Stressed Atoms and Their Recover. Charge Density Redistribution With Pressure in a Zeolite Framework

Abstract

Abstract As a result of external stress applied to crystals, ions relax, in addition to shortening the bond lengths, by changing their shape and volume. Modern mineralogy is founded on spherical ions/atoms, i.e. the close packing of spheres, ionic/atomic radii, and Pauling and Goldschmidt rules. More advanced, quantum crystallography has led to detailed quantitative studies of electron density in minerals. Here we innovatively apply it to high pressure studies up to 4.2 GPa of the mineral hsianghualite. With external stress, electron density redistributes inside ions and among them. For most ions, atomic volumes decrease; however, for silicon atomic volume increases. With growing pressure, we observed the higher contraction of cations in bonding directions, but a slighter expansion towards nonbonding directions. It is possible to trace the spatial redistribution of the electron density in ions even at the level of hundredths parts of an electron per cubic angstrom. This opens a new perspective to experimentally characterise mineral processes in the Earth’s mantle. The use of diamond anvil cells with quantum crystallography offer more than interatomic distances and elastic properties of minerals. Interactions, energetic features, a branch so far reserved only to the first principle DFT calculations at ultra-high pressures, become available experimentally.