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Mineralogy, Petrography, and Microstructural Evolution of The Primary and secondary pyrite textures from the Parys Mountain Volcanogenic Massive Sulphide Deposit, Wales: an electron backscatter diffraction investigation Michael A. Salter Department of Earth and Ocean Sciences, University of Liverpool, Liverpool, L69 3GP, UK. E-mail: [email protected] Abstract Colloform textures develop in a sequential manner and have the potential to record changing ore-forming conditions. Current understanding of colloform growth controls is limited. Recent studies invoke possible links between crystal morphology, degree of supersaturation, and development of crystallographic preferred orientations (CPOs) with common axes that switch across layer interfaces. Another possible factor is trace element sequestration. Further development of these ideas here utilises forescatter orientation contrast (OC) imaging and electron backscatter diffraction (EBSD) to investigate crystal morphology and CPOs in colloforms from the Parys Mountain polymetallic sulphide deposit. Results from two colloforms indicate development of CPO is commonly about <100> and only rarely about <110> and <111>. Both colloforms show weak CPOs consistent with coarse grain size and stronger CPOs consistent with small grain size, thereby demonstrating a possible link between crystal nucleation rate, degree of supersaturation, and strength of CPO development. In contrast to results of previous studies, common axes frequently lie parallel to nucleation surface and normal to growth direction. This is difficult to reconcile with ore-forming fluid and trace element growth controls and is most easily explained by syntaxial relationship with nucleation surfaces. Abrupt switching of common axis orientation across layer interfaces appears to eliminate this as a possible growth control, but a syntaxial relationship is demonstrated across at least one layer interface. Page | 1 Similar techniques are employed in the second part of this work to investigate the nature of deformation of pyrite in low-grade metamorphic terranes. Plastic deformation by dislocation creep is demonstrated at a likely maximum of ~260 °C, representing a new lower limit for such mechanisms. Slip of ~5-20° is demonstrated to be common about <100> directions and occurs more rarely about <110>. Individual grains commonly show multiple rotations about different axes. Introduction Understanding the primary and secondary mineralogical textures, and the mechanisms by which minerals deform, is central to comprehending the geological evolution of sulphide ore deposits (Gilligan & Marshall, 1987). Many ore deposits form at plate margins (Allen et al., 2002) and are commonly subject to metamorphism and/or deformation in subsequent orogenic events during basin closure. Most of the common economic sulphide minerals (e.g. sphalerite, chalcopyrite, and galena) are soft, and undergo intense recrystallisation and grain coarsening in all but the lowest metamorphic grades. Furthermore, they often only preserve deformation textures from retrograde metamorphic conditions (Vokes, 1969). Although not of economic importance, the refractory nature of pyrite, stable under a wide range of conditions and fS2, means it is capable of preserving primary and deformational textures produced prior to peak metamorphism (Craig and Vokes, 1993; Barrie et al., 2007), and is therefore important in understanding the genesis and deformational evolution of ore bodies, thus aiding their successful exploitation. Pyrite in ore deposits commonly takes the form of equant cubes, framboids, and colloforms. The latter two textures are regarded as the result of primary precipitation in open spaces in rocks, such as fissures or vugs (Craig, 2001). Colloform textures record conditions during precipitation of primary ore minerals, and their discrete layers provide sequential information Page | 2 about the evolution of chemical and physical conditions during ore formation (Foley et al., 2001; Barrie, 2009). They are considered to develop by direct crystallisation due to a high degree of supersaturation (Roedder, 1968) rather than an earlier postulated process invoking the accretion of colloidal gels (Rogers, 1917). Although widely reported as present in ore deposits (e.g. McClay, 1991), only recent work (Freitag et al., 2004; Barrie et al., 2009a; b) has investigated the mechanisms of colloform growth and what they reveal about ore forming environments. Freitag et al. (2004) use scanning electron microscope (SEM)-based electron backscatter diffraction (EBSD) facilities to analyse discrete colloform pyrite layers from Greens Creek, Alaska. They show a crystallographic preferred orientation (CPO) initially developed about a <100>, then a <110>, crystallographic axis associated with a change in grain size. CPO development and switching is considered a primary feature, conjectured to be controlled by changing redox conditions during precipitation, by analogy with models that explain grain size and ordering relationships in framboidal pyrite (Ohfuji et al., 2005). The significance of such a relationship in colloform texture is greater than in framboidal texture, as an evolutionary sequence of conditions is preserved rather than a single snapshot. Barrie et al. (2009a) find that colloform pyrite textures from Greens Creek, Alaska, and Ezuri, Japan, exhibit initially random crystal orientation followed by CPOs developed about <100>, <110>, and <111> crystallographic axes in subsequent layers. Similarity occurs despite δ34S isotope data that suggests quite different sulphur sources at these locations. Barrie et al. (2009b) find a similar style of switching between orientation axes in colloform sphalerite textures from Galmoy, Ireland. Such CPO changes are interpreted as the effect of changing temperature and degree of supersaturation during two-fluid mixing. Other possible controls include trace element sequestration, in situ bacteria-induced mineralisation, redox conditions, Page | 3 and sulphur source, although the results from Greens Creek and Ezuri imply that the latter is of low significance (Barrie et al., 2009a). Early studies of pyrite (e.g. Gill 1969; Graf and Skinner 1970) suggest that it is a very hard mineral that deforms by cataclasis over a large P-T field. Later experimental investigations reveal it is capable of deforming in a ductile manner and indicates a brittle–ductile transition at ~425 °C (Cox et al., 1981; Graf et al., 1981; McClay and Ellis, 1983). Cox et al. (1981) suggest that {100}<001> and possibly {100}<011> are major slip systems. {110} dislocation glide may also be important, but its critical resolved shear stress (CRSS) is several times higher than {100} glide, so it is probably less important. Barrie et al. (2007) demonstrate dislocation creep occurring principally as a lattice rotation about a single <100> axis, and less commonly about a single <110> axis. Further experimental studies (Barrie et al., 2008) involving shortening parallel to <100> and <110> confirm the dominant slip system is {001}<100>, with slip in this plane activated when <100> is oriented at >~5-15° to shortening direction. Slip on {110} planes is suggested to occur only when <100> is oriented parallel to shortening direction. Deformation mechanism maps for pyrite have been produced on the basis of experimental results (McClay and Ellis, 1983). These are of great value in determining the deformational behaviour of different phases in ore bodies that have experienced a known set of stress, strain, and temperature conditions (Siemes et al., 1991), and it is therefore important that they present accurate information. However, experimental deformation is limited by high strain- rates relative to those in nature, and thus yields temperatures that likely represent an upper limit for transition to the dislocation field of deformation. Recent work on naturally deformed pyrite (Freitag et al., 2004) indicates that dislocation glide and creep can take place at lower Page | 4 greenschist facies conditions, much lower temperature than indicated in experimental studies. A revision of the pyrite deformation mechanism map is therefore necessary. The aims of the present study, based on samples from the Parys Mountain polymetallic sulphide deposit, Anglesey, North Wales, are two-fold. The first part examines discrete layering in colloform pyrite textures, in order to offer comparison of colloform growth styles and mechanisms with those of Greens Creek, Ezuri (Freitag et al., 2004; Barrie et al., 2009 a), and Galmoy (Barrie et al., 2009b). The second part extends the investigation of naturally occurring plastic deformation of individual pyrite grains into lower anchizone metamorphic conditions (Merriman, 2006), as such representing a new low temperature constraint for initiation of plastic deformation. Both parts utilise EBSD facilities in combination with forescatter orientation contrast (OC) imaging. The results are coupled with energy dispersive X-ray (EDX) chemical mapping to explore the possibility of a link between microstructures and element distribution. Geological Setting Parys Mountain forms a low profile hill in the northeast of Anglesey, northwest Wales. Anglesey comprises a thin sequence of Lower Palaeozoic Welsh Basin strata that discontinuously and unconformably overlie a Precambrian basement of schists and gneisses (Barrett et al., 1999). Locally, sedimentation in the Ordovician and Silurian is considered to have been tectonically controlled (Bates, 1966), with the Carmel Head Thrust (fig 1) probably playing an important role.
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