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1 14 Preparation and characterization of barium strontium titanate thin films
2 X X LCR Sawyer-Tower (Ba x Sr 1-x )TiO SrTiO Pt(100)/MgO(100) Pt(100)/MgO(100) (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO 3
3 (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO Ba/(Ba+Sr) x Sr 1-x )TiO (Ba 0.6 Sr 0.4 )TiO (Ba 0.6 Sr 0.4 )TiO Ti/(Ba+Sr) Ti/(Ba+Sr) x 1-x )TiO Ti/(Ba+Sr) Ti/(Ba+Sr) Ti/(Ba+Sr) (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO
4 1 1.1 (FeRAM)Dynamic Random Access Memory(DRAM) (1) MOS FeRAM (2) (Pb(Zr,Ti)O 3 ) 1Gbit DRAM ((Ba x Sr 1-x )TiO 3 ) (3) 1.2 ( ) ABO A O B P E
5 cf (P r )b E=0 (P s )dg (E r ) 2 2 (4) T c Curie-Weiss (3) A B O ((Ba x Sr 1-x )TiO 3 ) 120 (Pb(Zr,Ti)O 3 ) 400 (Ba x Sr 1-x )TiO 3 ( 10,000 )DRAM (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 BaTiO3 SrTiO3 Ba/(Ba+Sr)Ti/(Ba+Sr) (Ba x Sr 1-x )TiO 3-2 -
6 (Ba x Sr 1-x )TiO 3 Ba/(Ba+Sr) Ti/(Ba+Sr) BaTiO 3 (Ba x Sr 1-x )TiO 3 (5),(6) A Ba Sr Ba/(Ba+Sr) Pt (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO X 3 (Ba x Sr 1-x )TiO 3 (x=1.00.5) 4 (Ba x Sr 1-x )TiO 3 Pt(100)/MgO(100) Ba/(Ba+Sr) 5 Ti/(Ba+Sr) 6 (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO
7 (1) P. Y. Leasaichene, et al IEDM Tech. Dig. 831 (1994) (2), IC RRAM,, (1996) (3), DRAM, (4) pratt, I.H. Proc, IEEE, 59, 1440, 1971 (5),,, (1997) (6), (Ba,Sr)TiO 3 DRAM,, (1993) - 4 -
8 (1) 2.1
9 - 6 - (2) (BaxSr1-x)TiO3 Pt RF (BaxSr1-x)TiO3 A B Pt Pt
10 - 7 - Ar O2 L C2 C1 (13.56MHz 2.2 (a) A B A B (b) B A B 2.3
11 - 8 - ) ( ) ( ) ( = = s m K T M Pa P nv J e e T(K) Pe(Pa) Je (M T a (a1)) Pe nm (3) (W)W Au 2.1 Au Au WMo 2.4 W
12 X X X X X X X 3 X X? d X? 2dsin?n? 2.5 X X X TiO2 2.5 X
13 X X X X X X X 2 X X X ( ) X X X X NaI X 2.6 X 10
14 ( )? µ? s? i±? µ? i 0 ( ) (4) (5) (514.5 nm) nm 2 ( ) TO
15 12 CCD nm /mm 1800 /mm CCD PC 2.7
16 (SEM)nm (SE) ( BSE) X ( ) (6) SEM 2.9 1kV40kV nm (AFM) AFM SEM
17 2 U(r) Lenard-Jones σ U( r) = 4ε r 12 σ r es r (7) 2.10 AFM AFM 3 (8) 100µm200µm 10 9 N/ AB (A-B) Z xy xy z 3 Ret CPU CRT Z 6 A B XY 2.10AFM 14
18 2.3.4 X X nm X X X X (9) 2.12 X X X d? X 2.11 X 2.12 X ( ) 15
19 tan X R Z R X jx R Z + = = + = θ tan B G Y G B jb G Y + = = + = φ LCR LCR LCR Z? Z Z Z (O)? (deg.)r (O)X (O) Y Y Y (O)G (S)B (S) 2.13 Z Y 2.13 Z Y j Z Z X R Y Y G B j
20 17 2 V I V I?? LCR (ESR) (10) LCR HCUR ( )HPOT ( High )LPOT ( Low )LCUR ( )GUARD
21 Sawyer-Tower Sawyer-Tower Sawyer-Tower 2.15 P E (11) O-A-B-M M 0 OR 0 MB OS OF( ) 0 (F-M ) M -R -B 2.15P-E M R F M E P F R B S
22 P-E Sawyer-Tower 2.16 Cx C0(C0 Cx) C0Cx C0 Q V = Q C 0 Vx Cx +q -q +q V C0C0Cx -q Vx 2.16Sawyer-Tower 19
23 2.4 (1),,, (1991) (2),,, (1998) (3),,, (1994) (4),,, (1995) (5),,, (1988) (6), QA,, (1996) (7), RD, vol.31 No.2 (1996.6) (8),,, (1995) (9),,, (1996) (10),, 70, 11, (2001) (11), 20
24 3 (Ba,Sr)TiO3 3.1 (1) ((BaxSr1-x)TiO3) (Pb(Zr,Ti)O3) (2) (SrBi2Ta2O9) (3) Pb Bi LSI Si (4) (BaxSr1-x)TiO3 MOCVD (BaxSr1-x)TiO3 (BaxSr1-x)TiO3 RF RF (BaxSr1-x)TiO3 21
25 3.2 SrTiO 3 pellet BaTiO 3 (5)(6) 3.1 BaTiO3 10mm SrTiO3 SrSrO SrSrO SrTiO SrTiO3 BaTiO3 SrTiO3 (BaxSr1-x)TiO3 MgO(100)MgO(100)(Ba,Sr)TiO3 1.0 (7) Si (100) (8) MgO Si MgO 3.2 BaTiO3 SrTiO3 070 Ba/(Ba+Sr) area ratio of STO/BTO target (%) 3.2BaTiO3 SrTiO3-22 -
26 MgO (BaxSr1-x)TiO3 Ba/(Ba+Sr)SrTiO3 Sr SrTiO3 60 Ba/(Ba+Sr) SrTiO3 3.4Pt(100)/MgO(100) (9) Pt MgO Pt 3.1 (BaxSr1-x)TiO3 c (001) Pt 3.1Pt(100) Pt (100) Substrate MgO(100) Pt Temperature 700 Pressure 1.0 Pa (111) Rf Power 70 W Ar : O2 1 :1 Thickness 100 nm MgO (100)
27 3.5Pt(100)/MgO(100) (BaxSr1-x)TiO3 Pt(100)/MgO(100)Ba0.9Sr0.1TiO3Ba0.5Sr0.5TiO3 Ar/O2 Ba0.8Sr0.2TiO3 Ar Thornton 4 (10) 3.3 Thornton 1(ZONE-1) Ar (TS/TM<0.3) 3.3Thornton T(ZONE-T) Ar (TS/TM<0.3) 2 1 T(Transition- ) 3(ZONE-2) TS/TM>0.3 1 T T 4(ZONE-3) TS/TM> TS
28 Thornton 0.3<TS/TM<0.5 (Ba,Sr)TiO RF Power 90W ( T-S ) Ba/(Ba+Sr) Ba/(Ba+Sr) Ti/(Ba+Sr) Ti/(Ba+Sr) Ba0.8Sr0.2TiO3 0.5 BaTiO3 SrTiO T-S PaAr/O2 3/1 Ba/(Sr+Sr)T-S 0.8 Ti./(Ba+Sr)T-S 55mm Substrate distance (mm) 3.4 Ti mm 60 mm MgO(200) (101) Pt(200) (002) Intensity (202) TiO 2 (003) (001) (202) q (deg.) Intensity (arb. units) 55 mm (003) Intensity (202) (003) 55 mm 50 mm q (deg.) 50 mm (202) Intensity q (deg.) TiO 2 (003) 3.5T-S XRD 3.6 XRD 2 q (deg.)
29 T-S XRD 3.6 XRD T-S 55mm XRD (Ba0.8Sr0.2)TiO3 T-S 50 60mm TiO2 TiO2 3.4 T-S 50 60mm Ti Ti TiO2 3.7 XRD FWHM T-S 55mm (001) Ba0.8Sr0.2TiO3 Pt XRD Pt T-S 55mm (001)/(001)+(101) FWHM Substrate distance (mm) 3.7XRD FWHM Ar O2 Ba0.8Sr0.2TiO3 T-S 55mm 0.5Pa 3.8 Ar O2 Ar O2 T-S 1.4 Ba/(Sr+Sr) Ti/(Ba+Sr) 0.8 O2 25 Ba/(Ba+Sr) O 2 /(Ar+O 2 ) (%) Ba/(Ba+Sr) Ti/(Ba+Sr) 3.8Ar/O Ti/(Ba+Sr)
30 O (11) 3.9 XRD O2 FWHM (001)/(001)+(101) O 2 /(Ar+O 2 ) (%) 3.9XRD FWHM FWHM 3.10 SEM SEM 25 O 2 : 20 % O 2 : 25 % O 2 : 33 % O 2 : 50 % O SEM Ba0.8Sr0.2TiO3-27 -
31 T-S 55mmAr/O2=3/ Ba/(Ba+Sr)1.5Pa 1.5Pa Pa Ba/(Ba+Sr)=0.72 Ti/(Ba+Sr) BaSrTiO (12) O Ti O Ti (001)/(001)+(101) FWHM XRD FWHM Ba/(Ba+Sr) Pressure (Pa) 3.12 XRD 3.13 SEM FWHM 2.5Pa 1.5Pa 1Pa 0.5Pa SEM Ba/(Ba+Sr) Ti/(Ba+Sr) Pressure (Pa) Ti/(Ba+Sr)
32 0.5Pa 2.5 Pa 1.5 Pa 1.0 Pa 0.5 Pa SEM BaTiO3 SrTiO3 Pt(100)/MgO(100) (BaxSr1-x)TiO3 (Ba0.8Sr0.2)TiO3 3.2 BaTiO3 (Ba0.9Sr0.1)TiO3 (Ba0.8Sr0.2)TiO3 (Ba0.7Sr0.3)TiO3 (Ba0.6Sr0.4)TiO3(Ba0.5Sr0.5)TiO3 3.2 (BaxSr1-x)TiO3 (Ba0.9Sr0.1)TiO3 Substrate Pt(100)/MgO(100) STO pellet/bto target 30 % Temperature 546 T-S distance 50 cm RF Power 90 W Pressure 0.5 Pa Ar : O2 3 :1 (Ba0.8Sr0.2)TiO3 Substrate Pt(100)/MgO(100) STO pellet/bto target 36 % Temperature 546 T-S distance 55 cm RF Power 90 W Pressure 0.5 Pa Ar : O2 3 :1-29 -
33 (Ba0.7Sr0.3)TiO3 Substrate Pt(100)/MgO(100) STO pellet/bto target 47 % Temperature 546 T-S distance 60 cm RF Power 90 W Pressure 1.5 Pa Ar : O2 3 :1 (Ba0.6Sr0.4)TiO3 Substrate Pt(100)/MgO(100) STO pellet/bto target 53 % Temperature 546 T-S distance 55 cm RF Power 90 W Pressure 0.5 Pa Ar : O2 3 :1 (Ba0.5Sr0.5)TiO3 Substrate Pt(100)/MgO(100) STO pellet/bto target 54 % Temperature 546 T-S distance 50 cm RF Power 90 W Pressure 1.5 Pa Ar : O2 3 :1 BaTiO3 Substrate Pt(100)/MgO(100) STO pellet/bto target 0 % Temperature 546 T-S distance 57 cm RF Power 250 W Pressure 0.8 Pa Ar : O2 3 :1 30
34 (1) K. Koyama, T. Sakuma, S. Yamammichi, H. Watanabe and H. Aoki IDEM ~826. (1991) (2) Won-Jae Lee, Young-Min Kim and Ho-Gi Kim Thin Solid Films ~79 (1995) (3) H. N. Al-Shareef, D. Dimons, T. J. Boyle, W. L. Warren, and B. A. Tuttle Appl. Phys. Lett. 68 (5) (1996) (4) S. Matsubara, T. Sakuma, S. Yamamichi and Y. Miyasaka. Mat. Res. Soc. Symp. Proc. 200, 243 (1990) (5) T. hata, S. Kawagoe, W. Zhang, K. sakai and Y. Yoshioka Vacuum Vol.51 No. 665~671 (1998) (6) Jr-Deok Kim, S. Kawagoe, K. Sasaki and T. Hata Jpn. J. Appl. Phys. Vol.38 (1999) (7),,, (1999) (8) Y. Yoshimura, K. Hamaishi, Y. Kamino and S. Nakamura Sutudy of substrate and electrode materials on ferroelectric films (1999) (9),, 70 9 (2001) (10),,, (1998) (11),,, (1991) (12) Ludmila Eckertova,,, (1994) 31
35 4 (BaxSr1-x)TiO3 4.1 LSI Dynamic Random Access Memory(DRAM) (1) DRAM Pb(Zr,Ti)O3(PZT)SrTiO3 (BaxSr1-x)TiO3 (BaxSr1-x)TiO3 SrTiO3 Ba Sr PZT (2) (Ba,Sr)TiO3 BaTiO3 SrTiO3 Ba/(Ba+Sr) Ba/(Ba+Sr)(BaxSr1-x)TiO3 (BaxSr1-x)TiO3 Ba/(Ba+Sr)(BaxSr1-x)TiO3 4.2(BaxSr1-x)TiO3 32
36 Pt(100)/MgO(100)x=1.0~0.5 (BaxSr1-x)TiO3 XRD (001) (002) MgO(200) Pt(200) BaTiO BaTiO3 (003) (Ba0.9Sr0.1)TiO3 (Ba0.8Sr0.2)TiO3 ( (Ba 0.9 Sr 0.1 )TiO 3 =1.0~0.8) (001) c (Ba0.7Sr0.3)TiO3 (Ba0.6Sr0.4)TiO3 Intensity (arb. units) (Ba0.5Sr0.5)TiO3 (x=0.7~0.5) (Ba 0.8 Sr 0.2 )TiO 3 (Ba 0.7 Sr 0.3 )TiO 3 (110) (100) (220) (Ba 0.6 Sr 0.4 )TiO 3 (110) Pt (Ba 0.5 Sr 0.5 )TiO 3 (BaxSr1-x)TiO3 (001) (100) x=0.7~ (BaxSr1-x)TiO3 Glass (BaxSr1-x)TiO3(x=1.0~0.5)XRD q (deg.) XRD (BaxSr1-x)TiO3 (BaxSr1-x)TiO3 BaTiO 3 (112) (101) (001) (002) (111) ( ) XRD BaTiO3 Sr (110) Intensity (relative) (Ba 0.8 Sr 0.2 )TiO 3 (Ba 0.7 Sr 0.3 )TiO Pt(100) (Ba 0.6 Sr 0.4 )TiO 3 (101) (Ba 0.9 Sr 0.1 )TiO 3 (Ba0.5Sr0.5)TiO3(x=1.0~0.5)x=1.0~0.8 (001) (Ba 0.5 Sr 0.5 )TiO 3 (200) x=0.7~ q (deg.) Sr 4.2(BaxSr1-x)TiO3/Glass (110) XRD 33
37 Intensity (001) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO 3 (Ba 0.7 Sr 0.3 )TiO 3 (Ba 0.6 Sr 0.4 )TiO 3 (Ba 0.5 Sr 0.5 )TiO 3 Lattice Parameter (nm) Tetragonal Cubic a axis c axis (100) q (deg.) (Ba x Sr 1-x )TiO 3 (x from 1.0 to 0.5) 4.3XRD Ba Sr (BaxSr1-x)TiO3 4.1 XRD (BaxSr1-x)TiO3 Sr 0.7 x0.5 (001) (100) XRD 2? a c 4.4 x0.8 a Sr x0.7 a (c/a)1 x=0.8~0.7 Sr SrTiO3 4.3(BaxSr1-x)TiO3 (BaxSr1-x)TiO3(x=1.0~0.5) 4.5 E(TO) cm cm cm -1 A1(TO1) A1(TO2) A1(TO3) (3) A1(TO1)A1(TO2) 34
38 4.6 A1(TO2) A1(TO1) A1(TO2) TiO6 Ba Sr (4) Ti 4+ Ba 2+, Sr 2+ O 2- Intensity (arb. units) E A 1 (TO 1 ) 1 (TO 1 ) A 1 (TO 2 ) A 1 (TO 3 ) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO 3 (Ba 0.7 Sr 0.3 )TiO ;; (Ba 0.6 Sr 0.4 )TiO (Ba 0.5 Sr 0.5 )TiO 3 - A1(TO1) A1(TO2) 4.5(BaxSr1-x)TiO3 4.6A1(TO1)A1(TO2) 4.5 (BaxSr1-x)TiO3 Sr Sr Ti (4) (BaxSr1-x)TiO3 4.7 (BaxSr1-x)TiO3 (x=1.0~0.8) A1(TO1)A1(TO2) Raman shift (cm -1 ) A1(TO1) x= x<0.8 (Ba0.5Sr0.5)TiO3 A1(TO1) Raman Shift (cm -1 ) A 1 (TO 2 ) A1(TO2) x=1.0~0.7 x< A1(TO1),A1(TO2) 160 (Ba x Sr 1-x )TiO 3 (x from 1.0 to 0.5) A 1 (TO 1 ) 35
39 A1(TO1) A1(TO2) 0.6 Ba/(Ba+Sr) 4.8 A1(TO2) A1(TO1) x=1.0~ A1(TO1)A1(TO2) x<0.7 Sr A1(TO2) Sr A1(TO2) A1(TO1)A1(TO2) 4.7 A1(TO1)A1(TO2) Ba/(Ba+Sr)x=0.5 A1(TO2) A1(TO1) A1(TO1) A1(TO2) 2 x=0.7 A 1 (TO 2 )/( A 1 (TO 1 )+A 1 (TO 2 ) ) (Ba x Sr 1-x )TiO 3 (x from 1.0 to 0.5) 4.4(BaxSr1-x)TiO ()
40 (6) G (7) (8) 4.9 (BaxSr1-x)TiO3(x=1.0~0.5) E 1 (TO 1 ) 4.7 x= x< Raman Shift (cm -1 ) (Ba x Sr 1-x )TiO 3 (x from 1.0 to 0.5) 37
41 ( ) 4.9 ( ) (BaxSr1-x)TiO3 (x=1.0~0.5) Ba Sr A 4.9 Sr (BaxSr1-x)TiO3 XRD x=0.8~ Ba/(Ba+Sr) (BaxSr1-x)TiO3 (x=1.0~0.5) Pt(100)/MgO(100) (BaxSr1-x)TiO3 (x=1.0~0.5) 600 Au 4.10 Ba/(Ba+Sr) Sr Dielectric Constant Ba/(Ba+Sr)= Ba/(Ba+Sr)4.10Ba/(Ba+Sr) (BaxSr1-x)TiO Sr SrTiO3 BaTiO3 (9) BaTiO3 SrTiO3 (BaxSr1-x)TiO3 Sr SrTiO3 (Ba0.6Sr0.4)TiO3 4.2 Sr SrTiO3 (Ba/(Ba+Sr)0.8) (Ba/(Ba+Sr)0.7) SrTiO3 (BaxSr1-x)TiO3 Ba/(Ba+Sr) 0 (Ba x Sr 1-x )TiO 3 (x from 1.0 to 0.5) 38
42 (Ba0.6Sr0.4)TiO3 (BaxSr1-x)TiO3 (x=1.0~0.5) (Ba0.6Sr0.4)TiO Hz~1MHz Dielectric Constant Loss Tangent k 10k 100k 1M Frequency (Hz) 100 1k 10k 100k 1M Frequency (Hz) (Ba0.6Sr0.4)TiO3 (Ba0.6Sr0.4)TiO nm nm 50nm ( > ) ( ) (10)(11) ( ) Dielectric Constant Thickness (nm) (Ba0.6Sr0.4)TiO3 4.14
43 4.6 Ba/(Ba+Sr)(BaxSr1-x)TiO3 4.1 (BaxSr1-x)TiO3 Sr XRD (BaxSr1-x)TiO3 x=0.8~0.7 Ba/(Ba+Sr) (BaxSr1-x)TiO3 Sr SrTiO3 Ba/(Ba+Sr) (Ba0.6Sr0.4)TiO3 4.1(BaxSr1-x)TiO3(x=1.00.5)substrate : Pt(100)/MgO(100) x (XRD) (001) (001) (001) (110) (110) (110) (110) (110) (110) c/a
44 (1) D. E. Kotecki, J. D. Baniecki, H. Shen, R.B. Laibowitz, J.J. Lian and T. M. Shaw IBM. RES. Delop. Vol. 43 No. 3 (1999) (2) R. Liedtke, S. Hoffmann, M. Grossmann and R. Waser STW, :044 (1999) (3) Qin-yu He, Xin-gui Tang, J.X. Zhang and Ming-mei Wu NanoStructured Materials, Vol. 11, No 2, pp , 1999 (4) Shou-Yi Kuo, Wen-Yi Liao and Wen-Feng Hsieh Physical Review B, Vol 64, (5),,, (1997) (6) Yu. I. Yuzyuk, A. Almedia, M. R. Chaves, V. A. Alyshin, I. N. Zakharchenko and E. V. Svirdov phys. Stat. sol. 2222, 535 (2000) (7) R. Naik and J. J. Nazarko Physical Review B Vol. 61, No. 17 (2000) (8) D. A. Tenne, A. M. Clark, A. R. James, K. chen and X. X. Xi Appl. Phys. Lett. Vol. 79, No23, (2001) (9),, (10),, Vol. 17, No. 11, pp. 660~665, (1996) (11) T. Horikawa, N. Mikami, H. Ito, Y. Ohno, T. Makita and L. Sato, IEICE Trans. Elwctron. E77-C p. 385 (1994) 41
45 5 Ti/(Ba+Sr) 5.1 (Ba,Sr)TiO 3 BaOSrO TiO 2 11 Ba/(Ba+Sr), Ti/(Ba+Sr)=1 (Ti/(Ba+Sr)1) 5.2Ti/(Ba+Sr) Ba Sr Ti (Ti/(Ba+Sr)<1)30 XRD Ti/(Ba+Sr)< Ti Intensity BST(101) BaO(200) (Ba 0.8 Sr 0.2) TiO 3 BaO BaO, SrO TiO 2 BaO TiO 2 (Ba 0.8 Sr 0.2) TiO 3 BaO 5.2 Ti (Ti/(Ba+Sr)>1) q (deg.) 5.1Ti XRD Ti/(Ba+Sr)>1.0 XRD 5.1 Ti (Ba 0.8 Sr 0.2) TiO 3 TiO 2 Intensity BST(003) TiO 2 (112) Ti BaO SrO TiO q (deg.) 5.2Ti XRD 42
46 TiO 2 (Ba 0.8 Sr 0.2) TiO 3 TiO 2 Ba,Sr Ti (Ba,Sr)TiO 3 Ti/(Ba+Sr)0.87~1.72 XRD Ti/(Ba+Sr)=1.0 Ba,Sr Ti Ti FWHM (deg.) Ti/(Ba+Sr) 5.3 Ti/(Ba+Sr) FWHM 5.3Ti/(Ba+Sr) Ti/(Ba+Sr) AFM 5.4 Ti/(Ba+Sr)=1.0 RMS Ti Ti/(Ba+Sr)<1.0 Ti/(Ba+Sr)=1.0 Ti Ti/(Ba+Sr)>1.0 Ti/(Ba+Sr)=1.15 RMS Ti Ti/(Ba+Sr)1.4 RMS 43
47 2 µm 2 µm 2 µm Ti/(Ba+Sr)= 0.87 Ti/(Ba+Sr)=0.87 Ti/(Ba+Sr)= 1.15 Ti/(B+Sr)= RMS : 12 µm 2 µm µm 0 2 µm RMS : 5 µm Ti/(B+Sr)=1.72 Ti/(B+Sr)= RMS : 5 µm 2 µm 2 µm 2 µm 2 µm Ti/(B+Sr)=1.4 0 RMS : 10 µm 0 RMS : 5 µm 0 2 µm RMS : 5 µm 2 µm 図 5.4 Ti/(Ba+Sr)の組成ずれに対する AFM 像 5.4 Ti/(Ba+Sr)比の組成ずれによる誘電率の変化 Ti/(Ba+Sr)比の組成ずれに対する誘 電率の変化を図 5.5 に示す それぞれ の膜厚は 200nm とした この図から Ti が不足している膜では誘電率が約 360 で あ り 化 学 量 論 組 成 で あ る Dielectric constant Ti/(Ba+Sr)=1.0(e=320)よりわずかに大 きくなっていることがわかる 一方 Ti/(Ba+Sr) Ti リ ッ チ な 膜 に お い て は 図 5.5 Ti/(Ba+Sr)の組成ずれに対する誘電率 Ti/(Ba+Sr)=1.15 の時 誘電率が 420 で 極大を示し それ以降は誘電率が低下し一定となることがわかった Ti/(Ba+Sr)= の膜において それぞれ(Ba 0.8Sr0.2) TiO 3 と BaO 及び(Ba0.8Sr0.2) TiO 3 と TiO 2 とが混在し結晶性 44
48 (1) 5.4 AFM Ti/(Ba+Sr)=1.0 Ti/(Ba+Sr)= Ti/(Ba+Sr)=1.0 Ti/(Ba+Sr)= BaO TiO 2 (Ba 0.8 Sr 0.2) TiO 3 TiO 2 Ti/(Ba+Sr)=1.15 Ti/(Ba+Sr)=0.87 Ti/(Ba+Sr) Ti/(Ba+Sr) Ti/(Ba+Sr) 4.6 Ti/(Ba+Sr)= Ti (Ti/(Ba+Sr)>1.0)Ba,Sr Ti 5.6Ti/(Ba+Sr) XRD FWHM Ti Ti Ti Loss Tangent Ti/(Ba+Sr) 45
49 4.6 Ti/(Ba+Sr) Ti/(Ba+Sr) (Ba 0.8 Sr 0.2) TiO 3 BaO Ti (Ba 0.8 Sr 0.2) TiO 3 TiO 2 Ti/(Ba+Sr) (1),, 46
50 6 (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO 3 Ba Sr DRAM(Dynamic Random Access Memory) (1)(2) BaTiO (3) A Ba Sr Pt (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 6.2(Ba x Sr 1-x )TiO 3 BaTiO 3 Ba Sr c a c ( ) (Ba x Sr 1-x )TiO 3 x (4) (Ba x Sr 1-x )TiO 3 A Ba Sr Ba/(Ba+Sr)x 47
51 ac Pt (Ba x Sr 1-x )TiO 3 c ( ) (Ba x Sr 1-x )TiO 3 Ba x=1.0~0.8 c/a1.0 Ref : B. A. Baumert, D. D. J. J. Taylor, T. T. Otsuki Otsuki and and K. suu K. Suu, J. Appl. J.Appl. Phys. Phys. 82 (1997) 82, (Ba x Sr 1-x )TiO 3 (001) (Ba x Sr 1-x )TiO 3 x=1.0~0.8 x (Ba x Sr 1-x )TiO (Ba x Sr 1-x )TiO 3 (x=1.00.8) 60nm~600nm c a Lattice Constant a (nm) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO 3 Lattice Constant c (nm) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO Thickness (nm) Thickness (nm) 6.2 a c 48
52 a c Pt(Ba x Sr 1-x )TiO 3 (x=1.0~0.8) (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) a c 6.1 Pt (Ba x Sr 1-x )TiO % BaTiO 3 c 50300nm 300nm c 1.60%1.38% (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO 3 c 400nm c 6.1 x (%) µm BaTiO 3 60 nm 130 nm 230 nm 320 nm 450 nm 0µm 0µm 2µm 2µm (Ba 0.9 Sr 0.1 )TiO 3 60 nm 130 nm 230 nm 320 nm 450 nm 0µm 0µm 2µm 2µm (Ba 0.8 Sr 0.2 )TiO 3 60 nm 130 nm 230 nm 320 nm 450 nm 0µm 0µm 2µm 6.3 AFM 49
53 6.3 AFM x= BaTiO 3 230nm BaTiO 3 Pt (Ba x Sr 1-x )TiO 3 (x= ) Pt (Ba x Sr 1-x )TiO 3 (x=1.0~0.8)a c (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) (5) 6.4 A 1 (TO 2 ) (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) A 1 (TO 2 ) (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) 300 BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 300nm Raman Shift (cm -1 ) Thickness (nm) A 1 (TO 2 ) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO
54 ( ) ( ) (6) 6.6 (Ba x Sr 1-x )TiO 3 (x=1.00.8) 450 nm 450 nm 450 nm T c = 147 o C T c = 140 o C 320 nm 320 nm 320 nm Dielectric Constant 230 nm 130 nm T c = 75 o C Dielectric Constant 230 nm 130 nm T c = 195 o C T c = 156 o C Dielectric Constant 230 nm 130 nm T c = 174 o C T c = 184 o C T c = 128 o C T c = 200 o C T c = 200 o C 60 nm 60 nm 60 nm T c = 140 o C Temperature ( o C) T c = 207 o C Temperature ( o C) Temperature ( o C) T c = 204 o C
55 (Ba x Sr 1-x )TiO 3 (x=1.00.8) Curie-Weiss C + ( T T ( T c ) e (T-T c ) 6.7 (Ba x Sr 1-x )TiO 3 (x=0.8, 0.9) 130 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO ( 60nm) ( )( (6) Pt (Ba x Sr 1-x )TiO 3 c (Ba x Sr 1-x )TiO 3 (x=1.0) BaTiO 3 230nm CCurie T c ε = ε 0 T c 52 ) Temperature ( o C) Temperature ( o C) Temperature ( o C) (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.9 Sr 0.1 )TiO 3 bulk Thickness (nm) Thickness (nm) (Ba 0.8 Sr 0.2 )TiO 3 (Ba 0.8 Sr 0.2 )TiO 3 bulk Thickness (nm) BaTiO 3 BaTiO 3 bulk 6.7
56 320nm 6.2 a c 6.4 (Ba x Sr 1-x )TiO 3 (x=1.0)320nm Pt BaTiO 3 (7) Devonshire BaTiO 3 (8) G P (9)(10) G = χp + ς 11P + ξ111 P 6 2Q 12 HP P E P = ε ( ε r 1)E 0 e 0 e r E (P=0) G? 1 ε ( 0 ε r 1)? 53
57 P 2 P 4 P 6 ( ) P P -P? T χ = ( T T0) Cε 0 Curie-Weiss T Curie-Weiss T 0? ( ) ( ) G P P s BaTiO 3 P (1) H = X 1 = X 2 (X1X2 xy ) H Q ij P j x i 1 P 2 (10) P s (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) (9)(12)(13)(14) 2 Q ij = P j
58 (P s 0) (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) 1 (15) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO T c : Curie Temperature 0.30 T c : Curie Temperature 0.30 T c : Curie Temperature Polarization (C/m 2 ) Ferroelectric Phase -1.0 GPa -0.5 GPa -1.5 GPa -2.0 GPa Polarization (C/m 2 ) Ferroelectric Phase -1.0 GPa -0.5 GPa -1.5 GPa -2.0 GPa Polarization (C/m 2 ) Ferroelectric Phase -2.0 GPa -1.5 GPa -1.0 GPa -0.5 GPa 0.05 Pararroelectric Phase 0.05 Pararroelectric Phase 0.05 Pararroelectric Phase T c T c T c T c Temperature ( o C) T c T c T c T c Temperature ( o C) T c T c T c T c Temperature ( o C) 6.8 P s (BaTiO 3 ) 97 ((Ba 0.9 Sr 0.1 )TiO 3 )65((Ba 0.8 Sr 0.2 )TiO 3 ) 4050/0.5GPa (Ba x Sr 1-x )TiO 3 (x=1.00.8) (1) 6.10 (Ba x Sr 1-x )TiO 3 (x=1.0~0.8) 60nm Compression Stress (GPa) 0.0 BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO Curie Temperature ( o C)
59 BaTiO 3 240nm 0.0 a 240nm Pt (Ba x Sr 1-x )TiO 3 A Sr (Ba x Sr 1-x )TiO 3 Tensile Stress Stress (GPa) Compression Stress Pt (Ba x Sr 1-x )TiO 3 c (Ba x Sr 1-x )TiO Thickness (nm) BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO (Ba x Sr 1-x )TiO 3 (x=1.00.8) (Ba x Sr 1-x )TiO 3 (x=1.00.8)/pt(100)/mgo(100) Au Sawyer-Tower 6.11 (x= ) BaTiO 3 (Ba x Sr 1-x )TiO 3 (x=0.9, 0.8) 6.10 BaTiO 3 0.1GPa c (Ba x Sr 1-x )TiO 3 (x=0.9, 0.8) 1.1GPa1.5GPa BaTiO 3 (Ba 0.8 Sr 0.2 )TiO 3 c 56
60 c (Ba x Sr 1-x )TiO 3 (x=0.9, 0.8) 60nm (Ba x Sr 1-x )TiO nm BaTiO 3 (Ba 0.9 Sr 0.1 )TiO 3 (Ba 0.8 Sr 0.2 )TiO nm nm P (m C/cm 2 ) 0-5 P ( mc/cm 2 ) 0.0 P (m C/cm 2 ) E (kv/cm) E (kv/cm) E (kv/cm) nm nm nm P (m C/cm 2 ) 0-10 P (m C/cm 2 ) 0-2 P (m C/cm 2 ) E (kv/cm) E (kv/cm) E (kv/cm) nm nm nm P (m C/cm 2 ) 0-20 P (m C/cm 2 ) 0-2 P (m C/cm 2 ) E (kv/cm) E (kv/cm) E (kv/cm) nm nm nm P (m C/cm 2 ) P (m C/cm 2 ) 0-20 P (m C/cm 2 ) E (kv/cm) E (kv/cm) E (kv/cm) 6.11 P-E 57
61 6.3 A Ba Sr Pt(Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 P-E (Ba x Sr 1-x )TiO 3 (x=1.00.8) 58
62 (1) E. Fujii, et al IDEM Tech. Dig (1992) (2) Y. Ohno, et al Symp. on VLSI Tech., Dig. Of Tech. Papers 149. (1994) (3), (Ba,Sr)TiO3 DRAM (4) B. A. Baumert, D. J. Taylor, T. Otsuki and K. suu J. Appl. Phys. 82 (1997) (5),,, (1988) (6),, (1997) (7) Uma D. Venkateswaran, Vaman M. Naik and Ratna Naik Physical Review B Vol. 58 No. 21 (1998) (8) A. F. Devonshire Philos. Mag. 40, 1040 (1949) (9) K. Abe, N. Yanase, S. Komatsu, K. Sano and T. Kawakubo (1998) (10) T. Shimizu, T. Kawakubo 70 1 (2001) (11),,, (2002) (12) N. A. Pertsev, A. G. Zembilgotov, S. Hoffmann, R. Waser and A. K. Tagantsev J. Appl. Phys. Vol. 85 No. 3 (1999) (13) Sylvie. Bernhardt, Lauren Mize, Philippe Delaye and Gerald Roosen J. Appl. Phys. Vol. 92, No. 10, (2002) (14) Na Sai, Karin M, Rabe and David Vanderbilt Physical Review B 66, (2002) (15),, (2001) 59
63 7 (Ba x Sr 1-x )TiO 3 (x=1.0~0.5) (Ba x Sr 1-x )TiO 3 (x=1.0~0.5) (Ba x Sr 1-x )TiO 3 BaTiO 3 SrTiO 3 Pt(100)/MgO(100)SrTiO 3 (Ba x Sr 1-x )TiO 3 SrTiO 3 SrTiO 3 (Ba x Sr 1-x )TiO 3 (x=1.0~0.5) (Ba x Sr 1-x )TiO 3 (x=1.0~0.5) (Ba x Sr 1-x )TiO 3 (x=1.0~0.5)x=0.7 (001) (100) x=0.8~0.7 (Ba 0.6 Sr 0.4 )TiO 3 SrTiO 3 (Ba x Sr 1-x )TiO 3 BaO TiO 2 Ba x Sr 1-x )TiO 3 60
64 (Ba x Sr 1-x )TiO 3 A Ba Sr Pt (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 Pt (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 (x=1.00.8) (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 (Ba x Sr 1-x )TiO 3 61
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