Slowing dynamics in supercooled liquids and other soft materials.

摘要

The slow structural dynamics displayed by supercooled liquids and the transition to an out-of-equilibrium glass state that they engender are among the most challenging issues in condensed matter physics. This thesis reports experimental studies designed to elucidate central aspects of these slow dynamics and the nature of the glass state. The subjects of these studies include glass forming molecular liquids and other soft materials that have been advanced as model glassy systems such as clay suspensions and block copolymer micelle solutions. The main experimental techniques employed in these investigations have been dielectric susceptibility and neutron scattering.; In the first half of this thesis, we report frequency-dependent dielectric susceptibility measurements characterizing the evolution in the dynamical properties, or aging, of two supercooled liquids, sorbitol and xylitol, quenched below their calorimetric glass transition temperatures, Tg. In addition to the alpha relaxation that tracks the structural dynamics, the susceptibilities of both liquids possess a secondary Johari-Goldstein relaxation at higher frequencies. Following a quench below Tg, the susceptibility slowly approaches equilibrium behavior. For both liquids features of the Johari-Goldstein relaxation display a dependence on the time since the quench, or aging time, that is very similar to the age dependence of the alpha peak. Implications of these findings for aging in glasses and the nature of Johari-Goldstein relaxation are discussed.; Further investigation of the aging in sorbitol reveals that it displays memory strikingly similar to that of a variety of glassy materials, particularly spin glasses. During a temporary stop in cooling, the susceptibility changes with time due to aging. The memory is revealed upon reheating as the susceptibility retraces these changes. To investigate the out-of-equilibrium state of the liquid as it displays this memory, we have employed a set of intricate thermal histories by interrupting the heating stage of the cycle and characterizing the subsequent aging. At temperatures above that of the original cooling stop, the liquid enters a state on heating with an effective age that is proportional to the duration of the stop, while at lower temperatures no effective age can be assigned and subtler behavior emerges. These results, which reveal differences with memory displayed by spin glasses, are discussed in the context of the liquid's energy landscape.; In the second half of the thesis, we report neutron scattering measurements and dielectric studies on a set of disordered soft materials. (Abstract shortened by UMI.)