Pressure-induced order–disorder transitions in β-In2S3: an experimental and theoretical study of structural and vibrational properties
Abstract
We report this joint experimental and theoretical study of the structural and vibrational properties of β-In2S3 upon compression shows that this tetragonal defect spinel undergoes two reversible pressure-induced order–disorder transitions up to 20 GPa. We propose that the first high-pressure phase above 5.0 GPa has the cubic defect spinel structure of α-In2S3 and the second high-pressure phase ($$\phi$$-In2S3) above 10.5 GPa has a defect α-NaFeO2-type (R$$\bar{3}$$) structure. This phase, related to the NaCl structure, has not been previously observed in spinels under compression and is related to both the tetradymite structure of topological insulators and to the defect LiTiO2 phase observed at high pressure in other thiospinels. Structural characterization of the three phases shows that α-In2S3 is softer than β-In2S3 while $$\phi$$-In2S3 is harder than β-In2S3. Vibrational characterization of the three phases is also provided, and their Raman-active modes are tentatively assigned. Our work shows that the metastable α phase of In2S3 can be accessed not only by high temperature or varying composition, but also by high pressure. On top of that, the pressure-induced β–α–$$\phi$$ sequence of phase transitions evidences that β-In2S3, a BIII2XV3 compound with an intriguing structure typical of AIIBIII2XVI4 compounds (intermediate between thiospinels and ordered-vacancy compounds) undergoes: (i) a first phase transition at ambient pressure to a disordered spinel-type structure (α-In2S3), isostructural with those found at high pressure and high temperature in other BIII2XV3 compounds; and (ii) a second phase transition to the defect α-NaFeO2-type structure ($$\phi$$-In2S3), a distorted NaCl-type structure that is related to the defect NaCl phase found at high pressure in AIIBIII2XVI4 ordered-vacancy compounds and to the defect LiTiO2-type phase found at high pressure in AIIBIII2XVI4 thiospinels. This result shows that In2S3 (with its intrinsic vacancies) has a similar pressure behaviour to thiospinels and ordered-vacancy compounds of the AIIBIII2XVI4 family, making β-In2S3 the union link between such families of compounds and showing that group-13 thiospinels have more in common with ordered-vacancy compounds than with oxospinels and thiospinels with transition metals.
- Authors:
-
[1];
[1];
[1];
[1];
[3];
[3];
[5];
[6];
[7];
[1]
- Polytechnic University of Valencia (Spain)
- University of Valencia (Spain)
- University of La Laguna, San Cristobal de La Laguna (Spain)
- West Virginia University, Morgantown, WV (United States)
- Uppsala University (Sweden); University of Montreal, QC (Canada)
- Uppsala University (Sweden); Indian Institute of Technology Ropar, Rupnagar (India)
- ALBA-CELLS, MALTA Consolider Team, Barcelona (Spain)
- Publication Date:
- Research Org.:
- West Virginia Univ., Morgantown, WV (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); Spanish Research Agency (AEI); Generalitat Valenciana; National Science Foundation (NSF); Swedish Research Council (SRC)
- OSTI Identifier:
- 1978755
- Grant/Contract Number:
- SC0016176; ACI-105357; 1726534; VR-2016-06014; VR-2020-04410
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 23; Journal Issue: 41; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Gallego-Parra, Samuel, Gomis, Óscar, Vilaplana, Rosario, Cuenca-Gotor, Vanesa Paula, Martínez-García, Domingo, Rodríguez-Hernández, Plácida, Muñoz, Alfonso, Romero, Aldo, Majumdar, Arnab, Ahuja, Rajeev, Popescu, Catalin, and Manjón, Francisco Javier. Pressure-induced order–disorder transitions in β-In2S3: an experimental and theoretical study of structural and vibrational properties. United States: N. p., 2021.
Web. doi:10.1039/d1cp02969j.
Gallego-Parra, Samuel, Gomis, Óscar, Vilaplana, Rosario, Cuenca-Gotor, Vanesa Paula, Martínez-García, Domingo, Rodríguez-Hernández, Plácida, Muñoz, Alfonso, Romero, Aldo, Majumdar, Arnab, Ahuja, Rajeev, Popescu, Catalin, & Manjón, Francisco Javier. Pressure-induced order–disorder transitions in β-In2S3: an experimental and theoretical study of structural and vibrational properties. United States. https://doi.org/10.1039/d1cp02969j
Gallego-Parra, Samuel, Gomis, Óscar, Vilaplana, Rosario, Cuenca-Gotor, Vanesa Paula, Martínez-García, Domingo, Rodríguez-Hernández, Plácida, Muñoz, Alfonso, Romero, Aldo, Majumdar, Arnab, Ahuja, Rajeev, Popescu, Catalin, and Manjón, Francisco Javier. Tue .
"Pressure-induced order–disorder transitions in β-In2S3: an experimental and theoretical study of structural and vibrational properties". United States. https://doi.org/10.1039/d1cp02969j. https://www.osti.gov/servlets/purl/1978755.
@article{osti_1978755,
title = {Pressure-induced order–disorder transitions in β-In2S3: an experimental and theoretical study of structural and vibrational properties},
author = {Gallego-Parra, Samuel and Gomis, Óscar and Vilaplana, Rosario and Cuenca-Gotor, Vanesa Paula and Martínez-García, Domingo and Rodríguez-Hernández, Plácida and Muñoz, Alfonso and Romero, Aldo and Majumdar, Arnab and Ahuja, Rajeev and Popescu, Catalin and Manjón, Francisco Javier},
abstractNote = {We report this joint experimental and theoretical study of the structural and vibrational properties of β-In2S3 upon compression shows that this tetragonal defect spinel undergoes two reversible pressure-induced order–disorder transitions up to 20 GPa. We propose that the first high-pressure phase above 5.0 GPa has the cubic defect spinel structure of α-In2S3 and the second high-pressure phase ($\phi$-In2S3) above 10.5 GPa has a defect α-NaFeO2-type (R$\bar{3}$) structure. This phase, related to the NaCl structure, has not been previously observed in spinels under compression and is related to both the tetradymite structure of topological insulators and to the defect LiTiO2 phase observed at high pressure in other thiospinels. Structural characterization of the three phases shows that α-In2S3 is softer than β-In2S3 while $\phi$-In2S3 is harder than β-In2S3. Vibrational characterization of the three phases is also provided, and their Raman-active modes are tentatively assigned. Our work shows that the metastable α phase of In2S3 can be accessed not only by high temperature or varying composition, but also by high pressure. On top of that, the pressure-induced β–α–$\phi$ sequence of phase transitions evidences that β-In2S3, a BIII2XV3 compound with an intriguing structure typical of AIIBIII2XVI4 compounds (intermediate between thiospinels and ordered-vacancy compounds) undergoes: (i) a first phase transition at ambient pressure to a disordered spinel-type structure (α-In2S3), isostructural with those found at high pressure and high temperature in other BIII2XV3 compounds; and (ii) a second phase transition to the defect α-NaFeO2-type structure ($\phi$-In2S3), a distorted NaCl-type structure that is related to the defect NaCl phase found at high pressure in AIIBIII2XVI4 ordered-vacancy compounds and to the defect LiTiO2-type phase found at high pressure in AIIBIII2XVI4 thiospinels. This result shows that In2S3 (with its intrinsic vacancies) has a similar pressure behaviour to thiospinels and ordered-vacancy compounds of the AIIBIII2XVI4 family, making β-In2S3 the union link between such families of compounds and showing that group-13 thiospinels have more in common with ordered-vacancy compounds than with oxospinels and thiospinels with transition metals.},
doi = {10.1039/d1cp02969j},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 41,
volume = 23,
place = {United States},
year = {Tue Oct 19 00:00:00 EDT 2021},
month = {Tue Oct 19 00:00:00 EDT 2021}
}
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