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Yishan Zhou

Publications and source records attributed to Yishan Zhou.

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muT2-NMR: Micro-Scale Correlation Relaxometry for in-situ High-Pressure Nuclear Magnetic Resonance

Over the last decade, frequency-domain in-situ high-pressure nuclear magnetic resonance (NMR) spectroscopy in diamond anvil cells (DACs) has been employed as a structural and electronic probe of condensed matter systems at pressures well into the megabar range. However, extensive spin interactions and sample heterogeneities under pressure often lead to significant spectral overlap, inhibiting independent observation of chemically similar spin sub-species in the same sample. In this work, we introduce a time-domain relaxometry framework specifically suited for DAC experiments, named muT2-NMR. Experimental flexibility and operational robustness are benchmarked on three hydrogen-rich molecular solids at pressures up to 72 GPa. We demonstrate that muT2-NMR can resolve individual molecular subunits in relaxation space, paving the way for novel high-pressure, high-resolution NMR applications in molecular solids.

physics.ins-det

Diffusion Driven Transient Hydrogenation in Metal Superhydrides at Extreme Conditions

In recent years, metal hydride research has become one of the driving forces of the high-pressure community, as it is believed to hold the key to superconductivity close to ambient temperature. While numerous novel metal hydride compounds have been reported and extensively investigated for their superconducting properties, little attention has been focused on the atomic and electronic states of hydrogen, the main ingredient in these novel compounds. Here, we present combined $^{1}H$- and $^{139}La$-NMR data on lanthanum superhydrides, $LaH_{x}$, ($x = 10.2 - 11.1$), synthesized after laser heating at pressures above 160 GPa. Strikingly, we found hydrogen to be in a highly diffusive state at room temperature, with diffusion coefficients in the order of $10^{-6}~cm^2s^{-1}$. We found that this diffusive state of hydrogen results in a dynamic de-hydrogenation of the sample over the course of several weeks, approaching a composition similar to its precursor materials. Quantitative measurements demonstrate that the synthesized superhydrides continuously decompose over time. Transport measurements underline this conclusion as superconducting critical temperatures were found to decrease significantly over time as well. This observation sheds new light on formerly unanswered questions on the long-term stability of metal superhydrides.

cond-mat.mtrl-sci

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