Baker, Don R

A compendium of diffusion measurements and their Arrhenius equations for water, carbon dioxide, sulfur, fluorine, and chlorine in silicate melts similar in composition to natural igneous rocks is presented. Water diffusion in silicic melts is well studied and understood, however little data exists for melts of intermediate to basic compositions. The data demonstrate that both the water concentration and the anhydrous melt composition affect the diffusion coefficient of water. Carbon dioxide diffusion appears only weakly dependent, at most, on the volatilefree melt composition and no effect of carbon dioxide concentration has been observed, although few experiments have been performed. Based upon one study, the addition of water to rhyolitic melts increases carbon dioxide diffusion by orders of magnitude to values similar to that of 6 wt% water. Sulfur diffusion in intermediate to silicic melts depends upon the anhydrous melt composition and the water concentration. In water-bearing silicic melts sulfur diffuses 2 to 3 orders of magnitude slower than water. Chlorine diffusion is affected by both water concentration and anhydrous melt composition; its values are typically between those of water and sulfur. Information on fluorine diffusion is rare, but the volatile-free melt composition exerts a strong control on its diffusion. At the present time the diffusion of water, carbon dioxide, sulfur and chlorine can be estimated in silicic melts at magmatic temperatures. The diffusion of water and carbon dioxide in basic to intermediate melts is only known at a limited set of temperatures and compositions. The diffusion data for rhyolitic melts at 800°C together with a standard model for the enrichment of incompatible elements in front of growing crystals demonstrate that rapid crystal growth, greater than 10-10 ms-1, can significantly increase the volatile concentrations at the crystal-melt interface and that any of that melt trapped by the formation of melt inclusions may not be representative of the bulk melt. However, basaltic melt inclusions trapped at 1300°C are more likely to contain bulk melt concentrations of water and carbon dioxide.

Volcanic degassing is directly linked to magma dynamics and controls the style of eruptive activity. To better understand how gas is transported within basaltic magma we perform a 3D investigation of vesicles preserved in scoria from the 2005 activity at Stromboli volcano (Italy). We find that clasts are characterized by the ubiquitous occurrence of one to a few large vesicles, exhibiting mostly irregular, tortuous, channel-like textures, orders of magnitude greater in volume than all the other vesicles in the sample. We compare observations on natural samples with results from numerical simulations and experimental investigations of vesicle size distributions and demonstrate that this type of vesicle invariably forms in magmas with vesicularities > 0.30 (and possibly > 0.10). We suggest that large vesicles represent pathways used by gas to flow non-explosively to the surface and that they indicate the development of an efficient system that sustains persistent degassing in basaltic systems.

Explosive activity at Stromboli is explained in terms of dynamics of large gas bubbles that ascend in the magma conduit and burst at the free surface generating acoustic pressure that propagates as infrasonic signals in the atmosphere. The rate and the amplitude of the infrasonic activity is directly linked to the rate and the overpressure of the bursting gas bubbles and thus reflects the rate at which magma column degasses under non-equilibrium pressure conditions. We investigate the link between explosive degassing and magma vesiculation by comparing the rate of infrasonic activity with the bubble size distributions (BSDs) of scoria clasts collected during several days of explosive activity at Stromboli. BSDs of scoria show a characteristic power law distribution, which reflect a gas bubble concentration mainly controlled by a combined process of bubble nucleation and coalescence. The cumulative distribution of the infrasonic pressure follows two power laws, indicating a clear separation between the frequent, but weak, bursting of small gas bubbles (puffing) and the more energetic explosions of large gas slugs. The exponents of power laws derived for puffing and explosive infrasonic activity show strongly correlated (0.96) changes with time indicating that when the puffing rate is high, the number of energetic explosions is also elevated. This correlation suggests that both puffing and explosive activity are driven by the same magma degassing dynamics. In addition, changes of both infrasonic power law exponents are very well correlated (0.92 with puffing and 0.87 with explosions) with variations of the BSD exponents of the scoria clasts, providing evidence of the strong interplay between scoria vesiculation and magma explosivity. Our analysis indicates that variable magma vesiculation regimes recorded in the scoria correlate with the event number and energy of the explosive activity. We propose that monitoring infrasound on active volcanoes may be an alternative way to look at the vesiculation process in open conduit systems.

We performed a series of X-ray tomographic experiments and lattice Boltzmann permeability simulations on pyroclastic products from explosive activity at Stromboli between December 2004 and May 2006. We reconstructed the 3-D textures of vesicles to investigate the relationship between the nature of vesiculation in the erupted products and the dynamics of gas transport in the shallow conduit in order to derive implications for the eruptive behavior of basaltic volcanoes. Scoriae from normal Strombolian explosions display remarkably consistent vesicle volume distributions fit by power laws with an exponent of 1 (±0.2). We ascribe the origin of such distributions to the combined effect of coalescence and continuous nucleation events in the steady state, shallow magma system that supplies normal Strombolian activity. Volume distributions and textures of vesicles in pumice clasts from the 5 April 2003 and 15 March 2007 paroxysmal activity are markedly different from those in the scoriae. Besides a power law function with a higher exponent, portions of these distributions can be also fit by an exponential function, suggesting the attempt of the system to reach near-equilibrium conditions. The investigated pumice clasts also lack the large, connecting vesicles responsible for the development of degassing pathways in the Stromboli magma that erupts the scoriae. This testifies to a decreased degassing efficiency of the magma associated with paroxysmal explosions and potential overpressure buildup at depth. By comparison with degassing experiments on basaltic melts, we derive a time constraint on the order of minutes to hours for the incubation of paroxysms at Stromboli.

Ambrym is one of the most actively erupting basaltic volcanoes in the Vanuatu island arc. Scoria clasts collected from a fallout deposit in the inner terrace of its Benbow active crater were analyzed through series of synchrotron X-ray computed microtomographic experiments, as well as permeability measurements and simulations. Our goal was to reconstruct and visualize scoria textures in 3D and to quantify vesicularity, permeability, vesicle sizes and distributions in order to understand how gas moves in and out of Ambrym basaltic magma. We find that vesicle size distributions in the volume range between ~ 103 and 1010 μm3 define two scoria classes. Vesicle size distributions in the low-to-moderately (0.44–0.67) vesicular samples can be fit by power laws with an exponent of 1 ± 0.2; distributions in the highly vesicular (0.86–0.88) samples can be fit by power laws with a higher exponent (1.4 to 1.7), as well as by exponential fits. Highly vesicular samples exhibit a very pronounced large vesicle, consisting of networks of smaller, interconnected vesicles, that is more than three orders of magnitude larger in volume than all other vesicles in each distribution. This type of vesicle is not found in the low-to-moderately vesicular samples. In addition, vesicle number density negatively correlates with vesicularity: less vesicular samples have the highest number density and vice versa, and contain far more numerous small-to-medium-sized vesicles than highly vesicular samples. Measured and calculated viscous (Darcian) permeabilities overlap in the range 10− 13 and 10− 9 m2, with higher values in the more vesicular samples. We ascribe these differences in the textural and physical properties of the scoria clasts to their derivation from distinct magma portions in the conduit that were driven by convective overturn and underwent different vesiculation histories and gas transport dynamics. Comparing basaltic scoria clasts from Ambrym to those from mild explosive activity at Stromboli volcano (Italy) reveals that differences in their vesicle size distributions may result from the influence of different crystal contents and shapes on the vesiculation and permeability of the respective magmas. Finally, we highlight how rheological properties have a fundamental role in determining the degassing behaviour of basaltic magma at Ambrym and other volcanoes in general.

Synchrotron X-ray computed microtomography (mCT) was applied for the first time to clasts of pumice and scoria generated by active, explosive volcanoes characterized by a range of eruptive styles (mild Strombolian to Plinian) and magmatic composition (basaltic to trachytic). The obtained two-dimensional (2D) tomographic images, corresponding to sample views at different rotation angles, were processed to reconstruct three-dimensional (3D) volumes and then used to make 3D measurements of vesicularity, vesicle number density, volume and connectivity for quantitative characterization of the investigated tephras. The results indicate a positive correlation between vesicle number density and eruption intensity that is used to investigate modes of magma degassing in explosive eruptions. In addition, the vesicle geometry affecting the connected gas flow pathways in pyroclasts from Strombolian eruptions is determined and related to the known permeabilities. Implications on the dynamics of explosive eruptions is discussed and, ultimately, used to quantitatively discriminate between different eruptive styles.

A series of computed microtomography experiments are reported which were performed by using a third-generation synchrotron radiation source on volcanic rocks from various active hazardous volcanoes in Italy and other volcanic areas in the world. The applied technique allowed the internal structure of the investigated material to be accurately imaged at the micrometre scale and three-dimensional views of the investigated samples to be produced as well as three-dimensional quantitative measurements of textural features. The geometry of the vesicle (gas-filled void) network in volcanic products of both basaltic and trachytic compositions were particularly focused on, as vesicle textures are directly linked to the dynamics of volcano degassing. This investigation provided novel insights into modes of gas exsolution, transport and loss in magmas that were not recognized in previous studies using solely conventional two-dimensional imaging techniques. The results of this study are important to understanding the behaviour of volcanoes and can be combined with other geosciences disciplines to forecast their future activity.

Fluorine and chlorine diffusion were measured in two natural phonolitic melts, from Vesuvius (Italy) and from Laacher See (Germany), at 0.5 and 1.0 GPa, between 1250 and 1450 °C at anhydrous conditions and with about 2 and 5 wt.% of dissolvedwater. The two different startingmaterials allowus to investigate the alkali effect,Na vs. K, on halogen diffusion.One compositionwas a K-rich (~10wt.%) phonoliticmelt corresponding to thewhite pumice phase of the 79ADeruption of Vesuvius, and the other aNa-rich (~10 wt.%) phonoliticmelt corresponding tomost differentiated melt of the 12,000 BC eruption of Laacher See. The diffusion-couple technique in a piston cylinder was used for the experiments. Experiments were performed with only one halogen diffusing and with the simultaneous diffusion of a halogenmixture (F, Cl, Br) in order to evaluate the interactions between the halogens during diffusion. Diffusion coefficients for F range between 2×10−11m2/s at 1250 °C and 7×10−11m2/s at 1450 °C for the Na-rich melt and between 1×10−11 m2/s at 1250 °C and 8×10−11 m2/s at 1450 °C for the K-rich melt at anhydrous conditions. Diffusion coefficients for Cl range between 2×10−12 m2/s at 1250 °C and 1×10−11 m2/s at 1450 °C for theNa-richmelt and between 7×10−12m2/s at 1250 °C and 2×10−11m2/s at 1450 °C for the K-richmelt at anhydrous conditions. Fluorine diffusivity is higher than Cl in the Na-rich-phonolitic melt by one order of magnitude,whereas in the K-rich-phonoliticmelt F and Cl diffusivities are similar. The effect ofwater is significant for Cl in both Na-rich and K-rich melts: the addition of water enhances Cl diffusivity by up to one order of magnitude, butwater does not significantly affect F diffusion. F and Cl diffusivities always differ fromone another in the same phonoliticmelt composition. F diffusivities are similar in both compositions. Conversely, Cl diffusion depends upon the dominant alkali. These results evidence that halogen diffusivitymay represent a limiting factor for their degassing during rapid syneruptive decompression and vesiculation of H2O-rich-phonolitic melts. The contrasting volatile diffusivities of F and Cl in silicate melts duringmagma vesiculation may be a key, controlling factor of the composition of the vapour phase (bubbles) produced. Such diffusion controlled degassingmodelmay explain the absence of F and Cl degassing observed during the 79AD eruption of Vesuvius.

Vesicle size distributions in two and three dimensions of two samples were independently measured by three different researchers to investigate whether or not such measurements are reproducible. Additionally, two different software programs were used to measure the three-dimensional vesicle size distributions: the 3D Object Counter plugin for ImageJ and Blob3D. Manual thresholding by each of the authors produced similar results for both samples using both programs; however, use of the automatic, maximum entropy technique for thresholding produced measurably different results because it did not discriminate between vesicles and plagioclase crystals in one case and between vesicles and some cracks in another. Use of asymmetric erosion and dilation processes on the images is shown to affect the vesicle size distribution, but it does not have a significant effect on the power-law exponent that describes intermediate-sized vesicles or on the vesicle number density in these samples. However, such a technique is not recommended.

A series of experiments created melt inclusions in plagioclase and pyroxene crystals grown from a basaltic melt at 1,150 C, 1.0 GPa to investigate diffusive fractionation during melt inclusion formation; additionally, P diffusion in a basaltic melt was measured at 1.0 GPa. Melt inclusions and melts within a few 100 microns of plagioclase– melt interfaces were analyzed for comparison with melt compositions far from the crystals. Melt inclusions and melt compositions in the boundary layer close to the crystal–melt interface were similar, but both differ significantly in incompatible element concentrations from melt found greater than approximately 200 microns away from the crystals. The compositional profiles of S, Cl, P, Fe, and Al in the boundary layers were successfully reproduced by a two-step model of rapid crystal growth followed by diffusive relaxation toward equilibrium after termination of crystal growth. Applying this model to investigate possible incompatible element enrichment in natural melt inclusions demonstrated that at growth rates high enough to create the conditions for melt inclusion formation, *10-9–10-8 m s-1, the concentration of water in the boundary layer near the crystal was similar to that of the bulk melt because of its high diffusion coefficient, but sulfur, with a diffusivity similar to major elements and CO2, was somewhat enriched in the boundary layer melt, and phosphorus, with its low diffusion coefficient similar to other high-field strength elements and rare earth elements, was significantly enriched. Thus, the concentrations of sulfur and phosphorus in melt inclusions may over-estimate their values in the bulk melt, and other elements with similar diffusion coefficients may also be enriched in melt inclusions relative to the bulk melt.