Abstract

Transparent, Crack-free and dense M′-type LuTaO4:Ln3+ (Ln = Eu, Tb) scintillator films have been successfully prepared by Pechini sol-gel technique. The structure, morphology, photoluminescence and X-ray excited luminescence (XEL) of the films were investigated in detail. The optical band gap of the LuTaO4 thin film was experimentally determined for the first time. Eu3+ or Tb3+ activated M′-type LuTaO4 thin films exhibited intensive 5D07F2 or 5D47F5 emission, corresponding to the decay time of 1.08 ms or 1.10 ms, respectively. It was demonstrated that the sol-gel derived M′-type LuTaO4:Ln3+ (Ln = Eu, Tb) scintillator films have a superior XEL performance, which indicates that this new type of scintillator film is expected to be a promising candidate for applications in high-spatial-resolution X-ray imaging.

© 2014 Optical Society of America

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  1. A. Koch, C. Raven, P. Spanne, and A. Snigirev, “X-ray imaging with submicrometer resolution employing transparent luminescent screens,” J. Opt. Soc. Am. A15(7), 1940–1951 (1998).
    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  18. B. Judd, “Optical absorption intensities of rare-earth ions,” Phys. Rev.127(3), 750–761 (1962).
    [CrossRef]
  19. G. S. Ofelt, “Intensities of crystal spectra of rare-earth ions,” J. Chem. Phys.37(3), 511–520 (1962).
    [CrossRef]

2013

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

2010

2009

2008

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

2007

J. Nedelec, “Sol-gel processing of nanostructured inorganic scintillating materials,” J. Nanomater.2007, 1–8 (2007).
[CrossRef]

2006

M. Nikl, “Scintillation detectors for x-rays,” Meas. Sci. Technol.17(4), R37–R54 (2006).
[CrossRef]

T. Martin and A. Koch, “Recent developments in X-ray imaging with micrometer spatial resolution,” J. Synchrotron Radiat.13(2), 180–194 (2006).
[CrossRef] [PubMed]

2004

C. Mansuy, J. M. Nedelec, and R. Mahiou, “Molecular design of inorganic scintillators: from alkoxides to scintillating materials,” J. Mater. Chem.14(21), 3274–3280 (2004).
[CrossRef]

M. J. Lambregts and S. Frank, “Application of Vegard’s law to mixed cation sodalites: a simple method for determining the stoichiometry,” Talanta62(3), 627–630 (2004).
[CrossRef] [PubMed]

1998

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

A. Koch, C. Raven, P. Spanne, and A. Snigirev, “X-ray imaging with submicrometer resolution employing transparent luminescent screens,” J. Opt. Soc. Am. A15(7), 1940–1951 (1998).
[CrossRef]

1995

S. Issler and C. Torardi, “Solid state chemistry and luminescence of X-ray phosphors,” J. Alloy. Comp.229(1), 54–65 (1995).
[CrossRef]

1994

G. Blasse, G. Dirksen, L. H. Brixner, and M. K. Crawford, “Luminescence of materials based on LuTaO4,” J. Alloy. Comp.209(1-2), 1–6 (1994).
[CrossRef]

1983

L. Brixner and H. Chen, “On the structural and luminescent properties of the M' LnTaO4 rare earth tantalates,” J. Electrochem. Soc.130(12), 2435–2443 (1983).
[CrossRef]

1966

G. Blasse, A. Bril, and W. Nieuwpoort, “On the Eu3+ fluorescence in mixed metal oxides: Part I-The crystal structure sensitivity of the intensity ratio of electric and magnetic dipole emission,” J. Phys. Chem. Solids27(10), 1587–1592 (1966).
[CrossRef]

1962

B. Judd, “Optical absorption intensities of rare-earth ions,” Phys. Rev.127(3), 750–761 (1962).
[CrossRef]

G. S. Ofelt, “Intensities of crystal spectra of rare-earth ions,” J. Chem. Phys.37(3), 511–520 (1962).
[CrossRef]

Bae, K. M.

Blasse, G.

G. Blasse, G. Dirksen, L. H. Brixner, and M. K. Crawford, “Luminescence of materials based on LuTaO4,” J. Alloy. Comp.209(1-2), 1–6 (1994).
[CrossRef]

G. Blasse, A. Bril, and W. Nieuwpoort, “On the Eu3+ fluorescence in mixed metal oxides: Part I-The crystal structure sensitivity of the intensity ratio of electric and magnetic dipole emission,” J. Phys. Chem. Solids27(10), 1587–1592 (1966).
[CrossRef]

Bril, A.

G. Blasse, A. Bril, and W. Nieuwpoort, “On the Eu3+ fluorescence in mixed metal oxides: Part I-The crystal structure sensitivity of the intensity ratio of electric and magnetic dipole emission,” J. Phys. Chem. Solids27(10), 1587–1592 (1966).
[CrossRef]

Brixner, L.

L. Brixner and H. Chen, “On the structural and luminescent properties of the M' LnTaO4 rare earth tantalates,” J. Electrochem. Soc.130(12), 2435–2443 (1983).
[CrossRef]

Brixner, L. H.

G. Blasse, G. Dirksen, L. H. Brixner, and M. K. Crawford, “Luminescence of materials based on LuTaO4,” J. Alloy. Comp.209(1-2), 1–6 (1994).
[CrossRef]

Chen, H.

L. Brixner and H. Chen, “On the structural and luminescent properties of the M' LnTaO4 rare earth tantalates,” J. Electrochem. Soc.130(12), 2435–2443 (1983).
[CrossRef]

Chen, S.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

Cheng, B. M.

Chiu, Y. C.

Courtheoux, L.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Crawford, M. K.

G. Blasse, G. Dirksen, L. H. Brixner, and M. K. Crawford, “Luminescence of materials based on LuTaO4,” J. Alloy. Comp.209(1-2), 1–6 (1994).
[CrossRef]

Den, T.

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

Dirksen, G.

G. Blasse, G. Dirksen, L. H. Brixner, and M. K. Crawford, “Luminescence of materials based on LuTaO4,” J. Alloy. Comp.209(1-2), 1–6 (1994).
[CrossRef]

Entine, G.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

Frank, S.

M. J. Lambregts and S. Frank, “Application of Vegard’s law to mixed cation sodalites: a simple method for determining the stoichiometry,” Talanta62(3), 627–630 (2004).
[CrossRef] [PubMed]

Gu, M.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

Gupta, T.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

Huang, S.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

Issler, S.

S. Issler and C. Torardi, “Solid state chemistry and luminescence of X-ray phosphors,” J. Alloy. Comp.229(1), 54–65 (1995).
[CrossRef]

Jallot, E.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Jang, S. M.

Judd, B.

B. Judd, “Optical absorption intensities of rare-earth ions,” Phys. Rev.127(3), 750–761 (1962).
[CrossRef]

Jung, P. G.

Kim, H. K.

Kinowski, C.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Klugerman, Y.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

Ko, J. S.

Koch, A.

T. Martin and A. Koch, “Recent developments in X-ray imaging with micrometer spatial resolution,” J. Synchrotron Radiat.13(2), 180–194 (2006).
[CrossRef] [PubMed]

A. Koch, C. Raven, P. Spanne, and A. Snigirev, “X-ray imaging with submicrometer resolution employing transparent luminescent screens,” J. Opt. Soc. Am. A15(7), 1940–1951 (1998).
[CrossRef]

Lambregts, M. J.

M. J. Lambregts and S. Frank, “Application of Vegard’s law to mixed cation sodalites: a simple method for determining the stoichiometry,” Talanta62(3), 627–630 (2004).
[CrossRef] [PubMed]

Lao, J.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Laquerriere, P.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Lee, C. H.

Lee, J. M.

Lee, S. M.

Lim, C. H.

Lin, C. C.

Liu, B.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

Liu, R. S.

Liu, W. R.

Liu, X.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

Mahiou, R.

C. Mansuy, J. M. Nedelec, and R. Mahiou, “Molecular design of inorganic scintillators: from alkoxides to scintillating materials,” J. Mater. Chem.14(21), 3274–3280 (2004).
[CrossRef]

Mansuy, C.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

C. Mansuy, J. M. Nedelec, and R. Mahiou, “Molecular design of inorganic scintillators: from alkoxides to scintillating materials,” J. Mater. Chem.14(21), 3274–3280 (2004).
[CrossRef]

Martin, T.

T. Martin and A. Koch, “Recent developments in X-ray imaging with micrometer spatial resolution,” J. Synchrotron Radiat.13(2), 180–194 (2006).
[CrossRef] [PubMed]

Miller, S.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

Nagarkar, V.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

Nedelec, J.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

J. Nedelec, “Sol-gel processing of nanostructured inorganic scintillating materials,” J. Nanomater.2007, 1–8 (2007).
[CrossRef]

Nedelec, J. M.

C. Mansuy, J. M. Nedelec, and R. Mahiou, “Molecular design of inorganic scintillators: from alkoxides to scintillating materials,” J. Mater. Chem.14(21), 3274–3280 (2004).
[CrossRef]

Ni, C.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

Nieuwpoort, W.

G. Blasse, A. Bril, and W. Nieuwpoort, “On the Eu3+ fluorescence in mixed metal oxides: Part I-The crystal structure sensitivity of the intensity ratio of electric and magnetic dipole emission,” J. Phys. Chem. Solids27(10), 1587–1592 (1966).
[CrossRef]

Nikl, M.

M. Nikl, “Scintillation detectors for x-rays,” Meas. Sci. Technol.17(4), R37–R54 (2006).
[CrossRef]

Ofelt, G. S.

G. S. Ofelt, “Intensities of crystal spectra of rare-earth ions,” J. Chem. Phys.37(3), 511–520 (1962).
[CrossRef]

Ohashi, Y.

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

Raven, C.

Renaudin, G.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Snigirev, A.

Spanne, P.

Squillante, M.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

Torardi, C.

S. Issler and C. Torardi, “Solid state chemistry and luminescence of X-ray phosphors,” J. Alloy. Comp.229(1), 54–65 (1995).
[CrossRef]

Turrell, S.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

Yasui, N.

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

Yeh, Y. T.

Yokota, Y.

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

Yoshikawa, A.

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

Yun, S.

Appl. Phys. Lett.

Y. Ohashi, N. Yasui, Y. Yokota, A. Yoshikawa, and T. Den, “Submicron-diameter phase-separated scintillator fibers for high-resolution X-ray imaging,” Appl. Phys. Lett.102(5), 051907 (2013).
[CrossRef]

IEEE Trans. Nucl. Sci.

V. Nagarkar, T. Gupta, S. Miller, Y. Klugerman, M. Squillante, and G. Entine, “Structured CsI(Tl) Scintillators for X-ray Imaging Applications,” IEEE Trans. Nucl. Sci.45(3), 492–496 (1998).
[CrossRef]

J. Alloy. Comp.

S. Issler and C. Torardi, “Solid state chemistry and luminescence of X-ray phosphors,” J. Alloy. Comp.229(1), 54–65 (1995).
[CrossRef]

G. Blasse, G. Dirksen, L. H. Brixner, and M. K. Crawford, “Luminescence of materials based on LuTaO4,” J. Alloy. Comp.209(1-2), 1–6 (1994).
[CrossRef]

J. Chem. Phys.

G. S. Ofelt, “Intensities of crystal spectra of rare-earth ions,” J. Chem. Phys.37(3), 511–520 (1962).
[CrossRef]

J. Electrochem. Soc.

L. Brixner and H. Chen, “On the structural and luminescent properties of the M' LnTaO4 rare earth tantalates,” J. Electrochem. Soc.130(12), 2435–2443 (1983).
[CrossRef]

J. Lumin.

S. Chen, X. Liu, M. Gu, C. Ni, B. Liu, and S. Huang, “Sol-gel synthesis and luminescent properties of M′-type LuTaO4:Eu3+ phosphors,” J. Lumin.140, 1–6 (2013).
[CrossRef]

J. Mater. Chem.

C. Mansuy, J. M. Nedelec, and R. Mahiou, “Molecular design of inorganic scintillators: from alkoxides to scintillating materials,” J. Mater. Chem.14(21), 3274–3280 (2004).
[CrossRef]

J. Nanomater.

J. Nedelec, “Sol-gel processing of nanostructured inorganic scintillating materials,” J. Nanomater.2007, 1–8 (2007).
[CrossRef]

J. Opt. Soc. Am. A

J. Phys. Chem. Solids

G. Blasse, A. Bril, and W. Nieuwpoort, “On the Eu3+ fluorescence in mixed metal oxides: Part I-The crystal structure sensitivity of the intensity ratio of electric and magnetic dipole emission,” J. Phys. Chem. Solids27(10), 1587–1592 (1966).
[CrossRef]

J. Sol-Gel Sci. Technol.

J. Nedelec, L. Courtheoux, E. Jallot, C. Kinowski, J. Lao, P. Laquerriere, C. Mansuy, G. Renaudin, and S. Turrell, “Materials doping through sol–gel chemistry: a little something can make a big difference,” J. Sol-Gel Sci. Technol.46(3), 259–271 (2008).
[CrossRef]

J. Synchrotron Radiat.

T. Martin and A. Koch, “Recent developments in X-ray imaging with micrometer spatial resolution,” J. Synchrotron Radiat.13(2), 180–194 (2006).
[CrossRef] [PubMed]

Meas. Sci. Technol.

M. Nikl, “Scintillation detectors for x-rays,” Meas. Sci. Technol.17(4), R37–R54 (2006).
[CrossRef]

Opt. Express

Phys. Rev.

B. Judd, “Optical absorption intensities of rare-earth ions,” Phys. Rev.127(3), 750–761 (1962).
[CrossRef]

Talanta

M. J. Lambregts and S. Frank, “Application of Vegard’s law to mixed cation sodalites: a simple method for determining the stoichiometry,” Talanta62(3), 627–630 (2004).
[CrossRef] [PubMed]

Other

G. Blasse and B. C. Grabmaier, Luminescent Materials (Springer, 1994), Chap. 3.

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Figures (6)

Fig. 1
Fig. 1

XRD patterns of the M'-type LuTaO4:Ln3+ (Ln = Eu, Tb) thin films.

Fig. 2
Fig. 2

The surface morphologies and cross-sectional views of the M′-type LuTaO4:Ln3+ thin films, (a) and (c) Ln = Eu, (b) and (d) Ln = Tb.

Fig. 3
Fig. 3

Transmission spectra of the M′-type LuTaO4:Ln3+ thin films, (a) Ln = Eu, (b) Ln = Tb, the insets present their photographs and optical band gaps.

Fig. 4
Fig. 4

Excitation and emission spectra of the M'-type LuTaO4:Ln3+ thin films, (a) Ln = Eu (λex = 209 nm, λem = 613 nm), (b) Ln = Tb (λex = 209 nm, λem = 548 nm).

Fig. 5
Fig. 5

Decay curves of the M′-type LuTaO4:Ln3+ thin films, (a) Ln = Eu (λex = 209 nm, λem = 613 nm), (b) Ln = Tb (λex = 209 nm, λem = 548 nm).

Fig. 6
Fig. 6

XEL spectra of the M'-type LuTaO4:Ln3+ thin films, (a) Ln = Eu, (b) Ln = Tb.

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