Temperature dependence of oxygen-and clumped isotope fractionation in carbonates: a study of travertines and tufas in the 6-95°C temperature range, Geochimica et Cosmochimica Acta (2015), doi: http://dx.doi.org/10.1016/j.gca. 2015.06.032 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. calibrations. For this reason there is a need to better understand the controls on isotope 25 fractionation especially on natural carbonates. In this study we analyzed oxygen, carbon and 26 clumped isotopes of a unique set of modern calcitic and aragonitic travertines, tufa and cave 27 deposits from natural springs and wells. Together these samples cover a temperature range 28 from 6 to 95°C. Travertine samples were collected close to the vents of the springs and from 29 pools, and tufa samples were collected from karstic creeks and a cave. The majority of our 30 vent and pool travertines and tufa samples show a carbonate-water oxygen isotope 31 fractionation comparable to the one of Tremaine et al. (2011)
Traditionally, fresh water carbonate research has focused on the sedimentology and palaeontology of ancient lacustrine deposits. Lithofacies in such low-energy deposits are typically fine-grained, developed uniformly in a generally concentric distribution ('bulls-eye' pattern) and are predictable even when preserved imperfectly. In contrast, because of their local lithofacies and palaeontological complexities, fluvial carbonates were either delegated to a status of 'minor geomorphological features' or barely considered prior to the 1970s. This viewpoint was based on the depositional record of fluvial and spring-fed fresh water carbonates, which were considered to be restricted generally to localized karstic areas. Such deposits are often preserved as scattered patches of ambient temperature tufa. Occasionally, however, in active tectonic areas, localized travertine deposits are also developed from deeply circulating hydrothermal waters. With a few exceptions (for example, basins with high subsidence rates or in arid climate zones), these fresh water carbonates are prone to erosion from continuing river incision and thus may not be preserved in the geological record. A partial record of fluvial and springdeposited carbonates is often preserved in Quaternary deposits, but the record in older deposits is typically fragmentary and often diagenetically modified. Yet once their unique facies architecture (and specialized nomenclature) is understood, these carbonates provide an important record of past sedimentological cycles of great value in palaeoenvironmental landscape modelling. The emphasis of modern research is to acquire information that explains how active systems function. In this respect, tufas reveal much of how carbonate precipitation is a shared product of physico-chemical and microbiological biomediation processes. Likewise, travertines not only show an intimate interrelation with active tectonism but also hold great potential as monitors of past volcanic carbon dioxide emissions. In addition, both tufas and travertines contain palynological records that can be used as proxy indicators of climate change. Perhaps no other field of sedimentology has witnessed more developments and applications over such a brief period of study.
In this paper we describe an example of travertine fissure-ridge development along the trace of a normal fault with metre displacement, located in the eastern margin of the Neogene-Quaternary Siena Basin, in the Terme S. Giovanni area (Rapolano Terme, Italy). This morphotectonic feature, 250 m long, 30 m wide and 10 m high, formed from supersaturated hot waters (39.9°C) flowing from thermal springs aligned along the trace of the normal fault dissecting travertines not older than Late Pleistocene (24 ± 3 ka). A straight, continuous fissure with a maximum width of 20 cm occurs at the top of the ridge, along its crest. Hot fluids flow from cones mainly located at the extremities of the ridge, where travertine is depositing. The travertine fissure-ridge shows an asymmetrical profile since it buries the fault scarp. The difference in height of slopes corresponds to the vertical displacement of the normal fault. Fissuring of the recent travertine deposits along the strike of the crestal fissure, as well as recent hydrothermal circulation, lead us to believe that the Terme S. Giovanni normal fault may be currently active. On the whole, the Terme S. Giovanni fissure ridge can be defined as a travertine fault trace fissure-ridge, adding a helpful example for studying the relationship between faulting and travertine deposition.
The terrestrial limestones forming at the emergence of thermal springs show a variety of unusual depositional facies. The specific lithological and petrological features of these deposits have few counterparts in the marine, and continental, karst-related carbonates, but they are typical of the epigean limestone that has been quarried since antiquity in the surroundings of Tivoli (Rome) under the name of travertine, where it is still forming in hydrogeothermal fields linked to extensional tectonics. The physicochemical, hydrodynamic and geological conditions specific to the Tivoli thermal spring system imply hypersaturated alkaline-sulphate, warm to hot waters, upwelling from springs fed through open fractures/faults in extensional and/or volcanic regimes. These features, together with the hydrodynamic behaviour of the water flows running from the vents, control the petrogenetic features of the travertine, a well-bedded, mostly finely laminated, porous but quite compact limestone. The results of a detailed comparative petrological analysis carried out on the lithofacies of travertine limestones, and of those observed during formation within numerous active thermal spring fields, provide the elements required for an exhaustive textural classification of the travertine lithofacies, which has not yet been described systematically. According to the genetic processes and fabrics, the thermal deposits that originate from such hypersaturated alkaline-sulphate, warm to hot waters, can be subdivided into: abiotic crystalline crusts, microbially mediated crusts (microbialites) and granular deposits mostly represented by small accumulations of limemudstone. Some of the granular deposits and the microbialites are only partially comparable with analogous sediments forming on tidal flats/sabkhas or other continental sites; however, the facies association of crystalline crusts and laminar curled microbialites has no counterpart in the marine realm. The widespread presence of thermophile bacteria and sulphobacteria, and the general absence of autochthonous eukaryote organisms, unable to live in poisonous sulphate waters, are also undeniable evidence of their thermal origin.
Middle-Late Pleistocene tectonic activity has been inferred through studies on travertine deposits exposed in a tract of the hinterland Northern Apennines. A detailed study on the relationships between tectonics and travertine deposition coupled with 230 Th/ 234 U age determination of travertines at Cava Oliviera quarry, located close to Serre di Rapolano village (southern Tuscany, Northern Apennines), allowed us to recognise Pleistocene faults, whose activity has been referred to 157-24 ka, at least. Travertine deposition was tectonically controlled by WSW-ENE striking, oblique and normal faults, associated to a main fault (named as the Violante Fault). This structure dissected a regional normal fault (known as the Rapolano Fault) Early-Middle Pliocene in age, which bounded the eastern side of the Pliocene Siena Basin, and gave rise to space accommodation for clayey and sandy marine sediments. Hydrothermal circulation (and related travertine deposition) was favoured by the damaging enhancement due to the fault-fault intersection. Tectonic activity has been also documented by deformation recorded by travertines, which suggest a main tectonic event between 64 ± 5 and 40 ± 5 ka. The tectonic activity described for the study area agrees with the Quaternary tectonic evolution documented in the surrounding areas (e.g. Mt. Amiata and Mt. Vulsini), as well as the Tyrrhenian margin of the Central Apennines, indicating that a widespread tectonic activity affected the inner part of the Apennines until the latest Quaternary.
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