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Ecological Burrow Network (Stochastic) GEOLOGICA ULTRAIECTINA MEDELINGEN VAN DE FACULTEIT GEOWETENSCHAPPEN UNIVERSITEIT UTRECHT No. 231 Heterogeneity, Uncertainty and Process Identi'fication in Early Diagenesis: New Model Developments with Applications to Biological Mixing Christof Meile Heterogeneity, Uncertainty and Process Identification in Early Diagenesis: New Model Developments with Applications to Biological Mixing Heterogeniteit, onzekerheid en proces-identificatie in vroege diagenese: Nieuwe modelontwikkelingen met toepassingen op het gebied van biologische menging (met een samenvatting in het Nederlands) Dissertation presented for the degree of doctor at Utrecht University under the authority of the rector Prof. W.H. Gispen to be defended in public on September 22,2003 at 12.45 o'clock, in accordance with the decision made by the Board for the of Doctoral Degrees by Christof Dieter Meile born in Miinsterlingen, Switzerland, on August 20, 1970 Supervisor: Prof. P. Van Cappellen Department of Geochemistry Faculty of Earth Sciences Utrecht University The doctoral dissertation was produced with the financial support of the Institute for Paleoenvironments and Paleoclimate Utrecht (IPPU) and the Netherlands Organisation of Scientific Research (NWO-Pionier) ISBN 90-5744-089-X Piaget: What makes the wind? Julia: The trees. Piaget: How do you know? Julia: I saw them waving their arms. Piaget: How does that make the wind? Julia (waiving her hands): Like this. Only they are bigger. And there are lots of trees. Piaget: What makes the wind on the ocean? Julia: It blows there from the land. No. It's the waves... Dialogue attributed to Jean Piaget (1896-1980) TABLE OF CONTENTS ACKNOWLEDGMENTS 9 SUMMARY/SAMENVATnNG 11 CHAPTER 1 13 Introduction CHAPTER 2 25 Meile, c., and Van Cappellen, P. (2003). Global estimates of enhanced solute transport in marine sediments. Limnology and Oceanography 48(2): 777-786. CHAPTER 3 43 Meile, C., Koretsky, C.M.. Van Cappellen, P. (2001). Quantifying bioirrigation in aquatic sediments: An inverse modeling approach. Limnology and Oceanography 46(l): 164-177. CHAPTER 4 63 Koretsky, C.M., Meile, C.. Van Cappellen, P. (2002). Quantifying bioirrigation using ecological parameters: A stochastic approach. Geochemical Transactions 3(3): 17-30. CHAPTERS 87 Meile, C., Tuncay, K., and Van Cappellen, P. (2003). Explicit representation of spatial heterogeneity in reactive transport models: Application to bioirrigated sediments. Journal ofGeochemical Exploration 78-79: 231-234. CHAPTER 6 93 Meile, c., and Van Cappellen, P. (in preparation). Particle age distribution and O2 exposure time: Timescales in bioturbated sediments. CHAPTER 7 111 Meile, C. and Regnier, P. (in preparation). Towards a flexible modeling framework for objective analysis of dynamic aquatic systems. CURRICULUM VITAE 135 Acknowledgments ACKNOWLEDGMENTS I would like to thank Philippe Van Cappellen for his advice, support, the freedom of exploration, friendship and the possibility for my extensive stays abroad. The members of my reading committee, B. Boudreau, C. Heip, R. Jahnke, J. Middelburg, M. Schluter, P. Regnier and B. van der Zwaan, are thanked for carefully reading the thesis and valuable feedback. Not to a small part, my life in Utrecht was fun due to the excellent company I had with Christelle, Parisa, and occasionally Jeff, in the office, and the Geochemistry department as a whole. I truly enjoyed the interactions with our more experimentally working group members. For getting the thesis printed, thanks go to C6line and Pien. I also would like to thank Anniet and Caroline for the Dutch translation of the summary and Kagan, Parisa, Pien'e, David and Ralf for the nice collaborations and common projects still to come. I also would like to thank Carla Koretsky for the continued collaboration and Bernhard Wehrli, who introduced me to science and made my initial journey across the Atlantic, which later lead to my move to the Netherlands, possible. Financial support from the Institute for Paleoenvironments and Paleoclimate Utrecht (IPPU) and the Netherlands Organisation of Scientific Research (NWO-Pionier), and the hospitality I experienced both at the School of Marine Sciences at the University of Georgia, USA. and at the Hanse Institute for Advanced Study in Delmenhorst, Germany, are gratefully acknowledged. Finally, I want to thank my parents for the strong and unconditional love and support. I hope to be able to follow their example. And I want to thank Mandy for not getting too tired of the long transatlantic commutes over the years. Support for mental balance from Casey Bubba, Ben "the animal" and Tobs is also acknowledged. Christof Meile 9 Summary SUMMARY Within the last decades, there have been spectacular developments in experimental and analytical techniques that allow geochemists and biologists to acquire ever more detailed data sets on aquatic sediments. These data sets often combine high-resolution chemical distributions with rate determinations, and information on resident biological communities and their activities. This wealth of data, in tum, creates a need for new diagnostic models that account for the complex interactions documented by field and experimental studies. Models of early diagenesis must therefore integrate knowledge from a wide variety of scientific fields, from transport theory and chemistry, to molecular biology and benthic ecology. Only by incorporating meaningful representations of the dominant processes, are these models able to scale reactive transport interactions from the local to the regional and, ultimately, global scale. This thesis focuses on the quantitative description of (1) biologically-induced transport processes, and (2) the coupling of reaction and transport processes. It presents three innovative approaches to quantify pore water transport other than molecular diffusion. Two of the approaches compute site-specific depth distributions of solute mixing intensities, but they differ fundamentally in the type of input data. One approach is based on chemical concentration and rate measurements, the other uses ecological data on the infaunal community. Despite their differences, both approaches yield comparable bioirrigation intensities. In the third approach, measured benthic oxygen uptake fluxes across a wide variety of oceanic environments are used to derive global relationships for enhanced solute transport rates in sediments. This last approach bridges the gap between site-specific studies of pore water irrigation and regional to global assessments of the role of benthic-pelagic coupling in ocean biogeochemistry. The estimates of enhanced solute transport intensities clearly demonstrate that bioirrigation has a major global impact on solute exchanges between the water column and sediments. Next, the fate of particulate matter in bioturbated sediments is modeled using a stochastic Lagrangian approach. Individual particle histories are explicitly computed from probability density functions that embody the nature of particle transport by bioturbation. The analysis of the results provides insight into the emergence and variability of particle properties relevant for the interpretation of the sedimentary record. In particular, the effect of bioturbation on the oxygen exposure time (OET) of unreactive and reactive particles is investigated. Finally, two advanced modeling environments for early diagenesis are presented. In the first one, a flexible reaction network simulator is coupled to one-dimensional (lD) transport descriptions. As the reaction network is easily modified and adapted by the user, it is ideally suited to explore biogeochemical reaction systems of increasing complexity. The ID forward reaction-transport model is further combined with local and global optimization algorithms to enhance model parameterization based on observational data. The second model environment is a preliminary version of a multidimensional reactive transport code for early diagenetic applications. 11 SAMENVATTING De laatste decennia zijn er spectaculaire ontwikkelingen geweest in experirnentele en analytische technieken op het gebied van de biogeochemie. Deze stellen geochemici en biologen in staat steeds meer gedetailleerde gegevens te verkrijgen over aquatische sedimenten. De gegevens zijn meestal een combinatie van chemische metingen in hoge resolutie, inclusief de bepaling van reactiesnelheden, en informatie over de aanwezige biologische gemeenschappen en hun activiteit. Deze rijkdom aan gegevens heeft geleid tot de vraag naar nieuwe diagnostische modellen die rekening houden met de complexe interacties die in veld- en laboratoriummetingen worden vastgesteld. Vroeg diagenetische modellen zijn noodzakelijk om de kennis te integreren van een breed scala aan wetenschapsgebieden, van transporttheorie en chemie, tot moleculaire biologie en benthische ecologie. AIleen door een zinvolle implementatie van de dominante processen, kan met deze modellen de wisselwerking van reactieve transportprocessen van lokaal tot regionaal en uiteindelijk mondiaal niveau worden opgeschaald. Dit proefschrift richt zich op de kwantitatieve beschrijving van (l) biologisch-geYnduceerde transportprocessen en (2) de koppeling van reactie en transportprocessen. Het presenteert 3 innovatieve methoden om poriewatertransport, anders dan door moleculaire diffusie, te kwantificeren. Twee van de methoden berekenen locatie-specifieke diepteverdelingen van de intensiteit van vloeistofmenging, maar verschillen fundamenteel in de wijze van invoer van gegevens. De eerste aanpak is gebaseerd
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