Abstrakti
High-pressure synthesis of denser glass has been a longstanding interest in condensed-matter physics and materials science because of its potentially broad industrial application. Nevertheless, understanding its nature under extreme pressures has yet to be clarified due to experimental and theoretical challenges. Here we reveal the formation of OSi4 tetraclusters associated with that of SiO7 polyhedra in SiO2 glass under ultrahigh pressures to 200 gigapascal confirmed both experimentally and theoretically. Persistent homology analyses with molecular dynamics simulations found increased packing fraction of atoms whose topological diagram at ultrahigh pressures is similar to a pyrite-type crystalline phase, although the formation of tetraclusters is prohibited in the crystalline phase. This critical difference would be caused by the potential structural tolerance in the glass for distortion of oxygen clusters. Furthermore, an expanded electronic band gap demonstrates that chemical bonds survive at ultrahigh pressure. This opens up the synthesis of topologically disordered dense oxide glasses.
| Alkuperäiskieli | Englanti |
|---|---|
| Artikkeli | 045153 |
| Julkaisu | Physical Review B |
| Vuosikerta | 99 |
| Numero | 4 |
| DOI - pysyväislinkit | |
| Tila | Julkaistu - 29 tammik. 2019 |
| OKM-julkaisutyyppi | A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä |
Rahoitus
The synchrotron radiation experiments were performed under the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposals No. 2009A1064, No. 2010A1048, No. 2010B1092, No. 2011A1239, No. 2011B1159, No. 2011B1153, No. 2013B1217). This research was supported by JSPS KAKENHI Grant Nos. JP22684028, JP24654170, JP25247087, JP15KK0148, a Grant for Program Research from Frontier Research Institute for Interdisciplinary Sciences, Tohoku University, and the Start-up funds at ETH Zürich (M.M.). This work was supported by JST PRESTO Grant No. JPMPR15N4, Japan (S.K.) and “Materials research by Information Integration” Initiative (MI2I) project of the Support Program for Starting Up Innovation Hub from JST (S.K., Y.H.) and JST CREST Grant No. 15656429 (Y.H.). The DFT calculations were carried out on the Cray XT4/XT5 computers at CSC, IT Center for Science Ltd., Finland, and Cray XC30 in Japan Advanced Institute of Science and Technology, Japan. J.A., J.K., T.M., and A.S.F. acknowledge financial support from the Academy of Finland through its Centres of Excellence Program (Project No. 284621). M.M. and S.K. designed the research conception. M.M. and N.H. conducted in situ high-pressure synchrotron x-ray diffraction experiments. S.K. performed the atomic structural analyses. H.I. constructed the structural model using MD simulations. N.K. and J.A. contributed to the electronic structural analyses. A.H., Y.H., and I.O. were involved in the topological analyses. T.M., A.S.F., and J.A. tested various parameterizations of the interatomic potentials for MD simulation. N.H. and Y.O. contributed to the optimization of in situ synchrotron x-ray diffraction measurements. Y.O. calculated the OPFs. J.K. and J.A. contributed to the cavity analyses. O.S. and Y.I. were involved in the data analyses for atomic and electronic structures, respectively. The authors declare no conflict of interest.
Julkaisufoorumi-taso
- Jufo-taso 2
!!ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics