Pressure-Driven Chemical Disorder in Glassy As2S3 up to 14.7 GPa, Postdensification Effects, and Applications in Materials Design
[2];
[5]
- Arizona State Univ., Mesa, AZ (United States). The Eyring Materials Center
- Russian Academy of Sciences (RAS), Moscow (Russia). Inst. for High Pressure Physics
- St. Petersburg State Univ. (Russia). Dept. of Chemistry
- European Synchrotron Radiation Facility (ESRF), Grenoble (France)
- Univ. du Littoral Côte d’Opale, Dunkerque (France). LPCA
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
A small difference in energy between homopolar and heteropolar bonds and the glass-forming ability of pure chalcogens leads to unexpected trends in densification mechanisms of glassy chalcogenides compared to vitreous oxides. Using high-precision compressibility measurements and in situ high-energy X-ray diffraction up to 14.7 GPa, we show herein a new densification route in a canonical glass As2S3. After the first reversible elastic step with a maximum pressure of 1.3 GPa, characterized by a strong reduction of voids and cavities, a significant bonding or chemical disorder is developed under higher pressure, reaching a saturation of 30% in the population of As-As bonds above 8-9 GPa. The pressure-driven chemical disorder is accompanied by a remarkable structural relaxation and a strongly diminished optical gap and determines structural, vibrational, and optical properties under and after cold compression. The decompressed recovered glass conserves a dark color and exhibits two relaxation processes: (a) fast (a few days) and (b) slow (months/years at room temperature). The enhanced refractive index of the recovered glass is promising for optical applications with improved functionalities. A nearly permanent red shift in optical absorption after decompression can be used in high-impact-force optical sensors.
- Research Organization:
- Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Région Hauts de France; Ministère de l’Enseignement Supérieur et de la Recherche (CPER Climibio); European Fund for Regional Economic Development; Russian Science Foundation; Saint- Petersburg State University; Grand Equipment National de Calcul Intensif (GENCI)
- Grant/Contract Number:
- AC02-06CH11357; 19-12-00111; 12.40.1342.2017; 2018-A0050910639
- OSTI ID:
- 1604982
- Journal Information:
- Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 124, Issue 2; ISSN 1520-6106
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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