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First-principles study of antisite defect configurations in ZnGa2O4:Cr persistent phosphors

Arthur De Vos (UGent) , Kurt Lejaeghere (UGent) , Danny Vanpoucke (UGent) , Jonas Joos (UGent) , Philippe Smet (UGent) and Karen Hemelsoet (UGent)
(2016) INORGANIC CHEMISTRY. 55(5). p.2402-2412
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Abstract
Zinc gallate doped with chromium is a recently developed near-infrared emitting persistent phosphor, which is now extensively studied for in vivo bioimaging and security applications. The precise mechanism of this persistent luminescence relies on defects, in particular, on antisite defects and antisite pairs. A theoretical model combining the solid host, the dopant, and/or antisite defects is constructed to elucidate the mutual interactions in these complex materials. Energies of formation as well as dopant, and defect energies are calculated through density-functional theory simulations of large periodic supercells. The calculations support the chromium substitution on the slightly distorted octahedrally coordinated gallium site, and additional energy levels are introduced in the band gap of the host. Antisite pairs are found to be energetically favored over isolated antisites due to significant charge compensation as shown by calculated Hirshfeld-I charges. Significant structural distortions are found around all antisite defects. The local Cr surrounding is mainly distorted due to a Zn-Ga antisite. The stability analysis reveals that the distance between both antisites dominates the overall stability picture of the material containing the Cr dopant and an antisite pair. The findings are further rationalized using calculated densities of states and Hirshfeld-I charges.
Keywords
EXTENDING HIRSHFELD-I, DENSITY-FUNCTIONAL THEORY, AUGMENTED-WAVE METHOD, DOPED ZINC GALLATE, PERIODIC MATERIALS, HIGH-BRIGHTNESS, VISIBLE-LIGHT, MN4+ EMISSION, LUMINESCENCE, ELECTRON

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Chicago
De Vos, Arthur, Kurt Lejaeghere, Danny Vanpoucke, Jonas Joos, Philippe Smet, and Karen Hemelsoet. 2016. “First-principles Study of Antisite Defect Configurations in ZnGa2O4:Cr Persistent Phosphors.” Inorganic Chemistry 55 (5): 2402–2412.
APA
De Vos, Arthur, Lejaeghere, K., Vanpoucke, D., Joos, J., Smet, P., & Hemelsoet, K. (2016). First-principles study of antisite defect configurations in ZnGa2O4:Cr persistent phosphors. INORGANIC CHEMISTRY, 55(5), 2402–2412.
Vancouver
1.
De Vos A, Lejaeghere K, Vanpoucke D, Joos J, Smet P, Hemelsoet K. First-principles study of antisite defect configurations in ZnGa2O4:Cr persistent phosphors. INORGANIC CHEMISTRY. 2016;55(5):2402–12.
MLA
De Vos, Arthur, Kurt Lejaeghere, Danny Vanpoucke, et al. “First-principles Study of Antisite Defect Configurations in ZnGa2O4:Cr Persistent Phosphors.” INORGANIC CHEMISTRY 55.5 (2016): 2402–2412. Print.
@article{7171939,
  abstract     = {Zinc gallate doped with chromium is a recently developed near-infrared emitting persistent phosphor, which is now extensively studied for in vivo bioimaging and security applications. The precise mechanism of this persistent luminescence relies on defects, in particular, on antisite defects and antisite pairs. A theoretical model combining the solid host, the dopant, and/or antisite defects is constructed to elucidate the mutual interactions in these complex materials. Energies of formation as well as dopant, and defect energies are calculated through density-functional theory simulations of large periodic supercells. The calculations support the chromium substitution on the slightly distorted octahedrally coordinated gallium site, and additional energy levels are introduced in the band gap of the host. Antisite pairs are found to be energetically favored over isolated antisites due to significant charge compensation as shown by calculated Hirshfeld-I charges. Significant structural distortions are found around all antisite defects. The local Cr surrounding is mainly distorted due to a Zn-Ga antisite. The stability analysis reveals that the distance between both antisites dominates the overall stability picture of the material containing the Cr dopant and an antisite pair. The findings are further rationalized using calculated densities of states and Hirshfeld-I charges.},
  author       = {De Vos, Arthur and Lejaeghere, Kurt and Vanpoucke, Danny and Joos, Jonas and Smet, Philippe and Hemelsoet, Karen},
  issn         = {0020-1669},
  journal      = {INORGANIC CHEMISTRY},
  keyword      = {EXTENDING HIRSHFELD-I,DENSITY-FUNCTIONAL THEORY,AUGMENTED-WAVE METHOD,DOPED ZINC GALLATE,PERIODIC MATERIALS,HIGH-BRIGHTNESS,VISIBLE-LIGHT,MN4+ EMISSION,LUMINESCENCE,ELECTRON},
  language     = {eng},
  number       = {5},
  pages        = {2402--2412},
  title        = {First-principles study of antisite defect configurations in ZnGa2O4:Cr persistent phosphors},
  url          = {http://dx.doi.org/10.1021/acs.inorgchem.5b02805},
  volume       = {55},
  year         = {2016},
}

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