Abstract

Through the use of complex core-shell structures, white light emissions are observed from a single nanoparticle doped with multiple trivalent rare-earth ions. The internal structuring of the nanoparticle to allow for a controlled degree of energy transfer a common excitation wavelength yielding the white light emission is obtained. Emissions with correlated color temperatures ranging from 2700K to 5000K were produced. The stability of the phosphors to excitation wavelength variations was examined.

© 2006 Optical Society of America

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  1. D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
    [Crossref]
  2. T. Jüstel, H. Nikol, and C. Ronda, “New Developments in the Field of Luminescent materials for Lighting and Displays,” Angew. Chem. Int. Ed. 37, 3084–3103 (1998).
    [Crossref]
  3. J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
    [Crossref]
  4. M. S. Shur and A. Žukauskas, “Solid-State Lighting: Toward Superior Illumination,” Proceedings of IEEE 93, 1691–1703 (2005).
    [Crossref]
  5. R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
    [Crossref]
  6. S. Sivakumar, F. C. J. M van Veggel, and M. Raudsepp, “Bright White Light through Up-conversion of a Single NIR Source from Sol-Gel Derived Thin Film Made with Ln3+-Doped LaF3 Nanoparticles,” J. Am. Chem. Soc. 127, 12464–12465 (2005).
    [Crossref] [PubMed]
  7. G.-S. Yi and G.-M. Chow, “Colloidal LaF3:Yb, Er, LaF3:Yb,Ho and LaF3:Yb,Tm nanocrystals with multicolor upconversion fluorescence,” J. Am. Chem. Soc. 15, 4460–4464 (2005)
  8. J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, and J. Ballato are preparing a manuscript to be called “Controlling Energy Transfer between Multiple Dopants within a Single Nanoparticle.”
  9. J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
    [Crossref]
  10. J. W. Stouwdam and F. C. J. M. van Veggel, “Improvement in the Luminescence Properties and Processability of LaF3/Ln and LaPO4/Ln Nanoparticles by Surface modification,” Langmuir 20, 11763–11771 (2004).
    [Crossref] [PubMed]
  11. J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, B. Kokuoz, T. James, and J. Ballato are preparing a manuscript to be called “Structure/Property Effects in Light Emissive Inorganic Nanoparticles with Complex Core-Shell Architectures.”
  12. M. Bettinelli and C. D. Flint, “Non-resonant energy transfer between Tb3+ and Eu3+ in the cubic hexachloroelpasolite crystals Cs2sNaTb1-xEuxCl6 (x=0.01–0.15),” J. Phys.: Condens. Matter2, 8417–8426 (1990).
    [Crossref]
  13. B. C. Joshi, “Enhanced Eu3+ emission by non-radiative energy transfer from Tb3+ in zinc phosphate glass,” J. Non-Cryst. Solids 180, 217–220 (1995).
    [Crossref]
  14. E. F. Schubert and J. K. Kim, “Solid-State Light Sources Getting Smart,” Science 308, 1274–1278 (2005).
    [Crossref] [PubMed]

Ballato, J.

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, and J. Ballato are preparing a manuscript to be called “Controlling Energy Transfer between Multiple Dopants within a Single Nanoparticle.”

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, B. Kokuoz, T. James, and J. Ballato are preparing a manuscript to be called “Structure/Property Effects in Light Emissive Inorganic Nanoparticles with Complex Core-Shell Architectures.”

Bettinelli, M.

M. Bettinelli and C. D. Flint, “Non-resonant energy transfer between Tb3+ and Eu3+ in the cubic hexachloroelpasolite crystals Cs2sNaTb1-xEuxCl6 (x=0.01–0.15),” J. Phys.: Condens. Matter2, 8417–8426 (1990).
[Crossref]

Bhat, J. C.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Choi, J. C.

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

Chow, G.-M.

G.-S. Yi and G.-M. Chow, “Colloidal LaF3:Yb, Er, LaF3:Yb,Ho and LaF3:Yb,Tm nanocrystals with multicolor upconversion fluorescence,” J. Am. Chem. Soc. 15, 4460–4464 (2005)

Collins, D.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Dang, H.

J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
[Crossref]

DiMaio, J.

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, B. Kokuoz, T. James, and J. Ballato are preparing a manuscript to be called “Structure/Property Effects in Light Emissive Inorganic Nanoparticles with Complex Core-Shell Architectures.”

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, and J. Ballato are preparing a manuscript to be called “Controlling Energy Transfer between Multiple Dopants within a Single Nanoparticle.”

Fletcher, R. M.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Flint, C. D.

M. Bettinelli and C. D. Flint, “Non-resonant energy transfer between Tb3+ and Eu3+ in the cubic hexachloroelpasolite crystals Cs2sNaTb1-xEuxCl6 (x=0.01–0.15),” J. Phys.: Condens. Matter2, 8417–8426 (1990).
[Crossref]

Hirosaki, N.

R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
[Crossref]

Holcomb, M. O.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

James, T.

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, B. Kokuoz, T. James, and J. Ballato are preparing a manuscript to be called “Structure/Property Effects in Light Emissive Inorganic Nanoparticles with Complex Core-Shell Architectures.”

Jeon, P. E.

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

Joshi, B. C.

B. C. Joshi, “Enhanced Eu3+ emission by non-radiative energy transfer from Tb3+ in zinc phosphate glass,” J. Non-Cryst. Solids 180, 217–220 (1995).
[Crossref]

Jüstel, T.

T. Jüstel, H. Nikol, and C. Ronda, “New Developments in the Field of Luminescent materials for Lighting and Displays,” Angew. Chem. Int. Ed. 37, 3084–3103 (1998).
[Crossref]

Kim, G. C.

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

Kim, J. K.

E. F. Schubert and J. K. Kim, “Solid-State Light Sources Getting Smart,” Science 308, 1274–1278 (2005).
[Crossref] [PubMed]

Kim, J.S.

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

Kokuoz, B.

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, B. Kokuoz, T. James, and J. Ballato are preparing a manuscript to be called “Structure/Property Effects in Light Emissive Inorganic Nanoparticles with Complex Core-Shell Architectures.”

Liu, W.

J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
[Crossref]

Ludowise, M. J.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Martin, P. S.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Mho, S. I.

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

Mitomo, M.

R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
[Crossref]

Nikol, H.

T. Jüstel, H. Nikol, and C. Ronda, “New Developments in the Field of Luminescent materials for Lighting and Displays,” Angew. Chem. Int. Ed. 37, 3084–3103 (1998).
[Crossref]

Park, H. L.

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

Raudsepp, M.

S. Sivakumar, F. C. J. M van Veggel, and M. Raudsepp, “Bright White Light through Up-conversion of a Single NIR Source from Sol-Gel Derived Thin Film Made with Ln3+-Doped LaF3 Nanoparticles,” J. Am. Chem. Soc. 127, 12464–12465 (2005).
[Crossref] [PubMed]

Ronda, C.

T. Jüstel, H. Nikol, and C. Ronda, “New Developments in the Field of Luminescent materials for Lighting and Displays,” Angew. Chem. Int. Ed. 37, 3084–3103 (1998).
[Crossref]

Rudaz, S. L.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Sakuma, K.

R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
[Crossref]

Schubert, E. F.

E. F. Schubert and J. K. Kim, “Solid-State Light Sources Getting Smart,” Science 308, 1274–1278 (2005).
[Crossref] [PubMed]

Shur, M. S.

M. S. Shur and A. Žukauskas, “Solid-State Lighting: Toward Superior Illumination,” Proceedings of IEEE 93, 1691–1703 (2005).
[Crossref]

Sivakumar, S.

S. Sivakumar, F. C. J. M van Veggel, and M. Raudsepp, “Bright White Light through Up-conversion of a Single NIR Source from Sol-Gel Derived Thin Film Made with Ln3+-Doped LaF3 Nanoparticles,” J. Am. Chem. Soc. 127, 12464–12465 (2005).
[Crossref] [PubMed]

Steigerwald, D. A.

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

Stouwdam, J. W.

J. W. Stouwdam and F. C. J. M. van Veggel, “Improvement in the Luminescence Properties and Processability of LaF3/Ln and LaPO4/Ln Nanoparticles by Surface modification,” Langmuir 20, 11763–11771 (2004).
[Crossref] [PubMed]

Takashi, K.

R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
[Crossref]

van Veggel, F. C. J. M

S. Sivakumar, F. C. J. M van Veggel, and M. Raudsepp, “Bright White Light through Up-conversion of a Single NIR Source from Sol-Gel Derived Thin Film Made with Ln3+-Doped LaF3 Nanoparticles,” J. Am. Chem. Soc. 127, 12464–12465 (2005).
[Crossref] [PubMed]

van Veggel, F. C. J. M.

J. W. Stouwdam and F. C. J. M. van Veggel, “Improvement in the Luminescence Properties and Processability of LaF3/Ln and LaPO4/Ln Nanoparticles by Surface modification,” Langmuir 20, 11763–11771 (2004).
[Crossref] [PubMed]

Wu, Z.

J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
[Crossref]

Xie, R.-J.

R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
[Crossref]

Yi, G.-S.

G.-S. Yi and G.-M. Chow, “Colloidal LaF3:Yb, Er, LaF3:Yb,Ho and LaF3:Yb,Tm nanocrystals with multicolor upconversion fluorescence,” J. Am. Chem. Soc. 15, 4460–4464 (2005)

Zhang, Z.

J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
[Crossref]

Zhou, J.

J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
[Crossref]

Žukauskas, A.

M. S. Shur and A. Žukauskas, “Solid-State Lighting: Toward Superior Illumination,” Proceedings of IEEE 93, 1691–1703 (2005).
[Crossref]

Other (14)

D. A. Steigerwald, J. C. Bhat, D. Collins, R. M. Fletcher, M. O. Holcomb, M. J. Ludowise, P. S. Martin, and S. L. Rudaz, “Illumination With Solid State Lighting Technology,” IEEE J. Selc Top Quantum Electronics 8, 310–320 (2002).
[Crossref]

T. Jüstel, H. Nikol, and C. Ronda, “New Developments in the Field of Luminescent materials for Lighting and Displays,” Angew. Chem. Int. Ed. 37, 3084–3103 (1998).
[Crossref]

J.S. Kim, P. E. Jeon, J. C. Choi, H. L. Park, S. I. Mho, and G. C. Kim, “Warm-white-light emitting diode utilizing a single-phase full-color Ba3MgSi2O8:Eu2+,Mn2+ phosphor,” Appl. Phys. Lett. 84, 2931–2933 (2004).
[Crossref]

M. S. Shur and A. Žukauskas, “Solid-State Lighting: Toward Superior Illumination,” Proceedings of IEEE 93, 1691–1703 (2005).
[Crossref]

R.-J. Xie, N. Hirosaki, M. Mitomo, K. Takashi, and K. Sakuma, “Highly efficient white-light-emitting diodes fabricated with short-wavelength yellow oxynitride phosphors,” Appl. Phys. Lett. 88, 101104 (2006).
[Crossref]

S. Sivakumar, F. C. J. M van Veggel, and M. Raudsepp, “Bright White Light through Up-conversion of a Single NIR Source from Sol-Gel Derived Thin Film Made with Ln3+-Doped LaF3 Nanoparticles,” J. Am. Chem. Soc. 127, 12464–12465 (2005).
[Crossref] [PubMed]

G.-S. Yi and G.-M. Chow, “Colloidal LaF3:Yb, Er, LaF3:Yb,Ho and LaF3:Yb,Tm nanocrystals with multicolor upconversion fluorescence,” J. Am. Chem. Soc. 15, 4460–4464 (2005)

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, and J. Ballato are preparing a manuscript to be called “Controlling Energy Transfer between Multiple Dopants within a Single Nanoparticle.”

J. Zhou, Z. Wu, Z. Zhang, W. Liu, and H. Dang, “Study on an antiwear and extreme pressure additive of surface coated LaF3 nanoparticles in liquid paraffin.” Wear 249, 333–337 (2001).
[Crossref]

J. W. Stouwdam and F. C. J. M. van Veggel, “Improvement in the Luminescence Properties and Processability of LaF3/Ln and LaPO4/Ln Nanoparticles by Surface modification,” Langmuir 20, 11763–11771 (2004).
[Crossref] [PubMed]

J. DiMaio, Center for Optical Materials Science and Engineering Technologies (COMSET), Clemson University, 107 Advanced Materials Research Laboratory, 91 Technology Drive, Anderson, S.C. 29625, B. Kokuoz, T. James, and J. Ballato are preparing a manuscript to be called “Structure/Property Effects in Light Emissive Inorganic Nanoparticles with Complex Core-Shell Architectures.”

M. Bettinelli and C. D. Flint, “Non-resonant energy transfer between Tb3+ and Eu3+ in the cubic hexachloroelpasolite crystals Cs2sNaTb1-xEuxCl6 (x=0.01–0.15),” J. Phys.: Condens. Matter2, 8417–8426 (1990).
[Crossref]

B. C. Joshi, “Enhanced Eu3+ emission by non-radiative energy transfer from Tb3+ in zinc phosphate glass,” J. Non-Cryst. Solids 180, 217–220 (1995).
[Crossref]

E. F. Schubert and J. K. Kim, “Solid-State Light Sources Getting Smart,” Science 308, 1274–1278 (2005).
[Crossref] [PubMed]

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Figures (5)

Fig. 1.
Fig. 1.

Scale models of the complex core-shell particles for white light applications. Red corresponds to the Eu0.2La0.8F3 core, green to the Tb0.2La0.8F3 shell, blue to the Tm0.2La0.8F3 shell, and yellow to the LaF3 passive shell. One can see the thickness of the shells have been modified in each model corresponding to the appropriate composition.

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Fig. 2.
Fig. 2.

XRD plot of LaF3 nanoparticles (inset: High-resolution TEM image with 2 nm scale bar.)

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Fig. 3.
Fig. 3.

Photoluminescence emission spectra of core-shell nanoparticles [(a) Nanoparticle A, (b) Nanoparticle B, and (c) Nanoparticle C] with different excitation wavelength.

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Fig. 4.
Fig. 4.

CIE diagrams of core-shell nanoparticles with excitation FWHM of (a) 1 nm and (b) 13 nm.

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Fig. 5.
Fig. 5.

Energy level diagrams showing the excitation scheme for obtaining white light from a single nanoparticle with a single UV excitation.

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Tables (1)

Tables Icon

Table 1. CIE color coordinates for core-shell nanoparticles.

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