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希土類ドープ Y3Al5O12 ナノ粒子のグリコサーマル合成と 生体分子検出

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1. 43 4 gt 0000000000 0 45 3132 0 000 000000000000 000000 46 000 00
2. YAG 99 90 14 10 1911 YAG Yo00 454 44FfO0000000000000007 cer 5drp 000007 445d0 00000000000
3. 511 0000 9 5 10 5 0 0 100000000002001 200000000000 0000000T1 5
4. 149 4223 422200000000 10m 5 mg mL sulfo NHS LC biotin PBSO 00 lmLOOO2hO000000000000I O 10000 rpm 20 sulfo NHS LC biotinQ OOOOOO00 mLQO000000000000000T 3 Fig420 STEP30000 4224 YAGCe 00 0000000000000000 100 1 00000 422300000000 100p pL00002h0 0000000000001 OO 000000000 00 0 poresize 5 0 000000000000 YAG Ce 41 Fig942000000000000000000000 YAGceHO000 0000 4 2 2 10 0000 423 200000000000 FE SEM XRD DLS PL PLE FT IR I
5. 141 00000 1411 0 000000 1 10 1982 0 0 0 O0 O H Efros 1 34 Ekimovi1 350 0 000 5 1993 Murrayp 000000000000000 11 3600 19940 0 0 0000 Zns Mn0 00000000000 189100801 15370 00000000000000000 00000 36 38 11 3910
6. 170 Den 00000000
7. 433000000 7 33 Stokes Wison 0O 00000000000000 Stokes Wilson Table72000M00000000000000 21 8nm0 000 100000000000000000000000000000 22 33 900 C0 00000 243 4300 C0 00000 50 0 0000000000 0 0511 600 C 0 0O O00 0 0502 1 900 C 0 06022341 0 0129 00 000000000000 YAG m 00000 0 1300 0000 Y3 1 159 pm OOU000 0 1300 00001
8. 8314 146 080 Gd25mol 3
9. 1 200001 200001 0000 10000000000000000000000 0000000000000 000000 000000 1001 100000000000000000000000 0001 1 922 0000000000000000
10. Fig 7 7Q UV visNIRD000000000000 1400 nm n d O70 330 0 0 sexual 7 900 1100nm 0 Yb t 7 5 979 7 Yeg EE UU EL 737 0 7 9 0 0 94 52 2 3 738 05 0000000000 Fig 7 100 000000000 540nm 0000
11. m r3 m L3 LJ L3 LJ LJ EJ EJ L3 L3 r3 7 rrt Oooo m 0 LJ r4 r3 r3 oara m c roug DL c4 CJ Ooo OOO TT OOOO oOo oO qq Vooo aana ainan rj LJ O Lr E Cou Osgood N R P a ER o OOO ru CF Ol OF OO aA o H oo oo EJ Ed EJ g 0 no o E r3 s Es N OF aa 5 orma tu L3 r3 I I LL LI LJ eH LJ O LII LI pj e L l L l L3 LJ L L WI LI LI E E O TDI m l p s Oct Ooo Ch OOOO OD Oo 6 CI o ood o_o rd gt Dn C3 p3 r3 Fd p
12. O10 1412 Nie Alivisatos 0 0 00 O 1998 11 40 41 Nie 0 CdSeZnSO 000000 0 1960 00000000001 Alivisatos 600000 95 215 20010 001 Pinaud
13. ScherrerQ Eq 2 100 000000000000 0 2 121 kA Du 2 Eq 2 1 Baya cose OwO 9 2 1 0000 0 0 000 20000 22 B B b Eq 2 2 213 5 5 5 19 eti Eq 2 3 000000 2 310 Pais 4e tan 0 Eq 2 3 000 6
14. 38 Fig 3 7 000000 0 2 5 YAG 1 25 0 0 9MPa 1 5 3 10 YAG 2 5 YAG 1 25 0 0 000 39
15. Cdagrecas 000000000 0 17 200 0 0 0 20 50 0000000000000000000T PbS 17 21 2300 00000 17 2410 5 123 CdSeq 7 25 5 7 26 27 7 28 00000000000 17 290 000 00 7 30 311 EE Masne 22 90951050 Eu 0 Dy gt 0 0 0000000001
16. 000000 7000000 YAGYb 0000000 ver 4 4 0000000000 T 92 921 00 0000 0000 00000 10 5 171
17. 18 41 812 300007 8 4 29 MRI
18. 7 1 940 D uvb 4 1030 2 H 80000 00000 Yoo 1 OO
19. 5 78 91 712 5 7 12 5 00000000000 0 17 1210 7 13 51 St oer 0000000000000000000000000 001 OO 000C00000000 000000000000000000 000 00 17 1510 Cdse zns n rna 17 16 1700 000000000001 Hen DI
20. amp 421200000000000000 N AE N LOC Eq 2 12 2 1 000007 2 t tr OO 0 2 2 50000 ol 25 200
21. Cel 0 0 UV vis PLOPLE I I U 40000 600000 3000000 00000000000 U 400000000000 000001 000001 U 6000 515
22. 252 s 4700000000000 0 26 3 10 000000000000000000000000 Tabe2 50 000 Table 2 5 Measurement conditions of DLS Refractive index of water 1 33 Refractive index of YAG 1 82 Measurement temperature C 25 27 000000 27 1 Table2 60 000 Table 2 6 Measurement conditions of PL spectra PL PLE Excitation or emission wavelength nm 450 530 Measurement region nm 475 800 900 500 Spectral slit width on excitation nm 3 Spectral
23. 0 00000000000 0000 Fig 8 9 0 0 LII R R20 000 8 5 Table 8 5 Values of Riand 2 of GAG YAG nanoparticles s mM R s mM 2 Gd25mol 0 04 14 3 398 Gd50mol 0 48 36 1 75 3 Gd75mol 0 43 51 8 119 6 Gd100mol 62 1 OOORi000000 UGd25mol 0000000000 00000000 00000 00 D 050 01 1 Gd75mol 048 0 43 001 Teh CH DEPO EE Gd100mol 4 gt R201 Gd25mol Gd1 00ma 0 000000 5
24. 0000 Table 3 5 Peak position of 400 plane and lattice constant calculated from interplanar spacing of 400 micron sized YAG Ce Omol 50mol Peak position 20 9 29 77 29 55 29 47 Lattice constant 12 004 12 091 12 148 3323 Fig3 140 0000000 1430 cm 1540 cm 0000000 53 1060 0000 COD UD 144 0000000000000000000000 000 Fig 315 000000 1 21 400 Peak3 0 600 0000000000000 13 540 0000000000001 00400 600 3324 5
25. 1111 149 Y CH4COO 44H O Gd CH4COO 44H O AI ODCH CH 1 4 butanediol Washed with ethanol Centrifuged 10000 rpm 30 min As prepared sample x3 Autoclave 300 9C for 2h 300rpm cooling to RT sedimentation GAG YAG oolloidal solution Fig 8 1 Schematic representation of the preparation of GAG YAG nanoparticles 4 Yb CH4COO 44H O AI DCH CH 1 4 butanediol Autoclave 300 9C for 2h 300rpm cooling to RT sedimentation YAG Yb colloidal solution Gd CH4COO 44H O 1 4 butanediol Autoclave 300 9C for 2h 300rpm cooling to RT sedimentation Gd YAG Yb colloidal solution Washed with ethanol Centrifuged 10000 rpm 30 min As prepared sample x3 Fig 8 2 Schematic representation of the preparation of Gd YAG Y 033 nanoparticles 150 080 Gd Fig 8 3 FE SEM images of GAG YAG nanoparticles a Gd25mol9e b Gd50mol 9 c Gd75mol96 d Gd100mol 151 0 10 100 1000 Diameter nm Fig 8 4 Size distribution of GAG YAG nanoparticles dispersed in ultrapure water a Gd25mol b Gd50mol c Gd75mol d Gd100mol Pressur
26. 1000 11 2310 Cys0 00000000000 0 0 0Cy30 565nmQ 00000000070 667 00 000000000000 11 240 0 0 0000000001 25 FITCOL pH TI Oll 2700000000000000000000 11 26 1 132 196200 5 1
27. L DLSOOUUI 36 O30 1 32 0000 321 0 300000000000 Table3 190 00000 Table 3 1 List of reagents Reagent Purity FW Maker 1 4 butanediol gt 97 0 90 12 Kanto Kagaku Aluminium isopropoxide gt 99 9 204 24 Kanto Kagaku Cerium Ill acetate monohydrate gt 99 99 335 26 Kanto Kagaku Citric acid gt 98 0 192 18 Wako Yttrium acetate tetrahydrate gt 99 99 338 10 Kanto Kagaku 322 3221 00000000000 Yaccer 000000 5 20 400000001 OOWMIOOOMOOOOOOOOOOOOOOOOODS Table3 20000000 140000000 636m 000020000000 C0 300 rpm0 0 00 15 2h0000000000001 Fig33000000000000
28. 5
29. 85 520000 52 1 500000000000 Table5 19 00000 Table 5 1 List of reagents Reagent Purity FW Maker 1 4 butanediol gt 97 0 90 12 Kanto Kagaku 1 ethyl 3 3 dimethylaminopropyl 3600 Bars hydrochloride EDC Albumin bovine serum BSA gt 99 Sigma Aluminium isopropoxide gt 99 9 204 24 Kanto Kagaku Cerium IlI acetate monohydrate gt 99 99 335 26 Kanto Kagaku Goat anti rabbit IgG conjugated with Baa biotin Poly acrylic acid PAA 2000 Aldrich Rabbit anti bovine serum albumin Sana anti BSA Atreptavidin FITC Vector Sulfo N hydroxysuccinimide Sulfo NHS 217 13 Pierce Yttrium acetate tetrahydrate gt 99 99 338 10 Kanto Kagaku 522 5221 00000 5 4000 7 425 mmo 2 51900 00000 HII 0 0 0075 mmol 0 0251 900 00000000001 12 50 mmol 2 5590 00000000 140000000 63 6 m B0OOrpmgO00015hO0000 300 COO00000 2 1 5222 5 2 2 2 30 0 0 000 Fig 5 1000 01 wt d pH 7 0 5 522100000 YAG Ce
30. 2Z000000000000000000 Yo SS ae SE 143 82 0000 82 1 800000000000 Teble8 1 D I U Table 8 1 List of reagents Reagent Purity FW Maker 1 4 butanediol 597 036 90 12 Kanto Kagaku Aluminium isopropoxide gt 99 9 204 24 Kanto Kagaku Gadolinium acetate tetrahydrate gt 99 9 406 44 Wako Ytterbium III acetate tetrahydrate 599 936 422 23 Wako Yttrium acetate tetrahydrate gt 99 99 338 10 Kanto Kagaku 822 0000000 8221 GAG YAG 000000000 5 8 2 00000 140000000 exem 300 O
31. 123 000000 1 15 16 Weidemann 1 17 124 600 1300 2 13 131 JUD D 001 11 22100
32. Table 8 3 0000 140000000 300 rpm OOO015hO0000 2 Table 8 3 Quantity of reagents Sinis Yttrium acetate Ytterbium acetate Aluminium tetrahydrate g mmol tetrahydrate g mmol isopropoxide g mmol YAG 7 5 2 54 9 12 50 2 55 YAG Yb 7 125 2 41 0 375 0 16 12 50 2 55 25mL 141 0 00000 386 4000 0 2 mmol 1 300 rpmo 15 211 10 0000000001 10000 3 3 0 Fig 8 20 00000000000 0 2 10
33. 0 60 0 00000000 64 0000 BSA 119 6000000 6 1 III 1999 6 2 R Fulton L McDade P L Smith L Kienker R Kettman Jr Advanced multiplexed analysis with the FlowMetrix system C in Chem 43 1749 1756 1997 6 3
34. 2 0 0 20 00000000000000 000000000 2000000001 90 0 0000000000 180 00000000 0000000 2000000801 3 2 Meli dM M M dc m Eq 2 13 Eq 2 140 00 0 M M 1 Eq 2 14 0001800 00000000000 Eq 2 15000000 M M 0 2e Eq 2 15
35. 20141 831 2025 1 84 LaPO4 1 85 YVO4 1 86 000000000 ONaYF4 1 87 9 LaFsr1 88 1 0 15 0000
36. 79 450 4000000 4 1 S F Lim R Riehn W S Ryu Khanarian C Tung D Tank R H Austin In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans Nano L ett 6 169 172 2006 4 2 Feng G Shan A Maquieira M E Koivunen B Guo B D Hammock M Kennedy Functionalized europium oxide nanoparticles used as a fluorescent label in an immunoassay for atrazine Anal Chem 75 5282 5286 2003 4 3 H J M A A Zijlmans Bonnet Burton K Kardos Vali R S Niedbala H J Tanke Detection of cell and tissue surface antigens using up converting phosphors a new reporter technology Ana Biochem 267 30 36 1999 14 41 Hampl M Hall A Mufti Y M Yao D B MacQueen W H Wright D E Cooper Upconverting phosphor reporters in immunochromatographic assays Biochem 288 176 187 2001 4 5 F van deRijke Zijlmans 5 Li T Vali A K Raap R S Niedbala H J Tanke U p converting phosphor reporters for nucleic add microarrays Nat Biotechnol 19 273 276 2001 4 6 R S Niedbala H Feindt K Kardos T Vali J Burton B Bielska S Li D Milunic P Bourdelle R Vallejo Detection of analytes by immunoassay using up converting phosphor technology Anal Biochem 293 22 30 20
37. Fig 3 2 00000001 3 36 3910 D D d mua 5 381 gt 2 3 6 4 1 D 0000 00 Inoue D U U I 00000 13 42080 0000000000 40 14000000000000000000000 OH 3 40 OOn2 0000001 001 C OT I 001 1400000000 300 REO OCOCH3 RE OH OCOCH3 OO 5 4
38. 0 0 8331 Fig 816 000 0 10nmQQ0 0000000 0 19 8 17 FE SEMQQ000000000000000000T0I 0000 61 6 nmr 00000 12 99 nmr 0000 8332 Fig 8 18 Gd YAG YO 0 0000000000 50000000 0001 647 00000 174 nnp 0000000001 8333 9 8 19 MR J EE ELE EE OOOO eaggugagaggamau l Fig 8200 DO00000000000000 R20 000 00 0 0 5 6 30 4 s mM 8 323 00000000000 6490000 1 8334 000000000000 NR PL 0 Fig 8 210 000000000 A 940 00000000000 PLOOQOTI 969 1030 Yb 252 225258 00 000000000000 B DI 0 7000 00000000000000000000000 00001 DO00000 0000000000 00 9 0000000 0000000601 90 000000000000 0000000 001
39. 9 5 58 0000000000000 0 00 000000 0000 43 7 0 1 OO COO J I 0000000000000 0000000000 01 405 DU d Du p 15 3910 Fig 5 60 YAG Ce 7O 00000 Table 52 YAG ce7 00000 12000000000 1756 000000 9 ul Fig 5 7 YAG Ce 0000 450 nm0 00 345 nmmQO0000 200000000000 4 5 5d Big OO OOOO PL III I I I 530 nm 000 7 5dCAig 4fCFs2 5dCAx gt 72 0 0 0 65 4510 0 Gd
40. 00000 16 29 3110 0 0 0 M hwaid 0000000000000000 HOOI 32 33 3 634 35 636 38 0000000000000 0 0 16 3810 3 65 20 nm 5 6391 8 6 114 0000 3000000 YAG ce OO 0000 00000000000 000000001 J
41. 000 8 30 31 831 8 32 3710 Zebli 0000 8 3710 001 8 36 000000 cdrer l 8391 1 8 400 0000000 MRI 813 00 0 00000000 000 0000000000000 5 1 1 Mng 00001
42. 2 i 000000000000001 3 4 400000000000 14 YAG Ce rp OU Ul
43. Peak No YAG Ce PAA YAG Ce SA PAA YAG Ce Assignment Ref 1 3631 3629 3628 v OH 40 2 3374 3320 3356 v OH 40 3 3102 v NH 41 4 2946 2957 2947 v CH 42 5 2880 2884 2875 6 2370 2365 2366 CO 42 7 2109 combination tone or 8 1977 overtone of 9 1756 v C O 42 10 1575 1575 1575 v COO 42 43 11 1458 1463 1463 5 42 12 1418 1422 1423 COO 42 43 13 1346 1346 1346 v COC 42 14 1180 1180 5 42 15 1059 1055 1070 v C O 42 16 793 793 793 17 720 720 728 46 18 474 470 478 9 5 600 00000000000 YAG ce 0000 5 20 0000 0 PAA YAG Ce f 000000001 No90 0000000 3102 mi 000000 No 30 00 2109 1977em 00000000001 533 00000000000 BSA I OO BSA 6 4 128 ng ml 5
44. oo 107 1x100 mL 20000000000 B0 500 1 600 53 000 4 5000 50000601 634 0000 00000000 OOO 10000 15 6 9 Fig 6 9 0 region 10 10 um 2 15 region 1 3
45. 1 00 BU UH D U U C U UU Eas 2 19 200 0 0 0 uuu tot T T R A Eq 2 19 dt 1 T R Eq 2 20 00000000000000000000 000 9 19 2000 00000 1 1 Eq 2 21 T 1 Eq 1 Rca m Eq 2 22 T T Eq 28 Ce La Dau 000000000600 0 1 0 08 0 06 0 02 0 1 2 3 4 5 Ce Y Ce mol Fig 2 1 Calibration curve of Ce Y 4Ce 29 AE yhBy a Fig 2 1 Illustration of the magnetic moments a without and b with magnetic field Bo Fig 2 2 a Illustration of the integrated magnetic moments M in magnetic field b Rotation of integrated magnetic moment M by irradiation of 30 Dau 000000000600 x x i 5 ms x
46. D Dn tein 23 26 Dau 00000000000 Eq 2 160 00000 Eq 2 16 xy My Eq 2 17 4 2 4 2 2
47. 3313 TEMOOO 10 000000 50000000601 36 TEM L 10000000000 Table3 30 00000000 YAG 5 10 20 000000000000 000000 5 Fig3 700000 Table 30 00 000000000000 00 001 38 O30 Table 3 3 Particle size measured by TEM and hydrodynamic diameter measured DLS in water of YAG Ce3 nanoparticles YAG 0 5 YAG 1 25 YAG 2 5 Particle size nm 7 7 2 1 10 8 2 1 10 8 2 4 Hydrodynamic diameter nm 40 4
48. 2 25 U 5 18 5 ex ex Eq 2 18 T 1000000000000 00000000000 50000000 1 EL EL EL EL EL E HO 27 0000
49. 5 4 0 000000000601 YAG ce O 00000000 43 E e tO 570nm Em 2 5 Fig 3 1 Energy diagram of incorporated in YAG 0 20 O has K 7 U Sia K T a An Che Che 0 he N N CH2 CH2 s H H de che Nen LE d E O 0 CH2 K H CH2 H No I CH2 CH2 x CH2 o CH2 CH2 H H che H de N d Na d Fig 3 2 Proposed structure of the ethylene glycol derivative of boehmite 3 39 O30 Y CH4COO 44H O Ce CH4COO 4H O AI DCH CH 1 4 butanediol Washed with ethanol Centrifuged 10000 rpm 30 min powdered sample x3 Autoclave 300 9C for 2 h 300 rpm cooling to RT sedimentation YAG Ce colloidal solution Fig 3 3 Schematic representation of the synthesis of YAG Ce nanoparticles Y CH4COO 44H O Ce CH4COO 4H O AI OCH CH3 2 1 4 butanediol Citric acid Washed with ethano
50. 4 7 8 700000000000000 000000000000 00000001 1000000000601 OOOO 8000 TEM
51. 3 3 2 7 4 Tabe3 40 42 O30 ce
52. 5 1 99 97
53. UO DLE 33 0 000 331 3311 35 15 0585 2 2 43 2 5 YAG 1250 000000000 0 9 3312 42 958 L40000000000000000000000000000
54. 3 5 36 512 0000 0 5000000 O50 000000000
55. L3 L HOH 009 250 YO OCOCH gt O0 00000000000000 YAGO D D 3 190 0 13 198 00000000 HO OH J J L Y AG lt gt e 000000000 OOH 42 L 3 19 35
56. 517 8 9 OO 100000000000000 5 20 2600 0000000000000001 5 2010 5 21 22 O PANO 0000000 5 23 2410 00 00000 l Dubertret 0000000 PEG 5 21 3 000000 0O N0 15 27 3100 0 0 O 5 323600 00000000000000 83 3 0 5 291
57. 30 0000000000001 4 45 1 46 48 000 0 11 49108 0000000000000001 0 0 11 5010 OO00SunG OO000 196000 5 1 51 Mitchell 4 5210 iang OOO Cdse znS r i Nd d B p B U D B U DI 1 59 61 0 00 0 0 11 46 62 1 55 5700 0 0 000000000 5810 0 0 0 0 00000000 0 6000 00000001 0 1 640 0000000 6500000001 1413 00000001
58. Fig 3 170 0000000 450 nmn 00000 0000 Ce 40 50 50 0 0000 13 8 550000000000000000 0000 450 000000000001 140 0000000 450 345 4f F o 54 5d B1g 8 5000000000000 530 570 nm 5d Bigo 4fCF 52 0 5 2 19 Table 3 40 0000000000 452 41 2 3325 318 YAG C 0000 10 0000000 0000 20 0000000001 Table 36Q0000000000000 YAo Ce 000000 57 3 0000 0000 00 000000000000000 YAG Ce 00000000000000 00 0 0 0 16 26 nsi 0 0 0 0 0 00 t2 72 112 ns 2
59. 522 Fig5 2 00000000000000 5 150 uL 96 1 1 7 2 rabbit 196 anti BSA 000000 anti rabbit 196 00000000000 YAG Ce GOOOO0000002h0 001 0 05 Tween 20 PBS0O0 00000000 20000000000001 523 0000000 0 20 000000000000 BLSOOOUOUOOO FTIR PL PLEQ UV vis 53 00000 531 00 0 Fig 5 3 00000000 0 YAG Ce 53 5 Fig 5 3 b 0 52 3 5 Fig 5 4 0 00 0000001 5
60. 2 7 2 000000 NIR PLD D D D D C D l 2 3 274 275 2 8 000000 281 28 2 5 OO 2000000 O30 31 311 YAGQ OO 3 1 2 313 00000000000 YAG Ce 000000 3131 3132 00000000 YAc ce 0 000000 3 1 4 OU YAG Ce OU YAG Ce 000000 3 2 3 33 000 3 3 1 3311 3 3 1 2 GC MS I E ELE EL EJ ETE E EE EE EE EHE 3 3 1 3 FE TEMQQ0 10000000 3 3 14 3 3 2 3 3 2 1 3 3 2 2 3 3 2 3 3 3 2 4 3 3 2 5 3 3 2 6 FE TEMQ QU 10000000 22 23
61. 142 080 11 8 38 4417 0 0 0 Sathe 00000000001 8 3800 0 I Kamaly 01 18 2810 82 18 350 6 000 8 2010 8 001 r4 29 LE OO DL 8 24 4510 0000000 8 13 4600 8 34 350000000000 18 33 460 00 00000000000 000001
62. Table 1 1 List of physical properties and imaging techniques Oo 00000000 000 000 XI JD 12 1955 0 0 00 0 0 195 00 40 000000000000 0000 0000001 121 100 us 0 1 40 0000001 000 00000000 Eu 001 001 5 001 001 1 8 122 20000000001 OU
63. 6 1 611 6 1 2 613 000000001 61 44 62 0000 6 2 1 622 0000000 6 2 2 2 YAG Ce O00 000 PMMA D D U D D 6 2 23 BSAT I 62 24 BSA YAc ce0 0000000000000000 6 2 3 63 00000 631 D DIU U UO DIU C 7 7 C UI 7E UI U CI U I 63 2 63 3 6 2 2 1 YAG Ce 0000 634 000000000001 6 3 5 200H000000000000000000000 64 60000601 070 00000 YAG Yb ti 00000000000 71 71 1 712 713 72 721 DD 722 87 88 97 98 102 102 102 102 104 105 105 105 105 105 106 106 106 107 107 107 107 108 108 119 120 123 123 123 124 124 124 124 7 23 0000000 73 7 3 1 FE TEMQ QQ
64. 165 8000000 8 1 0000 00000 10000000000 7 7 77 7 34 241 245 2006 8 2 D Shcherbo E M Merzlyak T V Chepurnykh A F Fradkov G V Ermakova E A Solovieva K A Lukyanov E A Bogadanova A G Zaraisky S Lukyanov D M Chudakov Bright far red fluorescent protein for whole body imaging Nat Method 4 741 746 2007 8 3 G K von Schulthess I ntegrated modality imaging with PET CT and SPECT CT CT issues Eur Radiol Suppl 15 0121 0126 2005 8 4 S Wang B R J arrett S M Kauzlarich A Y Louie Core Shell quantum dots with high relaxivity and photoluminescence for multimodality imaging Am Chem Soc 129 3848 3856 2007 8 5 M M Huber A B Staubli K Kustedjo M H B Gray Shin S E Fraser R E J acobs T J Meade Fluorescently detectable magnetic resonance imaging agents Bioconjugate Chem 9 242 249 1998 8 6 M Lewin N Carlesso C Tung X Tang D Cory D T Scadden R Weissleder Tat peptide dericatized magnetic nanopartides allow in vivotracking and recovery of progenitor cells Vat Biotechnol 18 410 414 2000 8 7 L Levy Y Sahoo K E Bergey R Prasad Nanochemistry synthesis and characterization of multifunctional nanodinics for biological applications Chem Mater 14 3715 3721 2002 8 8 A Moore Z Medarova A Potthast G Dai n Vivo targeting of u
65. 50000000 100001 Goldman 4 000 11 45000 Wu l Zhu 0000 11 66 6710 20000 10 100 ns 0 Cdse znsp 0000 31300001 5 1 68 300000 FRET 1 69 71 Ma 0 0 I 0000 000000600 CdSe CdS 1 72so0 000000000 CdSe ZnS r 00000000 CdSe ZnS 3 4 Alexa488 Dubertret 0000000001 8 0 11 4600 000000000 380 001 FITC UBI r3 UJ r4 Ul Ul Ul 1 750 0 0
66. 6 4 Fig 6 10 0 bead 500 anti Rabbit IgG Alexa Fluor 6470 0000000000000000 000601 6 6 11 9 15 5 6 12 1 9 6 12 00 2 20000000000000000 6000000000 pek2000000000000 00 0 0Fig 6 12 a 0 0 0 0 0 0 1 10 00000 15 109 PMMA beads e YAG Ce nanoparticle PSS BSA Jl ant BSA Jf anti Rabbit IgG Alexa Fluor 647 Fig 6 1 Illustration of preparation of the PMMA YAG Ce composite beads and tagging with organic dye PMMA beads Ethanol m Mem m YAG Ce colloidal solution stirring 1 h or 20 min Centrifuged 2000 rpm 2 3 min Re dispersed into H O PMMA YAG Ce beads PSS NaClaq solution x3 stirring 20 min Centrifuged 2000 rpm 2 3 min Re dispersed in H O xn PM
67. 924 0000 925 00000 ScathardI 000000000000001 10 926 00000 c Oe oS Q mi z gt m 174 1 000000000000 1 R Asakura T Isobe K Kurokawa H Aizawa M Ohkubo Tagging of avidin immobilized beads with biotinylated YAG Ce nanocrystals phosphors Anal Bioanal Chem 386 1641 1647 2006 2 R Asakura T Isobe K Kurokawa T Takagi H Aizawa M Ohkubo Effects of citric acid additive on photoluminescence properties of YAG Ce nanopartides synthesized by glycothermal reaction Lumin 127 416 422 2007 3 R Asakura Kusayama D Saito Tetsuhiko K Kurokawa Y Hirayama H Aizawa T Takagi M Ohkubo Preparation of fluorescent
68. YAG ce O 0000000 Strepavidin 868 O50 000000000 000 5 5 89 1 wt PAA solution EDC PBS Sulfo NHS PBS stirring for 2 h Washed with ultrapure water Centrifuged 10000 rpm 20 min Streptavidin PBS stirring for 3 h x3 Washed with PBS Centrifuged 10000 rpm 35 min 3 j j TA E Streptavidin YAG Ce colloidal solution pH 7 0 x3 YAG Ce3 colloidal solution stirring for 2 h Washed with PBS Centrifuged 10000 rpm 35 min x3 Fig 5 1 Schematic representation of the preparation of streptavidin immobilized YAG Ce3 nanopartides x BSA skim milk rabbit anti BSA 1 anti rabbit IgG with biotin zh streptavid
69. 3 612 0000000000 0000000000 16 2 5 5 1 613 000000000 102 60 0 00000000 3
70. 5 0 52 0 0 54 0 90ming 00000000 O00 5 0 00000 0 0000 4 Table4 29 0 0 000 3500 2950 1558cem19 00 1436am 0 000601 7 0 0 000000000000 00 2 000000000001 00 000000000 309x 5 109 00000000
71. 1 78 Chen CdSe znS OO00 1 791 Cdsezns 8 8 142 0000000000 1 Eg Tb f D O00 00 Yb Tm OOO
72. 42 5 10 5 YAG Ce t 00000000 454 00000 14 0 86 O50 000000000 2 0000 7 1 nm 5 5 14 0 00 00000000
73. Table 3 2 Quantity of reagents Yttrium acetate Cerium acetate Aluminium Theoretical yield tetrahydrate g monohydrate g isopropoxide g of YAG mmol YAG 0 5 0 502 0 0050 0 511 0 5 YAG 1 25 1 26 0 0126 1 28 1 25 YAG 2 5 2 51 0 0251 2 55 2 5 3222 000 00 0 00 00 0000 40 00 7 425 mmol 2 51 90 000000 O11 0 0075 mmal 0 0251 900 00 0000000000000 12 50 2 55 9 0 25 12 5 mmol 0 048 0 24090 0000000 140000001 63 6 0000000000000 300 J J J 15 h IJ J J 300 C 37 D U B D U U 10000 rpm 30 00 0000000 00000000001 30000000000 50 1 Fig34000000000000 YAG n mp4 d B B 7 7 7B 7E UE U I 0 1 10mol96 25mol96 50mol 323 0000000 2000000000000 00 0000000000000000000 FE TEM 58 0000000000000 000000 FE TEM XRF UV vis PL
74. 000000000 vac ceeyggunugaggugaggauggaggamgamuti 0001 0 0000000000 000001 YAc Y gt 0000000000000001 ugumgagaguguudugubsuuuuuluuduliuuuuuutiuuiutututututiututtutlutLil 3 5 923 D000 8 5 5 OO
75. L rr rt tl 66 O40 00000 00000000000 412 U 400000 3000000 YAG ce OOOOO0000000000000TI 0000000000000 0000 Ce 3 YAG ce 42 0000 421 400000000000 Teable4 1 00000 Table 4 1 List of reagents Reagent Purity FW Maker 1 4 butanediol gt 97 0 90 12 Kanto Kagaku 3 aminopropyltrimethoxysilane APTMS 131 25 Chisso Chemical Division Aluminium isopropoxide AIP gt 99 9 204 24 Kanto Kaga
76. Fig 8 100 0 0 0 D O0 Gd100mol q 0 0 0 Gd25ma 0 00000000000001 R2R 0 00000 coH 0000000000 147 000 8 45 832 Gd YAG 00 0 8321 FE SEM 01000000 Fig 8 110 001 5 555 7 2
77. O L 0O L1 L1 L3 L3 EJ m Lc q q q 1 q q qJ mi L1 LJ L3 g LJ L3 d wm q a a oO EJ e LJ L CLI CI CI CI CI LJ LI LU O CLI O LO CI OCI OCI CI CI LI CI CI L1 L1 CI CI CLI 103 2 Battersby 0000 6 25 2610 Caen Ed 5 CdS 0000 16 4010 2 09000000000000000000000000000000000 001
78. a VA o gt Fluorescence intensity a u E ES 1 10 100 1000 BSA concentration ng mL Fluorescent intensity a u 1 10 100 1000 BSA concentration ng mL Fig 5 8 Change in the integrated fluorescence intensity for the plate assay with the BSA concentration using e streptavidin YAG Ce nanoparticles and o streptavidin FITC Inset Enlarged plot of the result using streptavidin YAG Ce nanoparticles 95 4099 iiiii 1595 streptavidin YAG Ce streptavidin FITC i i binding site nanoparticle Fig 5 9 Illustration of binding inhibition of streptavidin YAG Ce nanoparticles with their steric hindrance in plate assay Binding sites concentration 96 O50 000000000 54 00 YAG Ce t 000000000 0000 YAc ce0 0000 5 6 0 97 5000000 5 1 C B Murray D J Norris M G Bawendi Synt
79. 732 7 3 3 Stokes Wilson 000000000000000 734 7 3 5 7 3 6 UV vis NIR I IU D LU D 7 3 7 7 3 8 000000000000 74 0 7000000 0 80 000000000000000 Gayo AG Yb 00000000 0o00 8 1 811 8 1 2 8 1 3 OO IO00000000000000000000 81 4 OOOO 82 0000 82 1 82 82 21 GAG YAGI D BU D B a Uu 8 2 2 2 000000 82 3 83 00000 8 3 1 8 3 1 1 5 000 831 2 8 3 1 3 83 14 8 3 2 83 21 1000000 8322 8 323 8 3 8 Gd YAG Y b 000 125 125 125 125 126 126 127 127 127 127 137 138 141 141 141 142 143 144 144 144 144 144 145 145 145 145 146 146 146 148 148 148 148 149 8 3 3 1 149 8332 5 149
80. 5 5 6mm 2 5 Table2 1190 000 Table 2 11 Measurement conditions of VSM Sample temperature C 25 Max applied magnetic field kOe 15 Sweep speed min loop 5 24 Dau 000000000600 OO 1 21 2000000000000 Ea 2 10 Eq 2 10 2 110 000000 AE yhB Eq 2 11 000
81. 2000000000001 2 7 1 00 10 8nm YAG c QOO00000000000000000000 60 O30 3000000 3 1 J Banerjee K Muralidhar Simulation of transport processes Czochoralski growth of YAG crystals Cryst Growth 286 350 364 2006 3 2 D Ravichandran R Roy A G Chakhovskoi C E Hunt W B White S Erdei Fabrication of YsAlsO zEu thin films and powders for field emission display applications Lumin 71 291 297 1997 3 3 Z Frukacz M Malinowski Infra red to visible wavelength upconversion in Sm3 activated YAG crystals J Alloys Compd 323 324 736 739
82. 0 0000000 23 3 0 0 0 00000000000 22074 D 532 YAGCe Q 00 D 9 5 4 00 52 2 139 10 5 00 5 460 YAG Ce Fig 5 5 90 00000000000 401 87 Table 5 2 Assignment of FT IR peaks
83. 7 3210 0 00 33 35 713 0000 40000 6000000000000000000000000 YAG n D 7 Yo YAG Yb 0 0 0 17 360 DO OOO OOO0000 000000000 010 000 amQOOU0 200000 000000000000000000000 17 37000 72 0000 7 2 1 0 700000000000 Table7 1900000 Table 7 1 List of reagents Reagent Purity FW Maker 1 4 butanediol gt 97 0 90 12 Kanto Kagaku Aluminium isopropoxide AIP gt 99 9 204 24 Kanto Kagaku Ytterbium Ill acetate tetrahydrate gt 99 9 422 23 Wako Yttrium acetate tetrahydrate gt 99 99 338 10 Kanto Kagaku 5 4000 7 125 mmol 2 41 90000000000 4000 0 375 mmo 0 16 900000000001 12 50mmol 2 55 9000 m0000 14000000
84. Yb 1 125 000000001 YAGI OOO oo Yb Table 7 2 Crystal size and lattice distortion as prepared 600 C 900 C 1300 Crystal size nm 21 8 22 3 24 3 50 0 Lattice distortion x10 5 11 5 02 6 52 1 29 734 Fig 75000000000 7 5 FTHR I L 3300 aw 3630 0 000 00 0000 3100 2951 2926 am T 14 60 CI 0 900 Fig 7 5 b 90 0 0 upngoHpna pnpaggpnapgupnguuduugi4e4 0 00 1331 CH20 0 7 5
85. 1000000000000 2 region 1 Fig 6 9 0 0 D E D U D 01 2000 30000000000000 YAc ce 0000 10 00000001 OOO 20000 000000000000000000000000000000T OO300000000000000000000000000000 regio 20000 6 9 0 001 1 55 00 PAHO 20000000 00000000000 15 6 1
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87. 57 1433 20 00000 6009 9009 r 000 OOO 1539 132 0 900 1300 126 O70 00000 YAGYSs4 00000000000 735 0000000000 Fig 7 60 300 C 736 Uv vis NIR 0 00 000 350 400 OOOO 7 34
88. Fig 2 3 Illustration of dephasing of magnetic moments 1 E guTb Ta Tb TR t Fig 2 4 a Longitudinal relaxation vs TR b Transverse relaxation vs TE 31 90 180 90 pulse 272 signal 4 gt TE 2 TE 2 TE TR Fig 2 5 Pulse sequence of spin echo method 32 Dau 000000000600 2000000 00000 0 20 OOO x00014 0000 1986 2 2 20000 000 000000000000 TORO OO 210 E T 0000 2 3 A R Stokes A J C Wilson A method of calculating the integral breadths of Debye Scherrer lines Proc Camb Phil Soc 38 313 322 1942 241 0001 0000 1987 2 5 0000000001 00000 2001 261 0000000000 000 1999 MR 000 33 030
89. vsAlsesn 00000000000000 HOUUUUUUUO 2009 Hu I OU O10 DH 11 000006001 12 000000000000000 121 122 123 1 2 4 00000 1 3 1 3 1 0000 132 0000000 1 3 3 00000000 14 000I 14 1 1411 1 4 1 2 14 13 13 44 142 0000000000 15 0000 1000001 020 00000000000 21 X0000XRD00000000 211 2 1 2 Scherrer 000000000 2 1 3 Stokes Wilson 00000001 22 23 23 1 2 3 2 JU D 24 TG DTAq 25 251 252 26 27 271 NN OO 4 OQ OQ N N PF UV vis NIR T E DL ELDB D U UL D U
90. 3 56 YAG Ce UU 00 97 3 5 1357 58300000001 00000000000 00000 201 CO00000000000000000040 Alisn 0000000000001 1 00000000000 0 8 2010 zhu 00000000000001 1 0000000 000000000000 0000 0000000001 5 Cet ut 25 5 5 60 61 0000 01
91. 5 2 001 2 1 332 3321 10000000 Fig 3 11 00000000 00 0000000 001 Table 3 40 OUI rig3 10 eX O00 3 Table 3 4 Properties of YAG Ce nanoparticles prepared with and without citric acid Citric acid dav Ce 9 Absorbance ample 5 mol nm Y Ce a u 0 10 2 42 8 3 75 0 144 10 9 3 3 1 3 50 0 121 Nanosize 25 5 9 0 8 3 64 0 085 50 4 0 0 8 3 71 0 078 Reference 0 097 1 the number average particle diameter 2 the Ce Ce Y atomic ratio measured by XRF 3 the absorbance at 450nm 4 Fsample and Fret values in Eq 2 9 i e the integrated PL intensity at 530nm 5 IQEsampie Value calculated by Eq 2 9 PL intensity 7690 8921 6113 75
92. 6 10 YAG Ce Dn Do DU UU UI PSSPAH 000000000000 YAG ce 000000000000 Fig 6 10 b 6354 0 20000000000 000000 00000000 108 60 0 00000000 Fig 11 a OL 000001 Fig 6 11 000001 5 BSA
93. 8 1 1000 200 00 0 11 40100 0000000001 POR OO DOOD EET tooo oe oo ooo 1414 Cd 1 76 00000000 Dubertret CdSe ZnS O10 ul 46 Derfus 0 Casen 0000 215 000 11 77100 0 5 8 8 Deufus 0000 2950001
94. Fig8 50 0000000000000 2 8 312 2 2 115 9 00000000000 Gd 119 3 pm I B U U U D U U I 8312 Gd Y 4Gd Table8 4 000000000 edd 8313 8 98 Uni
95. 5600 nmi 00000 10 0 nm 0000 8322 Fig 8 1200 000000 813 8323 Fig 8 14 0000001 Gd YAG L Gd YAG T2 000 2 Fig 8 15 000 sl mM 0 sdi 00000 OO 52 442 Gd DOTA Ri R20 0 4 1 4 9 5 1 1 8 20 Rif 01 GdYAGO OOOO 83 19 Gd25mol9q 00000 ed25mol9 4 0 0 O Gd Gd4Y O Table 8 A Gd YAG I 0 0 0 Gd Gd Y 23 5mol94
96. 6223 YAGCe nn d d 00000 BSAD DI 6 2 2 3 40 00000 Fig 6 30 0 0 Obead30 0 0 0 550 00000000001 1mg mL 0 5 NaclQ 000000 bead 4 000 1 mg mL 0 5 bead 5 50 000001 0 5mL 1 3 mg mL EDC PBS 0 501 5mg mL BSA PBS 01 15 6 2221 5 3 5 bead 6 T 6224 YAG CeQ 0000000000000000 bead6Q 000 0 5mL 100000000 rabbit anti BSA O0lmLQO0015hOO000000006222Q0 000000000 PBS 300071 0000000000000 O5SmL QO 00000 5 bead 7 0 00 U PBS 1000 Alexa 647 goat anti rabbitlgG 1mL EH 1 5 7 d DB U U 00 rabbitloGO 00 6 2 2 20 000000000 PBSOOUOUO 300000000 1 000000 bead ST 623 2 5 Edipse Tablee 2 0000
97. UU UU 18 26106 000000000000 CdSMn 2Zns LavOaEu 000 0 8410 00 0 00000 amp 0 0000001 8 170 00 00001 Feet 000 18 420 ud 00 000000000000 000000 2 Cog Oo OOO Eu 20000000000000 00000 H ber 5 FePtu Cas 10 0 0 UU O U CU CI U U D I cas rePt 0000000 843 0 Choi in vitro 01 3000000000000000000000T0I cyS50000001 ID d dat utle151 D UI 000000 8 21 360000 260100001 0000 CdTe
98. 4 Forward scattering intensity 2 40 103 40 Fluorescence intensity 104 1 Forward scattering intensity Fig 6 10 Dot plot for the mixture of the bare PMMA beads and the composite beads of 5 10 and 15 mm in size measured by FCM a bare beads and PMMA YAG Ce gt b bare beads PMMA YAG Ce3 PSS PAH 116 60 0 00000000 Fig 6 11 Microscopic bright field images and fluorescence images b f of beads a b c bead 8 of 15 umin sizein Fig 6 1 d e f bead 3 treated with anti Rabbit gG Alexa Fluor 647 of 15 um sizein Fig 6 1 Images b were obtained under the condition of the filter block set 1 Images c f were obtained under the condition of the filter block set 2 117 10 103 10 Fluorescence intensity 10 10 1023 Forward scattering intensity 123 0 4 Peak 2 10 107 103 ot Red fluorescence intensity Number of beads Fig 6 12 Dot plot a and histogram of red fluorescence intensity b for the mixture of the bare and composite beads of 10 and 15 um in size measured by FCM The beads corresponding to the peak 2 shown in the b were detected as red dots shown in a by gating 118
99. p p rpm p C3 C3 Ej r rm b p p o SS oo o oo Sie a a Ld LJ E Oooo C3 E LJ pr E DL p C p E p B pr Oooo Oooo rr t i rir a Q avana n ao c3 og Soe ooo EE a u Er o L LI LI LCI CI L3 Too Oooo a CLI LI ol ALL L LS 9 0 LER a e cce o rid adii rn um Em em mmu WR omi 500100 0000000 Eje oe o Soo 1 O E3 m Ed 3 C3 o oo LJ m 5 Ooo ccc FFF oof ee ee eee 22 EI Cid ele EIE mL E ES LL LL LJ Ls o E m UC U OG VEU m ee TRITT m ooo oo O 0 A g Oooo m m ooo rm rt L a
100. 31 311 000000 Y Als0x 1970 CQOOO0O000BI0DO00000000000000000000T 2 5 ngu 0 B U U I Czochralski 0 5 41 00 000000000000000 3 610 0000 B 7 900 0 0 0 8 1000 0 0 8 1100 0 0 1 2 D 3 130 YAPO 0 4 2 700 1500 C0 0000000000 5 13 16 1700 0 000 13 18 2010 00000000000000000000 9 0000000 3 17 312 0000 YAGOHOOOOOY00000 00000 196700 Blasse
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102. 7 0mol94 GGd25mol 30 MRI O00 U Gd25mol q 00000 eeYAGr I J 1 Gd YAG Gd25mol 6 OO000 Gd YAG 148 080 833 0 8 3 20 Gd YAGQO OOOO T1000000000000000000000000 I
103. D pnaunpgle13 3200000000000 18 6 20 0 0 00000 Feud 8 240 0 NaYFa ErYb 8 3310 000 001 Ga OU 0 T 2000000000 000 8 200001 89 18 814 23 814 70000 6 21 2 20 0001 100 Gd 1i
104. 000000000060 Intensity 32 5 33 33 5 20 deg Fig 7 4 XRD peak of 420 plane a as prepared b calcined at 600 c calcined at 900 d calcined at 1300 131 KM intensity 4000 8 3500 3000 2500 2000 1500 1000 Wavenumber cm Fig 7 5 FT IR spectra of YAG Y b nanoparticles a as prepared b calcined at 600 C c calcined at 900 C d calcined at 1300 C 132 Weight loss O70 00000 000000000060 exoo lt endo 0 200 400 600 800 1000 1200 Temperature C Fig 7 6 TG DTA profile of as prepared YAG Y b nanoparticles 133 0 15 Absorbance o 5 400 600 800 1000 1200 1400 Wavelength nm Fig 7 7 UV vis NIR spectra of YAG Y b nanoparticles b calcined at 600 c calcined at 900 C d calcined at 1300 C Absorbance me 950 960 970 980 990 1000 Wavelength nm Fig 7 8 Absorption peaks assigned tof f transition of Y b3 a as prepared b calcined at 600 C c calcined at 900 C d calcined at 1300 C 134 O70 00000 000000000060 400 300 200 PL intensity a 100 0 960 1000 1040 1080 1120 1160 1200 Wavelength nm Fig 7 9 PL spectra of samples under irradiation of NIR laser 940 nm a as prepared b calcined at 600 C c calcined at 900 C d calcined at 1300 C 135 Number 1 10 100 1000 Diameter nm
105. 5 2hO 0000000007 10000 rpm 35 ming D rb t 5 5223 5 2 22 00000 000000 15 mL 10 mg mL Sulfo NHS PBS 15 mL 20 mg mL EDC PBSQ 0 24mLQQ00002h 0 i 10000 rpm 35 3 10 1 5 850 D UD 00 10000 rpm 35 301 10 5224
106. Fig 7 10 Particle size distribution measured by DLS for YAG Yb nanoparticles diluted in ultrapure water 110 zeii ke ee 90 80 70 60 50 40 30 Normalized PL intensity e 20 40 60 80 100 120 Time min Fig 7 10 The change in the PL intensity with time a YAG Y b nanoparticles under irradiation of NIR laser A 940 nm b Alexa680 under irradiation of 680 nm light 136 O70 00000 000000000060 74 YAGYb 0000 1000000 1 Yeo 2 137 0 7000000 7 1 V R Kondepati H M Heise J Backhaus Recent applications of near infrared spectroscopy in cancer diagnosis and therapy Anal Bioanal Chem 390 125 139 2008 7 2 R Weissleder Tung U Mahmood A Bogdanov r In vivo imaging of tumors with protease activated near infrared fluorescent probes Nat Biotechnol 17
107. G00mL ming 823 0000000 0 200000000000 FE SEM XRD XRF DLS MRI NIR PL 83 0000000 831 GAG YAGH LH E I UE 8311 050001 Fig 8 3 FE SEMQ 0000 GAG YAG I 5 Fig 8 40 8 4 lt Gd Gaun Table84 145 Table 8 4 Properties of GAG YAG nanoparticle Sample d nm d nm Gd Gd Y 96 GdOmol 56 0 45 0 0 Gd25mol 64 6 49 2 23 5 Gd50mol 74 8 67 8 50 2 Gd75mol 97 3 81 3 73 1 Gd100mol 125 1 126 9 100 1 calculated from SEM images 2 measured by DLS
108. 104 60 0 00000000 62 0000 621 0 600000000000 Tableo 19 00000 Table 6 1 List of reagents Reagent Purity FW Maker 1 4 butanediol gt 97 0 90 12 Kanto Kagaku 1 ethyl 3 3 dimethylaminopropyl 191 70 Pierce hydrochloride EDC 3 aminopropyltrimethoxysilane 131 25 Chisso Chemical Division Albumin bovine serum BSA gt 99 Sigma Alexa Fluor 647 goat anti rabbit IgG Molecular probe Aluminium isopropoxide gt 99 9 204 24 Kanto Kagaku Avidin immobilized agarose gel beads Sigma Avidin immobilized Micromod Partikeltechnologie polystyrene copolymer beads Cerium Ill acetate monohydrate gt 99 99 335 26 Kanto Kagaku Sulfosuccinimidyl 6 biotinamido hexanoate biotinyl agent Poly acrylic acid PAA 2000 Alrich Poly allylamine hydrochloride PAH 15 000 Aldrich Poly sodium 4 styrenesulfonate PSS 70 000 Aldrich Rabbit anti bovine serum albumin Sign anti BSA Yttrium acetate tetrahydrate 299 9996 338 10 Kanto Kagaku 622 0000000 6221 YAGCe 00 00060 5 4000 7 425 mmol 2 5190 000000 11 1000 0 0075 mmol 0 025190 000000000000 12 50 mmol 2 55 90 0 000000
109. Ce 4f amp F 25dCA sgU 0000001 2 72 92 1 93 94 OU 10 000 000 200 1 951000 9 7 1 000000000000 Kasuya 0 0000000014000001 1000000 10 11 97 980 0 0000000000000 UU 2 4050 3
110. Omol b 10mol c 25mol d 50mol 55 Absorbance 350 400 450 500 550 Wavelength nm Fig 3 16 UV vis absorption spectra of the samples prepared with and without citric acid Omol b LOmol c 25mol d 50mol 96 56 O30 250 200 150 100 PL intensity 0 2 300 350 400 450 500 550 600 650 700 Wavelength Fig 3 17 PL and PLE spectra of the samples prepared with and without citric acid a Omol b 10mol96 c 25mol d 50mol 57 0 50 100 150 200 250 300 Time ns Fig 3 18 PL decay curves of YAG Ce nanoparticles prepared by without and with citric acid a Omol96 b 10mol96 c 25 01 d 50mol and micronsized commercial bulk Lines are obtained by curve fitting 58 O30 Number C potential mV Fig 3 19 C potential distribution of the samples prepared with and without citric ad d a Omol b 10mol9 c 25mol d 50mol 59 34 00 0000000 40nm 000 2001 16 26 ns v 72 112 ns 20 000001 YAG Ce 0000 0000
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112. 10 0 45 4 9 2 43 4 9 4 3314 000000000000 4900000000000 000 13 4410 00000 0 0000000000000000000 0000001 Fig3 80 00 0000000000000 0000000000000 00 0000 14 00000 3 M M O M 47 3 46 39 458 4900 52 3 18
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115. Assignment Ref YAG Ce 1 3700 3700 v OH 4 25 2 3400 3400 v OH 4 25 3 3091 v NH 4 26 4 2950 v CH 4 27 5 2370 2370 4 27 6 2118 combination tone or 7 1975 overtone of 2 8 1643 4 26 9 1551 1558 v5 COO 4 27 28 10 1458 5 4 27 11 1436 v5 COO 4 27 28 12 1358 1352 CHz2 4 27 13 1176 v Si O X 14 1067 X Al Y Ce 15 1061 v C O 4 27 16 1023 v C O 4 27 17 700 700 v 5 Al O 4 30 Fig4 9000 Ce 1 L1 L1 LI I Fig 4 9 a 000 00 0 0 1l 000 FE SEM Fig 4 10 0 0 Fig 4 10 a o 00000001 70 O40 00000 000000000060 0 000 5 0000000001 Fig41090 0000000000000000000 Fig4 10d 0 DU t 71 Y CH4COO 44H O Ce CH COO H O AIP H O APTMS stirring for 2 h 1 4 butanediol Washed with ultrapur
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120. 23 23 24 24 24 25 33 34 34 34 34 34 36 36 37 37 37 37 37 38 38 38 38 38 38 39 40 40 40 41 41 42 42 3 3 2 7 OO 0000 34 03001 YAG Ce7 00000000000 41 411 412 42 O00 421 422 4221 D D B 42 2 4223 D Dl 4224 423 D 43 DDD 4 3 1 D 4 3 2 APT YAG Ce 43 3 44 04001 050 51 512 5 2 000 521 522 5 2 2 1 5 2 2 2 5 2 2 3 YAG Ce 000000 5 2 2 4 5 23 0000000 3 00000 5 3 1 PAA 000 42 60 61 66 66 67 67 67 67 67 68 68 68 68 68 69 70 79 80 83 83 84 85 85 85 85 85 86 86 86 86 86 5 3 2 0000000001 53 3 0000000001 54 5000000 YAG Ce 000 BSA 60 YAG Ce 7 000000000 LU DL ELO EI UT
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122. 83 33 149 83 34 NIR PE T C 149 84 165 D 8000001 166 O90 00000000 91 000000 170 92 171 9 2 1 171 922 10 D D 172 923 0000 172 924 0000 173 925 173 926 174 175 UU 179 vi O10 11 00000001 Table 1 100000 1
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127. 00 3 000 0000 0000 0000 01 0 00001 0000000000000 000 0 52 0 0 000000001 2005 3000 4 0000 000 0000 1 u t YAG Ce 00001 0 5200000001 20050 30 00 510000 0000 0000 0000 000 1 0000000000 00 0 4601 0 20050 100 6 000 0001 7 53000000 2006 30 1710000 D UI 0 00000 000 00 0 000800 YAG Ces L 0 20070 1 0 PMMA 0000 0 45000000080 1810 000 000 0000 0000 000 00 EE ED 2000001 000000 YAG ce0 00 0 PMMA 40000001 OO0000 20079 30 00 191000 0000 000 OO 0 00000 00000 00 0 2440000000 2007 50 10 000 0000 000 0000 000000000 000 0000 0000 mam 20 000000000000 2007 6 176 110 000 0010 0000 0000 000 00 0 000
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131. Bate D D U LU LI D I Cauchy Lorentz 0000 Bota Bow Pee Eq 2 4 gt 5000 5 DB ota df df Eq 2 5 Eq 2 3 ScherreQ OOEq2 190 0000000000000 d ice 2es Eq 2 6 k k s Eq 2 7 0 d Eq 2 600 25000000 DB oat Eu 2es Eq 2 8 Du Eq 2 80 0 0 22 00 XO D U 5 30000000 203 03 Ceo Y Ce Al 3 1 x 3x 5 Osx lt 0 04 9 000000 Cel 00000001 20 Dau 000000000600 Fig 2 10 000 23 231 0000 Bio Rad FTS 60A 0 0 0 00 6 Tab
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133. Ce nanoparticles dispersed in ultra purewater b FITC dispersed in ultra purewater Normalized PL intensity 75 Transmittance 3500 2500 1500 500 Wavenumber Fig 4 8 FT IR spectra YAG Ce nanoparticles APTMS YAG Ce nanoparticles O40 00000 00000000000 a rn J 100um 100um Fig 4 9 Microscopic images of avidin immobilized agarose gel beads a b treated with biotinylated YAG Ce nanopartides c d treated with YAG Ce nanoparticles without biotin a bright field image b d fluorescent i mage 77 Fig 4 10 Microscopic images of avidin immobilized polystyrene copolymer beads a b d e after treating with biotinylated nanoparticles c before treating with biotinylated YAG Ce nanoparticles a bright field image b fluorescent image c e FE SEM images 78 O40 00000 00000000000 44 DD 1000000 10 00000000001 YAG Ce 1 0 00 D YAG Ce n 0000000 0000000601 YAG Ce
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136. Table 3 6 PL decay parameters obtained by curve fitting Citric acid Time constant ns Relative amplitude Sample mol 0 16 1 74 2 35 5 64 5 10 26 3 107 7 30 8 69 2 25 24 5 115 0 28 5 71 5 50 25 5 113 3 27 7 72 3 Microsize 57 3 100 1 lo As exp t t1 A2exp t t2 2 lo Av exp t z 3326 0001 000000000000000000000000000000000000 00 3314 Fig38 0 0000 01 0 0 0000000000000 0000000000000000 001 14 42 319
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138. precursor in glycothermal reaction a low precursor concentration b high precursor concentration 50 O30 Fig 3 11 FE TEM images of the samples prepared with and without citric acid Nominal percentage of citric acid for the theoretical yield of YAG a e Omoal b 10mol96 25mol and d f 50mol 51 Intensity Fig 3 12 XRD profiles of the samples prepared with and without citric acid Omoal b 10mol96 c 25mol96 d 50moal e 3 5 12 J CP DS 33 40 52 O30 Intensity 28 285 29 295 30 305 31 20 deg Fig 3 13 Precisely measured XRD peak of 400 plane a micronsized commercial YAG Ce bulk b nanosized prepared without citric c nanosized YAG Ce prepared with citric acid 50mol 53 KM intensity 0 5 nile 0 W 2200 2000 1800 1600 1400 1200 1000 800 Wavenumber cm Fig 3 14 FT IR spectra of the samples prepared with and without citric acid a Omol b 10mol c 25mol d 50mol The Kubelka Munk KM intensity relative to the peak at 1060 corresponding to v C O is shown in this figure 54 O30 900 800 700 600 500 400 Wavenumber cm Fig 3 15 FT IR spectra of the samples prepared with and without citric acid
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140. 0 0000 1 0000 0000000000000 0 0000000000000 0000 000 6 amp 0000000000000 2007 9 000 1210 000 4010 000 0000 460 0000000000000 2008 10 000 2008 0 10 000 141 II 0000 0000 0000 0000 0000 4 0000000601 7 3000071 OOOU0000 20080 50 151000 0000 0000 000 250000000 2008 5 0 00 161 0000 000 0000 000000000000 00 O00 250000000 2008 5 00 1710 000 000 0000 0000 0000 00000 0000 Gd YAc Yb 000000000 0 250000000 20080 5 00 4 0000060 110000 000 0000 00 0000 00 0 00000 0000 7 O0 O J P2006 162284 20040 120 2000 2 0000 0
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142. 0 1154 nm 0 7B CD U 7 7 D I I Fig 7 11 YAG Yb T 0 U D U U U U I Alexa680 0 0 0 00 35 2 127 Y CH COO 44H O Yb CH COO 4H O AI DCH CH 1 4 butanediol Washed with ethanol Centrifuged 10000 rpm 30 min x3 Autoclave As prepared sample 300 C for 2 h 300 rpm Calcination for 2 h at 600 1300 C cooling to RT sedimentation Calcined sample YAG Yb colloidal solution Fig 7 1 Schematic representation of the synthesis of YAG Y b nanoparticles 128 O70 00000 YAGYS 4 00000000000 Fig 7 2 a c TEM images of samples a as prepared b calcined at 600 C calcined at 900 C d SEM micrograph of sample calcined at 1300 C 129 Intensity 10 20 30 40 50 60 20 deg Fig 7 3 XRD profiles of samples as prepared b calcined at 600 C calcined at 900 C d calcined at 1300 C 130 O70 00000
143. 0 63 6 300 rpm I 00125h00000 300 COOU000 O2hOOO000000000000000000000000000 1 O70 00000 YAGYSs4 00000000000 30000000000 60 C 1 day 0 2 300 71 10000 rpm 30 ming 0000000 OOo t OOo t OHHH HH Lr 723 0000000 0 20000000000 OFE TEM FE SEM XRD PL PLE FT IR VSM Stokes Wilson L 73 00000 731 Fig7 20 0000000000000 FE TEMT ED UU UFig 7 2 a 0000001 14 5nm 00000 2 6nm 0 0O 0 19 7 2000 00000 se0 cOOOO00000000000000007 001 900 C0 0000000 0 Fig
144. 000 000 0000 0000 00 0 00000 000 00 PCT 2007 230877 20060 20 27000 31000 0000 00 0000000000 0 pp 225 232 2007 41 000 0000 0000 0000 0000 0400000000000 177 D00000 000000000000000 vo 2 No1 00000 pp13 16 2009 178 3832000000000001 0 ut 179
145. 000000000 106 60 0 00000000 Table 6 2 Condition of filter block set Excitation wavelength Dichroic wavelength Emission wavelength Filter block set 1 430 440 nm 505 nm 515 555 nm Filter block set 2 605 655nm 650 nm 667 5 722 5 nm 63 00000 631 Fig64a0 000 YAG ce 7OOOO0000000000000000000000000 4 55 2 000000 5 20min 0 6 2 YAG Ce 0000 305 632 9 660 0000000000 5 000 0 00 000000000 0 19 6 6
146. 000000000 13 210 00 LED U U U U L OOO LEDI3 222240 y0 0 000000000 0 32252617 000000000801 OUUU Fig 3 10 0 YAGI I III Cet 00000 3270 4 00 0000 O00071 FseQ Fr 200000000000 000S5d00000000I 5 5 4 0 0000000000801 5d00000000000000000000000000000T 3 6 28 313 00000000000 ua 0000 3131 JUD D d B dab u d Bn p uut 140000000000000TT I 3 29 FesO4 3 301 0000 OOOOD I331N 0000000000 ZnGa 2043 320 00000000000001 34 O30 0 000000000000000600 13 33000 0 5 340 00 00 3 350 000000000000 UL UD BL BL BL BL EL E noue 1 DE D E C C D E EE CO D D D D B D OI E 7T CIO 00001 0000 014 YAG p 0 DD U I 3 190 0000 350 600 75 150 MPa 4 280 300 4
147. 000000000 La0 S Yb Er 00000000000000 48 9 00 14 10 5 411121 1 ILaF 4 13 15 NaYF 4 4 16 001 OU L WengD Dl a 20nm NaYFaYb Er 1 4 1810 00 00 II O Chatterjee 4 17 0 419 1 4 13 1600 0 0000000000000001 4 15 000000000001 8 0 00 42019 YVO Eu 0 0 14 210 Eu 4 220 00 0000000000000000 0000000
148. 00000000000000000000000000001 1 1 000000 10mm 00000000 3 47 49 0000 0 5 00080 548 60000001 4 14 00000000 13 4900 0 001409 0000000000000000000001 08000000000 2 0000000 04 0000000000000 0000000000 4710 314 0000 Kasuyap 0 0000000000000 00000 0000 0100 OOO 0 50nmg 20000000000000000 5 3 1I 1 3 500 0 0 0 00000 3 51
149. 00000001 432 APTMS YAG Ce 00 0 YAG Ce DES 1D UO D I D U U I 41 45 5 3nmU0 0000 9 1nm l 0000001 APTMSQ O00 0000 Fig 4 80 00000 Table 4 20 0 00APTMSO0OO000000000000 0 3091 1643 r3 OU 2 1176 cm 0 0 1067 em 0 L 69 v stretching 5 bending o wagging as asymmetric s symmetric 433 00000 YAGCe 000 0000000 si O xgo00 X Al Y ce 00000510 00000601 APTMS 370 000000 UUUOUUI 000 42 Table 4 2 Assignment of FT IR spectra Peak number SRM E YAG Ce
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151. 140000000 636m 300 000 15 0000 300 COO00000 2 0000001 100000000000000000000000000000000 6222 YAGCe 000000000 62 2249 000000 Fig6 10 00000000000 Fig6 2000000071 1 O2bET or O3ET bead 10 6 2 2 1 105 100000000 2000 rpm 2 3 0 00000001 3 000 bead 20 0 0 bead20 0000 1 mg mL 55 0 5 25mL 20 2000rpm 2 3 00000000 00 55 3 255 bead 300 00 000 000 PMMA YAG Ce PSS n
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153. 28 19920 5 29 2 133 0000000 0 19420 0 Weissman 00 0 Eu 7O00000000000000000CT 1 330 000000 300000000000000000000000dD3 1 4f 4f 100 us D T D L L 14 0000000000000000
154. 5 172 Den 00000000 1 4 3000000000000001 10 102 0000 001 173 3 100000
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156. 6000000000000 0000 55080 0000000000000 Fig 6 6 c ID 0000 YAc ce0 0000000000000 000 00060 0000 PSSO 2000000000000 6 6 0000 0 0000000000000 67 2 67 1 Fig 6 700 0000000000000000 633 TG DTAQD 000000001 Fig 6 80 000000 5 250 400 600 00 0000000 000 YAG ce 0000 PSSO 1 20 0800000000000 DD DI 0 54 2 2 wt 0 0000000000 40000
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160. 96 16933 70 22 0 30 2 29 5 40 1 72 0 3322 9 312 YAG D 0000 3 13 400 001 350000000000001 OU YAG Ce Kasei Optnix P46 Y 1 ul 001 40 O30 YAG Ce I 4000 000000000 4000 000000000000T0I
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164. LJ Li Nicon E600 0 0 0000 Table4 2Q 00000 Table 4 2 Condition of filter block set Excitation wavelength Dichroic wavelength Emission wavelength 430 440 nm 505 nm 515 555 nm 43 00000 431 00000 YAGCe D 43 YAG ce 000 68 O40 00000 Yaecedmnaupna gpnannun OOO Fig 4 7 488am 00000000001 4 23 2410 100000 95nmp 00000 1 2nm0 0 000000 Fig440 00 XRD 5 Fig 45 D t D U LU 46 8 0000 7 5 nm 100000000000 2 9 4 6 450nm 00 345 nm 200000000000 5 4f amp F o 5d Big 530 0 0 570
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166. MA YAG Ce PSS beads Fig 6 2 Schematic representation of the preparation of PMMA YAG Ce composite beads 110 0 60 0 00000000 PMMA YAG Ce PSS beads EDC PBS solution PAH NaClaq solution PSAP E stirring 20 min stirring 1 5 h Centrifuged 2000 rpm 2 3 min Centrifuged 2000 rpm 2 3 min Re dispersed in H O x3 Re dispersed in H O x3 BSA tagged PMMA YAG beads PMMA YAG Ce PSS PAH beads rabbit anti BSA PAA NaClaq solution stirring 1 5 h stirring 20 min i Centrifuged 2000 rpm 2 3 min x3 Centrifuged 2000 rpm 2 3 min Re dispersed in Re dispersed in H O x3 rabbit IgG tagged beads PMMA YAG Ce PSS PAH PAA beads anti rabbit IgG with Alexa 647 stirring 1 5 h Centrifuged 2000 rpm 2 3 min Re dispersed in H O x3 Alexa tagged PMMA Y AG beads Fig 6 3 Schematic representation of the conjugation with BSA and tagging with organic dye 111 Zeta potential mV 0 20 40 60 80 100 120 Time min Fig 6 4 Change in zeta potential of composite beads with mixing time b PMMA YAG Ce3 PSS c PMMA YAG Ce2 PSS YAG Ce d PMMA YAG Ce3 PSS 2 60 PMMA YAG Ce PMMA YAG Ce PSS YAG Ce 40 20 Zeta Potential mV eo PMMA YAG Ce PSS Layer Number Fig 6 5 Change in saturated zeta potentials by sequential ads
167. OMS5hOO000 2 D L1 D 20000 rpm 30 0000000000 30000000000 60 9 8 108 00000000000 Gd0mol Gd25mol Gd50mol Gd75mol Gd100mol Table 8 2 Quantity of reagents Yttrium acetate tetrahydrate g mmol 7 5 2 54 1 902 5 63 1 268 3 75 0 634 1 87 Gadolinium acetate tetrahydrate g mmol 0 762 1 87 1 524 3 75 2 286 5 63 3 048 7 5 Aluminium isopropoxide g mmol 12 50 2 55 12 50 2 55 12 50 2 55 12 50 2 55 12 50 2 55 8222 Gd YAG J 0 0 00 YAG L1 L I I YAG Yb D 000000 cad 000000000001 2 40000000 144 080
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172. e MPa 0 00 05 10 15 20 25 30 3 5 Time h Fig 8 5 Plots of temperature and pressure vs time a GdOmol b Gd25mol96 50 1 d Gd75mol e Gd100mol96 152 080 vc Yb OOOO0O0000000 Intensity YAG 33 40 10 20 30 40 50 60 Fig 8 6 XRD profiles of GAG YAG nanoparticles 8 GdOmol b Gd25mol96 Gd50mol d Gd75mol e Gd100mol 153 Intensity 32 4 32 6 32 9 33 1 33 4 33 6 20 deg Fig 8 7 XRD peaks of 420 plane a GdOmol b 25 1 Gd50mol d Gd75mol96 Gd100 mol 154 080 69 OOOOOO000000 0 mg mL 20 mg mL T weighted 100 mg mL 500 mg mL 0 mg mL 20 mg mL T weighted 100 mg mL 500 mg mL Fig 8 8 MR images a Gd25mol b Gd50mol9o c Gd75mol9e d Gd100mol96 155 0 0 5 1 1 5 2 0 0 0 2 0 4 0 8 1 0 1 2 Gd mM 0 6 Gd mM 0 0 0 0 0 5 1 0 1 5 2 0 2 5 3 0 0 0 0 5 1 0 1 5 2 0 2 5 Gd mM Gd mM Fig 8 9 Plots of 1 1 and 1 T2 vs Gd concentration a Gd25mol96 b Gd50mol Gd75mol9 d Gd100mol 90 156 gnetization emu Ma 080 0 15 0 1 0 1 1 6 10 1 2 10 8000 4000 4000 8000 1 210 1 6 10 Magnetic field Oe Fig 8 10 VSM measurement of a Gd25mol and b Gd100mol 96 157 Fi
173. e water Centrifuged 10000 rpm 20 min Autoclave 300 C for 2 h 300 rpm APTMS YAG Ce colloidal solution cooling to RT sedimentation sulfo NHS LC biotin YAG Ce colloidal solution stirring for 2 h Washed with ultrapure water x3 Centrifuged 10000 rpm 20 min Biotinylated YAG Ce colloidal solution Fig 4 1 Schematic representation of the preparation of biotinylated YAG Ce nanoparticles Sulfo NHS LC Biotin APTMS 2 lt MeO OMe Fig 4 2 Illustration of the preparation of the biotinylated nanoparticles O40 00000 00000000000 Fig 4 3 TEM micrograph of YAG Ce nanoparticles 73 Intensity 33 40 Er 10 20 30 40 50 60 20 deg Fig 4 4 XRD profile of YAG Ce nanoparticles 30 25 20 15 10 Number 1 10 100 1000 Diameter nm Fig 4 5 Particlesize distribution measured by DLS for YAG Ce nanoparticles diluted in ultrapure water solid line APTMS YAG Ce nanoparticles diluted in ultra purewater broken line O40 00000 00000000000 120 100 80 60 40 PL intensity a u 20 0 300 350 400 450 500 550 600 650 700 Wavelength nm Fig 4 6 PL and PLE spectra of the YAG Ce nanoparticles dispersed in 1 4 butanediol 110 100 90 80 70 60 50 40 30 0 30 60 90 Time min Fig 4 7 The change in the PL intensity with time under irradiation of 488 nm light a YAG
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177. g 8 11 FE SEM images of a YAG nanoparticles and b Gd YAG nanoparticles 158 080 Intensity YAG 33 40 Fig 8 12 XRD profiles of a YAG nanoparticles and b Gd YAG nanoparticles Intensity we 32 6 32 8 33 0 33 2 33 4 33 6 20 deg Fig 8 13 XRD peaks of 420 plane a YAG nanoparticles and b Gd YAG nanoparticles 159 T weighted T weighted 0 mg mL 20 mg mL 100 mg mL 500 mg mL Fig 8 14 MR images of Gd YAG nanoparitcle dispersed in agalose gel 30 25 0 0 00 0 05 0 10 0 15 0 20 0 25 0 30 0 35 0 40 Gd mM Fig 8 15 Plots of 1 T1 and 1 T2 vs Gd concentration of Gd YAG nanoparticles 160 080 vAcvbesmuggaadgpiuutuuntu Fig 8 16 FE TEM image of Gd YA Y b nanoparticle Fig 8 17 FE SEM image of Gd YA Y b nanoparticles 161 30 25 20 15 Number 96 10 1 10 100 1000 Diameter nm Fig 8 18 Partide size distribution measured by DLS for Gd YAG Yb nanoparticles diluted in ultrapure water 162 0 80 00000000000000 Gd 000000000000 T weighted T weighted 0 mg mL 20 mg mL 100 mg mL 500 mg mL Fig 8 19 MR images of Gd YAG Y b nanoparitcle dispersed in agalose gel 30 25 VT 5 s N O O O 0 1 0 2 0 3 0 4 0 5 Gd mM Fig 8 20 Plots of 1 and 1 T2 vs Gd concentration 163 PL i
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182. in YAG Ce nanoparticle Fig 5 2 Illustration of plate assay for detecting BSA 90 O50 000000000 Fig 5 3 Photographs of YAG Ce nanoparticles dispersed in water a and PBS b and PAA modified YAG Ce nanoparticles dispersed in PBS c Number 96 T 0 0 50 100 150 Diameter nm Fig 5 4 Particle size distribution in water measured by DLS a nanoparticles b PAA modified YAG Ce nanoparticles c streptavidin immobilized YAG Ce nanoparticles 91 30 25 20 L 15 2 z 10 0 100 50 0 50 100 C potential mV Fig 5 5 C potential distribution of a YAG Ce nanoparticles b PAA modified YAG Ce nanopartides and c streptavidin immobilized YAG Ce nanoparticles 92 O50 000000000 Transmittance 4000 3500 3000 2500 2000 1500 1000 500 Wavenumber Fig 5 6 FT IR spectra of a YAG Ce nanoparticles b PAA modified YAG Ce3 nanoparticles and c streptavidin immobilized YAG Ce nanoparticles 93 u O Co e N O O O O O Normalized PL intensity a N 0 300 350 400 450 500 550 600 650 Wavelength nm Fig 5 7 PL and PLE spectra of PAA modified YAG Ce nanoparticles O50 000000000 o a o m T
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184. ku Avidin immobilized agarose gel beads Sigma Avidin immobilized Micromod Partikeltechnologie polystyrene copolymer beads Cerium Ill acetate monohydrate gt 99 99 335 26 Kanto Kagaku Sulfosuccinimidyl 6 biotinamido 556 59 Pierce hexanoate biotinyl agent Yttrium acetate tetrahydrate gt 99 99 338 10 Kanto Kagaku 422 4221 0000000 000000 TVS 120 N29 00000000 4000 7 425 mma 190000000 1009 0 0075 mmol 0 025190 0 00001 Uil 2 5 OU 12 50 mma 2 55 90 00000000 140000000 63 6 mL 300 00015h00000 2 1 67 4222 422100000 5 0000 1 5 150nL 2 10000 rpm 20 ul 1 Fig4 2Q STEP 1 2 UU 5
185. l Centrifuged 10000 rpm 30 min powdered sample x3 Autoclave 300 9C for 2 h 300 rpm cooling to RT sedimentation YAG Ce colloidal solution Fig 3 4 Schematic representation of the synthesis of YAG Ce nanoparticles with citric acid 45 350 lt 300 250 T _ 200 2 D 150 n 100 50 3 5 aunyesodwa Fig 3 5 Change in pressure during glycothermal reaction a YAG 0 5 b YAG 1 25 YAG 2 5 d programmed temperature O30 20 nm Fig 3 6 FE TEM images of YAG Ce nanoparticles YAG 0 5 b YAG 1 25 0 YAG 2 5 47 Number 1 10 100 1000 Diameter nm Fig 3 7 Particle size distribution measured by DLS for YAG Ce nanoparticles diluted in ultrapure water a YAG 0 5 b YAG 1 25 YAG 2 5 O30 RO AI OR HO CH OH RO RO 1 RO AI O CH 7 Z R A 2 AI OH 7 CH RO RO RO JAI OH M OR RO OR AI O M RO OR Fig 3 8 Formation of Al O M M Al Y or Ce bond during glycothermal reaction 49 exo lt endo 0 200 400 600 800 1000 1200 Temperature C Fig 3 9 DTA profiles of a powder obtained from supernatant and b powder obtained from whole sample Precursor concentration Precursor concentration Fig 3 10 Illustration of the distribution of the
186. le2 20 000 000 FT IR Table 2 2 Measurement conditions of FT IR spectra FTS 60A FT IR 6100 Matrix KBr CaF2 Measurement region cm 400 4000 800 2200 Resolution cm 2 2 Acquisition time 32 100 232 Ul OUUU 6100 Table2 3 Table 2 3 Measurement conditions of FT IR spectra Matrix 08 2 Measurement region cm 400 4000 Resolution 4 Acquisition time 128 24 D ED B D LITG DTAT ul Tabi e2 4 D lU TG8120 0000 e Al2Os 00000 Table 2 4 Measurement conditions of TG D TA Sample weight mg 10 Heating rate K Jmin 10 Maximum temperature C 1300 Air flow mL min 200 22 21 251 D E E E U E EFE TEMTT 00000 FEI Temai 1200 00 00001
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189. ntensity a u 140 120 100 80 60 40 20 0 960 990 1020 1050 1080 1110 Wavelength nm Fig 8 21 PL spectra of Gd YAG Y b nanoparticles 164 080 vAcvbesmugmugagaugpiuuuuntu 84 Gd II 56 125 0 00 0 0000000000000 208 00000000000 OOO 1000000 10
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191. orption 112 0 60 0 00000000 Fig 6 6 FE SEM images of beads b bare PMMA c d PMMA YAG Ce PSS f PMMA YAG Ce PSS b d f expanded images of marked areas in a C e Fig 6 7 Fluorescence images and bright field images inset of beads a bare PMMA b PMMA YAG Ce3 PSS c PMMA YAG Ce PSS Fluorescence images were obtained under the condition of the filter block set 1 113 20 fom 5 2 2 40 100 O 200 300 400 500 600 700 800 m Temperature C 60 80 100 0 200 400 600 800 1000 1200 Temperature C Fig 6 8 TG profile of a PMMA YAG Ce3 PSS b PMMA YAG Ce PSS of 15 umin size 114 60 0 00000000 10 region region 2 Fluorescence intensity 10 104 103 103 8 b 3 2 o ji Q E 101 107 1032 10 2 Fluorescence intensity 64 O Number of beads a 10 107 10 10 Fluorescence intensity Fig 6 9 Histograms of fluorescence intensity a b and dot plot c for the mixture of the bare PMMA beads and the composite beads PMMA YAG Ce PSS and PMMA YAG Ce PSS z of 10 and 15 um in size measured by FCM a 10 um beads b 15 um beads c 10 and 15 um beads 115 10 103 10 Fluorescence intensity 10
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