Abstract
The most viscous volcanic melts and the largest explosive eruptions1 on our planet consist of calcalkaline rhyolites2,3. These eruptions have the potential to influence global climate4. The eruptive products are commonly very crystal-poor and highly degassed, yet the magma is mostly stored as crystal mushes containing small amounts of interstitial melt with elevated water content5. It is unclear how magma mushes are mobilized to create large batches of eruptible crystal-free magma. Further, rhyolitic eruptions6,7,8 can switch repeatedly between effusive and explosive eruption styles and this transition is difficult to attribute to the rheological effects of water content or crystallinity9,10. Here we measure the viscosity of a series of melts spanning the compositional range of the Yellowstone volcanic system and find that in a narrow compositional zone, melt viscosity increases by up to two orders of magnitude. These viscosity variations are not predicted by current viscosity models11,12 and result from melt structure reorganization, as confirmed by Raman spectroscopy. We identify a critical compositional tipping point, independently documented in the global geochemical record of rhyolites, at which rhyolitic melts fluidize or stiffen and that clearly separates effusive from explosive deposits worldwide. This correlation between melt structure, viscosity and eruptive behaviour holds despite the variable water content and other parameters, such as temperature, that are inherent in natural eruptions. Thermodynamic modelling demonstrates how the observed subtle compositional changes that result in fluidization or stiffening of the melt can be induced by crystal growth from the melt or variation in oxygen fugacity. However, the rheological effects of water and crystal content alone cannot explain the correlation between composition and eruptive style. We conclude that the composition of calcalkaline rhyolites is decisive in determining the mobilization and eruption dynamics of Earth’s largest volcanic systems, resulting in a better understanding of how the melt structure controls volcanic processes.
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Acknowledgements
This study was supported by a European Research Council Advanced Grant to D.B.D. on ‘Explosive volcanism in the Earth system: experimental insights’ (EVOKES, grant number 247076). E.D. was supported by DFG grant ED 1757/1-1. We thank M. Kaliwoda and R. Hochleitner for Raman measurements at the Mineralogical State Collection Munich (SNSB). In addition, we thank H. W. Lohringer, D. Mueller, and A. Wimmer for assistance during the sample preparation, microprobe analyses and iron titration. Scientific discussions with M. Diez, D. Morgavi and C. M. P. De Campos were greatly appreciated. D.D.G. thanks C. Chelle-Michou and J. Lourenço for their assistance with R programming and H. Mader for comments and suggestions.
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D.D.G. conceptualized the original idea, performed the low-temperature viscosity, calorimetric, Raman spectroscopic measurements, and Rhyolite-MELTS simulations. D.D.G., S.K. and S.W. synthetized the samples and performed the high-temperature viscosity measurements, wrote the original draft paper, finalized the figures, and compiled the database of chemical compositions. E.D. performed the magnetic measurements, wrote the associated text and finalized the figures. D.R.N, K.U.H. and D.B.D. advised on the optimal experimental methods and contributed to producing a final manuscript.
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Reviewer Information Nature thanks M. Manga and Y. Zhang for their contribution to the peer review of this work.
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Extended data figures and tables
Extended Data Figure 1 High- and low-temperature viscosity measurements of samples investigated in this study.
See Extended Data Table 2 for experimental data and Extended Data Table 1 for sample chemistry.
Extended Data Figure 2 Comparison between measured and calculated viscosities of all samples at 850 °C.
The solid black line is a 1:1 reference line. Symbols are values predicted by the HZ11 (red) and GRD12 (black) models. The red and black dotted lines show linear fits to the model results. The two models generally agree, with the exception of samples J, C and F, which are described better by the HZ model than by the GRD model.
Extended Data Figure 3 Raman spectra of samples F, J and L.
These samples show increasing FeO content. Spectra were acquired before the low-temperature viscosity measurements. The peak at about 670 cm−1 (sample L) indicates the magnetite peak. The FeO content (in wt%) is given in parentheses in the key; see Extended Data Table 1.
Extended Data Figure 4 Magnetic-hysteresis analyses of samples F, J, and L.
These samples show increasing FeO content. (See Extended Data Table 1 for sample chemistry.) a, Hysteresis loops of six sub-samples of samples F and J. M is magnetization. b, Hysteresis loops of ten sub-samples of sample L. c, Hysteresis as in b corrected for a paramagnetic slope calculated using the linear portion of every loop for fields >1.25 T and normalized for the saturation magnetization Ms. The red vertical band indicates all values of B90, calculated for every loop as the field where M/Ms = 0.9. The B90 values are used in d to estimate the size of the magnetic particles as described in Methods.
Extended Data Figure 5 Differential thermal analysis data for samples F, J and L.
These samples show increasing FeO content at a heating or cooling rate of 10 °C min−1 under an argon atmosphere. (FeO content in wt% is given in parentheses in the key; see Extended Data Table 1.) The temperatures given are . Thin lines represent the first heating scans; thick lines represent the second heating scan. The nanolite-bearing sample (L) shows two endothermic peaks during the first heating scan, revealing two distinct amorphous domains (nanolite-free and nanolite-bearing). The lower glass transition temperature (peak at 692.4 °C) represents the nanolite-free amorphous domain. Except for the topmost curve, the curves were shifted along the y axis for clarity.
Extended Data Figure 6 Total alkali versus silica diagram of all effusive and explosive samples plotted in Fig. 4.
Note that the classic total alkali versus silica classification of these samples does not allow us to distinguish between explosive and effusive behaviour. Only through the newly developed RAI can these populations be clearly separated (Fig. 4).
Extended Data Figure 7 Calculated viscosities at the measured Tgpeak.
Data reported in Extended Data Table 1 after ref. 125 (see Methods for further details). The viscosity remains constant over the investigated range of silica content with the exception of sample L. This sample exhibits an extremely high viscosity owing to the iron depletion effect (see main text). The error in the viscosity measurements was estimated to be ±0.05 logarithmic units (see Methods).
Supplementary information
Supplementary Data
This file contains Supplementary Table 1. (XLSX 93 kb)
Supplementary Data
This file contains Supplementary Table 2. (XLSX 172 kb)
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Di Genova, D., Kolzenburg, S., Wiesmaier, S. et al. A compositional tipping point governing the mobilization and eruption style of rhyolitic magma. Nature 552, 235–238 (2017). https://doi.org/10.1038/nature24488
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DOI: https://doi.org/10.1038/nature24488
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