JOURNAL OF CHEMICAL PHYSICS, cilt.137, sa.22, 2012 (SCI-Expanded)
Pressure induced densification in a molecular arsenic sulfide glass is studied at ambient temperature using x-ray scattering, absorption and Raman spectroscopic techniques in situ in a diamond anvil cell. The relatively abrupt changes in the position of the first sharp diffraction peak, FSDP, and the pressure-volume equation of state near similar to 2 GPa suggest a phase transition between low-and high-density amorphous phases characterized by different densification mechanisms and rates. Raman spectroscopic results provide clear evidence that the phase transition corresponds to a topological transformation between a low-density molecular structure and a high-density network structure via opening of the constituent As4S3 cage molecules and bond switching. Pressure induced mode softening of the high density phase suggests a low dimensional nature of the network. The phase transformation is hysteretically reversible, and therefore, reminiscent of a first-order phase transition. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4769794]