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1 Scintillation 5 1.1 Scintillation process .......... .......... ....... 5 1.2 Conversion process ................... ....... 7 1.2.1 Interaction of radiation with matter . ............ 7 1.2.2 Multiplication, relaxation and thermalization electron-hole pairs ........ . ...... ..... ....... 9 1.3 Formation of defects and transfer process ............ . . 10 1.3.1 Formation of defects ..................... 10 1.3.2 Energy transport ................. ...... 12 1.4 Emission process ......... .................. 16 2 Scintillation materials 19 2.1 Introduction ....... ........ ......... ..... 19 2.2 Applications and drivers of scintillator development ........ 19 2.2.1 High energy physics . ......... ....... ..... 19 2.2.2 Medical imaging ............. ......... 20 2.2.3 Neutron physics ................... .. . . 20 2.3 Known scintillators and their properties . ............. 21 2.4 Fundamental limits and directions in the search for the new scin- tillator ................... ........... .. 24 2.4.1 Scintillation speed ............... ....... 24 2.4.2 Light yield ................... ...... . 25 2.4.3 Energy resolution ................... .... 25 2.4.4 Density ................... ....... . 26 2.5 Selection of the studied compounds . ................ 27 3 Experimental 31 3.1 Crystals ................... .......... .. 31 3.2 Scintillation Measurements ................... ...... 32 3.2.1 X-ray excited emission and afterglow measurements . . . . 32 3.2.2 Pulse height measurements .................. 33 3.2.3 Scintillation decay measurements ........ ...... 38 3.3 Luminescence characteristics measurements . ............ 40 3.3.1 UV/VIS spectroscopy . ............ .... ... . 40 3.3.2 Vacuum Ultraviolet (VUV) excitation and emission spec- troscopy ...... ... ............... . . 40 3.3.3 Optically excited decay time measurements ..... .... .. 41 3.3.4 Time resolved excitation and emission spectroscopy . . . . 42 3.4 Temperature-dependent measurements . .............. 43 4 LuI3: Ce3+: High light yield scintillator for photodiode readout 45 4.1 Introduction .................. .......... ..45 4.2 Materials .................. . .......... . 46 4.3 Scintillation properties of 2-4 mm3 crystals . ............ 46 4.3.1 X-ray excited emission spectra ..... ......... .. 46 4.3.2 Light detection . ................... .. . 47 4.3.3 Pulse height experiments .......... ...... ... 49 4.3.4 Time profile ............. .......... ..52 4.4 Scintillation properties of 2 x 6 x 8 mm3 crystals ......... . 53 4.4.1 X-ray excited emission spectra . ............... 53 4.4.2 Pulse height experiments ................... 55 4.4.3 Time profile . ........ ................ . 56 4.5 Conclusion. ............... ............... 58 5 Optical spectroscopy and luminescence quenching of LuI3: Ce3+ 61 5.1 Introduction .................. .......... ..61 5.2 Crystal lattice of LuI3 .......... .............. 61 5.3 Results ................... ........... ..62 5.4 Discussion .............. ................. 66 5.4.1 Host properties ................... ..... 66 5.4.2 Ce3+ Spectroscopy .................. .... 69 5.4.3 Luminescence quenching in LuI3: Ce3+ .......... 71 5.5 Conclusion ....... ............... ........ . 71 6 GdI3: Ce3+: Iodide scintillator 73 6.1 Introduction ................... .......... 73 6.2 Properties of GdI3: Ce"3 . . .. ................ . 74 6.3 Results and discussion ................... ..... 74 6.3.1 Scintillation and luminescence properties at RT ...... 74 6.3.2 Temperature dependence ..... .............. 78 6.4 Summary ................... .......... ..84 7 New fast lanthanide scintillators: PrC13: Ce3+ and PrBr3: Ce3+ 85 7.1 Introduction .................... ......... 85 7.2 Materials .................. ........... ..85 7.3 Scintillation properties of PrC13: Ce3+ ............... 86 7.4 Scintillation properties of PrBr3: Ce3+ ............... 89 7.5 Conclusion. . . . . .. ....................... 93 8 Thermal quenching of Ce3+ emission in PrX3 (X = Cl, Br) 95 8.1 Introduction . . . . . . . .................. ...... 95 8.2 Crystal lattice of PrX3 (X = Cl, Br) . ............... 96 8.3 Results.. .. ........ . .. ..... ....... . 97 8.3.1 Luminescence Characteristics ............. ... 97 8.3.2 Temperature dependence . .................. 100 8.4 Discussion ................... ............ 103 8.4.1 Radiative lifetimes of Ce3+ in PrC13: Ce3+ and PrBr3: Ce3+ 104 8.4.2 Quenching mechanisms of Ce3+ emission ........ .. 105 8.4.3 Energy level schemes in LaBr3: Ce3+ and PrBr3: Ce3+ . . 106 8.4.4 A model for the thermal luminescence quenching .... . 107 8.5 Conclusion . ................... .......... 109 9 Ce3+ doped Cs2NaREBr6 (RE=La,Y,Lu) 113 9.1 Introduction ....... ............... ....... 113 9.2 Materials .............. ................. 114 9.3 Results ................... ............ ..114 9.3.1 X-ray excited emission spectra . .............. . 114 9.3.2 Gamma spectroscopy . ............... ..... 116 9.3.3 Scintillation and intrinsic Ce3+ emission decay times . . . 116 9.3.4 Spectroscopy ................... ...... 118 9.3.5 Temperature Dependence of Anomalous Emission ..... 121 9.4 Discussion. ................... ............ 124 9.4.1 Host properties ...... ...... ............ 124 9.4.2 Ce3+ spectroscopy ................... ... 124 9.4.3 Scintillation mechanism ................... 126 9.4.4 Anomalous Emission . .................. .. 127 9.5 Conclusion . ................ ............... 132 10 Rb2LiYBr6: Ce3+ and other Li-based thermal-neutron scintilla- tors 135 10.1 Introduction ................... . .......... 135 10.2 Ce3+ activated Rb2LiYBr6: Ce3+ ........... ....... 136 10.2.1 Materials ...... ................ ..... 136 10.2.2 Results and Discussion . ................... 136 10.3 Other Li-based thermal-neutron scintillators . ........... 140 10.3.1 Thermal-neutron detection efficiencies of new scintillators . 141 10.3.2 Results and Discussion .... ................ 142 10.4 Conclusion. ................... ........... 146 11 Ce3+ doped ternary cesium halides 149 11.1 Introduction. ................... . ......... 149 11.2 Sample preparation and gamma interaction properties ....... 149 11.3 Results and discussion ................... ..... 150 11.3.1 X-ray excited emission spectra . ............... 150 11.3.2 Luminescence characteristics . ................ 153 11.3.3 Scintillation light yield and energy resolution ....... . 157 11.3.4 Scintillation decay curves . .................. 160 11.4 Conclusion. ................... ........... 162 12 Emission, light yield and time response of Ce3+ doped halides 165 12.1 Introduction. ................... . ......... 165 12.2 5d--4f Ce3+ emission wavelength . ................. 166 12.3 Light yield. . .................. . . ...... . 168 12.3.1 Influence of the structure, the type of lanthanide and the type of anion to the fundamental limit . .......... 169 12.3.2 Influence of the structure, the type of lanthanide and the type of anion to light yield losses . ............. 171 12.4 Time response. ................... ......... 178 12.4.1 Radiative lifetime of Ce3+ . ................. 178 12.4.2 Influence of self absorption on the scintillation decay curve 179 12.4.3 Influence of the anion on the scintillation decay curve . . . 182 12.5 Discussion and Conclusion ................... ... 184 Summary and Conclusion 189 Samenvatting en Conclusie 195 Acknowledgments 201 Curriculum Vitae 203 List of Publications 205