Investigation of new models pressure-induced amorphization for two distinct topological classes of minerals


For verification of the new amorphization model [M.H. Cohen et al., Journal of Non-Cryst. Solids 307, 602 (2002)] which is considered in
our work, it is necessary to know, whether amorphization results in a change of topology of minerals or it remains the same. It is not generally accepted - within the extensive literature - that there are two distinct classes of materials which could be labelled as pressure amorphized. To the first class, belong a conventional glass, whose atomic structure is not topologically equivalent to any crystalline structure. To the second class, belong the materials with random displacements of the nuclei which do not destroy the crystalline topology. The authors of this new model suppose that since the above distinction has not been clearly made, a general physical picture of the microscopic processes underlying amorphization under pressure has not been available yet. For these two cases, the effective Hamiltonians, describing the elastic deformation energy in terms of atomic displacements will be constructed in a different manner and hence amorphization models should be different.
For gaining a complete understanding of to which on of these two classes belong amorphization substances, we have investigated the
dynamic and the static mechanisms of amorphization of a number of frame minerals subject to the external pressure and, also, to the cation exchange.To reveal universal laws the amorphization mechanisms we investigated phase transitions of some frame minerals in the triclinic structure as an intermediate stage of amorphization. We have shown that transition in the amorphous phase of anorthite, berlinite, quartz, natrolite and edingtonite is described by the common equation, obtained in the process of considering the microscopic model of the phase transition. According to our model in the above-mentioned minerals, one or more branches of the phonon spectrum, connected to the module C44 softens and flattens with increasing pressure. In this case, the calculation of the lattice dynamics shows the following picture of amorphization pressure: The random displacements in the amorphous phase are associated with the incipient instability of at least one nearly flat phonon branch. These random displacements are large enough to eliminate the diffraction picture through reduction of the Debye-Waller factor, but not so large as to distroy the crystal structure topology. In this case, the amorphization arises from a random displacive or orientational transition instead of from a reconstructive transition and the memory of the original topology of the low-pressure crystal structure being retained through the remaining stable branches. For verification whether the memory of the original topology of the crystal structure in the minerals in question is retained or not, the amorphization of natrolite Na2[Al2Si3O10] 2H2O (Khibiny, Kola Peninsula, Russia) end edingtonite Ba[Al2Si3O10] 4H2O (Bohlet, Sweden) was investigated at high pressures up to 11 GPa, using the Raman spectroscopy. It turned out that after release of pressure amorphization, these minerals recover their Raman spectra, suggesting that flat branches of the phonon spectrum hold in the memory about the original topology of the crystal structure, and therefore the new model is suitable for describing the microscopic processes underlying the amorphization of these minerals.