Synthesis of SrGa S :Eu Phosphor and Its Luminescent Properties SrGa S :Eu
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(2) (2002. 1. 18 ). †. †. Synthesis of SrGa2S4 : Eu Phosphor and Its Luminescent Properties Young-Duk Huh*, Jae-Hoon Shim, and Young Rag Do† Department of Chemistry, Dankook University, Seoul 140-714, Korea † Electronic Material Development Team, Samsung SDI, Kyunggi-do 442-390, Korea (Received January 18, 2002). . SrGa S : Eu !"#, $%& '() *+ , -./ 01. 2345 SrGa S : Eu6 7 8 SrCO , Ga O , 9+/ Eu O : H S; Ar < : =>?@ A /B)A CD /E3,F5 7 G1. H IJ)A SrS, Eu KL, 9+/ Ga KL6 'M 3 , NMA SrGa S : Eu : 7 G1. # F6 OP8 Ar < Q R STU V 6 H S: WX Y Z#1. SrGa S : Eu 6 7 [\ ] ^_G1. : SrGa S : Eu , ] 2. 4. 2 4. 2. 3. 2. 3. 2. 3. 2. 4. 2. 2 4. 2. 4. ABSTRACT. SrGa2S4 : Eu is a green emitting phosphor which is applied for field emission display, and cathodoluminescence. Conventionally, SrGa2S4 : Eu is synthesized by solid state reaction, in which a mixture of SrCO3, Ga2O3, and Eu2O3 is fired at high temperatures under flowing H2S and Ar gases. In this study, SrGa2S4 : Eu phosphor is synthesized by using a decomposition method, where SrS, Eu complex, and Ga complex are used. The advantage of this method is that toxic H2S gas and Ar gas are not used. The synthetic conditions and luminescent properties of SrGa 2S4 : Eu phosphor are also investigated. Key words: SrGa2S4 : Eu phosphor, luminescent property. . 2. !"#(FED, field emission display), $%& (CL, cathodoluminescence) '( `) *+ W-./ 01. a
(3) bX SrGa S : Eu8 4c /E3,F 5 7 G1. d, SrCO , Ga O , Eu O : ef Lg W-/ hi6 -jk: l< m n h 900 C )A h 2oi C p 7 m1. #q 500 C #E) A H S < : r =>?s tc uvwx y SrGa2S4 : Eu. 1-3. 2. 4. 3-5. 3. 2. 3. 2. 3. o. o. 2. z{(strontium thiogallate, SrGa S ) 7 /, 500 C #)A Ar < : =>?sA uvwx yz{# |. Z SrGa S : Eu 6 } kc Eu #B# |.sA Eu 5 . Z~ X m1. #; 8 7 8 QR STU V 6 H S < : W-M( , H S < +) 8 f>(R m1. k SrGa S : Eu : 7 0 # ) m.s 01. SrGa S : Eu : 7 01@ SrGa S : Eu p '() # ,- Z 4. o. 2. 2+. 4. 3+. 2. 2. 2. 2. 2. 164. 4. 4. 4.
(4) SrGa2S4 : Eu. . #1. UA H S < : W-X Y/ SrGa S : Eu : 7 F6 8 45 1. Sastry `8 SrCl , GaCl , EuCl : Na S; 3,o SrGa S : Eu : 7 G1. # 7 m 6 f H S < : W-p 7 m 6 f6 40% ) .X Y1. H S < : W-X Y¡XR ¢£# ¤8 SrGa S : Eu : ¥ < ¦§1. Kobayashi ` 8 EuGa S : Ce; CaGa S : Ce : #y¨©ª# u(dithiocarbamate) «r KL W-p 7 ¬1. 9+/ Jiang `8 #; 8 F5 SrGa S : Eu : 7 G1. #6 7 F8 V< c H S: W-X Y¡XR 7L6 | Xf ® MA Ar < : =>?sA 7L 7 ¬1. 9+/ 7 ) W-¯ °4 [\R ±²) ³: G5´, sµ p <X °4 [\ ¶8 X) m IJ ³.X Y¡1. H ±²)A H S; Ar < : · W-X Y/ SrGa S : Eu : 7 / ¸, 7 6 °4 [\ ¹c/ m1. H I J)A H S; Ar < : · W-X Y5 º (tube furnace) ») ¼½ W-. E (box furnace): W- 01. UA H IJ6 7 F8 fH4c : W-p SrGa S : Eu : ¾5 7 0 F km1. 2. 2. 2. 3. 3. 165. 4. 2. 7. 2. 4. 2. 2. 2. 4. 2. 4. 2. 4. Fig. 1. Flow chart of a synthetic method.. 7. 2. 4. 8. 2. 2. 2. 4. 2. 2 4.
(5) ¿8 Fig. 1) ´ÀÁ§1. H ¿8 #~ <T: W-¬5¸ ÁÂ6 ~<T) 7 ) Ãm o : ħ/, ÅÂ6 ~<T) |: Xf ® MA Æǯ Á ~<T6 ÅÂ) } È ÉÊ Ä§ 1. H ¿)A 7 / SrGa S : Eu 6 ¹m J[Ë6 ³a8 Sr Ga S : Eu #1. Eu #B# Sr ®Ì) ÌÍ. 7 ) 0.95 mol SrS, 2.0 mol Ga KL, 0.05 mol Eu KL W-G1. 9 +/ p'6 y(sulfur) hi6 -jk(flux): l<m n C p : 7 m1. #q Ga KL, Ga [(CH ) NCS ] 8 Ga(NO) ; (CH ) NCS Na6 Î: 1:35 Ïm Z L) c n Ðp 7 G1. Ñm Eu KL, [(CH ) N]{Eu[(CH ) NCS ] }, 8 (CH ) NCl, Eu(NO) , (CH ) NCS Na: 1:1:4 L) c n ¥s 2. 4. 2+. 0.95. 2. 4. 0.05. 2+. 3 2. 2 3. 3. 3 4. 3. 3 2. 3 2. 3 2. 2. 2. 2 4. 3 4. Ò ÐL#1. 7 °4 [\ ¶/ W-. p '6 y(sulfur)6 Ó, -jk6 ÔÕ, -jk6 Ó, 9+ / C B~ ` Öo×@A ¿ G1. 7 ¯ SrGa S : Eu 6 ØJ[ Ù ] 8 SDI)A H S; Ar < : W-p RÚ SrGa S : Eu ; G1. H S; Ar < : W-p RÚ SrGa S : Eu 6 7 8 SrCO , Ga O , Eu O : ef Lg W-/ hi6 NaBr: l< m n h 800 C)A h 2oi C p 7 G1. #q 500 C #E)A H S < : r =>?/, 500 C #) A Ar < : =>?§1. 7 ) W-¯ (furnace) E (Siliconit Muffle furnace, Model IS-F105)#1. H S; Ar < : W-p 7 q º (Lindberg model BF51664PC): W-G1. 6 ] 8 ' ~ (photoluminescence spectroscopy): W-p ¹cG1. pf) W-¯ Û8 500 W6 Xe ÜÝ#1. o 6 ³@) Þ5 pf ßs ?§5¸, ^ ®Ì pf ) MA 45 G1. W-¯ OÌ 0.275 m6 OÌ(triple grating monochromator, Acton Research Co): WG/, àáº(photomultiplier tube)8 PHV 400 W-G1. 6 â 6 Ø Ù ØJ[: ¹ cf ®MA X-& ãä 'åf(X-ray diffractometer, Rigaku, Model D/Max-3C): W-G1. 2. 4. 2. 2. 4. 2. 2. 4. 3. 2. 3. o. 2. 3. o. o. 2. 2. o. H ¿8 #~<T: W-¬5¸ ÁÂ6 ~<T ) 7 ) Ãm o : ħ/, ÅÂ6 ~<T) Journal of the Korean Chemical Society.
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(8) . 166. |: Xf ®MA } È Ä§1. H ¿)A SrGa S : Eu 7 8 4äm Ó6 SrS, Ga KL, Eu K L, -jk, 9+/ p'6 S6 Ó Ïp 850 C) A 2oi C G1. #q Ga KL, Ga[(CH ) NCS ] , 8 Ga(NO) ; (CH ) NCS Na6 Ð5 ¥§1. 9+ / Eu KL, [(CH ) N]{Eu[(CH ) NCS ] }8 (CH ) NCl, Eu(NO) , (CH ) NCS Na6 Ð5 ¥§1. SrGa S : Eu «r KL6 'M 3, NMA 7 # ¯1. H ¿)A H S; Ar < : W- X Y/ SrGa S : Eu : 7 Z) æ4 ç§1. ¿)A p'6 y(sulfur) ÁÂ6 ~<T) l<p 7 )A è'm y ép ê. m SrGa S : Eu: 7 / m1. W-¯ SrS6 Î : fë5 p'5 l< y6 Ó8 50%Âì 500%bX [äG1. l<m y6 Ó) í 6 îuï Fig. 2) ´ÀÁ§1. W-¯ y6 Ó# 400% 2 q <O ¤8 f: ¥§1. U A 4äm Ó6 y l< Z# SrGa S : Eu : 7 m ð Z ¹cG1. H ¿)A H S; Ar < : W-X Y5 4 äm Ó6 y l< Z# ñm 6 Ø ¥ m ð +U ò¯1. ñm 6 ØJ[: ¥X ó@ f< ôI½ õs g Z#1. l<m y6 Ó) í 6 X-& ãä îuï Fig. 3) ´ÀÁ§1. 9ö)A ¹c 0÷# W-¯ y6 Ó# 200%bX ñm SrGa S : Eu : 7 # .X Y$ ¹cG1. 300%Âì 500%bX 6 øm ~6 Ø <ù ú 2. 4. o. 3 2. 3. 3 2. 2. 3 4. 3. 2. 3 2. 2 3. 3 2. 2 4. 3 4. 2. 4. 2. 2. 2. 4. 4. 2. 4. 2. 2 4. Fig. 2. Emission spectra of SrGa2S4:Eu at different sulfur concentrations; (a) 50%, (b) 100%, (c) 200%, (d) 300%, (e) 400%, and (f) 500%. 2002, Vol. 46, No. 2. Fig. 3. X-ray diffraction patterns of SrGa2S4:Eu at different sulfur concentrations; (a) 50%, (b) 100%, (c) 200%, (d) 300%, (e) 400%, and (f) 500%.. 01. UA îuï5 ¥8 Ø: ûü ÐM ë1. 6 X-& ãä îuï5Âì 7 ¯ 6 Ø ¹c# <ý1. Ø # ¤5 @ 6 f< ¤SXXR #m Z8 45 <ý´, ¾45 'å Z8 þ <ý1. UA X-& ãä îuï8 ÿ[ #ì W-./ ¹m f6 îuï5 Âì ¹cM(R m1. 6 7 )A 2345 -jk: W-m1. -jk6 W-8 6 7 B~: QR ST U, 6 Ø ¤ R ð m1. H IJ)A~ 6 7 ) 4<X6 -jk: W- G1. Fig. 4)A ¹c 0÷# KBr: -jk W-¬ q <O ¤8 Ø: ¥§1. #q W-¯ p. Fig. 4. Emission spectra of SrGa2S4:Eu using different fluxes; (a) NaBr, (b) NaCl, (c) KBr, and (d) Li2CO3..
(9) SrGa2S4 : Eu. . Fig. 5. Emission spectra of SrGa2S4:Eu with different KBr amounts; (a) 0.2%, (b) 0.5%, (c) 0.8%, (d) 1.0%, and (e) 1.5%.. 167. Fig. 7. X-ray diffraction patterns and Miller indices of SrGa2S4:Eu synthesized by (a) using H2S and Ar gases flowing and (b) decomposition method without gas flowing.. } È5 É ÅÂ ~<T: ) Ä/ 900 C 2 oi C m1. #; 8 F5 7 m ; H S; Ar < : W-p /E3,F5 7 m ; G1. Fig. 78 6 6 -& ã ä îuï#1. H IJ F5 7 m ; /E3,F5 7 m < 8 Ø J[: < ù ú 01. SrGa S W Ø #¸, Ø E a=20.84 , b=20.50 , 9+/ c=12.21 #1. EuGa S ~ SrGa S ; 8 W Ø #¸, Ø E a=20.72 , b=20.40 , 9+/ c=12.20 #1. EuGa S ; SrGa S # 8 Ø J[) ØE~ 6 ø, Sr Ga S :Eu 6 Ø8 SrGa S ; 6 1/ ò¯1. UA H ±²6 SrGa S : Eu 6 Æ X(Miller index) SrGa S 6 Ø6 Æ X:
(10) / p G1. H ¿)A 7 m SrGa S : Eu SrGa S ; 6 8 X-& ã ä îuï6 ÿ#/ 05, H IJ6 7 F5 SrGa S : Eu < 7 ¹c 0§1. 9´ » $(S/N) ÿ@ H S; Ar < : W-p ¥8 < Ø # ¤1. UA H IJ6 7 F5 7 m < S? ñ ¯ : ¥X ó 6m1. Fig. 88 SrGa S : Eu 6 pf Ù îu ï#1. pf îuï8 O(λ ) 535 nm) / / G1. 9+/ îuï8 pf O (λ ) 465 nm) // G1. SrGa S :Eu 320~480 nm6 8 ð)A < 2s1. o. 2. 2. 2. Fig. 6. The emission intensities SrGa2S4:Eu at different firing temperatures; (a) 750 oC, (b) 800 oC, (c) 850 oC, (d) 900 oC, (e) 950 oC and (f) 1000 oC.. '6 y8 Ó8 400%5 /o1. Fig. 5 KBr6 W-¯ Ó) í îuï ÿpë1. UA KBr6 Ó# 0.5%(w/w)2 q f< <O ¤8 Z ú 01. # q KBr6 Ó6 ³a8 W-¯ SrS, Ga KL, 9+/ Eu KL6 7) m (weight ratio)#1. 1í -jkÿ1 KBr# ¤ 8 ð X ¹½ ú < ¦5´, KBr: W -@ 6 Ø # ¤Sù ú 0§1. Ñm, H IJ)A 7 B~: Öo×@A : 7 G1. Fig. 68 p B~)A 7 ¯ 6 îuï6 f: ´ÀÁ§1. 900 C# ° 4 7 B~ ¹cG1. )A6 °46 7 F +@ 1$ 1. SrS, Ga KL, Eu KL ) 400% p'6 y -jkc KBr: 0.5%(w/w) l < m Z ÁÂ~<T) Ä/, Á ~<T6 ÅÂ: o. 4. 2. 4. 4. 5. 2 4. 2. 4. 0.95. 2. 4. 0.05. 2. 4. 2 4. 2. 2 4. 2. 4. 4. 2 4. 2. 2 4. em. ex. 2. 4. Journal of the Korean Chemical Society.
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(13) . 168. IJ6 F8 * n SrGa S : Eu : 7 p W- Z#1. UA 5 SrGa S : Eu !"#, $%& , 9+/ 1 # '( `)A # IJ Z#1. 2 4. 2. 4. !"#, $%& '() *+ ,-./ 01.. 4c SrGa S :Eu6 7 8 SrCO , Ga O , 9+/ Eu O : H S; Ar < : =>?@A CD /E3 ,F5 7 G1. 9´ V< c H S: + M( SrGa S : Eu6 7 8 +1. H I J)A SrS, Eu KL, 9+/ Ga KL6 'M 3, NMA SrGa S : Eu : 7 G1. # F6 OP8 V 6 H S< QR STU Ar < ~ W- X Y5, 7 # i/ ®¿X< Y1. °46 7 F8 SrS, Ga KL, Eu KL) 400% p'6 y -jkc KBr: 0.5%(w/w) l< m Z ÁÂ~<T) Ä/, ÁÂ ~<T6 ÅÂ: } È5 É ÅÂ ~<T: 900 C 2oi C Z5 ,·-1. 9+/ SrGa S : Eu : 1# '() ,-# <ý ¹cG1. SrGa2S4 : Eu. 2. 2. Fig. 8. Excitation (λem=535 nm) and emission (λex=465 nm) spectra of SrGa2S4:Eu synthesized by (a) using H2S and Ar gases flowing and (b) decomposition method without gas flowing.. 3. 4. 3. 2. 3. 2. 2. 2 4. 2 4. ð)A6 tc SrGa S 6 Û < . ~ #(valance-to-conduction band transition) q²) 2s1. 3@) 535 nm ð)A6 8 Eu 6 4f 5d 4f #) 6MA 2s1. H IJ )A îuï q 465 nm: pf O5 G1. 9 # 465 nm 1# (LED, light emitting diode)) SrGa S : Eu : !"@ # ¯1. #$<X ð)A < 0/, 4 : 1# ) : !"@ 4# ¯1. UA 1# ) SrGa S : Eu; 4 : % 4ä½ !"@ )A ´ 4# ¯1. 1# )A ´ # ê ½ .X Y~ 4 6 Ó [ä@ , , 9+/ 4# t ç . O 1# : R 0 ¯ 1. UA 1# 6 Oc 465 nm: pf O5 G1. H IJ6 Ø SrGa S : Eu O 1# : R 4äm < ¹cG1. O 1# ) ºm Á-8 a
(14) IJ #/, & ±² ³ '#1. #X(5 Fig. 8)A ÿ@ H ¿ F5 7 m 6 f H S; Ar < : W-p ¥8 6 f6 h 93%#1. hi6 ¢ £8 õsXXR, H IJ6 7 F8 Av)A )é m ©; # p <X OP <X/ 01. UA H 350 nm. 2+. 2 4. 6. 1. 7. 2 4. 2 4. 2 4. 2. 2002, Vol. 46, No. 2. 2. o. 2 4. 1. Yang, S.; Zhang, F.; Stoffers, C.; Jacobsen, S. M.; Wagner, B. K.; Summers, C. J.; Yocom, N.; McClelland, S. Appl. Phys. Lett. 1998, 72, 158. 2. Stoffers, C.; Yang, S.; Jacobsen, S. M.; Summers, C. J. J. SID. 1996, 4, 337. 3. Do, Y. R.; Bae, J. W.; Kim, Y.; Yang, H. G. Bull. Kor. Chem. Soc. 2000, 21, 295. 4. Eichenauer, L.; Jarofke, B.; Mertins, H.C.; Dreysig, J.; Busse, W.; Gumlich, H. E.; Benalloul, P.; Barthou, C.; Benoit, J.; Fouassier, C.; Garcia, A. Phys. Stat. Sol. 1996, A153, 515. 5. Peters, T. E.; Baglio, J. A. J. Electrochem. Soc. 1972, 119, 230. 6. Sastry, I. S. R.; Bacalski, C. F.; McKittrick, J. J. Electrochem. Soc. 1999, 146, 4319. 7. Kobayashi, T.; Uheda, K.; Naruke, H.; Yamase, T. Chem. Let. 1996, 26, 567. 8. Jiang, Y. D.; Villaobos, G.; Souriau, J. C.; Paris, H.; Summers, C. J.; Wang, Z. L. Solid State Commun. 2000, 113, 475..
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