Abstract

A new blue-emitting phosphor, K2ScSi4O10F:Eu2+ (KSSOF:Eu2+), was synthesized through a solid-state reaction. The structural and optical properties of KSSOF:Eu2+ phosphor, in addition to its thermal quenching and fabrication of white LEDs (WLEDs), were investigated for the first time. The phosphor showed broad blue emission, with a maximum at 434nm under near-ultraviolet excitation due to 5d4f transition of the Eu2+ ion. The critical distance was calculated to be 12 Å using the critical concentration of Eu2+ and Dexter’s theory for energy transfer. WLEDs were fabricated by blending KSSOF:Eu2+, commercial Lu3Al5O12:Ce3+, and (Sr,Ca)AlSiN3:Eu2+ phosphors, showed a high color rendering index of 88 at a correlated color temperature of 4134 K under a forward bias current of 100 mA.

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  1. W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
    [CrossRef]
  2. T. Nishida, T. Ban, and N. Kobayashi, Appl. Phys. Lett. 82, 3817 (2003).
    [CrossRef]
  3. J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
    [CrossRef]
  4. U. Kolitsch and E. Tillmanns, Eur. J. Mineral. 16, 143 (2004).
    [CrossRef]
  5. R. Shannon, Acta Crystallogr. 32, 751 (1976).
    [CrossRef]
  6. R. A. Young, The Rietveld Method (Oxford University, 1995).
  7. W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
    [CrossRef]
  8. S. Shionoya, W. M. Yen, and T. Hase, Phosphor Handbook (CRC Press, 1999), Vol. 1.
  9. G. Blasse, Phys. Lett. A 28, 444 (1968).
    [CrossRef]
  10. D. L. Dexter, J. Chem. Phys. 21, 836 (1953).
    [CrossRef]
  11. G. Blasse, J. Solid State Chem. 62, 207 (1986).
    [CrossRef]
  12. S. Bhushan and M. V. Chukichev, J. Mater. Sci. Lett. 7, 319 (1988).
    [CrossRef]

2011 (1)

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

2009 (1)

W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
[CrossRef]

2004 (2)

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

U. Kolitsch and E. Tillmanns, Eur. J. Mineral. 16, 143 (2004).
[CrossRef]

2003 (1)

T. Nishida, T. Ban, and N. Kobayashi, Appl. Phys. Lett. 82, 3817 (2003).
[CrossRef]

1988 (1)

S. Bhushan and M. V. Chukichev, J. Mater. Sci. Lett. 7, 319 (1988).
[CrossRef]

1986 (1)

G. Blasse, J. Solid State Chem. 62, 207 (1986).
[CrossRef]

1976 (1)

R. Shannon, Acta Crystallogr. 32, 751 (1976).
[CrossRef]

1968 (1)

G. Blasse, Phys. Lett. A 28, 444 (1968).
[CrossRef]

1953 (1)

D. L. Dexter, J. Chem. Phys. 21, 836 (1953).
[CrossRef]

Ban, T.

T. Nishida, T. Ban, and N. Kobayashi, Appl. Phys. Lett. 82, 3817 (2003).
[CrossRef]

Bhushan, S.

S. Bhushan and M. V. Chukichev, J. Mater. Sci. Lett. 7, 319 (1988).
[CrossRef]

Blasse, G.

G. Blasse, J. Solid State Chem. 62, 207 (1986).
[CrossRef]

G. Blasse, Phys. Lett. A 28, 444 (1968).
[CrossRef]

Brinkley, S.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Chmelka, B. F.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Choi, J. C.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Chukichev, M. V.

S. Bhushan and M. V. Chukichev, J. Mater. Sci. Lett. 7, 319 (1988).
[CrossRef]

DenBaars, S. P.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Dexter, D. L.

D. L. Dexter, J. Chem. Phys. 21, 836 (1953).
[CrossRef]

George, N.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Hase, T.

S. Shionoya, W. M. Yen, and T. Hase, Phosphor Handbook (CRC Press, 1999), Vol. 1.

Hu, J.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Im, W. B.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
[CrossRef]

Jeon, D. Y.

W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
[CrossRef]

Jeon, P. E.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Kim, G. C.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Kim, J. S.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Kim, Y.-I.

W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
[CrossRef]

Kobayashi, N.

T. Nishida, T. Ban, and N. Kobayashi, Appl. Phys. Lett. 82, 3817 (2003).
[CrossRef]

Kolitsch, U.

U. Kolitsch and E. Tillmanns, Eur. J. Mineral. 16, 143 (2004).
[CrossRef]

Kurzman, J.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Mikhailovsky, A.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Nishida, T.

T. Nishida, T. Ban, and N. Kobayashi, Appl. Phys. Lett. 82, 3817 (2003).
[CrossRef]

Park, H.-L.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Park, Y. H.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Seshadri, R.

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Shannon, R.

R. Shannon, Acta Crystallogr. 32, 751 (1976).
[CrossRef]

Shionoya, S.

S. Shionoya, W. M. Yen, and T. Hase, Phosphor Handbook (CRC Press, 1999), Vol. 1.

Tae Whan, K.

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Tillmanns, E.

U. Kolitsch and E. Tillmanns, Eur. J. Mineral. 16, 143 (2004).
[CrossRef]

Yen, W. M.

S. Shionoya, W. M. Yen, and T. Hase, Phosphor Handbook (CRC Press, 1999), Vol. 1.

Yoo, H. S.

W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
[CrossRef]

Young, R. A.

R. A. Young, The Rietveld Method (Oxford University, 1995).

Acta Crystallogr. (1)

R. Shannon, Acta Crystallogr. 32, 751 (1976).
[CrossRef]

Adv. Mater. (1)

W. B. Im, N. George, J. Kurzman, S. Brinkley, A. Mikhailovsky, J. Hu, B. F. Chmelka, S. P. DenBaars, and R. Seshadri, Adv. Mater. 23, 2300 (2011).
[CrossRef]

Appl. Phys. Lett. (2)

T. Nishida, T. Ban, and N. Kobayashi, Appl. Phys. Lett. 82, 3817 (2003).
[CrossRef]

J. S. Kim, P. E. Jeon, Y. H. Park, J. C. Choi, H.-L. Park, G. C. Kim, and K. Tae Whan, Appl. Phys. Lett. 85, 3696 (2004).
[CrossRef]

Eur. J. Mineral. (1)

U. Kolitsch and E. Tillmanns, Eur. J. Mineral. 16, 143 (2004).
[CrossRef]

Inorg. Chem. (1)

W. B. Im, Y.-I. Kim, H. S. Yoo, and D. Y. Jeon, Inorg. Chem. 48, 557 (2009).
[CrossRef]

J. Chem. Phys. (1)

D. L. Dexter, J. Chem. Phys. 21, 836 (1953).
[CrossRef]

J. Mater. Sci. Lett. (1)

S. Bhushan and M. V. Chukichev, J. Mater. Sci. Lett. 7, 319 (1988).
[CrossRef]

J. Solid State Chem. (1)

G. Blasse, J. Solid State Chem. 62, 207 (1986).
[CrossRef]

Phys. Lett. A (1)

G. Blasse, Phys. Lett. A 28, 444 (1968).
[CrossRef]

Other (2)

S. Shionoya, W. M. Yen, and T. Hase, Phosphor Handbook (CRC Press, 1999), Vol. 1.

R. A. Young, The Rietveld Method (Oxford University, 1995).

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Figures (5)

Fig. 1.
Fig. 1.

(a) Unit cell representation of the crystal structure of K2ScSi4O10F, with the blue, black, red, orange, and white spheres representing K, Sc, Si, O, and F atoms, respectively. (b) The potassium site is depicted as eight-coordination with oxygen and fluorine atoms.

Fig. 2.
Fig. 2.

Rietveld refinement of K1.99Eu0.01ScSi4O10F (KSSOF:Eu2+) using (a) x-ray powder diffraction and (b) NPD data. The black filled circles represent observed intensities and the solid line represents the ones that were calculated.

Fig. 3.
Fig. 3.

(a) Excitation spectra of K1.99Eu0.01ScSi4O10F at λem=434nm and emission spectra under λex=370nm. (b) Position of the emission maxima. (c) Relative emission intensity as a function of Eu2+ concentration in the KSSOF host.

Fig. 4.
Fig. 4.

(a) Temperature-dependent normalized emission intensities of KSSOF:Eu2+ and commercial (Sr,Ba)2SiO4:Eu2+ phosphor, and (b) activation plots for thermal quenching of KSSOF:Eu2+ and commercial (Sr,Ba)2SiO4:Eu2+ phosphor using Arrhenius equation.

Fig. 5.
Fig. 5.

Electroluminescence of InGaN LED + phosphor under different forward bias currents, representing: (a) excitation and emission PL spectra of KSSOF:Eu2+, Lu3Al5O12:Ce3+, and (Sr,Ca)AlSiN3:Eu2+ phosphors, and the emission spectrum of NUV LED (λmax=365nm) using a prototype WLED; (b) InGaN LED (λmax=365nm)+KSSOF:Eu2++Lu3Al5O12:Ce3++(Sr,Ca)AlSiN3:Eu2+; and (c) CIE chromaticity coordinates of the device under different forward bias currents. The Planckian locus line and points corresponding to color temperatures of 3500 and 6500 K are indicated. (The inset shows digital camera images of the WLED fabricated using KSSOF:Eu2+ phosphor, Lu3Al5O12:Ce3+, and (Sr,Ca)AlSiN3:Eu2+ using a UV LED.)

Equations (3)

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Rc12(3V4πχcN)13,
Rc260.63×1028(48×1016E4·p)fs(E)fa(E)dE,
I(T)=I01+Ae(EkT),

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