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1.
Sci Rep ; 14(1): 12239, 2024 May 28.
Article in English | MEDLINE | ID: mdl-38806565

ABSTRACT

Laser-driven dynamic compression experiments of plastic materials have found surprisingly fast formation of nanodiamonds (ND) via X-ray probing. This mechanism is relevant for planetary models, but could also open efficient synthesis routes for tailored NDs. We investigate the release mechanics of compressed NDs by molecular dynamics simulation of the isotropic expansion of finite size diamond from different P-T states. Analysing the structural integrity along different release paths via molecular dynamic simulations, we found substantial disintegration rates upon shock release, increasing with the on-Hugnoiot shock temperature. We also find that recrystallization can occur after the expansion and hence during the release, depending on subsequent cooling mechanisms. Our study suggests higher ND recovery rates from off-Hugoniot states, e.g., via double-shocks, due to faster cooling. Laser-driven shock compression experiments of polyethylene terephthalate (PET) samples with in situ X-ray probing at the simulated conditions found diamond signal that persists up to 11 ns after breakout. In the diffraction pattern, we observed peak shifts, which we attribute to thermal expansion of the NDs and thus a total release of pressure, which indicates the stability of the released NDs.

2.
Phys Rev E ; 108(3-2): 035210, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37849197

ABSTRACT

We present experimental observations of K_{ß} emission from highly charged Mg ions at solid density, driven by intense x rays from a free electron laser. The presence of K_{ß} emission indicates the n=3 atomic shell is relocalized for high charge states, providing an upper constraint on the depression of the ionization potential. We explore the process of state relocalization in dense plasmas from first principles using finite-temperature density functional theory alongside a wave-function localization metric, and find excellent agreement with experimental results.

3.
Struct Dyn ; 10(5): 054501, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37841290

ABSTRACT

Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray-matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L3-edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm2. We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale.

4.
Proc Natl Acad Sci U S A ; 119(43): e2200405119, 2022 Oct 25.
Article in English | MEDLINE | ID: mdl-36256805

ABSTRACT

The magnetotransport behavior inside the nematic phase of bulk FeSe reveals unusual multiband effects that cannot be reconciled with a simple two-band approximation proposed by surface-sensitive spectroscopic probes. In order to understand the role played by the multiband electronic structure and the degree of two-dimensionality, we have investigated the electronic properties of exfoliated flakes of FeSe by reducing their thickness. Based on magnetotransport and Hall resistivity measurements, we assess the mobility spectrum that suggests an unusual asymmetry between the mobilities of the electrons and holes, with the electron carriers becoming localized inside the nematic phase. Quantum oscillations in magnetic fields up to 38 T indicate the presence of a hole-like quasiparticle with a lighter effective mass and a quantum scattering time three times shorter, as compared with bulk FeSe. The observed localization of negative charge carriers by reducing dimensionality can be driven by orbitally dependent correlation effects, enhanced interband spin fluctuations, or a Lifshitz-like transition, which affect mainly the electron bands. The electronic localization leads to a fragile two-dimensional superconductivity in thin flakes of FeSe, in contrast to the two-dimensional high-[Formula: see text] induced with electron doping via dosing or using a suitable interface.

5.
Sci Adv ; 8(35): eabo0617, 2022 Sep 02.
Article in English | MEDLINE | ID: mdl-36054354

ABSTRACT

Extreme conditions inside ice giants such as Uranus and Neptune can result in peculiar chemistry and structural transitions, e.g., the precipitation of diamonds or superionic water, as so far experimentally observed only for pure C─H and H2O systems, respectively. Here, we investigate a stoichiometric mixture of C and H2O by shock-compressing polyethylene terephthalate (PET) plastics and performing in situ x-ray probing. We observe diamond formation at pressures between 72 ± 7 and 125 ± 13 GPa at temperatures ranging from ~3500 to ~6000 K. Combining x-ray diffraction and small-angle x-ray scattering, we access the kinetics of this exotic reaction. The observed demixing of C and H2O suggests that diamond precipitation inside the ice giants is enhanced by oxygen, which can lead to isolated water and thus the formation of superionic structures relevant to the planets' magnetic fields. Moreover, our measurements indicate a way of producing nanodiamonds by simple laser-driven shock compression of cheap PET plastics.

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