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Contents 5.3 Energy Transfer and Quenching at low temperature . . . . . . . . . . 214 5.4 Modeling the temperature effect on crude oil fluorescence . . . . . . . 216 5.5 Quenching of crude oil fluorescence . . . . . . . . . . . . . . . . . . . 227 5.6 Viscosity effect on crude oil fluorescence . . . . . . . . . . . . . . . . 229 5.7 Thermodynamic Considerations of crude oil photophysics . . . . . . . 231 5.8 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 238 6 Conclusions and Future Work 240 A Reference Lifetime Standards 243 A.1 Standards for FD lifetime measurements . . . . . . . . . . . . . . . . 243 A.2 HPTS: 8-hydroxypyrene-1,3,6-trisulphonic acid trisodium salt (com- mon name: Pyranine) . . . . . . . . . . . . . . . . . . . . . . . . . . . 244 A.3 SPA N-(3-sulfopropyl) acridinium salt . . . . . . . . . . . . . . . . . . 247 A.4 Rhodamine B . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 249 A.5 Acridone . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 251 A.6 Coumarin 6 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 254 A.7 Coumarin 30 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 256 A.8 Coumarin 314 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 258 A.9 Lucifer Yellow CH di-potassium salt . . . . . . . . . . . . . . . . . . . 260 B Supplementary Data 262 B.1 Frequency Domain Lifetime Data . . . . . . . . . . . . . . . . . . . . 262 C HCFI analysis - an application of crude oil fluorescence lifetime analysis 272 C.1 FD analysis of HCFI . . . . . . . . . . . . . . . . . . . . . . . . . . . 273 C.1.1 Distinguishing HCFI by lifetime . . . . . . . . . . . . . . . . . 276 C.2 A final word . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 279 D Published Work 281 Bibliography I vii
List of Publications and Presentations The work outlined in this has been published, in part, in the following manuscripts: Publications 1. P. Owens, A.G. Ryder and N.J.F. Blamey (2008), Frequency Domain Flu- orescence Lifetime Study of Crude Petroleum Oils, Journal of Fluorescence, 18(5):997–1006. 2. P. Owens and A.G. Ryder, “Low temperature lifetime study of crude petroleum oils,” manuscript in preparation. Co-authored Papers 1. Blamey N.J.F., Ryder A.G., Feely M., Dockery P., Owens P. (2008), The application of structured-light illumination microscopy to hydrocarbon-bearing fluid inclusions, Geofluids 8(2): 102 -112. 2. Blamey N.J.F., Ryder A.G., Owens P. and Feely M., “Accurate characterisa- tion of hydrocarbon-bearing fluid inclusions using frequency domain fluorescence lifetime measurements”, Manuscript in preparation. Abstracts and Presentations 1. Owens P. and Ryder A.G.,“Dynamics of crude oil fluorescence revealed by low temperature time-resolved single photon counting studies”, XXII IUPAC Symposium on Photochemistry, Gothenburg, Sweden, 28th July -1st August 2008.[Poster] viii
Page 1 and 2: Time-Resolved Fluorescence Spectros
Page 3 and 4: Abstract behaviour allowing calcula
Page 5 and 6: Contents List of Publications and P
Page 7: Contents 2.3 Temperature based Life
Page 11 and 12: Abbreviations Abbrev Definition API
Page 13 and 14: Chapter 1 Introduction For many yea
Page 15 and 16: Introduction temperature increases
Page 17 and 18: A seal or cap-rock that prevents th
Page 19 and 20: Introduction Figure 1.2: Crude oil
Page 21 and 22: Introduction eroatoms (O, S, N) and
Page 23 and 24: Introduction toluene, dichlorometha
Page 25 and 26: 1.2 Fluorescence Spectroscopy 1.2.1
Page 27 and 28: Introduction S1 state for a certain
Page 29 and 30: Introduction The peaks in the absor
Page 31 and 32: Introduction Figure 1.9: Jablonski
Page 33 and 34: Introduction Figure 1.10: Static qu
Page 35 and 36: Introduction the ratio of τ 0/τ i
Page 37 and 38: 1.2.5 Measuring fluorescence lifeti
Page 39 and 40: Introduction Figure 1.14: Time-reso
Page 41 and 42: Introduction The autocorrelation fu
Page 43 and 44: Introduction case, the molecules ex
Page 45 and 46: From Equation 1.26, Introduction ω
Page 47 and 48: m = 1 P 2 + Q 2 Introduction (1.36
Page 49 and 50: Introduction based average lifetime
Page 51 and 52: Introduction Figure 1.21: General p
Page 53 and 54: Introduction TAC output pulse is gi
Page 55 and 56: Introduction at each frequency acco
Page 57 and 58: Introduction diagram showing the op
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Introduction Figure 1.26: Schematic
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Introduction provides enhanced cont
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Introduction PAH’s. It has been s
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to heavy oils (low API gravity). In
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Introduction The balance between en
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Introduction Figure 1.34: Fluoresce
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Introduction used [126, 129, 132] a
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Introduction Figure 1.36: Plot of a
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fractional contributions over time
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Introduction concentration and Ksv
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1.5 Crude oil photophysics Introduc
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Introduction stages of thermal matu
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Introduction yellow to red fluoresc
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1.7 Thesis goal Introduction This i
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Materials and Methods concentration
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Table 2.2: Fractionation Data for B
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Materials and Methods 2.2 Frequency
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Materials and Methods was within ±
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Materials and Methods The dichroic
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Figure 2.5: Transmission characteri
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Materials and Methods Figure 2.7: S
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Materials and Methods The variation
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Materials and Methods Figure 2.9: L
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Materials and Methods Figure 2.10:
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Materials and Methods Comparison ca
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Materials and Methods with ρ param
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Materials and Methods 2.3 Temperatu
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Materials and Methods IRF of the sy
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Materials and Methods 2.4 Temperatu
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Materials and Methods a series of w
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Materials and Methods 2. Using the
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Lifetime study on crude oils by the
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Table 3.3: Average lifetime and sin
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Table 3.5: Average lifetime and sin
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3.5 Single Lifetime distributions L
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Energy Transfer and Quenching proce
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Influence of low temperature on flu
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Conclusions and Future Work model (
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Appendix A Reference Lifetime Stand
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Appendix Figure A.2: FD response fo
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A.3 SPA N-(3-sulfopropyl) acridiniu
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A.4 Rhodamine B Appendix Rhodamine
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A.5 Acridone Appendix The highly ph
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Appendix Figure A.11: FD response f
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Table B.1: Frequency Domain average
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Appendix Table B.3: Emission λmax
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Table B.5: Frequency Domain lifetim
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Appendix for the determination of t
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Appendix Figure C.3: Multifrequency
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Appendix Figure C.5: FLIM intensity
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Appendix Table C.1: Fluorescence li
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Appendix D Published Work 281
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998 J Fluoresc (2008) 18:997-1006 s
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1000 J Fluoresc (2008) 18:997-1006
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1002 J Fluoresc (2008) 18:997-1006
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1004 J Fluoresc (2008) 18:997-1006
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1006 J Fluoresc (2008) 18:997-1006
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Bibliography [10] W. G. Dow (1977),
Page 307 and 308:
Bibliography [31] M. A. Ali and W.
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Bibliography [53] R. D. Spencer and
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Bibliography [75] K. Konig (2000),
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Bibliography [93] C. Pasquini and A
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Bibliography [113] C. Ralston, X. W
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Bibliography [132] A. Ryder (2004),
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Bibliography variable-angle synchro
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Bibliography [171] R. K. McLimans (
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Bibliography using fluorescence spe
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Bibliography [210] H. Mishra, S. Pa
Page 327 and 328:
Bibliography [229] N. Boens, W. W.
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