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«THE ROLE OF FLUIDS IN GEOLOGICAL PROCESSES by Tristan Azbej Dissertation submitted to the faculty of the Virginia Polytechnic Institute and State ...»

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THE ROLE OF FLUIDS IN GEOLOGICAL PROCESSES

by

Tristan Azbej

Dissertation submitted to the faculty of the Virginia Polytechnic Institute and State

University in partial fulfillment of the requirements for the degree of

Doctor of Philosophy in Geosciences

Committee Chairman: Robert J. Bodnar

Committee: James Beard, Erdogan Kiran, Donald Rimstidt, Csaba Szabo,

Robert Tracy

August 22nd, 2006

Blacksburg, Virginia

Key words: critical fluids, laser raman spectrometry, melt inclusions, ocelli

THE ROLE OF FLUIDS IN GEOLOGICAL PROCESSES

Azbej Tristan (ABSTRACT) The role and behavior of fluids in hydrothermal and magmatic environments have been studied. Experimental studies have been carried out to determine fluid properties, in natural environments and in both synthetic and natural fluid and melt inclusions.

One of these studies dealt with the effect of composition on the critical P-T-X properties of aqueous salt solutions approximated by the H2O-NaCl-KCl-CaCl2 system. The results indicate a systematic variation in critical properties as a function of composition over the range of P-T-X studied.

A technique for analyzing individual H2O-CO2 inclusions using Raman spectroscopy has also been developed. The resulting empirical equation relating Raman intensities and composition is valid for compositions ≤50mol% CO2. The technique has been applied to H2O-CO2 inclusions from the Butte, MT Porphyry CuMo deposit and the results agree with compositions estimated from microthermometric and petrographic observations.

The aim of another study was to study water loss from melt inclusions during laboratory heating. Melt inclusions had lost insignificant amounts of water when held at experimental conditions (800°C, 1 kbar) for ≤24 hours. However, significant water loss was observed for longer duration experiments.

Ocelli, which are globular bodies of felsic minerals are interpreted as products of magmatic melt immiscibility. As such, the carbonate aggregates in Cretaceous lamprophyres from Hungary with similar petrographic characteristics have also generally been interpreted to be products of magmatic immiscibility. Petrographic and geochemic studies have shown three three distinct genetic groups for these aggregates, none of which were consistent with a magmatic origin.

Table of contents Chapter I – Introduction I.1 Synthetic fluid inclusions XVII: Critical PTX properties of H2O-NaCl-KCl solutions……………………………………………………………………….1 I.2 In Situ Quantitative Analysis of Individual H2O-CO2 Fluid Inclusions by Laser Raman Spectroscopy…………………………………………………....2 I.3 Experimental determination of H2O loss from melt inclusions during laboratory heating……………………………………………………………...4 I.4 Genesis of carbonate aggregates in lamprophyres from the northeastern Transdanubian Central Range, Hungary: Magmatic or hydrothermal origin?...5 CHAPTER 2. – Synthetic fluid inclusions XVII: PTX properties of H2O-NaCl-KClCaCl2 solutions in the vicinity of the critical point II.1. Introduction………………………………………………………………7 II.2. Phase Equilibria in Aqueous Salt Solutions……………………………...8 II.3. Experimental Methods…………………………………………………..14 II.4. Results and Discussion………………………………………………….18 II.5. Summary………………………………………………………………...30 II.6. Acknowledgements……………………………………………………...30 II.7.References………………………………………………………………..31 CHAPTER 3. - In Situ Quantitative Analysis of Individual H2O-CO2 Fluid Inclusions by Laser Raman Spectroscopy III.1. Introduction……………………………………………………………35 III.2. Analytical Methods…………………………………………………....36 III.3. Results and Discussion………………………………………………..40 III.4. Application to Natural Inclusions……………………………………..48 III.5. Conclusions……………………………………………………………50 III.6. Acknowledgements……………………………………………………51 III.7. References……………………………………………………………..51 iii CHAPTER IV - Experimental determination of H2O loss from melt inclusions during laboratory heating IV.1. Introduction……………………………………………………….……56 IV.2. Raman Spectra of Hydrous Glass………………………….……….….57 IV.3. Calibration of the Raman spectra……………………………………....61 IV.4. Water loss from melt inclusions……………………………..……...….66 IV.5. Conclusions………………………………………………………….....80 IV.6. Acknowledgements………………………………………………..…...81 IV.7. References Cited..……………………………………………...………81 CHAPTER V. - Genesis of carbonate aggregates in lamprophyres from the northeastern Transdanubian Central Range, Hungary: Magmatic or hydrothermal origin?





V.1. Introduction…………………………………………………….……….88 V.2. Geological Background and Lamprophyre Petrology…………….…….89 V.3. Samples Studied and Analytical Methods…………….………….……..92 V.4. Petrography……………………………………………………………..93 V.5. Chemical Composition of Carbonate Aggregates………………………95 V.6. Microthermometric Analyses…………………………………….……..99 V.7. Discussion…………………………………………………..…………103 V.8. Conclusions……………………………………………………………108 V.9. Acknowledgements…………………………………………………....110 V.10. References……………………………………...…………………….110

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Figure 1.3.

Relationship between water content of melt inclusions in quartz 5 from the Bishop Tuff and the amount of time held at 800ºC and 1 kbar.

Figure 1.4.

Estimates of P-T formation conditions for carbonate aggregates in 6 the TCR lamprophyres.

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Figure 2.2.

Schematic phase diagram of H2O and the critical curves of the H2O- 10 NaCl.

Figure 2.3.

Schematic segment of the phase diagram H2O-NaCl phase diagram. 12

–  –  –

Figure 2.5.

Determination of critical conditions of a solution using the slope- 16 intercept technique.

Figure 2.6.

Critical temperature curves of H2O-KCl-NaCl solutions. 21

–  –  –

Figure 2.10.

Critical points of 2 molal H2O-NaCl-KCl–CaCl2 solutions. 29 Figure 3.1.

Raman spectrum (at 350°C) showing the peaks for CO2 (1388 cm-1) 39 and H2O (3600 cm-1).

Figure 3.2.

Raman linear peak intensity ratios calculated for different 40 acquisition times.

Figure 3.3.

Relationship between composition of H2O-CO2 inclusions and 42 Raman spectral intensity ratios.

Figure 3.4.

Raman linear peak intensity ratios of CO2-H2O inclusions. 44

–  –  –

Figure 4.2.

Comparison of Raman spectra of a melt inclusion (inset) in quartz. 60 Figure 4.3.

Summary of the procedures used to treat Raman spectra obtained on 63 hydrous glasses.

Figure 4.4.

Relationship between the amount of water in hydrous glass and the 64 ratio between the water peak area at 3550 cm-1 and the T-O-T peak area band centered at 1050 cm-1.

Figure 4.5.

Relationship between water content of melt inclusions in quartz 73 from the Bishop Tuff and the amount of time held at 800°C and 1 kbar.

Figure 4.6.

Relationship between ratio of the bubble area to the total area of the 78 melt inclusion and amount of time the inclusion was held at 800°C and 1 kbar.

Figure 4.7.

Comparison between the single-standard technique used by Thomas 79 et al. (2006) & Di Muro et al. (2006), and the multiple standard calibration technique.

Figure. 5.1. Geological map of the northeastern Transdanubian Central Range 91 (TCR).

Figure. 5.2. Photomicrographs (A, C, D, E, H) and BSE images (B, F) of 94 carbonate aggregates in the TCR lamprophyres.

Figure 5.3.

Ternary CaO–MgO–FeO diagrams showing compositions of 96 carbonate phases in aggregates from the TCR lamprophyres.

Figure 5.4.

Homogenization temperatures of fluid inclusions hosted in 101 carbonate aggregates.

Figure 5.5.

Estimates of P-T formation conditions for carbonate aggregates in 106 the TCR lamprophyres.

–  –  –

Table 2.1.

Homogenization temperatures of and behavior of synthetoc H2O– 19 KCl inclusions Table 2.2.

Homogenization temperatures of and behavior of synthetic H2O– 23 NaCl-KCl inclusions (mNaCl:mKCl = 1:1) Table 2.3.

Homogenization temperatures of and behavior of synthetic H2O– 25 NaCl-KCl inclusions (mNaCl:mKCl = 3:1 and 1:3) Table 3.1. Raman linear peak intensity ratios of H2O-CO2 synthetic fluid 42 inclusion standards.

Table 3.2.

Raman spectral linear peak intensity ratios of H2O-CO2 synthetic 44 fluid inclusion standards collected at various temperatures Table 3.3.

Raman spectral peak area ratios of H2O-CO2 synthetic fluid 47 inclusion standards collected at various temperatures.

Table 3.4.

Raman spectral peak area ratios of H2O-CO2 synthetic fluid inclusion 47 standards.

–  –  –

Table 4.2.

Results of Raman analysis of melt inclusions in early-erupted Bishop 69 Tuff quartz Table 5.1a.

Table 1a. Average composition of carbonate minerals in Type-I 97 aggregates from the TCR lamprophyres.

Table 5.1b.

Table 1b. Average composition of carbonate minerals in Type-II 98 and -III aggregates from the TCR lamprophyres.

Table 5.1c.

Table 1c. Average composition of carbonate minerals in veins from 99 the TCR lamprophyres.

Table 5.2.

Average ice-melting temperatures and salinities of fluid inclusions in 102 carbonate aggregates from the TCR lamprophyres.

Table 5.3.

Summary of petrographic, geochemical and microthermometric 109 characteristics of different carbonate aggregate types in the TCR lamprophyres.

–  –  –

This dissertation includes, in addition to this introductory chapter, four chapters each describing a different project. The overriding theme that ties all of these studies together is the role and behavior of fluids in hydrothermal and magmatic environments.

These projects include experimental studies to determine fluid properties, as well as studies of fluids in both synthetic and natural fluid and melt inclusions.

I.1. Critical PTX properties of H2O-NaCl-KCl solutions

Hydrothermal fluids in their critical or near-critical states exhibit anomalous physical and thermodynamic properties that affect mass and energy transport in hydrothermal systems. This project investigated the effect of composition on the critical P-T-X properties of aqueous salt solutions. Fluids approximated by the H2O-NaCl-KClCaCl2 system are common in many geologic environments including submarine hydrothermal environments and other hydrothermal ore-forming systems. In this study, P-T location of the critical point and the projection of the critical isochore have been determined for various compositions in the H2O-NaCl-KCl-CaCl2 system, for salinities ≤3 molal. The results indicate a systematic variation in critical properties as a function of composition over the range of P-T-X studied (Fig 1.1.).

Figure 1.1.

Critical points of 2 molal H2O-NaCl-KCl–CaCl2 solutions. Dashed lines represent projected mixing curves between the binary end-member solutions. Ratios represent the molar ratio of solutes in ternary and quaternary solutions.

I.2. In Situ Quantitative Analysis of Individual H2O-CO2 Fluid Inclusions by Laser Raman Spectroscopy Fluids approximated by the H2O-CO2±salt system are common in hydrothermal ore deposits and in medium- to high-grade metamorphic rocks. Interpretation of fluid inclusions from these environments requires information on the H2O-CO2 ratio of the fluids because the isochores and metamorphic phase equilibria vary with fluid composition. In this study a technique for analyzing individual H2O-CO2 inclusions using Raman spectroscopy is described (Fig. 1.2.). This technique eliminates the need to know the geometry of the inclusions and the host sample as required for quantitative FTIR analysis and allows much smaller inclusions to be analyzed. The resulting empirical equation relating Raman intensities and composition is valid for compositions ≤50mol% CO2. The technique has been applied to H2O-CO2 inclusions from the Butte, MT Porphyry Cu-Mo deposit and the results agree with compositions estimated from microthermometric and petrographic observations.

Figure 1.2.



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