Light source using a yellow-to-red-emitting phosphor

Details Light source using a yellow-to-red-emitting phosphor Light source using a yellow-to-red-emitting phosphor

2002-01-22

2003-11-18

Nelms, David (Department: 2818)

Active solid-state devices (e.g., transistors, solid-state diode

Field effect device

Charge transfer device

C257S233000, C257S098000

Reexamination Certificate

active

06649946

ABSTRACT:

TECHNICAL FIELD
This invention relates to an electrical Light source using a yellow-to-red-emitting phosphor and more particularly, but not exclusively to Light Emitting Diodes (LED). The phosphor belongs to the class of rare-earth activated silicon nitrides. Other application fields are electrical lamps, especially high intensity discharge lamps or fluorescent lamps.
BACKGROUND ART
For Eu
2+
-doped material normally UV-blue emission is observed (Blasse and Grabmeier: Luminescent Materials, Springer Verlag, Heidelberg, 1994). Several studies show that also emission in the green and yellow part of the visible spectrum is possible (Blasse: Special Cases of divalent lanthanide emission, Eur. J. Solid State Inorg. Chem. 33 (1996), p. 175; Poort, Blokpoel and Blasse: Luminescence of Eu
2+
in Barium and Strontium Aluminate and Gallate, Chem. Mater. 7 (1995), p. 1547; Poort, Reijnhoudt, van der Kuip, and Blasse: Luminescence of Eu
2+
in Silicate host lattices with Alkaline earth ions in a row, J. Alloys and Comp. 241 (1996), p. 75). Hitherto, red Eu
2+
luminescence is observed only in some exceptional cases, such as in alkaline earth sulphides and related lattices of the rock-salt type (Nakao, Luminescence centers of MgS, CaS and CaSe Phosphors Activated with Eu
2+
Ion, J. Phys. Soc. Jpn. 48(1980), p. 534), in alkaline earth thiogallates (Davolos, Garcia, Fouassier, and Hagenmuller, Luminescence of Eu
2+
in Strontium and Barium Thiogallates, J. Solid. State Chem. 83 (1989), p. 316) and in some borates (Diaz and Keszler; Red, Green, and Blue Eu
2+
luminescence in solid state Borates: a structure-property relationship, Mater. Res. Bull. 31 (1996), p. 147). Eu
2+
luminescence in alkaline-earth silicon nitrides has hitherto only been reported for MgSiN
2
:Eu (Gaido, Dubrovskii, and Zykov: Photoluminescence of MgSiN
2
Activated by Europium, Izv. Akad. Nauk SSSR, Neorg. Mater. 10 (1974), p. 564; Dubrovskii, Zykov and Chernovets: Luminescence of rare earth Activated MgSiN
2
, Izv. Akad. Nauk SSSR, Neorg. Mater. 17 (1981), p. 1421) and Mg
1−x
Zn
x
SiN
2
:Eu (Lim, Lee, Chang: Photoluminescence Characterization of Mg
1−x
Zn
x
SiN
2
:Tb for Thin Film Electroluminescent Devices Application, Inorganic and Organic Electroluminescence, Berlin, Wissen-schaft und Technik Verlag, (1996), p. 363). For both Eu
2+
luminescence in the green and green/blue part of the spectrum was found.
New host lattices of the nitridosilicate type are based on a three dimensional network of cross-linked SiN
4
tetrahedra in which alkaline earth ions (M=Ca, Sr and Ba) are incorporated. Such lattices are for example Ca
2
Si
5
N
8
(Schlieper and Schlick: Nitridosilicate I, Hochtemperatursynthese und Kristallstruktur von Ca
2
Si
5
N
8
, Z. anorg. allg. Chem. 621, (1995), p. 1037), Sr
2
Si
5
N
8
and Ba
2
Si
5
N
8
(Schlieper, Millus and Schlick: Nitridosilicate II, Hochtemperatursynthesen und Kristallstrukturen von Sr
2
Si
5
N
8
and Ba
2
Si
5
N
8
, Z. anorg. allg. Chem. 621, (1995), p. 1380), and BaSi
7
N
10
(Huppertz and Schnick: Edge-Sharing SiN
4
tetrahedra in the highly condensed Nitridosilicate BaSi
7
N
10
, Chem. Eur. J. 3 (1997), p. 249). The lattice types are mentioned in Table 1.
Sulfide based phosphors (e.g. earth alkaline sulfides) are less desirable for lighting applications, especially for LED applications, because they interact with the encapsulating resin system, and partially suffer from hydrolytic attack. Red emitting Eu
2+
activated borates show already temperature quenching to a certain degree at the operating temperature of LEDs.
DISCLOSURE OF THE INVENTION
It is, therefore, an object of this invention to obviate the disadvantages of the prior art. It is another object of the invention to provide a light source with improved red color rendition R9. It is a further object to provide a light source with an improved overall color rendition Ra. It is a further object to provide a white LED with high color rendition.
Especially high stability up to at least 100° C. is desirable for LED applications. Their typical operation temperature is around 80° C.
These objects are accomplished by the characterising features of claim
1
. Advantageous embodiments can be found in the dependant claims.
The light source uses a new yellowish-red emitting phosphor. Its absorption is at least within the blue to green spectral region. Furthermore they show fluorescent emission under absorption. Those Eu
2+
-doped luminescent materials show emission within the yellow to red spectral region, especially long wavelength red, orange or yellow emission. These phosphors are based on alkaline-earth silicon nitride material as host-lattices. They are very promising, especially for LED applications, when used as phosphors. Hitherto white LEDs were realised by combining a blue emitting diode with a yellow emitting phosphor. Such a combination has only a poor colour rendition. A far better performance can be achieved by using a multicolor (for example red-green-blue) system. Typically the new material can be used together with a green-emitting (or yellow-emitting) phosphor, for example strontiumaluminate SrAl
2
O
4
:Eu
2+
, whose emission maximum is around 520 nm.
In detail, the new Light source using a yellow-to-red-emitting phosphor, uses a host lattice of the nitridosilicate type M
x
Si
y
N
z
:Eu, wherein M is at least one of an alkaline earth metal chosen from the group Ca, Sr, Ba and wherein z=2/3x+4/3y. The incorporation of nitrogen increases the proportion of covalent bond and ligand-field splitting. As a consequence this leads to a pronounced shift of excitation and emission bands to longer wavelengths in comparison to oxide lattices.
Preferably, the phosphor is of the type, wherein x=2, and y=5. In another preferred embodiment, the phosphor is of the type, wherein x=1, and y=7.
Preferably, the metal M in the phosphor is strontium because the resulting phosphor is emitting at relatively short yellow to red wavelengths. Thus the efficiency is rather high in comparison to most of the other elected metals M.
In a further embodiment the phosphor uses a mixture of different metals, for example Ca (10 atom.-%) together with Ba (balance), as component M.
These materials show high absorption and good excitation in the UV and blue visible spectrum (up to more than 450 nm), high quantum efficiency and low temperature quenching up to 100° C.
It can be used for luminescence conversion LEDs with a blue light emitting primary source together with one or more phosphors (red and green). Another field of application are compact fluorescent lamps and replacement of yttrium vanadate in high intensity discharge lamps.


REFERENCES:
patent: 6252254 (2001-06-01), Soules et al.
patent: 6255670 (2001-07-01), Srivastava et al.
patent: 6287993 (2001-09-01), Fu et al.
US patent application publication US 2003/0024438 A1 by Botty et al. pub date Feb. 6, 2003.
Soon-Seok Lee et al: “Development and luminescent characteristics of CaSiN/sub 2/ based phosphors”, Journal of the Institute of Electronics Engineers of Korea D, Oct. 1999, Inst. Electron. Eng. Korea, South Korea, vol. 36-D, No. 10, pp. 31-36, XP002136109, ISSN: 1226-5845, p. 31.

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