WO2007080541A1 - Light emitting device with a eu-comprising phosphor material - Google Patents
Light emitting device with a eu-comprising phosphor material Download PDFInfo
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- WO2007080541A1 WO2007080541A1 PCT/IB2007/050068 IB2007050068W WO2007080541A1 WO 2007080541 A1 WO2007080541 A1 WO 2007080541A1 IB 2007050068 W IB2007050068 W IB 2007050068W WO 2007080541 A1 WO2007080541 A1 WO 2007080541A1
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Definitions
- the present invention is directed to light emitting devices, especially to the field of LEDs and to a light converting Eu-comprising phosphor material.
- Line emitting phosphors are widely applied as red emitters in fluorescent light emitting devices and emissive displays, e.g. in fluorescent lamps, CRTs, and PDPs.
- Eu-containing light emitting devices suffer from the drawback that the common Eu-doped materials such as CaS :Eu or Sr 2 SIsNgIEu comprises Eu 2+ ions, which are subject of instability due to its oxidation or reaction with other components present in the light emitting device.
- Another drawback of Eu 2+ activated red-emitting phosphors according to prior art is their relatively wide emission band, which results in a low lumen equivalent.
- Eu 3+ activated red-emitting phosphors show a better lifetime stability compared to Eu 2+ , but showing a strong absorption only in the UV-C and VUV spectral range, while the absorption is very weak below the low edge of the charge transfer state around 300nm.
- phosphor-converted light emitting diodes pcLEDs
- the LED emits a primary radiation, which is at least partly converted into a secondary radiation with a longer wavelength by the light converting material, the so-called phosphor material.
- a light emitting device comprising an excitation energy source to deliver a primary energy and a converting element essentially comprising Eu 3+ - phosphor material to at least partly convert the primary energy into a secondary radiation whereby in the excitation spectrum of the Eu-comprising phosphor material at 298 K and 1,013 bar the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is >5% of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm.
- the term “intensity” denotes the amount of absorbed light (corresponding to an absorption strength).
- the term “essentially comprising Eu 3+ -phosphor material” means and/or includes especially that >90%, according to another embodiment >95% and according to another embodiment >98% of the Eu comprised in the Eu-comprising material are in the form of Eu 3+ .
- the spectral (absorption and emission) properties of Eu 3+ materials are more stable over time as compared to Eu 2+ materials, because of the lesser tendency to be oxidized. The lower the remaining Eu 2+ content, the better the lifetime behaviour of the Eu-phosphor material.
- the excitation energy source can be any suitable energy source to excite the secondary light emission of Eu 3+ -comprising phosphor materials such as electron beam sources (e.g. electron guns in CRTs) or light sources such as organic LEDs, inorganic LEDs or laser diodes. Therefore the primary energy can be the energy of an electron beam or the energy of a radiation.
- electron beam sources e.g. electron guns in CRTs
- light sources such as organic LEDs, inorganic LEDs or laser diodes. Therefore the primary energy can be the energy of an electron beam or the energy of a radiation.
- the terms “wavelength range” or more specific "UV-A spectral range” or “blue spectral range” denote energy ranges not limited only to electro-magnetic radiation energy.
- a light-emitting device could be operated efficiently with LEDs with blue primary radiation (primary energy).
- the absorption strength of a converting element depends on the absorption strength of the material itself and on the thickness of the converting element in primary energy, e.g. primary light energy, propagation direction.
- a more effective light conversion material for instance enables the application of thinner phosphor materials for more compact devices and/or to reduce the risk of re-absorption of the secondary emission and following radiation-less transition leading to an enhanced efficiency of the light emitting device due to a thinner converting element.
- An enhancement of the blue absorption capability simultaneously also enhances the absorption capability in the near UV-A range between 350nm and 420nm. Therefore, also LEDs emitting within the UV- A spectral range can be used to emit the primary radiation of the pcLED by using a phosphor material according to the present invention.
- the peak area in the wavelength range between > 680 nm to ⁇ 720 nm is >15% of the peak area in the wavelength range between > 570 nm to ⁇ 720 nm.
- the LED shows an improved deep red emittance characteristics in that for some applications efficiencies of 100 - 200 Lumen/Watt are feasible. Additionally, the LED shows improved colour point stability due to the stability of the red emitter.
- peak area denotes the integral amount of light within the specified wavelength range.
- the atomic dopant level (in atom-% of the trivalent cation of the host lattice) of Eu in the Eu-comprising phosphor material is up to 20%.
- Higher Eu 3+ concentration would led to pronounced energy transfer of the absorbed energy to the surface and defect sites and thus to quenching of the Eu3+ luminescence, a phenomenon which is known as concentration quenching.
- the Eu-comprising phosphor material furthermore comprises a co-dopant M selected out of the group comprising Bi, In, Tl, Sb or mixtures thereof.
- M co-dopant
- the atomic dopant concentration of M (in atom- %) in the Eu-comprising material is up to 20%. Higher M 3+ concentration would led to pronounced energy transfer of the absorbed energy to the surface and defect sites and thus to quenching of the activator luminescence.
- the ratio of Eu (in atom-%) towards M (in atom-%) in the Eu comprising material is > 0.1:1 to ⁇ 10:1.
- the term "the ratio of Eu towards M” means or includes especially that M represents the sum of all co-dopants as described above.
- the Eu-comprising material is selected out of the group comprising oxides, oxyhalogenides, garnets, vanadates, tungstates, borates, silicates, germanates or mixtures thereof. These materials offer a high electron density at the sites of the oxygen anions within the host lattice leading to improved absorption properties of Eu 3+ .
- the Eu-comprising material is selected out of the group comprising (Gdi_ x _ z Lu x ) 2 ⁇ 3 :Eu z , (Y 1-x-y- z Gd x Lu y ) 3 Al 5 0i 2 :Eu z , Ba 2 (Yi- ⁇ - y - z Gd x Lu y ) 2 Si 4 ⁇ i 3 :Eu z , (Yi- x - y - z Gd x Lu y )VO 4 :Eu z , (Yi- x - y - z Gd x Lu y )OF:Euz, (Yi -x-y-z Gd x Lu y )OCl:Eu z , Ba(Yi -x-y- z Gd x Lu y )B 9 Oi 6 :Eu z , Ba 3 (Yi-
- a light-emitting device may be of use in a broad variety of systems and/or applications, amongst them one or more of the following:
- Fig. 1 shows an excitation spectrum of a Y 2 O 3 IEu material according to prior art
- Fig. 2 shows an emission spectrum of the material of Fig. 1
- Fig. 3 shows an excitation spectrum of a Eu-comprising material according to a first Example of a first embodiment of the present invention
- Fig. 4 shows an emission spectrum of the material of Fig. 3
- Fig. 5 shows an excitation spectrum of a Eu-comprising material according to a second Example of a second embodiment of the present invention
- Fig. 6 shows an emission spectrum of the material of Fig. 5
- Fig. 7 shows an excitation spectrum of a Eu-comprising material according to a third Example of a third embodiment of the present invention
- Fig. 8 shows an emission spectrum of the material of Fig. 7
- Fig. 9 shows an excitation spectrum of a Eu-comprising material according to a fourth Example of a fourth embodiment of the present invention
- Fig. 10 shows an emission spectrum of the material of Fig. 9
- Fig. 11 shows an emission spectrum of an LED according to a fifth
- Fig. 12 shows an emission spectrum of an LED according to a sixth
- Fig. 1 and 2 refer to Y 2 O 3 IEu material with a Eu-doping level of 5% (prior art Eu-component).
- Fig. 1 shows an excitation spectrum
- Fig. 2 shows an emission spectrum. It can be clearly seen that the intensity as well as the peak area as described above is much lower than according to materials within the present invention. While the absorption of Eu 3+ phosphors in the UV-C and VUV spectral range is strong, it is only very weak below the low energy edge of the charge transfer state around 300nm.
- the present invention describes red line emitting Eu 3+ phosphors with relatively strong absorption of UV-A radiation and/or blue radiation due to the enhancement of the weak absorption lines at around 395nm ( 7 Fo - 5 D 3 ) and 465nm ( 7 Fo - 5 D 2 ). This is achieved by using lattices with a high covalency or by co-doping the host lattice by ions having the [Ar]3d 10 , [Kr]4d 10 or [Xe]4f 14 5d 10 electron configuration.
- the spin forbidden character of the 4f-4f transitions of Eu 3+ is relaxed to a certain extent, which results in an enhanced absorption strength of these transitions.
- the improved absorption properties enable the efficient application of these materials as a colour converter for organic or inorganic state of the art phosphors converted light emitting diodes with emission wavelength in the UV-A and/or blue spectral range.
- Suitable Eu-comprising phosphor materials for the absorption enhancement according to the present invention are high covalent lattices such as (Gdi_ x Lu x ) 2 O 3 :Eu, (Yi_ x _ y Gd x Lu y ) 3 Al 5 0i2:Eu, Ba 2 (Y 1-x-y Gd x Lu y ) 2 Si4 ⁇ 13 :Eu, Ba 2 (Y 1-x- y Gd x Lu y ) 2 Ge 4 0i 3 :Eu, (Yi_ x _ y Gd x Lu y )VO 4 :Eu, (Yi_ x _ y Gd x Lu y )OF:Eu, (Yi_ x .
- high covalent lattices such as (Gdi_ x Lu x ) 2 O 3 :Eu, (Yi_ x _ y Gd x Lu y ) 3 Al 5
- Eu 3+ is surrounded from ions with high negative charge density. Suitable Eu-doping levels are levels up to atomic 20%. Within these materials, Eu 3+ exhibits a strong covalent interaction with the host lattice influencing the transition probability of the spin forbidden transition in comparison to atomic transition probabilities.
- the covalent interaction of Eu 3+ with the host lattices can be even more enhanced by co-doping of the host lattice with other triple positive charged ions such as Bi 3+ , In 3+ , Tl 3+ or Sb 3+ or mixtures thereof.
- suitable In 3+ co-doping levels are up to atomic 10%.
- the atomic dopant level of M in the Eu-comprising phosphor material is up to 5%.
- the atomic dopant level of M in the Eu-comprising phosphor material is up to 1%.
- the ratio in atom% of Eu towards M in the Eu-comprising phosphor material is > 0.5:1 to ⁇ 5:1. According to an embodiment of the present invention, the ratio in atom% of Eu towards M in the Eu-comprising phosphor material is > 1:1 to ⁇ 3:1. In case that more than one co- dopant is present, the term "the ratio of Eu towards M" means or includes especially that M represents the sum of all co-dopants as described above.
- the absorbed excitation energy will be released by a secondary radiation with longer wavelength.
- the excited D-levels relax radiation-less to the excited D-ground state 5 Do.
- transitions to the 7 F 2 state are allowed, while transitions to the 7 F 4 state leading to a deep red emission are spin forbidden.
- a deep red emission with wavelengths around 700nm are preferred.
- the high electron density of the Eu 3+ -comprising phosphor materials according to the present invention also influencing the emission properties, where the spin forbidden transition 5 D 0 - » 7 F 4 is enhanced in comparison to the allowed transition 5 Do- » 7 F 2 .
- Fig. 3 and 4 refer to LaOCl: Eu.
- Fig.3 shows an excitation spectrum
- Fig. 4 shows an emission spectrum.
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is approx. 21 % of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm.
- the peak area in the wavelength range between > 680 nm to ⁇ 720 nm is 22% of the peak area in the wavelength range between > 570 nm to ⁇ 720 nm.
- Fig. 5 and 6 refer to Sr 3 In 2 Ge 3 Oi 2 IEu.
- Fig.5 shows an excitation spectrum
- Fig. 6 shows an emission spectrum.
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is approx. 25 % of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm.
- the peak area in the wavelength range between > 680 nm to ⁇ 720 nm is 25 %of the peak area in the wavelength range between > 570 nm to ⁇ 720 nm.
- Fig. 7 and 8 refer to Y 2 SiOs:Eu.
- Fig.7 shows an excitation spectrum
- Fig. 8 shows an emission spectrum.
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is approx. 11 % of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm.
- Fig. 9 and 10 refer to Ca 3 Ga 2 Ge 3 Oi 2 IEu. Fig.9 shows an excitation spectrum
- Fig. 10 shows an emission spectrum
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is approx. 11 % of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm.
- the peak area in the wavelength range between > 680 nm to ⁇ 720 nm is 27% of the peak area in the wavelength range between > 570 nm to ⁇ 720 nm.
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is >10% of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm as shown for example for Y 2 SiOsIEu and Ca 3 Ga 2 Ge 3 Oi 2 IEu.
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is >15% of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm.
- the maximum intensity in the wavelength range between > 460 nm to ⁇ 470 nm is >20% of the maximum intensity in the wavelength range between > 220 nm to ⁇ 320 nm as shown for example for LaOCliEu and Sr 3 In 2 Ge 3 Oi 2 IEu.
- the peak area in the wavelength range between > 680 nm to ⁇ 720 nm is >20% of the peak area in the wavelength range between > 570 nm to ⁇ 720 nm as shown for example for Ca 3 Ga 2 Ge 3 Oi 2 IEu, Y 2 SiOsIEu, Sr 3 In 2 Ge 3 Oi 2 IEu and LaOCIiEu.
- Other Eu-comprising phosphor materials can show different peak area ratios.
- EXAMPLE V Fig. 11 shows an emission spectrum of an LED according to a fifth Example of a fifth embodiment of the present invention. The LED was manufactured as follows:
- a powder mixture of 20% (Y 5 Gd) 3 Al 5 Oi 2 ICe and 80%Y 2 SiO 5 :Eu were suspended in a fluid silicon precursor compound. A drop of this silicon precursor was placed on a Chip emitting light of the wavelength 465 nm and the silicon polymerized. The LED is then sealed with a plastic lens.
- Fig. 11 shows a good optical characteristic with a T c value of 3000K.
- Fig. 12 shows an emission spectrum of an LED according to a sixth
- Example of a sixth embodiment of the present invention The LED was manufactured as follows:
- a powder mixture of 20% (Y,Gd) 3 Al 5 Oi 2 :Ce and 80% LaOChEu were suspended in a fluid silicon precursor compound. A drop of this silicon precursor was placed on a Chip emitting light of the wavelength 465 nm and the silicon polymerized. The LED is then sealed with a plastic lens.
- Eu-doping levels different from 5atom% can be chosen in order to adapt for instance the converting element size or the spectral properties of the converting element to the desired application.
- the light source of this spectrofluorimeter system is a 150W Xe-lamp in an airflow-cooled housing.
- the lamp output is focused on the entrance slit of the excitation monochromator (Bentham) with a focal length of 0.5 m.
- the escaping light from the exit slit of the excitation monochromator is fed into a sample chamber and focused onto the sample material under test via several mirrors. While the sample under test is horizontal orientated the optical axis of the excitation and the emission branch are oriented vertically and nearly parallel. This geometric orientation ensures reliable and quantitative comparative measurements of different samples.
- the sample chamber is coupled optically to the emission monochromator (Bentham, focal length 0.5m) via a mirror system. Detection of the emitted light occurs with a thermo-electrically cooled photomultiplier tube (PMT) unit mounted to the exit slit of the emission monochromator.
- PMT thermo-electrically cooled photomultiplier tube
- the sample under test is shaped as a powder layer of 2 mm thickness and the spot size of the excitation light beam is approx. 2x3 mm 2 .
- the spectral resolution of the excitation and emission branch was in the order of 1-2 nm.
- a 1 nm step size was chosen for the determination of the excitation and emission spectra.
Abstract
Description
Claims
Priority Applications (2)
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JP2008549959A JP2009524212A (en) | 2006-01-16 | 2007-01-10 | Light emitting device having Eu-containing phosphor material |
EP07700560A EP1979439A1 (en) | 2006-01-16 | 2007-01-10 | Light emitting device with a eu-comprising phosphor material |
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EP06100385 | 2006-01-16 | ||
EP06100385.1 | 2006-01-16 |
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WO2007080541A1 true WO2007080541A1 (en) | 2007-07-19 |
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PCT/IB2007/050068 WO2007080541A1 (en) | 2006-01-16 | 2007-01-10 | Light emitting device with a eu-comprising phosphor material |
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US (1) | US7446343B2 (en) |
EP (2) | EP1979439A1 (en) |
JP (2) | JP2009524212A (en) |
KR (1) | KR20080089486A (en) |
CN (2) | CN101370907A (en) |
RU (1) | RU2008133603A (en) |
TW (2) | TW200738847A (en) |
WO (1) | WO2007080541A1 (en) |
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JP2009096986A (en) * | 2007-07-26 | 2009-05-07 | Jiaotong Univ | New phosphor and fabrication of the same |
Also Published As
Publication number | Publication date |
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JP5628394B2 (en) | 2014-11-19 |
TW200738847A (en) | 2007-10-16 |
JP2014039053A (en) | 2014-02-27 |
US20080023712A1 (en) | 2008-01-31 |
EP1979438A1 (en) | 2008-10-15 |
KR20080089486A (en) | 2008-10-06 |
EP1979439A1 (en) | 2008-10-15 |
JP2009524212A (en) | 2009-06-25 |
US7446343B2 (en) | 2008-11-04 |
CN101370907A (en) | 2009-02-18 |
EP1979438B1 (en) | 2015-08-19 |
TWI422057B (en) | 2014-01-01 |
CN101370906B (en) | 2015-01-28 |
RU2008133603A (en) | 2010-02-27 |
TW200746465A (en) | 2007-12-16 |
CN101370906A (en) | 2009-02-18 |
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