January, 2005, the series was published under the title Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology.)

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