This paper presents the technical details and commissioning results of a newly upgraded platform for ion-irradiation experiments under multi-GPa static pressure conditions at the GSI Helmholtz Center for Heavy Ion Research (Darmstadt, Germany), now accessible to external users. The GSI SIS18 accelerator provides heavy ions with tens of GeV kinetic energies, capable of penetrating through diamond anvil cells and depositing extremely high energy densities within the pressurized samples. This energy deposition triggers ultrafast, localized structural and phase transformations at the nanoscale. The platform integrates online optical microscopy and Raman spectroscopy, providing real-time monitoring of material modifications during stepwise fluence accumulation. By enabling controlled studies of structural responses and phase transitions under coupled extreme conditions, this setup opens unprecedented opportunities for research across condensed-matter physics, materials science, geoscience, high-pressure chemistry, and planetary science.

Understanding the phase diagram of carbon is challenging due to large energy barriers between phases and the presence of extensive metastability fields. We examine the phase composition and microstructure in the poorly understood region of the pressure-temperature diagram from the vicinity of the graphite-diamond-liquid triple point up to pressures of similar to 35 GPa using flash laser heating of glassy carbon. Consistent with previous studies of the carbon phase diagram, above the triple point pressure (at similar to 11 GPa) and temperatures below similar to 2000 K, the graphite to diamond transformation was inhibited. Above this temperature and above the triple point pressure, a graphite/diamond nanocomposite was observed, arising from a partial transformation to diamond via solid state diffusion processes. As the pressure increased further to above similar to 16 GPa, phase pure nanodiamonds were formed with crystal sizes down to similar to 1 nm, depending on the temperature. At higher temperatures above the triple point pressure, clear evidence for melting was observed, resulting in the formation of larger diamond crystals, up to 0.5 mu m in diameter consistent with growth from a liquid. Below the triple point pressure, glassy carbon gradually graphitizes up to the melting point of similar to 5000 K, while above this temperature larger crystals with pillar-like morphology grow from the liquid phase. Our work demonstrates that the complex phase behaviour of carbon leads to a wide variety of microstructures in the vicinity of the graphite-diamond-liquid triple point including nanocomposites with crystallite sizes down to the nanoscale.

A miniature sized end-loaded piston cylinder cell with radial side windows for neutron scattering experiments is described. The principle of the bicone-shaped cylinders used was first presented by McWhan in 1974. The present cell is of compact portable design yet significantly enlarges the scattering angles. Its small size allows neutron scattering experiments at low temperatures. The bicone-shaped cylinders are made from various ceramics or a highly neutron-transmissive Ni-free Cr-Mo-V steel. Successful neutron scattering experiments up to 5 GPa have been demonstrated on the CORELLI single-crystal diffractometer and the VISION vibrational spectrometer of the Spallation Neutron Source at the Oak Ridge National Laboratory.

Diamond's unique properties on the nanoscale make it one of the most important materials for use in biosensors and quantum computing and for components that can withstand the harsh environments of space. We synthesize oriented, faceted diamond particles by flash laser heating of glassy carbon at 16 GPa and 2300 K. Detailed transmission electron microscopy shows them to consist of a mosaic of diamond nanocrystals frequently joined at twin boundaries forming microtwins. Striking 3-fold translational periodicity was observed in both imaging and diffraction. This periodicity was shown to originate from nanodimensional wedge-shaped overlapping regions of twinned diamond and not from a possible 9R polytype, which has also been reported in other group IVa elements and water ice. Extended bilayers of hexagonal layer stacking were observed, forming lonsdaleite nanolaminates. The particles exhibited optical fluorescence with a rapid quench time (<1 ns) attributed to their unique twinned microstructure.

The phase behavior of carbon at high pressure and the search for carbon structures denser than diamond has been explored for decades showing large discrepancies, with many fundamental questions remaining unresolved. Here we show evidence of melting above the graphite-diamond-liquid (GDL) triple point (similar to 13 GPa, 4000 K) up to 50 GPa on samples recovered from single flash-heating events using spectroscopic and electron microscopic methods. The results show that for all pressures, diamond melts below the triple point temperature contradicting previous studies, most of which predict a positive slope of the melting curve.

We have synthesized hydrogenated and deuterated amorphous carbon materials that have a density, 2.7 ± 0.1 g/cm3, consistent with almost entirely tetrahedral bonding. In hydrogen-free tetrahedral amorphous carbon, the presence of a minority of sp2 bonded atoms leads to localized states that could be passivated with hydrogen by analogy with hydrogenated amorphous silicon. Neutron diffraction analysis demonstrated that the local bonding environment is consistent with ab initio models of high density hydrogenated tetrahedral amorphous carbon and with the related tetrahedral molecular structure neopentane. The optical bandgap of our material, 4.5 eV, is close to the bandgap in the density of states determined by scanning tunneling spectroscopy (4.3 eV). This bandgap is considerably larger than that of hydrogen-free tetrahedral amorphous carbon, confirming that passivation of sp2 associated tail-states has occurred. Both the structural and electronic measurements are consistent with a model in which the tetrahedrally bonded carbon regions are terminated by hydrogen, causing hopping conductivity to dominate.

Over the last 60 years, the diamond anvil cell (DAC) has emerged as the tool of choice in high pressure science because materials can be studied at megabar pressures using X-ray and spectroscopic probes. In contrast, the pressure range for neutron diffraction has been limited due to low neutron flux even at the strongest sources and the resulting large sample sizes. Here, we introduce a neutron DAC that enables break-out of the previously limited pressure range. Key elements are ball-bearing guides for improved mechanical stability, gem-quality synthetic diamonds with novel anvil support and improved in-seat collimation. We demonstrate a pressure record of 1.15 Mbar and crystallographic analysis at 1 Mbar on the example of nickel. Additionally, insights into the phase behavior of graphite to 0.5 Mbar are described. These technical and analytical developments will further allow structural studies on low-Z materials that are difficult to characterize by X-rays.

Although long-chain aliphatic hydrocarbons are documented in meteorites, their origin is poorly understood. A key question is whether they are pristine or a byproduct of terrestrial alteration? To understand if these long-chain hydrocarbons are indigenous, it will be important to explore their thermodynamic and mechanical stability at conditions experienced by extraterrestrial objects during atmospheric entry and passage. Extreme pressures and temperatures experienced by meteorites are likely to alter the molecular organization of these long-chain hydrocarbons. These structural changes associated with extreme conditions are often documented via laboratory-based Raman spectroscopic measurements. So far, Raman spectroscopic measurements have investigated the effect of static compression on the aliphatic hydrocarbons. The effect of temperature on the structural changes remains poorly explored. To bridge this gap, in this study, we have explored the behavior of two aliphatic hydrocarbons at simultaneously high pressures and temperatures. We have used a resistively heated diamond anvil cell. On compression to moderate pressures, the appearance of new vibrational modes in the low-energy region confirms prior studies and is related to the bending of the linear chains. Upon heating to ∼220 °C, we note that the new low-energy mode undergoes softening. The mode softening is likely due to the combination of unbending of the alkane chain and mode anharmonicity.

Ten years ago, Dave Mao, director of Energy Frontier Research in Extreme Environments (EFree), a Department of Energy (DOE) energy frontier, recognized the importance of neutron science for energy research. The subsequent establishment of a neutron group within EFree lead to the formation of an Instrument Development Team for SNAP, the dedicated high-pressure beamline at the Spallation Neutron Source at Oak Ridge National Laboratory in Tennessee. The core concept was to develop novel high-pressure techniques to expand the pressure range for neutron diffraction. A quite ambitious goal was set to reach half megabar levels (50 GPa), which at the time was considered extremely challenging. Here we will give a brief overview of the developments during the last decade in this novel area of research. An important factor was that during this period multicarat diamond anvils have become available grown by chemical vapor deposition (CVD), making research in this pressure range and beyond rather routine. This chapter shows the latest developments in large anvil and anvil support designs, compact multiple ton diamond cells, and new neutron methodologies. Achievements are illustrated with some examples of high-quality neutron diffraction patterns collected on sample sizes much small than conventional sizes.

Three concepts for the application of multi-extreme conditions under in situ neutron scattering are described here. The first concept is a neutron diamond anvil cell made from a non-magnetic alloy. It is shrunk in size to fit existing magnets and future magnet designs and is designed for best pressure stability upon cooling. This will allow for maximum pressures above 10 GPa to be applied simultaneously with (steady-state) high magnetic field and (ultra-)low temperature. Additionally, an implementation of miniature coils for neutron diamond cells is presented for pulsed-field applications. The second concept presents a set-up for laser-heating a neutron diamond cell using a defocused CO2 laser. Cell, anvil, and gasket stability will be achieved through stroboscopic measurements and maximum temperatures of 1500 K are anticipated at pressures to the megabar. The third concept presents a hybrid levitator to enable measurements of solids and liquids at temperatures in excess of 4000 K. This will be accomplished by a combination of bulk induction and surface laser heating and hyperbaric conditions to reduce evaporation rates. The potential for deployment of these multi-extreme environments within this first instrument suite of the Second Target Station is described with a special focus on VERDI, PIONEER, CENTAUR, and CHESS. Furthermore, considerations for deployment on future instruments, such as the one proposed as TITAN, are discussed. Overall, the development of these multi-extremes at the Second Target Station, but also beyond, will be highly advantageous for future experimentation and will give access to parameter space previously not possible for neutron scattering.

Multi-anvil and laser-heated diamond anvil methods have been used to subject Ge and Si mixtures to pressures and temperatures of between 12 and 17 GPa and 1500-1800 K, respectively. Synchrotron angle dispersive X-ray diffraction, precession electron diffraction and chemical analysis using electron microscopy, reveal recovery at ambient pressure of hexagonal Ge-Si solid solutions (P6(3)/mmc). Taken together, the multi-anvil and diamond anvil results reveal that hexagonal solid solutions can be prepared for all Ge-Si compositions. This hexagonal class of solid solutions constitutes a significant expansion of the bulk Ge-Si solid solution family, and is of interest for optoelectronic applications.

When powders of polycrystalline transparent materials are compressed in the diamond cell, they undergo a change from translucent to transparent. This effect is due to plastic deformation of the grains leading to a reduction in the size of voids responsible for light scattering. The pressures of the onset and saturation of the optical transmission corelate respectively well with the previously reported yield strengths and hardness obtained by different techniques. From ten measurements on MgO, SiO2, Al2O3, olivine, pyroxene, garnet and a perovskite, we find a ratio between hardness and yield strength of three, which is generally accepted. Preliminary high temperature measurements with the double-sided laser heating technique show that this method may be used for determining rheological properties of minerals at P-T conditions of the deep Earth. This technique for obtaining high optical transmission in polycrystalline materials may also be of interest for modern solid state laser materials.

Octadecane (C18H38) is an aliphatic hydrocarbon that is abundant in carbonaceous chondritic meteorites. It is debated whether these hydrocarbons found in the meteorite are pristine or are a result of subsequent modifications as these meteorites are delivered to the Earth. It is well-known that meteorites are often subjected to extreme pressures and temperatures upon entering the Earth's atmosphere. To explore the behavior of octadecane at high pressures, that is, how its molecular structure responds to compression, we use a diamond anvil cell in conjunction with Raman spectroscopy. We find that at room temperatures, upon compression to similar to 5 GPa, a linear-chain octadecane molecule transforms into a bent-chain configuration. Similar transitions from linear to a bent configuration in other hydrocarbons have been documented. We find a linear correlation between the transition pressure from linear to bent configuration, and the chain length of the alkane, that is, longer chain lengths, is likely to be less stable in the linear configuration under compression. These kinks in the bent-chain configuration are likely sites for the dissociation of the longer chain hydrocarbons to smaller hydrocarbons. The octadecane sample examined in this study did not undergo any additional transition to the highest pressure (similar to 18 GPa) explored in this study.

High-pressure neutron diffraction is an extremely useful technique in the quest for making and understanding novel hydride superconductors. Neutron diffraction can be used to directly determine elemental stoichiometries and atomic positions of many light elements such as hydrogen or deuterium, even in the presence of heavy elements such as rare-earth metals. Here, we report on the current status and ongoing developments on high-pressure neutron diffraction for hydride superconductors and other metal hydrides with a special focus on current advancements at the Spallation Neutrons and Pressure (SNAP) beamline of the Spallation Neutron Source at Oak Ridge National Laboratory. For broader context, an overview of high-pressure neutron diffractometers and pressure cells is included together with insight into critical sample considerations. There, attention is given to the requirements for powdered hydride samples and the need for deuterium rather than hydrogen. Additionally, the advantages of angular access and data representation as possible at SNAP are described. We demonstrate the current capability for high-pressure neutron diffraction on two different samples created via hydrogen gas loading, specifically pure deuterium and nickel-deuteride. The deuterium example highlights the usefulness of adding sample materials that facilitate the formation of a good powder while the nickel-deuteride example demonstrates that atomic deuterium positions and stoichiometry can be directly determined. Both examples highlight the importance of large scattering apertures. These enable investigation of the data resolved by scattering angle that is needed to identify parasitic peaks and background features. Finally, future directions beyond current high-pressure neutron powder diffraction are also discussed.

Leadership in materials science underpins future technologies in energy, security, and other applications that drive this nation’s economy. Neutron scattering is among the crucial characterization techniques necessary to ensure a world-leading position in materials science for the United States. The Second Target Station (STS) at the Spallation Neutron Source (SNS) will provide transformative new capabilities for the study of a broad range of materials using neutron scattering and will support users in many fields of research—materials science, physics, chemistry, geology, biology, and engineering, among others—and from academia, government laboratories, and industry.

The amount of literature on both melting and thermal conductivity of iron at Earth’s core conditions is overwhelming and the discrepancies are very large. There is a broad range of experimental techniques each of which is flawed to a certain degree, which may explain the discrepancy. In this report, we present new data using a different method for determining the phase behavior and resistivity of iron in the laser-heated diamond cell by measuring the electrical resistance of both solid and liquid iron wires. The experiment avoids some of the major flaws of previous experiments, the most important of which is the detection of the onset of melting. These measurements confirm a shallow melting curve found earlier and the resistivity data imply a trend towards low thermal conductivity in the liquid outer core.

Quantitative single crystal neutron-diffraction in diamond anvil cells has so far been limited by the neutron flux available at the various neutron sources. As a result, highly precise measurements of the exact position of light elements have not been possible preventing, for example, structural studies of hydrogen and hydrogen bonds under pressure. Here we report experiments carried out on SNAP at the Spallation Neutron Source (ORNL, TN, USA) to explore the possibility and current limits of such studies. Furthermore, we benchmarked the obtained data quality with reference experiments carried out on TOPAZ, a dedicated single-crystal instrument. We show that measuring single-crystal diffraction intensities on SNAP is possible to such a precision that we are able to resolve the hydrogen bonds in potassium dideuterium phosphate (DKDP) as well as in ice VI.

Exploring the behavior of hydrocarbon under pressure is important for understanding its role in planetary sciences and also for exploring novel organic chemistry. In this study, we explored the high-pressure behavior of a linear-chain hydrocarbon, tricosane (C23H48), using Raman spectroscopy. We compressed tricosane up to 23 GPa and did not find any evidence for pressure-induced amorphization within the conditions explored in this study. Upon compression, we observe new modes in the low energy region 100–300 cm−1. In order to understand the appearance of these new modes at high pressures, we used complementary ab initio calculations and explored the effect of chain configurations (linear and bent) on the predicted Raman spectra. We find that these new modes observed at higher pressures are better explained by bent configuration of tricosane chains. Thus, based on high-pressure Raman spectra, it is very likely that a linear chain of tricosane is bent under pressure, i.e., it undergoes a pressure-induced trans-gauche transformation. It is also likely that such bent regions (i.e., kinks) will act as sites along which large chain hydrocarbons could dissociate into smaller chain lengths at extreme conditions relevant to the interiors of Jovian planets.