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We demonstrate a significantly simplified experimental approach for investigating liquid metallic hydrogen, which is crucial to understand the internal structure and evolution of giant planets. Plastic samples were shockcompressed and then probed by short pulses of X-rays generated by free electron lasers. By comparison with ab initio simulations, we provide indirect evidence for the creation of elemental hydrogen in shock-compressed plastics at ∼150GPa and ∼5,000K and thus in a regime where hydrogen is predicted to be metallic. Being the most common form of condensed matter in our solar system, and ostensibly the simplest of all elements, hydrogen is the model case for many theoretical studies and we provide a new possibility to benchmark models for conditions with extreme pressures and temperatures. Moreover, this approach will also allow to probe the chemical behavior of metallic hydrogen in mixture with other elements, which, besides its importance for planetary physics, may open up promising pathways for the synthesis of new materials.

The insulator-metal transition in liquid hydrogen is an important phenomenon to understand the interiors of gas giants, such as Jupiter and Saturn, as well as the physical and chemical behavior of materials at high pressures and temperatures. Here, the path toward an experimental approach is detailed based on spectrally resolved x-ray scattering, tailored to observe and characterize hydrogen metallization in dynamically compressed hydrocarbons in the regime of carbon-hydrogen phase separation. With the help of time-dependent density functional theory calculations and scattering spectra from undriven carbon samples collected at the European x-ray Free-Electron Laser Facility (EuXFEL), we demonstrate sufficient data quality for observing C-H demixing and investigating the presence of liquid metallic hydrogen in future experiments using the reprated drive laser systems at EuXFEL.

This work presents first insights into the dynamics of free-surface release clouds from dynamically compressed polystyrene and pyrolytic graphite at pressures up to 200 GPa, where they transform into diamond or lonsdaleite, respectively. These ejecta clouds are released into either vacuum or various types of catcher systems, and are monitored with high-speed recordings (frame rates up to 10 MHz). Molecular dynamics simulations are used to give insights to the rate of diamond preservation throughout the free expansion and the catcher impact process, highlighting the challenges of diamond retrieval. Raman spectroscopy data show graphitic signatures on a catcher plate confirming that the shock-compressed PS is transformed. First electron microscopy analyses of solid catcher plates yield an outstanding number of different spherical-like objects in the size range between ten(s) up to hundreds of nanometres, which are one type of two potential diamond candidates identified. The origin of some objects can unambiguously be assigned, while the history of others remains speculative.

We present measurements of the nucleation rate into a diamond lattice in dynamically compressed polystyrene obtained in a pump-probe experiment using a high energy laser system and in situ femtosecond X-ray diffraction. Different temperature-pressure conditions that occur in planetary interiors were probed. For a single shock reaching 70GPa and 3000K no diamond formation was observed while with a double shock driving polystyrene to pressures around 150GPa and temperatures around 5000K nucleation rates between 1029 m-3s-1 and 1034 m-3s-1 were recorded. These nucleation rates do not a agree with predictions of recent theoretical models for carbon-hydrogen mixtures by many orders of magnitude. Our data suggests that there is indeed significant diamond formation to be expected inside icy giant planets like Neptune and Uranus.

We discuss the possibility of obtaining highly precise measurements of the ionization potential depression in dense plasmas with spectrally resolved X-ray scattering, while simultaneously determining the electron temperature and the free electron density. A proof-of-principle experiment at the Linac Coherent Light Source, probing isochorically heated carbon samples, demonstrates the capabilities of this method and motivates future experiments at X-ray free electron laser facilities.

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N. J. Hartley, N. Ozaki, T. Matsuoka, B. Albertazzi, A. Faenov, Y. Fujimoto, H. Habara, M. Harmand, Y. Inubushi, T. Katayama, M. Koenig, A. Krygier, P. Mabey, Y. Matsumura, S. Matsuyama, E. E. McBride, K. Miyanishi, G. Morard, T. Okuchi, T. Pikuz, O. Sakata, Y. Sano, T. Sato, T. Sekine, Y. Seto, K. Takahashi, K. A. Tanaka, Y. Tange, T. Togashi, Y. Umeda, T. Vinci, M. Yabashi, T. Yabuuchi, K. Yamauchi, and R. Kodama , "Ultrafast observation of lattice dynamics in laser-irradiated gold foils", Appl. Phys. Lett. 110, 071905 (2017) https://doi.org/10.1063/1.4976541., We have observed the lattice expansion before the onset of compression in an optical-laser-driven target, using diffraction of femtosecond X-ray beams generated by the SPring-8 Angstrom Compact Free-electron Laser. The change in diffraction angle provides a direct measure of the lattice spacing, allowing the density to be calculated with a precision of ±1%. From the known equation of state relations, this allows an estimation of the temperature responsible for the expansion as <1000 K. The subsequent ablation-driven compression was observed with a clear rise in density at later times. This demonstrates the feasibility of studying the dynamics of preheating and shock formation with unprecedented detail.

We have observed lattice expansion before the onset of compression in an optical-laser-driven target, using diffraction of femtosecond X-ray beams generated by the SACLA X-ray Free Electron Laser. The change in diffraction angle provides a direct measure of the lattice spacing, allowing the density to be calculated with a precision of +-1%. From known equation of state relations this allows estimation of the temperature responsible for the expansion as <1000 K. The subsequent ablation-driven compression was observed with a clear rise in density at later times. This demonstrates the feasibility of studying the dynamics of preheating and shock formation with unprecedented detail.

The effects of hydrocarbon reactions and diamond precipitation on the internal structure and evolution of icy giant planets like Neptune and Uranus have been discussed for more than three decades. Inside these celestial bodies, gravity compresses mixtures of light elements to densities of several grams per cubic centimeter while the temperature reaches thousands of kelvins resulting in thermal energies on the order of chemical bond energies and above. Under these conditions, simple hydrocarbons like methane, which are highly abundant in the atmospheres, are believed to undergo structural transitions that release hydrogen from deeper layers and may lead to compact stratified cores. Indeed, the isentropes of Uranus and Neptune intersect a temperature-pressure regime where first polymerization occurs, whereas in deeper layers, a phase separation into diamond and hydrogen may be possible. Here we show experimental evidence for this phase separation process obtained by in situ X-ray diffraction from polystyrene (C8H8)n samples dynamically compressed to conditions around 150 GPa and 5000 K, which resembles the environment ~10,000 km below the surfaces of Neptune and Uranus [1]. Our findings demonstrate the necessity of high pressures for initiating carbon-hydrogen demixing and imply that diamond precipitation may require ~10x higher pressures than previously suggested by static compression experiments. In addition to their relevance for planetary modelling, by showing the formation of nanodiamonds from laser-irradiated plastic, our results identify a possible method to produce diamond nanoparticles for material science and industrial applications.

T. A. Pikuz, A. Ya. Faenov, N. Ozaki, N. J. Hartley, B. Albertazzi, T. Matsuoka, K. Takahashi, H. Habara, Y. Tange, S. Matsuyama, K. Yamauchi, R. Ochante, K. Sueda, O. Sakata, T. Sekine, T. Sato, Y. Umeda, Y. Inubushi, T. Yabuuchi, T. Togashi, T. Katayama, M. Yabashi, M. Harmand, G. Morard, M. Koenig, V. Zhakhovsky, N. Inogamov, A. S. Safronova, A. Stafford, I. Yu. Skobelev, S. A. Pikuz, T. Okuchi, Y. Seto, K. A. Tanaka, T. Ishikawa, and R. Kodama, "Indirect monitoring shot-to-shot shock waves strength reproducibility during pump–probe experiments", Journal of Applied Physics 120, 035901 (2016) https://doi.org/10.1063/1.4958796., We present an indirect method of estimating the strength of a shock wave, allowing on line monitoring of its reproducibility in each laser shot. This method is based on a shot-to-shot measurement of the X-ray emission from the ablated plasma by a high resolution, spatially resolved focusing spectrometer. An optical pump laser with energy of 1.0 J and pulse duration of ∼660 ps was used to irradiate solid targets or foils with various thicknesses containing Oxygen, Aluminum, Iron, and Tantalum. The high sensitivity and resolving power of the X-ray spectrometer allowed spectra to be obtained on each laser shot and to control fluctuations of the spectral intensity emitted by different plasmas with an accuracy of ∼2%, implying an accuracy in the derived electron plasma temperature of 5%-10% in pump-probe high energy density science experiments. At nano- and sub-nanosecond duration of laser pulse with relatively low laser intensities and ratio Z/A ∼ 0.5, the electron temperature follows Te ∼ Ilas2/3. Thus, measurements of the electron plasma temperature allow indirect estimation of the laser flux on the target and control its shot-to-shot fluctuation. Knowing the laser flux intensity and its fluctuation gives us the possibility of monitoring shot-to-shot reproducibility of shock wave strength generation with high accuracy.

We present an indirect method of estimating the strength of a shock wave, allowing on line monitoring of its reproducibility in each laser shot. This method is based on a shot-to-shot measurement of the X-ray emission from the ablated plasma by a high resolution, spatially resolved focusing spectrometer. An optical pump laser with energy of 1.0 J and pulse duration of ∼660 ps was used to irradiate solid targets or foils with various thicknesses containing Oxygen, Aluminum, Iron, and Tantalum. The high sensitivity and resolving power of the X-ray spectrometer allowed spectra to be obtained on each laser shot and to control fluctuations of the spectral intensity emitted by different plasmas with an accuracy of ∼2%, implying an accuracy in the derived electron plasma temperature of 5%-10% in pump-probe high energy density science experiments. At nano- and sub-nanosecond duration of laser pulse with relatively low laser intensities and ratio Z/A ∼ 0.5, the electron temperature follows Te ∼ Ilas2/3. Thus, measurements of the electron plasma temperature allow indirect estimation of the laser flux on the target and control its shot-to-shot fluctuation. Knowing the laser flux intensity and its fluctuation gives us the possibility of monitoring shot-to-shot reproducibility of shock wave strength generation with high accuracy., T. A. Pikuz, A. Ya. Faenov, N. Ozaki, N. J. Hartley, B. Albertazzi, T. Matsuoka, K. Takahashi, H. Habara, Y. Tange, S. Matsuyama, K. Yamauchi, R. Ochante, K. Sueda, O. Sakata, T. Sekine, T. Sato, Y. Umeda, Y. Inubushi, T. Yabuuchi, T. Togashi, T. Katayama, M. Yabashi, M. Harmand, G. Morard, M. Koenig, V. Zhakhovsky, N. Inogamov, A. S. Safronova, A. Stafford, I. Yu. Skobelev, S. A. Pikuz, T. Okuchi, Y. Seto, K. A. Tanaka, T. Ishikawa, and R. Kodama, "Indirect monitoring shot-to-shot shock waves strength reproducibility during pump–probe experiments", Journal of Applied Physics 120, 035901 (2016) https://doi.org/10.1063/1.4958796.

We have observed the lattice expansion before the onset of compression in an optical-laser-driven target, using diffraction of femtosecond X-ray beams generated by the SPring-8 Angstrom Compact Free-electron Laser. The change in diffraction angle provides a direct measure of the lattice spacing, allowing the density to be calculated with a precision of ±1%. From the known equation of state relations, this allows an estimation of the temperature responsible for the expansion as <1000 K. The subsequent ablation-driven compression was observed with a clear rise in density at later times. This demonstrates the feasibility of studying the dynamics of preheating and shock formation with unprecedented detail., N. J. Hartley, N. Ozaki, T. Matsuoka, B. Albertazzi, A. Faenov, Y. Fujimoto, H. Habara, M. Harmand, Y. Inubushi, T. Katayama, M. Koenig, A. Krygier, P. Mabey, Y. Matsumura, S. Matsuyama, E. E. McBride, K. Miyanishi, G. Morard, T. Okuchi, T. Pikuz, O. Sakata, Y. Sano, T. Sato, T. Sekine, Y. Seto, K. Takahashi, K. A. Tanaka, Y. Tange, T. Togashi, Y. Umeda, T. Vinci, M. Yabashi, T. Yabuuchi, K. Yamauchi, and R. Kodama , "Ultrafast observation of lattice dynamics in laser-irradiated gold foils", Appl. Phys. Lett. 110, 071905 (2017) https://doi.org/10.1063/1.4976541.

N. J. Hartley, N. Ozaki, T. Matsuoka, B. Albertazzi, A. Faenov, Y. Fujimoto, H. Habara, M. Harmand, Y. Inubushi, T. Katayama, M. Koenig, A. Krygier, P. Mabey, Y. Matsumura, S. Matsuyama, E. E. McBride, K. Miyanishi, G. Morard, T. Okuchi, T. Pikuz, O. Sakata, Y. Sano, T. Sato, T. Sekine, Y. Seto, K. Takahashi, K. A. Tanaka, Y. Tange, T. Togashi, Y. Umeda, T. Vinci, M. Yabashi, T. Yabuuchi, K. Yamauchi, and R. Kodama , "Ultrafast observation of lattice dynamics in laser-irradiated gold foils", Appl. Phys. Lett. 110, 071905 (2017) https://doi.org/10.1063/1.4976541., We have observed the lattice expansion before the onset of compression in an optical-laser-driven target, using diffraction of femtosecond X-ray beams generated by the SPring-8 Angstrom Compact Free-electron Laser. The change in diffraction angle provides a direct measure of the lattice spacing, allowing the density to be calculated with a precision of ±1%. From the known equation of state relations, this allows an estimation of the temperature responsible for the expansion as <1000 K. The subsequent ablation-driven compression was observed with a clear rise in density at later times. This demonstrates the feasibility of studying the dynamics of preheating and shock formation with unprecedented detail.

T. A. Pikuz, A. Ya. Faenov, N. Ozaki, N. J. Hartley, B. Albertazzi, T. Matsuoka, K. Takahashi, H. Habara, Y. Tange, S. Matsuyama, K. Yamauchi, R. Ochante, K. Sueda, O. Sakata, T. Sekine, T. Sato, Y. Umeda, Y. Inubushi, T. Yabuuchi, T. Togashi, T. Katayama, M. Yabashi, M. Harmand, G. Morard, M. Koenig, V. Zhakhovsky, N. Inogamov, A. S. Safronova, A. Stafford, I. Yu. Skobelev, S. A. Pikuz, T. Okuchi, Y. Seto, K. A. Tanaka, T. Ishikawa, and R. Kodama, "Indirect monitoring shot-to-shot shock waves strength reproducibility during pump–probe experiments", Journal of Applied Physics 120, 035901 (2016) https://doi.org/10.1063/1.4958796., We present an indirect method of estimating the strength of a shock wave, allowing on line monitoring of its reproducibility in each laser shot. This method is based on a shot-to-shot measurement of the X-ray emission from the ablated plasma by a high resolution, spatially resolved focusing spectrometer. An optical pump laser with energy of 1.0 J and pulse duration of ∼660 ps was used to irradiate solid targets or foils with various thicknesses containing Oxygen, Aluminum, Iron, and Tantalum. The high sensitivity and resolving power of the X-ray spectrometer allowed spectra to be obtained on each laser shot and to control fluctuations of the spectral intensity emitted by different plasmas with an accuracy of ∼2%, implying an accuracy in the derived electron plasma temperature of 5%-10% in pump-probe high energy density science experiments. At nano- and sub-nanosecond duration of laser pulse with relatively low laser intensities and ratio Z/A ∼ 0.5, the electron temperature follows Te ∼ Ilas2/3. Thus, measurements of the electron plasma temperature allow indirect estimation of the laser flux on the target and control its shot-to-shot fluctuation. Knowing the laser flux intensity and its fluctuation gives us the possibility of monitoring shot-to-shot reproducibility of shock wave strength generation with high accuracy.