Remarkably Stable Glassy GeS 2 Densified at 8.3 GPa: Hidden Polyamorphism, Contrasting Optical Properties, Raman and DFT Studies, and Advanced Applications - Université du Littoral Côte d'Opale Accéder directement au contenu
Article Dans Une Revue Journal of Physical Chemistry B Année : 2023

Remarkably Stable Glassy GeS 2 Densified at 8.3 GPa: Hidden Polyamorphism, Contrasting Optical Properties, Raman and DFT Studies, and Advanced Applications

Andrey Tverjanovich
Oleg Tsiok
  • Fonction : Auteur
Maria Bokova
Arnaud Cuisset

Résumé

Glassy GeS2, densified at 8.3 GPa, exhibits a strongly reduced bandgap, predominantly tetrahedral Ge environment, enhanced chemical disorder and partial 3-fold coordination of both germanium and sulfur, assuming two possible reaction paths under high pressure: (i) a simple dissociation 2Ge–S ⇄ Ge–Ge + S–S and (ii) a chemical disproportionation GeS2 ⇄ GeS + S. The observed electronic and structural changes remain intact for at least seven years under ambient conditions but are gradually evolving upon heating. The relaxation kinetics at elevated temperatures, up to the glass transition temperature Tg, suggests that complete recovery of the densified glassy GeS2 over a typical operational T-range of optoelectronic devices will take many thousands of years. The observed logarithmic relaxation and nearly infinite recovery time at room temperature raise questions about the nature of millennia-long phenomena in densified GeS2. Two alternative explanations will be discussed: (1) hidden polyamorphism and (2) continuous structural and chemical changes under high pressure. These investigations offer valuable insights into the behavior of glassy GeS2 under extreme conditions and its potential applications in optoelectronic devices and other advanced technologies.
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Dates et versions

hal-04295266 , version 1 (20-11-2023)

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Citer

Andrey Tverjanovich, Oleg Tsiok, Vadim Brazhkin, Maria Bokova, Arnaud Cuisset, et al.. Remarkably Stable Glassy GeS 2 Densified at 8.3 GPa: Hidden Polyamorphism, Contrasting Optical Properties, Raman and DFT Studies, and Advanced Applications. Journal of Physical Chemistry B, 2023, 127 (45), pp.9850-9860. ⟨10.1021/acs.jpcb.3c05773⟩. ⟨hal-04295266⟩

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