Ph.D. thesis (pdf) - dirac

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vi Acknowledgement Raymond Herren. The technical assistance and help of the staff at IMFUFA has also been indispensable for this work and I thank Ib Hst Petersen, Peter Jensen and Ebbe Hyldahl Larsen. A special thank also goes to Jens Christian Niss for proofreading the whole manuscript in a very short time. Albena Nielsen and coworkers are thanked for making available dielectric data prior to publication and I would at the same time like to thank every one in “Glass and Time” (Denmark) for moral support. My three years in the TESMaC group have been a real pleasure, and I am greatly thankful to everyone for helping me out, supporting me and being overbearing with my French. I would especially like to thank Jean-Marie Teuler for solving at least million software problems, and Anne Boutin for strong support when it was most needed. I would also like to thank the former <strong>Ph</strong>.D.-student Aude Chauty-Cailliaux, from whom I overtook many results and experiences. Finally I would like to thank ... Maj and Bo for being present at all times no matter how far away (and for coming closer). Niels for being there at the best (or worst) time possible. Paola, Carmelo, Elisa, Javier and Kosima for making Grenoble feel like a second home. Christelle, Angela, Ricardo, Aurelie, Frederic, Silvian, Gilbert, Pernille, Jean Luc, Margrethe, Stephan, Lucie, Anders, Guara and all of ECAP for making Paris home. And all my other friends and my family - I am grateful that they are far too numerous to be listed here. Kristine Niss April 2007 This work was supported by grant No. 645-03-0230 from Forskeruddannelsesrådet (Denmark).
Contents Abstract iii Acknowledgement v 1 Introduction 1 2 Slow and fast dynamics 7 2.1 The glass transition . . . . . . . . . . . . . . . . . . . . . . . . . . . 7 2.2 Fragility . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10 2.3 Non-Debye relaxation . . . . . . . . . . . . . . . . . . . . . . . . . . 13 2.4 Energy landscape . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14 2.5 Fast dynamics and glassy dynamics . . . . . . . . . . . . . . . . . . . 15 2.6 Fragility and other properties . . . . . . . . . . . . . . . . . . . . . . 17 2.7 Relation between fast and slow dynamics . . . . . . . . . . . . . . . 20 3 What we learn from pressure experiments 29 3.1 Isochoric and isobaric fragility . . . . . . . . . . . . . . . . . . . . . . 29 3.2 Empirical scaling law and some consequences . . . . . . . . . . . . . 31 3.3 Correlations with fragility . . . . . . . . . . . . . . . . . . . . . . . . 36 3.4 Temperature dependences . . . . . . . . . . . . . . . . . . . . . . . . 39 3.5 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41 vii
Page 1: THÈSE présentée par Kristine NIS
Page 5: Acknowledgement First of all I woul
Page 9: CONTENTS ix 9 Summarizing discussio
Page 12 and 13: 2 Introduction fragility with other
Page 15: Résumé du chapitre 2 De manière
Page 18 and 19: 8 Slow and fast dynamics glass. The
Page 20 and 21: 10 Slow and fast dynamics energy in
Page 22 and 23: 12 Slow and fast dynamics increasin
Page 24 and 25: 14 Slow and fast dynamics (linear)
Page 26 and 27: 16 Slow and fast dynamics The dynam
Page 28 and 29: 18 Slow and fast dynamics T > T 2
Page 30 and 31: 20 Slow and fast dynamics as theore
Page 32 and 33: 22 Slow and fast dynamics and sugge
Page 34 and 35: 24 Slow and fast dynamics The boson
Page 36 and 37: 26 Slow and fast dynamics modulus 3
Page 39 and 40: Chapter 3 What we learn from pressu
Page 41 and 42: 3.2. Empirical scaling law and some
Page 47 and 48: 3.3. Correlations with fragility 37
Page 49 and 50: 3.4. Temperature dependences 39 mea
Page 51: 3.5. Summary 41 assumption that the
Page 55 and 56: Chapter 4 Experimental techniques a
Page 57 and 58:
4.2. Dielectric spectroscopy 47 4.1
Page 59 and 60:
4.2. Dielectric spectroscopy 49 fie
Page 61 and 62:
4.3. Inelastic Scattering Experimen
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Page 67 and 68:
Page 69 and 70:
Page 71 and 72:
Page 73 and 74:
Page 75 and 76:
Page 77 and 78:
Page 79:
Résumé du chapitre 5 La relaxatio
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72 Alpha Relaxation the dielectric
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74 Alpha Relaxation Measuring the c
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76 Alpha Relaxation 4 2 0 This work
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78 Alpha Relaxation for the 1 s iso
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80 Alpha Relaxation log10(τ α ) 2
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82 Alpha Relaxation 2 1 0 216.4K th
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84 Alpha Relaxation function has a
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86 Alpha Relaxation 2.5 2.5 2 2 log
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88 Alpha Relaxation 0.4 log 10 Im(
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90 Alpha Relaxation keeping the rel
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92 Alpha Relaxation correlation bet
Page 105 and 106:
Chapter 6 High Q collective modes I
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6.1. Inelastic X-ray scattering 97
Page 109 and 110:
6.2. Sound speed and attenuation 99
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Page 113 and 114:
Page 115 and 116:
6.3. Nonergodicity factor 105 where
Page 117 and 118:
6.3. Nonergodicity factor 107 1 0.9
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6.3. Nonergodicity factor 109 high
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6.4. Nonergodicity factor and fragi
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Page 125 and 126:
Page 127 and 128:
6.5. Summary 117 d log (e(ρ))/ d l
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Résumé du chapitre 7 Dans ce chap
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122 Mean squared displacement colle
Page 134 and 135:
124 Mean squared displacement 1.5 I
Page 136 and 137:
126 Mean squared displacement 1.4 1
Page 138 and 139:
128 Mean squared displacement a cen
Page 140 and 141:
130 Mean squared displacement cumen
Page 142 and 143:
132 Mean squared displacement / a
Page 144 and 145:
134 Mean squared displacement I P i
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136 Mean squared displacement as be
Page 149:
Résumé du chapitre 8 Le pic de bo
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142 Boson Peak The FEC-model sugges
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144 Boson Peak the Qout Q in factor
Page 156 and 157:
146 Boson Peak We are mainly intere
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148 Boson Peak 1.5 x 10−3 ω [meV
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150 Boson Peak comparison of the ev
Page 162 and 163:
152 Boson Peak In figure 8.6 we sho
Page 164 and 165:
154 Boson Peak Predictions/explanat
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156 Boson Peak meaning that the Deb
Page 168 and 169:
158 Boson Peak g(ω)/ω 2 [arb. uni
Page 170 and 171:
160 Boson Peak are equivalent becau
Page 172 and 173:
162 Boson Peak m P /m ρ 2 1.8 1.6
Page 174 and 175:
164 Boson Peak S(ω) [arb.unit] S(
Page 176 and 177:
166 Boson Peak 3 2.5 S(ω) [arb. un
Page 178 and 179:
168 Boson Peak perature effect on t
Page 181 and 182:
Chapter 9 Summarizing discussion Wh
Page 183 and 184:
173 temperature in the harmonic app
Page 185:
Chapter 10 Perspectives In this wor
Page 188 and 189:
178 BIBLIOGRAPHY Angell, C. A. [199
Page 190 and 191:
180 BIBLIOGRAPHY Casalini, R. and R
Page 192 and 193:
182 BIBLIOGRAPHY Farago, B., Arbe,
Page 194 and 195:
184 BIBLIOGRAPHY Inamura, Y., Arai,
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186 BIBLIOGRAPHY Monaco, A., Chumak
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188 BIBLIOGRAPHY Patkowski, A., Gap
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190 BIBLIOGRAPHY Sekula, M., Pawlus
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Appendix A Details on the samples T
Page 205 and 206:
A.1. Cumene 195 the value found fro
Page 207 and 208:
A.2. PIB 197 The temperature depend
Page 209 and 210:
A.4. DBP 199 peak differently at di
Page 211 and 212:
A.6. Other samples 201 NH 2 tempera
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Appendix B Data compilations B.1 Da
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B.1. Data compilation 205 DHIQ = De
Page 217 and 218:
B.1. Data compilation 207 Triphenyl
Page 219 and 220:
Appendix C Dielectric setup Figure
Page 222:
Abstract The degree of departure fr
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