Ph.D. thesis (pdf) - dirac

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162 Boson Peak m P /m ρ 2 1.8 1.6 1.4 1.2 1 OTP PB glycerol salol DHIQ sorbitol PC DBP m−fluorAni cumene PIB strong 0.8 0 0.5 1 1.5 R Figure 8.13: The relative contribution of density to the viscous slowing down, measured by m P /m ρ a function of the inverse relative boson peak intensity, R. Red symbols are R values of this work. Blue symbols represent data from literature. See the appendix for values and references. DBF and Bose Scaled S(ω) 2 1.5 1 0.5 0 T=T g P=1400 MPa Patm 0 2 4 6 8 10 12 14 16 ω / meV Figure 8.14: The boson peak of PIB3580 at atmospheric pressure and at 1.4 GPa at T ≈ T g (P). The data are corrected for the temperature dependent bosefactor.
8.3. Boson Peak and fragility 163 1.2 1 S(omega)/S(ω BP ) 0.8 0.6 0.4 0.2 P=1400 MPa Patm 0 1 2 3 4 5 ω / ω BP Figure 8.15: The boson peak of PIB3580 at atmospheric pressure and at 1.4 GPa at T ≈ T g (P). The axis are scaled with the boson peak position and intensity. The data are corrected for the temperature dependent bosefactor. from this scaling that R is independent of pressure. Two systems are not sufficient to state that this is a universal behavior of R. However if the finding is general, then it strongly supports the suggestion that the correlation between R and the isochoric fragility m ρ , as the latter also stays constant as a function of pressure along the T g -line (chapter 3). 8.3.3 The quasi-elastic intensity The quantity R is a measure of the boson peak intensity relative to the minimum intensity at the low energy side of the peak. This latter is sometimes clearly influenced by quasi elastic scattering. It is therefore not a priori the boson peak intensity that determines R. In figures 8.18 and 8.19 we show the S(ω) of two liquids which both follow the correlations seen in figures 8.11 and 8.12 namely DBP and DHIQ. For both samples we show the data at T = 100 K and at T = T g = 180 K, (all data at atmospheric pressure). The spectra deep in the glass at T = 100 K are quite similar for the two liquids, while this is not the case at T g . For the less fragile DBP the main effect is an increase in intensity due to the temperature dependence of the bose factor. In the case of the very fragile DHIQ on the other hand, there is a quasi-elastic signal at T g which totally swarms the boson peak. Hence, it is this quasi-elastic signal, rather than the nature of the boson peak which gives DHIQ its large value of R. This observation questions the proposed relation between R and
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THÈSE présentée par Kristine NIS
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Acknowledgement First of all I woul
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Contents Abstract iii Acknowledgeme
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CONTENTS ix 9 Summarizing discussio
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2 Introduction fragility with other
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Résumé du chapitre 2 De manière
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8 Slow and fast dynamics glass. The
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10 Slow and fast dynamics energy in
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12 Slow and fast dynamics increasin
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14 Slow and fast dynamics (linear)
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16 Slow and fast dynamics The dynam
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18 Slow and fast dynamics T > T 2
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20 Slow and fast dynamics as theore
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22 Slow and fast dynamics and sugge
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24 Slow and fast dynamics The boson
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26 Slow and fast dynamics modulus 3
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Chapter 3 What we learn from pressu
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3.2. Empirical scaling law and some
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3.3. Correlations with fragility 37
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3.4. Temperature dependences 39 mea
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3.5. Summary 41 assumption that the
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Chapter 4 Experimental techniques a
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4.2. Dielectric spectroscopy 47 4.1
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4.2. Dielectric spectroscopy 49 fie
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4.3. Inelastic Scattering Experimen
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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
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Chapter 6 High Q collective modes I
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6.1. Inelastic X-ray scattering 97
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6.2. Sound speed and attenuation 99
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6.3. Nonergodicity factor 105 where
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6.3. Nonergodicity factor 107 1 0.9
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6.3. Nonergodicity factor 109 high
Page 121 and 122: 6.4. Nonergodicity factor and fragi
Page 127 and 128: 6.5. Summary 117 d log (e(ρ))/ d l
Page 129: Résumé du chapitre 7 Dans ce chap
Page 132 and 133: 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
Page 146 and 147: 136 Mean squared displacement as be
Page 149: Résumé du chapitre 8 Le pic de bo
Page 152 and 153: 142 Boson Peak The FEC-model sugges
Page 154 and 155: 144 Boson Peak the Qout Q in factor
Page 156 and 157: 146 Boson Peak We are mainly intere
Page 158 and 159: 148 Boson Peak 1.5 x 10−3 ω [meV
Page 160 and 161: 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
Page 166 and 167: 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 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,
Page 196 and 197: 186 BIBLIOGRAPHY Monaco, A., Chumak
Page 198 and 199: 188 BIBLIOGRAPHY Patkowski, A., Gap
Page 200 and 201: 190 BIBLIOGRAPHY Sekula, M., Pawlus
Page 203 and 204: 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
Page 213 and 214: Appendix B Data compilations B.1 Da
Page 215 and 216: 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
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Abstract The degree of departure fr
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