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Diamond precipitation dynamics from hydrocarbons at icy planet interior conditions

Nature Astronomy volume 8, pages 174–181 (2024)Cite this article

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A Publisher Correction to this article was published on 22 January 2024

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Abstract

The pressure and temperature conditions at which precipitation of diamond occurs from hydrocarbon mixtures is important for modelling the interior dynamics of icy planets. However, there is substantial disagreement from laboratory experiments, with those using dynamic compression techniques finding much more extreme conditions are required than in static compression. Here we report the time-resolved observation of diamond formation from statically compressed polystyrene, (C8H8)n, heated using the 4.5 MHz X-ray pulse trains at the European X-ray Free Electron Laser facility. Diamond formation is observed above 2,500 K from 19 GPa to 27 GPa, conditions representative of Uranus’s and Neptune’s shallow interiors, on 30 μs to 40 μs timescales. This is much slower than may be observed during the ∼10 ns duration of typical dynamic compression experiments, revealing reaction kinetics to be the reason for the discrepancy. Reduced pressure and temperature conditions for diamond formation has implications for icy planetary interiors, where diamond subduction leads to heating and could drive convection in the conductive ice layer that has a role in their magnetic fields.

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Fig. 1: State diagram of hydrocarbons at high pressure and temperature.
Fig. 2: Experimental set-up.
Fig. 3: Time-resolved data from a run starting at 20 GPa with average pulse energy of 71 μJ.
Fig. 4: Integrated X-ray diffraction patterns in the region of interest from a run starting at 19 GPa.
Fig. 5: Raman spectra of the sample after removal from the DAC.

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The datasets used during the current study are available from the corresponding author on reasonable request.

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Acknowledgements

We thank N. Hartley for fruitful discussions. This work was supported by US Department of Energy (DOE) Office of Fusion Energy Sciences funding no. FWP100182. A.F.G. and E.E. are grateful for the support of Carnegie Science and NSF EAR-2049127. We acknowledge European XFEL in Schenefeld, Germany, for provision of X-ray free-electron laser beamtime at Scientific Instrument HED and thank the staff for their assistance. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III beamline P02.2. Beamtime was allocated from in-house beamtime from the beamline. Lawrence Livermore National Laboratory is operated by Lawrence Livermore National Security, LLC, for the US DOE, National Nuclear Security Administration under Contract DE-AC52-07NA27344. S.N. and L.M.A. acknowledge financial support from Sorbonne University under grant Emergence HP-XFEL. Y.L. is grateful for support from the Leader Researcher programme (NRF-2018R1A3B1052042) of the Korean Ministry of Science and ICT (MSIT). We are indebted to the HIBEF user consortium for the provision of instrumentation and staff that enabled this experiment. G.M. has been supported by a grant from Labex OSUG@2020 (Investissements d’avenir - ANR10 LABX56) and PNP-INSU programme. M.B. acknowledges the support of Deutsche Forschungsgemeinschaft (DFG Emmy-Noether project BY112/2-1).

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Author notes

  1. Stephan Stern

    Present address: X-Spectrum GmbH, Hamburg, Germany

Authors and Affiliations

  1. High Energy Density Science Division, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Mungo Frost & Siegfried H. Glenzer

  2. SUPA, School of Physics and Astronomy, and Centre for Science at Extreme Conditions (CSEC), University of Edinburgh, Edinburgh, UK

    R. Stewart McWilliams, Bernhard Massani, Orianna B. Ball, Matthew J. Duff, James D. McHardy & Malcolm I. McMahon

  3. University Bayreuth, Bayreuth, Germany

    Elena Bykova & Saiana Khandarkhaeva

  4. Mathematisch-Naturwissenschaftliche Fakultät - Institut für Anorganische Chemie, Universität zu Köln, Cologne, Germany

    Maxim Bykov

  5. Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany

    Rachel J. Husband, Heinz Graafsma, Torsten Laurus, Hanns-Peter Liermann, Stephan Stern & Cornelius Strohm

  6. Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie (IMPMC), Sorbonne Université, CNRS UMR 7590, MNHN, Paris, France

    Leon M. Andriambariarijaona, Guillaume Fiquet & Sandra Ninet

  7. European XFEL, Schenefeld, Germany

    Karen Appel, Valerio Cerantola, Anand Dwivedi, Zuzana Konôpková, Motoaki Nakatsutsumi, Jolanta Sztuk-Dambietz & Monica Turcato

  8. Radiation Physics/High Energy Density, Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden, Germany

    Carsten Baehtz

  9. Consortium for Advanced Radiation Sources, The University of Chicago, Chicago, IL, USA

    Stella Chariton & Vitali B. Prakapenka

  10. Department of Earth System Sciences, Yonsei University, Seoul, South Korea

    Jinhyuk Choi & Yongjae Lee

  11. Physical and Life Sciences, Lawrence Livermore National Laboratory, Livermore, CA, USA

    Hyunchae Cynn

  12. Earth and Planets Laboratory, Carnegie Institution for Science, Washington DC, USA

    Eric Edmund & Alexander F. Goncharov

  13. School of Earth Sciences and Environmental Engineering, GIST, Gwangju, South Korea

    Huijeong Hwang

  14. Université Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, IRD, Université Gustave Eiffel, ISTerre, Grenoble, France

    Nicolas Jaisle & Guillaume Morard

  15. Department of Physics, Hanyang University, Seoul, South Korea

    Jaeyong Kim, Lan Anh Nguyen & Zhongyan Wu

  16. Institute of Earth and Environmental Sciences, Albert-Ludwigs University of Freiburg, Freiburg, Germany

    Clemens Prescher & Stephan Stern

  17. Institut für Physik, Universität Rostock, Rostock, Germany

    Ronald Redmer

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  1. Mungo Frost
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Contributions

All authors were involved in experimental planning. M.F., E.B., M.B., R.J.H., C.S., H.-P.L., Z.K. and A.F.G. coordinated the experiment. M.F. prepared the samples. H.-P.L., J.D.M., L.M.A., S.K. and B.M. performed the prescreening at P02.2 at PETRA III. M.F., C.S., C.B., H.-P.L., Z.K., S.N., J.D.H., C.P., E.E., R.S.M., S.C., O.B.B., M.J.D. and A.F.G. conducted the experiment. T.L., S.S., C.S. and J.S.-D. operated the AGIPD detector. R.R., S.H.G. and A.F.G. advised. M.F., R.S.M., O.B.B., R.J.H., Z.K., C.P., E.E. and A.F.G. analysed the data. M.F. and R.S.M. wrote the paper.

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Correspondence to Mungo Frost.

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Extended data

Extended Data Fig. 1 FEA Model of Sample Temperature.

FEA model (cylindrical section) of sample temperature at the time of XFEL probing at 30 μs in Fig. 3d. Bold white lines indicate boundaries between DAC components; light white lines indicate additional boundaries required by the analysis; XFEL radiation is from below26. Black lines indicate solid-liquid boundaries, with the melting point of Au taken to be 2350 K31,32 and the melting point of polystyrene taken to be 1000 K (representing a likely minimum bound, considering an ambient melting point of 510 K and steep rise with pressure). The model shows high temperatures are localized near the coupler hole, with cold material surrounding the hotspot, including several microns of cold and solid polystyrene separating the sample from the diamond anvils and significantly more separating the hot sample from the gasket.

Extended Data Fig. 2 Time resolved data from a run with 1% beam power.

No thermal emission or diamond is observed. a: XRD in region of interest, vertical stripes are artifacts from diode normalization. b: SOP spectrogram showing no emission. c: Time evolution of intensity at q where diamond is expected shows no diamond formation, the line is smoothed with 15 pulse wide Hamming window. Time 0 is estimated first arrival of X-rays based on other runs.

Extended Data Fig. 3 Time resolved data from a run with 5% beam power.

Thermal emission and diamond formation are observed. a: XRD in region of interest normalized to beam intensity monitoring diode. The diamond 111 reflection is visible after 40 μs. b: SOP spectrogram. c: Temperature from SOP fitting and equation of state of gold30. d: Time evolution of diamond peak intensity, line is smoothed with 15 pulse wide Hamming window. Time 0 corresponds to first X-ray pulse based on rising edge of thermal emission. Temporal error bars represent the time bin of the SOP, temperature error bars represent one-half standard deviation confidence and are derived from the fitting uncertainty of a Planck function to the spectrographic data and statistical analysis of these data27.

Extended Data Fig. 4 Time resolved data from a run with 25% beam power.

This is a different run than is presented in Fig. 3, but shows similar temperatures and diamond formation. a: XRD in region of interest normalized to beam intensity monitoring diode. The diamond {111} reflection is visible after 35 μs. b: Emissivity as a function of time. c: SOP spectrogram. d: Temperature from SOP fitting and equation of state of gold30. e: Time evolution of diamond peak intensity, line is smoothed with 15 pulse wide Hamming window. Time 0 corresponds to first X-ray pulse based on rising edge of thermal emission. Temporal error bars represent the time bin of the SOP, temperature error bars represent one-half standard deviation confidence and are derived from the fitting uncertainty of a Planck function to the spectrographic data and statistical analysis of these data27.

Extended Data Fig. 5 Unintegrated Diffraction Image.

Raw diffraction pattern from a single XFEL pulse taken 40.2 μs into a run starting at 19 GPa. The SOP temperature is 2540(30) K. The integrated pattern is shown in Fig. 4b. λ = 0.6965 Å. Lighter shades correspond to higher signal, brightness and contrast are optimized for visibility. The pattern is azimuthally unwrapped such that vertical lines are at constant q (also known as ‘caked’). The shadow at low q is from the mirror used to observe the sample, the dark panel (top right) was faulty and masked when integrating the diffraction patterns.

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Supplementary Figs. 1–11, Tables 1 and 2, and minimal supporting text to contextualize these.

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Frost, M., McWilliams, R.S., Bykova, E. et al. Diamond precipitation dynamics from hydrocarbons at icy planet interior conditions. Nat Astron 8, 174–181 (2024). https://doi.org/10.1038/s41550-023-02147-x

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