arXiv subjects

Thomas Meier

Publications and source records attributed to Thomas Meier.

At least 37 records · Page 2Linked to original sources

arXiv2024

Hexagonal to Monoclinic Phase Transition in Dense Hydrogen Phase III Detected by High-Pressure NMR

Conclusive crystal structure determination of the high pressure phases of hydrogen remains elusive due to lack of core electrons and vanishing wave vectors, rendering standard high-pressure experimental methods moot. Ab-initio DFT calculations have shown that structural polymorphism might be solely resolvable using high-resolution nuclear magnetic resonance (NMR) spectroscopy at mega-bar pressures, however technical challenges have precluded such experiments thus far. Here, we present in-situ high-pressure high-resolution NMR experiments in hydrogen phase III between 181 GPa and 208 GPa at room temperature. Our spectra suggest that at lower pressures phase III adopts a hexagonal P6122 crystal structure, transitioning into a monoclinic C2/c phase at about 197 GPa. The high resolution spectra are in excellent agreement with earlier structural and spectral predictions and underline the possibility of a subtle P6122 to C2/c phase transition in hydrogen phase III. These experiments show the importance of a combination of ab-initio calculations and low-Z sensitive spectral probes in high-pressure science in elucidating the structural complexity of the most abundant element in our universe.

cond-mat.mtrl-sci↗

arXiv2024

Parts-per-billion Trace Element Detection in Anhydrous Minerals by Micro-scale Quantitative NMR

Nominally anhydrous minerals (NAMs) composing Earth's and planetary rocks incorporate microscopic amounts of volatiles. However, volatile distribution in NAMs and their effect on physical properties of rocks remain controversial. Thus, constraining trace volatile concentrations in NAMs is tantamount to our understanding of the evolution of rocky planets and planetesimals. Here, we present a novel approach of trace-element quantification using micro-scale Nuclear Magnetic Resonance (NMR) spectroscopy. This approach employs the principle of enhanced mass-sensitivity in NMR microcoils formerly used in \textit{in-situ} high pressure experiments. We were able to demonstrate that this method is in excellent agreement with standard methods across their respective detection capabilities. We show that by simultaneous detection of internal reference nuclei, the quantification sensitivity can be substantially increased, leading to quantifiable trace volatile element amounts of about $50$ wt-ppb measured in a micro-meter sized single anorthitic mineral grain, greatly enhancing detection capabilities of volatiles in geologically important systems.

physics.geo-ph↗

arXiv2024

Unveiling a Novel Metal-to-Metal Transition in LuH2: Critically Challenging Superconductivity Claims in Lutetium Hydrides

Following the recent report by Dasenbrock-Gammon et al. (2023) of near-ambient superconductivity in nitrogen-doped lutetium trihydride (LuH3-δNε), significant debate has emerged surrounding the composition and interpretation of the observed sharp resistance drop. Here, we meticulously revisit these claims through comprehensive characterization and investigations. We definitively identify the reported material as lutetium dihydride (LuH2), resolving the ambiguity surrounding its composition. Under similar conditions (270-295 K and 1-2 GPa), we replicate the reported sharp decrease in electrical resistance with a 30% success rate, aligning with Dasenbrock-Gammon et al.'s observations. However, our extensive investigations reveal this phenomenon to be a novel, pressure-induced metal-to-metal transition intrinsic to LuH2, distinct from superconductivity. Intriguingly, nitrogen doping exerts minimal impact on this transition. Our work not only elucidates the fundamental properties of LuH2 and LuH3 but also critically challenges the notion of superconductivity in these lutetium hydride systems. These findings pave the way for future research on lutetium hydride systems while emphasizing the crucial importance of rigorous verification in claims of ambient temperature superconductivity.

cond-mat.supr-con↗

arXiv2023

A systematic survey of Moon-forming giant impacts: Non-rotating bodies

In the leading theory of lunar formation, known as the giant impact hypothesis, a collision between two planet-size objects resulted in a young Earth surrounded by a circumplanetary debris disk from which the Moon later accreted. The range of giant impacts that could conceivably explain the Earth-Moon system is limited by the set of known physical and geochemical constraints. However, while several distinct Moon-forming impact scenarios have been proposed -- from small, high-velocity impactors to low-velocity mergers between equal-mass objects -- none of these scenarios have been successful at explaining the full set of known constraints, especially without invoking controversial post-impact processes. In order to bridge the gap between previous studies and provide a consistent survey of the Moon-forming impact parameter space, we present a systematic study of simulations of potential Moon-forming impacts. In the first paper of this series, we focus on pairwise impacts between non-rotating bodies. Notably, we show that such collisions require a minimum initial angular momentum budget of approximately $2~J_{EM}$ in order to generate a sufficiently massive protolunar disk. We also show that low-velocity impacts ($v_{\infty} \lesssim 0.5~v_{esc}$) with high impactor-to-target mass ratios ($γ\to 1$) are preferred to explain the Earth-Moon isotopic similarities. In a follow-up paper, we consider impacts between rotating bodies at various mutual orientations.

astro-ph.EP↗

arXiv2022

Forming Iron-rich Planets with Giant Impacts

We investigate mantle stripping giant impacts (GI) between super-Earths with masses between 1 M$_{\oplus}$ and 20 M$_{\oplus}$. We infer new scaling laws for the mass of the largest fragment and its iron mass fraction, as well as updated fitting coefficients for the critical specific impact energy for catastrophic disruption, $Q_{RD}^{*}$. With these scaling laws, we derive equations that relate the impact conditions, i.e., target mass, impact velocity and impactor-to-target mass ratio, to the mass and iron mass fraction of the largest fragment. This allows one to predict collision outcomes without performing a large suite of simulations. Using these equations we present the maximum and minimum planetary iron mass fraction as a result of collisional stripping of its mantle for a given range of impact conditions. We also infer the radius for a given mass and composition using interior structure models and compare our results to observations of metal-rich exoplanets. We find good agreement between the data and the simulated planets suggesting that GI could have played a key role in their formation. Furthermore, using our scaling laws we can further constrain the impact conditions that favour their masses and compositions. Finally, we present a flexible and easy-to-use tool that allows one to predict mass and composition of a planet after a GI for an arbitrary range of impact conditions which in turn allows to assess the role of GI in observed planetary systems.

astro-ph.EP↗

arXiv2022

High-Pressure Synthesis of Seven Lanthanum Hydrides with a Significant Variability of Hydrogen Content

The lanthanum-hydrogen system has attracted significant attention following the report of superconductivity in LaH10 at near-ambient temperatures and high pressures. Here, we present the results of our single-crystal X-ray diffraction studies on this system, supported by density functional theory calculations, which reveal an unexpected chemical and structural diversity of lanthanum hydrides synthesized in the range of 50 to 180 GPa. Seven lanthanum hydrides were produced, LaH3, LaH~4, LaH4+δ, La4H23, LaH6+δ, LaH9+δ, and LaH10+δ, and the atomic coordinates of lanthanum in their structures determined. The regularities in rare-earth element hydrides unveiled here provide clues to guide the search for other synthesizable hydrides and candidate high-temperature superconductors. The hydrogen content variability in lanthanum hydrides and the samples' phase heterogeneity underline the challenges related to assessing potentially superconducting phase(s) and the nature of electronic transitions in high-pressure hydrides.

cond-mat.mtrl-sci↗

arXiv2022

Direct Hydrogen Quantification in High-pressure Metal Hydrides

High-pressure metal-hydride (MH) research evolved into a thriving field within condensed matter physics following the realisation of metallic compounds showing phonon mediated near room-temperature superconductivity. However, severe limitations in determining the chemical formula of the reaction products, especially with regards to their hydrogen content, impedes a deep understanding of the synthesized phases and can lead to significantly erroneous conclusions. Here, we present a way to directly access the hydrogen content of MH solids synthesised at high pressures in (laser-heated) diamond anvil cells using nuclear magnetic resonance (NMR) spectroscopy. We show that this method can be used to investigate MH compounds with a wide range of hydrogen content, from MHx with x=0.15 (CuH0.15) to x < 6.4 (H 6+-0.4 S 5).

cond-mat.mtrl-sci↗

arXiv2022

Universal Hydrogen Bond Symmetrisation Dynamics Under Extreme Conditions

The experimental study of hydrogen bonds and their symmetrisation under extreme conditions is predominantly driven by diffraction methods, despite challenges of localising or probing the hydrogen subsystems directly. Until recently, H-bond symmetrisation has been addressed in terms of either nuclear quantum effects, spin crossovers or direct structural transitions; often leading to contradictory interpretations when combined. Here, we present high-resolution \textit{in-situ} $^1$H-NMR experiments in diamond anvil cells investigating a wide range of hydrogen bonded systems at pressure ranges of up to 90 GPa covering their respective H-bond symmetrisation. We found pronounced minima in the pressure dependence of the NMR resonance line-widths associated with a maximum in hydrogen mobility, precursor to a localisation of hydrogen atoms. These minima, independent of of the chemical environment of the linear O -- H-O unit, can be found in a narrow range of oxygen-oxygen distances between 2.44 and 2.45 Å, leading to an average critical oxygen-oxygen distance of $\bar{r}_{\rm OO}^{crit}=2.443(1)$ Å.

physics.chem-ph↗

arXiv2021

Tailoring Luminescent Properties of SrS:Ce by Modulating Defects: Sr-Deficiency and Na+ Doping

Ce3+ doped SrS phosphors with a charge-compensating Na+ for light-emitting diode (LED) applications have been successfully synthesized via a solid-state reaction method, which can be indexed to rock-salt-like crystal structures of Fm-3m space group. SrS:(Ce3+)x(x=0.005-0.05) and SrS:(Ce3+)0.01,(Na+)y(y=0.005-0.030) phosphors were excited by 430nm UV-VIS light, associated to the 5d1-4f1 transition of Ce3+. The composition-optimized SrS:(Ce3+)0.01,(Na+)0.015 phosphors showed an intense broad emission band at 430-700nm. The doping of Na+ was probed by solid-state nuclear magnetic resonance. The 430 nm pumped with white LED (w-LED) combining SrS:(Ce3+)0.01,(Na+)0.015 phosphors and Sr2Si5N8:Eu2+ phosphors shows a color-rendering index (Ra) of 89.7. The proposed strategy provides new avenues for design and realization of novel high color quality solid-state lighting emitting diodes (SS-LEDS).

cond-mat.mtrl-sci↗

arXiv2021

Absence of proton tunneling during the hydrogen bond symmetrization in $δ$-AlOOH

$δ$-AlOOH is of significant crystallochemical interest due to a subtle structural transition near 10 GPa from a $P2_1nm$ to a $Pnnm$ structure, the nature and origin of hydrogen disorder, the symmetrization of the O-H$\cdots$O hydrogen bond and their interplay. We perform a series of density functional theory based simulations in combination with high-pressure nuclear magnetic resonance experiments on $δ$-AlOOH up to 40 GPa with the goal to better characterize the hydrogen potential and therefore the nature of hydrogen disorder. Simulations predict a phase transition in agreement with our nuclear magnetic resonance experiments at $10-11$ GPa and hydrogen bond symmetrization at $14.7$ GPa. Calculated hydrogen potentials do not show any double-well character and there is no evidence for proton tunneling in our nuclear magnetic resonance data.

cond-mat.mtrl-sci↗

arXiv2021

In-situ High Pressure Nuclear Magnetic Resonance Crystallography

Our recent developments in in-situ nuclear magnetic resonance (NMR) spectroscopy under extreme conditions led to the observation of a wide variety of physical phenomena not accessible with standard high pressure experimental probes. However, inherent di- or quadrupolar line broadening in diamond anvil cell (DAC) based NMR experiments often limit detailed investigations of local atomic structures, especially if different phases or local environments are coexisting. Here, we present our progress in the development of high resolution NMR experiments in DACs using one and two-dimensional homonuclear decoupling experiments at pressures up to the Mbar regime. Using this technique, spectral resolutions in the order of 1 ppm and below have been achieved, enabling high pressure structural analysis. Several examples will demonstrate the wide applicability of this method for extreme conditions research.

cond-mat.mtrl-sci↗

arXiv2021

High-Pressure Na3(N2)4, Ca3(N2)4, Sr3(N2)4, and Ba(N2)3 Featuring Nitrogen Dimers with Non-Integer Charges and Anion-Driven Metallicity

Charged nitrogen dimers are ubiquitous in high-pressure binary metal-nitrogen systems. They are known to possess integer formal charges x varying from one through four. Here, we present the investigation of the binary alkali- and alkaline earth metal-nitrogen systems, Na-N, Ca-N, Sr-N, Ba-N to 70 GPa. We report on compounds-Na3(N2)4, Ca3(N2)4, Sr3(N2)4, and Ba(N2)3-featuring charged nitrogen dimers with paradigm-breaking non-integer charges, x = 0.67, 0.75 and 1.5. The metallic nature of all four compounds is deduced from ab initio calculations. The conduction electrons occupy the pi* antibonding orbitals of the charged nitrogen dimers that results in anion-driven metallicity. Delocalization of these electrons over the pi* antibonding states enables the non-integer electron count of the dinitrogen species. Anion-driven metallicity is expected to be found among a variety of compounds with homoatomic anions (e.g., polynitrides, carbides, and oxides), with the conduction electrons playing a decisive role in their properties.

cond-mat.mtrl-sci↗

arXiv2021

The EOS/Resolution Conspiracy: Convergence in Proto-Planetary Collision Simulations

We investigate how the choice of equation of state (EOS) and resolution conspire to affect the outcomes of giant impact (GI) simulations. We focus on the simple case of equal mass collisions of two Earth-like $0.5\,M_\oplus$ proto-planets showing that the choice of EOS has a profound impact on the outcome of such collisions as well as on the numerical convergence with resolution. In simulations where the Tillotson EOS is used, impacts generate an excess amount of vapour due to the lack of a thermodynamically consistent treatment of phase transitions and mixtures. In oblique collisions this enhances the artificial angular momentum (AM) transport from the planet to the circum-planetary disc reducing the planet's rotation period over time. Even at a resolution of $1.3 \times 10^6$ particles the result is not converged. In head-on collisions the lack of a proper treatment of the solid/liquid-vapour phase transition allows the bound material to expand to very low densities which in turn results in very slow numerical convergence of the critical specific impact energy for catastrophic disruption $Q_{RD}^*$ with increasing resolution as reported in prior work. The simulations where ANEOS is used for oblique impacts are already converged at a modest resolution of $10^5$ particles, while head-on collisions converge when they evidence the post-shock formation of a dense iron-rich ring, which promotes gravitational re-accumulation of material. Once sufficient resolution is reached to resolve the liquid-vapour phase transition of iron in the ANEOS case, and this ring is resolved, the value of $Q_{RD}^*$ has then converged.

astro-ph.EP↗

arXiv2021

Proton dynamics in high-pressure ice-VII from density functional theory

Using a density-functional-theory-based approach, we explore the symmetrization and proton dynamics in ice-VII, for which recent high-pressure NMR experiments indicate significant proton dynamics in the pressure-range of $20-95$ GPa. We directly sample the potential seen by the proton and find a continuous transition from double- to single-well character over the pressure range of 2 to 130 GPa accompanied by proton dynamics in agreement with the NMR experiments.

cond-mat.mtrl-sci↗

arXiv2020

Nuclear Spin Crossover in Dense Molecular Hydrogen

The laws of quantum mechanics are often tested against the behaviour of the lightest element in the periodic table, hydrogen. One of the most striking properties of molecular hydrogen is the coupling between molecular rotational properties and nuclear spin orientations, giving rise to the spin isomers ortho- and para-hydrogen. At high pressure, as intermolecular interactions increase significantly, the free rotation of H2 molecules is increasingly hindered, and consequently a modification of the coupling between molecular rotational properties and the nuclear spin system can be anticipated. To date, high-pressure experimental methods have not been able to observe nuclear spin states at pressures approaching 100 GPa and consequently the effect of high pressure on the nuclear spin statistics could not be directly measured. Here, we present in-situ high-pressure nuclear magnetic resonance data on molecular hydrogen in its hexagonal phase I up to 123 GPa at room temperature. While our measurements confirm the presence of I=1 ortho-hydrogen at low pressures, above 70 GPa, where inter- and intramolecular distances become comparable, we observe a crossover in the nuclear spin statistics from a spin-1 quadrupolar to a spin-1/2 dipolar system, evidencing the loss of spin isomer distinction. These observations represent a unique case of a nuclear spin crossover phenomenon in quantum solids.

cond-mat.mtrl-sci↗

arXiv2020

Metallic Hydrogen Sublattice and Proton Mobility in Copper Hydride at High Pressure

Atomic and electronic structures of Cu2H and CuH have been investigated by high pressure NMR spectroscopy, X-ray diffraction and ab-initio calculations. Metallic Cu2H was synthesized at a pressure of 40 GPa, and semi-metallic CuH at 90 GPa, found stable up to 160 GPa. Experiments and computations suggest the formation of a metallic 1H-sublattice as well as a high 1H mobility of ~10-7 cm2/s in Cu2H. Comparison of Cu2H and FeH data suggests that deviations from Fermi gas behavior, formation of conductive hydrogen networks, and high 1H mobility could be common features of metal hydrides.

cond-mat.mtrl-sci↗

arXiv2019

Table-top NMR system for high-pressure studies with in-situ laser heating

High pressure Nuclear Magnetic Resonance (NMR) is known to uncover behavior of matter at extreme conditions. However, significant maintenance demands, space requirements and high costs of superconducting magnets render its application unfeasible for regular modern high pressure laboratories. Here, we present a table-top NMR system based on permanent Halbach magnet arrays with dimensions of 25 cm diameter and 4 cm height. At the highest field of 1013 mT, 1H-NMR spectra of Ice VII have been recorded at 25 GPa and ambient temperature. The table-top NMR system can be used together with double sided laser heating set-ups. Feasibility of high-pressure high-temperature NMR was demonstrated by collecting 1H-NMR spectra of H2O at 25 GPa and 1063(50) K. We found that the change in signal intensity in laser-heated NMR diamond anvil cell yields a convenient way for temperature measurements.

physics.app-ph↗

arXiv2019

Improving Resolution of Solid State NMR in Dense Molecular Hydrogen

Recent advancements in radio-frequency resonator designs have led to the implementation of nuclear magnetic resonance in diamond anvil cells (DACs) at pressures well above 100 GPa. However, a relatively low resolution and the absence of decoupling sequences complicate the analysis of the results of solid state NMR in DACs. Here, we present the first application of homo-nuclear Lee-Goldburg (LG) decoupling at extreme conditions on high density molecular hydrogen. Lenz lens based two-dimensional resonator structures were found to generate a homogeneous B1 field across sample cavities as small as 12 picolitres, a prerequisite for optimal decoupling. At ideal LG conditions, the broad 1H resonance of molecular ortho-hydrogen was narrowed 1600-fold, resulting in line-widths of 3.1 ppm.

physics.app-ph↗