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Register a new userImproving Resolution of Solid State NMR in Dense Molecular Hydrogen
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Added by
Thomas Meier Dr. rer. nat.
Publication date
2019
fields
Physics
and research's language is
English
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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.
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We present an accurate computational study of the electronic structure and lattice dynamics of solid molecular hydrogen at high pressure. The band-gap energies of the $C2/c$, $Pc$, and $P6_3/m$ structures at pressures of 250, 300, and 350 GPa are calculated using the diffusion quantum Monte Carlo (DMC) method. The atomic configurations are obtained from ab-initio path-integral molecular dynamics (PIMD) simulations at 300 K and 300 GPa to investigate the impact of zero-point energy and temperature-induced motion of the protons including anharmonic effects. We find that finite temperature and nuclear quantum effects reduce the band-gaps substantially, leading to metallization of the $C2/c$ and $Pc$ phases via band overlap; the effect on the band-gap of the $P6_3/m$ structure is less pronounced. Our combined DMC-PIMD simulations predict that there are no excitonic or quasiparticle energy gaps for the $C2/c$ and $Pc$ phases at 300 GPa and 300 K. Our results also indicate a strong correlation between the band-gap energy and vibron modes. This strong coupling induces a band-gap reduction of more than 2.46 eV in high-pressure solid molecular hydrogen. Comparing our DMC-PIMD with experimental results available, we conclude that none of the structures proposed is a good candidate for phases III and IV of solid hydrogen.
Being the simplest element with just one electron and proton the electronic structure of the Hydrogen atom is known exactly. However, this does not hold for the complex interplay between them in a solid and in particular not at high pressure that is known to alter the crystal as well as the electronic structure. Back in 1935 Wigner and Huntington predicted that at very high pressure solid molecular hydrogen would dissociate and form an atomic solid that is metallic. In spite of intense research efforts the experimental realization, as well as the theoretical determination of the crystal structure has remained elusive. Here we present a computational study showing that the distorted hexagonal P6$_3$/m structure is the most likely candidate for Phase III of solid hydrogen. We find that the pairing structure is very persistent and insulating over the whole pressure range, which suggests that metallization due to dissociation may precede eventual bandgap closure. Due to the fact that this not only resolve one of major disagreement between theory and experiment, but also excludes the conjectured existence of phonon-driven superconductivity in solid molecular hydrogen, our results involve a complete revision of the zero-temperature phase diagram of Phase III.
Solid-state lithium-ion batteries (SSLIBs) are considered to be the new generation of devices for energy storage due to better performance and safety. Poly (ethylene oxide) (PEO) based material becomes one of the best candidate of solid electrolytes, while its thermal conductivity is crucial to heat dissipation inside batteries. In this work, we study the thermal conductivity of PEO by molecular dynamics simulation. By enhancing the structure order, thermal conductivity of aligned crystalline PEO is obtained as high as 60 W/m-K at room temperature, which is two orders higher than the value (0.37 W/m-K) of amorphous structure. Interestingly, thermal conductivity of ordered structure shows a significant stepwise negative temperature dependence, which is attributed to the temperature-induced morphology change. Our study offers useful insights into the fundamental mechanisms that govern the thermal conductivity of PEO but not hinder the ionic transport, which can be used for the thermal management and further optimization of high-performance SSLIBs.
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.
We theoretically investigate thermalization and spin diffusion driven by a quantum spin bath for a realistic solid-state NMR experiment. We consider polycrystalline L-alanine, and investigate how the spin polarization spreads among several $^{13}$C nuclear spins, which interact via dipole-dipole coupling with the bath of strongly dipolar-coupled $^1$H nuclear (proton) spins. We do this by using direct numerical simulation of the many-spin time-dependent Schrodinger equation. We find that, although the proton spins located near the carbon sites interact most strongly with the $^{13}$C spins, this interaction alone is not enough to drive spin diffusion and thermalize the $^{13}$C nuclear spins. We demonstrate that the thermalization within the $^{13}$C subsystem is driven by the collective many-body dynamics of the proton spin bath, and specifically, that the onset of thermalization among the $^{13}$C spins is directly related to the onset of chaotic behavior in the proton spin bath. Therefore, thermalization and spin diffusion within the $^{13}$C subsystem is controlled by the proton spins located far from the C sites. In spite of their weak coupling to the $^{13}$C spins, these far-away protons help produce a network of strongly coupled proton spins with collective dynamics, that drives thermalization.
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