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LumiLab
Department of Solid State Sciences
Ghent University
Belgium
iCom, Budva, Montenegro
September 4, 2015
Jonas J. Joos, Dirk Poelman, Philippe F. Smet
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Nonequivalent lanthanide defects: energy level modeling
Energy levels, a tool for spectroscopy
1
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
4f2 4f5d CT host*
many-body diagram
Pr3+
Energy levels, a tool for spectroscopy
1
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
4f2 4f5d CT host*
many-body diagram
Pr3+
Energy levels, a tool for spectroscopy
1
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
4f2 4f5d CT host*
many-body diagram
one-electron diagram
Pr3+
Energy levels, a tool for spectroscopy
1
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
4f2 4f5d CT host*
many-body diagram
one-electron diagram
charge-state transition level
Pr3+
Empirical energy level schemes
2
CaGa2S4
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Empirical energy level schemes
2
CaGa2S4
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Empirical energy level schemes
2
CaGa2S4
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
easy!
Multiple defects
3
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Easy: All lanthanide ions do the same
example: CaGa2S4
Harder: All lanthanides do the same
example: SrAl2O4
Hard: Some lanthanides act “special”
example: SrGa2S4
Sr1 Sr2
Eu2+ Ce3+
Multiple defects
3
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Easy: All lanthanide ions do the same
example: CaGa2S4
Harder: All lanthanides do the same
example: SrAl2O4
Hard: Some lanthanides act “special”
example: SrGa2S4
Sr1 Sr2
Eu2+ Ce3+
Site-selective PL spectroscopy
4
Eu2+
J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
Sr1 Sr2
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Site-selective PL spectroscopy
4
Eu2+
Ce3+
D. D. Jia, J. Lumin. 117, 170 (2006)
Sr1 Sr2
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Site-selective PL spectroscopy
4 J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
VB
Eu2+
Ce3+
Eu3+
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Site-selective PL spectroscopy
4 J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
VB
vacuum
EuSr1 EuSr2
Eu2+
Ce3+
Eu3+ Sr1 Sr2
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Two-site energy level scheme
5
Trivalent lanthanides
Sr1
Sr2
J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Two-site energy level scheme
6
Divalent lanthanides
Sr1
Sr2
Sr1
Sr2
J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Two-site energy level scheme
7
Divalent lanthanides
J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Sr1
Sr2
Two-site energy level scheme
7
Divalent lanthanides
J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014)
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Multiple defects
3
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Easy: All lanthanide ions do the same
example: CaGa2S4
Harder: All lanthanides do the same
example: SrAl2O4
Hard: Some lanthanides act “special”
example: SrGa2S4
Sr1 Sr2
Eu2+ Ce3+
Multiple defects
3
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Easy: All lanthanide ions do the same
example: CaGa2S4
Harder: All lanthanides do the same
example: SrAl2O4
Hard: Some lanthanides act “special”
example: SrGa2S4
Sr1 Sr2
Eu2+ Ce3+
PL spectroscopy Eu2+ and Ce3+
8
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
energy (eV)
PL spectroscopy Eu2+ and Ce3+
8
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
energy (eV)
PL spectroscopy Eu2+ and Ce3+
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
8 energy (eV)
PL spectroscopy Eu2+ and Ce3+
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
8 energy (eV)
PL spectroscopy Eu2+ and Ce3+
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
8 energy (eV)
PL spectroscopy Eu2+ and Ce3+
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
8 energy (eV)
PL spectroscopy Eu2+ and Ce3+
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
8 energy (eV)
Local environment from EPR
9
SrGa2S4:Eu2+ SrGa2S4:Ce3+
W. L. Warren et al., Appl. Phys. Lett. 70, 478 (1997)
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
SrGa2S4:Ce3+
Repercussions on E-level scheme
10
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Repercussions on E-level scheme
10
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Multiple defects
3
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Easy: All lanthanide ions do the same
example: CaGa2S4
Harder: All lanthanides do the same
example: SrAl2O4
Hard: Some lanthanides act “special”
example: SrGa2S4
Sr1 Sr2
Eu2+ Ce3+
Conclusions
11
Realistic materials often require more complex models
Very distinct experimental features burried in uncertainty intervals
General physical insight most important merit
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
LumiLab
Department of Solid State Sciences
Ghent University
Belgium
iCom, Budva, Montenegro
September 4, 2015
Jonas J. Joos, Dirk Poelman, Philippe F. Smet
Jonas Joos Nonequivalent lanthanide defects: energy level modeling
Nonequivalent lanthanide defects: energy level modeling

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Nonequivalent lanthanide defects: energy level modeling

  • 1. LumiLab Department of Solid State Sciences Ghent University Belgium iCom, Budva, Montenegro September 4, 2015 Jonas J. Joos, Dirk Poelman, Philippe F. Smet Jonas Joos Nonequivalent lanthanide defects: energy level modeling Nonequivalent lanthanide defects: energy level modeling
  • 2. Energy levels, a tool for spectroscopy 1 Jonas Joos Nonequivalent lanthanide defects: energy level modeling 4f2 4f5d CT host* many-body diagram Pr3+
  • 3. Energy levels, a tool for spectroscopy 1 Jonas Joos Nonequivalent lanthanide defects: energy level modeling 4f2 4f5d CT host* many-body diagram Pr3+
  • 4. Energy levels, a tool for spectroscopy 1 Jonas Joos Nonequivalent lanthanide defects: energy level modeling 4f2 4f5d CT host* many-body diagram one-electron diagram Pr3+
  • 5. Energy levels, a tool for spectroscopy 1 Jonas Joos Nonequivalent lanthanide defects: energy level modeling 4f2 4f5d CT host* many-body diagram one-electron diagram charge-state transition level Pr3+
  • 6. Empirical energy level schemes 2 CaGa2S4 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 7. Empirical energy level schemes 2 CaGa2S4 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 8. Empirical energy level schemes 2 CaGa2S4 Jonas Joos Nonequivalent lanthanide defects: energy level modeling easy!
  • 9. Multiple defects 3 Jonas Joos Nonequivalent lanthanide defects: energy level modeling Easy: All lanthanide ions do the same example: CaGa2S4 Harder: All lanthanides do the same example: SrAl2O4 Hard: Some lanthanides act “special” example: SrGa2S4 Sr1 Sr2 Eu2+ Ce3+
  • 10. Multiple defects 3 Jonas Joos Nonequivalent lanthanide defects: energy level modeling Easy: All lanthanide ions do the same example: CaGa2S4 Harder: All lanthanides do the same example: SrAl2O4 Hard: Some lanthanides act “special” example: SrGa2S4 Sr1 Sr2 Eu2+ Ce3+
  • 11. Site-selective PL spectroscopy 4 Eu2+ J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) Sr1 Sr2 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 12. Site-selective PL spectroscopy 4 Eu2+ Ce3+ D. D. Jia, J. Lumin. 117, 170 (2006) Sr1 Sr2 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 13. Site-selective PL spectroscopy 4 J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) VB Eu2+ Ce3+ Eu3+ Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 14. Site-selective PL spectroscopy 4 J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) VB vacuum EuSr1 EuSr2 Eu2+ Ce3+ Eu3+ Sr1 Sr2 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 15. Two-site energy level scheme 5 Trivalent lanthanides Sr1 Sr2 J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 16. Two-site energy level scheme 6 Divalent lanthanides Sr1 Sr2 Sr1 Sr2 J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 17. Two-site energy level scheme 7 Divalent lanthanides J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) Jonas Joos Nonequivalent lanthanide defects: energy level modeling Sr1 Sr2
  • 18. Two-site energy level scheme 7 Divalent lanthanides J. Botterman, J. J. Joos, P. F. Smet, Phys. Rev. B 90, 085147 (2014) Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 19. Multiple defects 3 Jonas Joos Nonequivalent lanthanide defects: energy level modeling Easy: All lanthanide ions do the same example: CaGa2S4 Harder: All lanthanides do the same example: SrAl2O4 Hard: Some lanthanides act “special” example: SrGa2S4 Sr1 Sr2 Eu2+ Ce3+
  • 20. Multiple defects 3 Jonas Joos Nonequivalent lanthanide defects: energy level modeling Easy: All lanthanide ions do the same example: CaGa2S4 Harder: All lanthanides do the same example: SrAl2O4 Hard: Some lanthanides act “special” example: SrGa2S4 Sr1 Sr2 Eu2+ Ce3+
  • 21. PL spectroscopy Eu2+ and Ce3+ 8 Jonas Joos Nonequivalent lanthanide defects: energy level modeling energy (eV)
  • 22. PL spectroscopy Eu2+ and Ce3+ 8 Jonas Joos Nonequivalent lanthanide defects: energy level modeling energy (eV)
  • 23. PL spectroscopy Eu2+ and Ce3+ Jonas Joos Nonequivalent lanthanide defects: energy level modeling 8 energy (eV)
  • 24. PL spectroscopy Eu2+ and Ce3+ Jonas Joos Nonequivalent lanthanide defects: energy level modeling 8 energy (eV)
  • 25. PL spectroscopy Eu2+ and Ce3+ Jonas Joos Nonequivalent lanthanide defects: energy level modeling 8 energy (eV)
  • 26. PL spectroscopy Eu2+ and Ce3+ Jonas Joos Nonequivalent lanthanide defects: energy level modeling 8 energy (eV)
  • 27. PL spectroscopy Eu2+ and Ce3+ Jonas Joos Nonequivalent lanthanide defects: energy level modeling 8 energy (eV)
  • 28. Local environment from EPR 9 SrGa2S4:Eu2+ SrGa2S4:Ce3+ W. L. Warren et al., Appl. Phys. Lett. 70, 478 (1997) Jonas Joos Nonequivalent lanthanide defects: energy level modeling SrGa2S4:Ce3+
  • 29. Repercussions on E-level scheme 10 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 30. Repercussions on E-level scheme 10 Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 31. Multiple defects 3 Jonas Joos Nonequivalent lanthanide defects: energy level modeling Easy: All lanthanide ions do the same example: CaGa2S4 Harder: All lanthanides do the same example: SrAl2O4 Hard: Some lanthanides act “special” example: SrGa2S4 Sr1 Sr2 Eu2+ Ce3+
  • 32. Conclusions 11 Realistic materials often require more complex models Very distinct experimental features burried in uncertainty intervals General physical insight most important merit Jonas Joos Nonequivalent lanthanide defects: energy level modeling
  • 33. LumiLab Department of Solid State Sciences Ghent University Belgium iCom, Budva, Montenegro September 4, 2015 Jonas J. Joos, Dirk Poelman, Philippe F. Smet Jonas Joos Nonequivalent lanthanide defects: energy level modeling Nonequivalent lanthanide defects: energy level modeling