Spectral proxies for bonding transitions in 
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 and 
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 polymorphs at high pressure up to 270 GPa by O 
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-edge x-ray Raman scatte

Yi, Yoo Soo; Khim, Hoon; Kim, Yong-Hyun; Lee, Sung Keun

doi:10.1103/physrevb.103.214109

Cited by 9 publications

(42 citation statements)

References 69 publications

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“…We note that the full optimization of all atomic positions at constant volume may lead to an unwanted relaxation of the amorphous structures, reducing the extent of topological variation. Calculations of 25 Mg, 17 O, and 29 Si NMR parameters were carried out with the GIPAW method, implemented in CASTEP. 68,86,87 The electronic interactions were represented with on-the-fly ultrasoft pseudopotential.…”

Section: Methodsmentioning

confidence: 99%

“…[39,[43][44][45][46][47][48][49] and references therein). We note that the residual second-order quadrupolar interaction is often predominant in the one-dimensional MAS NMR spectrum involving quadrupolar nuclides (spin >1/2, e.g., 17 O and 25 Mg) in diverse noncrystalline oxides (e.g., Refs. [50,51]).…”

Section: Introductionmentioning

confidence: 96%

“…[22, 23] and references therein). Advances in element‐specific nonresonant inelastic X‐ray scattering (IXS) revealed the densification of MgSiO 3 glass, suggesting the formation of tricluster oxygen and related changes in medium‐range structures above 20 GPa 8 and the reduction of O–O distance up to 130 GPa 24,25 . However, overlap among the binary correlation functions in the pair distribution functions (from X‐ray and neutron scattering) of oxide glasses is more prevalent at elevated pressure conditions.…”

Section: Introductionmentioning

confidence: 99%

“…Furthermore, the experimental NMR investigation of MgSiO 3 poses an additional challenge due to pronounced structural disorder intrinsic to Mg-bearing glasses, leading to substantial NMR peak broadening. 67 Therefore, the nature of nuclear spin interactions involving 17 O, 25 Mg, and 29 Si under extreme compression is not known.…”

Section: Introductionmentioning

confidence: 99%

“…[6,24,80,81]), these two ab initio techniques can be combined to reveal the hidden nature of nuclear spins under extreme compression. This study explores the evolution of MgSiO 3 glasses under pressure above 1.5 Mbar based on ab initio calculations of the NMR parameters of 25 Mg, 29 Si, and 17 O to unravel the detailed nature of bonding transitions and nuclear spin interactions under compression. We develop solid-state NMR protocols operating at high pressure, from which the densification mechanisms of oxide glasses and the unique properties of the compressed melts and glasses under compression can be inferred.…”

Section: Introductionmentioning

confidence: 99%

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Structure and disorder in MgSiO₃ glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Lee

Parq

et al. 2022

J Am Ceram Soc.

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The structural modifications in oxide glasses under extreme compression may account for the pressure‐induced increase in their mechanical toughness and rigidity, rendering potential for technological applications of the compressed glasses. High‐resolution solid‐state nuclear magnetic resonance has provided a structural information regarding glasses by identifying how nuclear spins behave and interact with nearby elements. However, knowledge of nuclear spins resonance in oxide glasses under extreme pressure above 1 million atmospheres has not been available, making the origins of glass densification illusive. In this article, ab initio calculations of prototypical magnesium silicate glasses quantify how structural changes in glasses affect the nature of nuclear spin interactions at high pressure beyond megabars. The calculated results establish novel correlations between pressure‐induced evolution of atomic structures, such as oxygen and cation coordination numbers, bond angle and lengths, and structurally relevant nuclear magnetic resonance parameters for Mg, Si, and O in compressed oxide glasses above megabar pressures. The established correlations highlight that the nuclear spins in glasses can serve as a new indicator to the extreme densification paths. Pressure‐induced dispersion in nuclear spin parameters also reveals an overall increase in the topological entropy. This entropy gain may weaken glasses at an elevated pressure conditions, accounting for potential softening of the compressed glasses. The proposed relationships open a new window to the evolution of diverse complex glasses under extreme stress and compression with high‐resolution solid‐state nuclear magnetic resonance.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 96%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Structure and disorder in MgSiO₃ glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Lee

Parq

et al. 2022

J Am Ceram Soc.

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Polymeric nitrogen: A review of experimental synthesis method, structure properties and lattice dynamic characterization from large scientific facilities and extreme spectroscopy perspectives

Lei,

Liu,

Zhang

2023

Energetic Materials Frontiers

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Reductive Adsorption of Atmospheric Oxidized Mercury on Ice: Insights from Density Functional Calculations

Han

Hur

2021

ACS Earth Space Chem.

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The fate of atmospheric mercury (Hg) has been intensively investigated due to concerns about its global dispersion. The reduction of reactive oxidized Hg (Hg II ) to the stable form (Hg 0 ) is a significant process, in that it extends the mean atmospheric lifetime of Hg and allows for its long-range transport. While the reduction mechanisms of Hg II in aqueous, particulate, and gas phases have drawn much attention, the reaction pathway and mechanism of Hg II reduction in icy environments are still elusive, despite that ice particles have been expected to play an active role, from field and laboratory observations. With density functional theory calculations, we reveal the adsorptive and dissociative pathways of Hg II on ice, including the catalytic role of the ice surface that facilitates the dissociative adsorption of Hg dihalides. Because ice is the most common phase of water in the upper atmosphere and cryosphere, its influence on Hg speciation can have profound implications on the global Hg cycle.

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Spectral proxies for bonding transitions in SiO2 and MgSiO3 polymorphs at high pressure up to 270 GPa by O K -edge x-ray Raman scatte

Cited by 9 publications

References 69 publications

Structure and disorder in MgSiO₃ glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Structure and disorder in MgSiO₃ glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Polymeric nitrogen: A review of experimental synthesis method, structure properties and lattice dynamic characterization from large scientific facilities and extreme spectroscopy perspectives

Reductive Adsorption of Atmospheric Oxidized Mercury on Ice: Insights from Density Functional Calculations

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Spectral proxies for bonding transitions in SiO2 and MgSiO3 polymorphs at high pressure up to 270 GPa by O K -edge x-ray Raman scatte

Cited by 9 publications

References 69 publications

Structure and disorder in MgSiO3 glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Structure and disorder in MgSiO3 glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Polymeric nitrogen: A review of experimental synthesis method, structure properties and lattice dynamic characterization from large scientific facilities and extreme spectroscopy perspectives

Reductive Adsorption of Atmospheric Oxidized Mercury on Ice: Insights from Density Functional Calculations

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Product

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Structure and disorder in MgSiO₃ glasses above megabar pressures via nuclear magnetic resonance: DFT calculations

Structure and disorder in MgSiO₃ glasses above megabar pressures via nuclear magnetic resonance: DFT calculations