硫系玻璃的熔体均匀化和自组织：GexSe100-x二元体系中锐刚性、应力和纳米级相分离转变的证据
Melt homogenization and self-organization of chalcogenides glasses: evidence of sharp rigidity, stress and nanoscale phase separation transitions in the GexSe100-x binary
摘要：
拉曼分析方法用于监测GexSe 100-x熔体的生长，并揭示了两个步骤的均匀化过程。所得均匀玻璃显示在Tg下的非可逆焓ΔHnr（x），以显示随x的方井状变化，其中在xc（1）= 19.5（5）%附近的刚性转变和在xc（2）= 26.0（5）%附近的应力转变表示刚性但无应力的中间相（IP）的边界。ΔHnr（x）的方阱状变化形成倾斜的壁，三角形形状，并最终在具有增加的不均匀性的玻璃中消失。ΔHnr项在IP外但不在IP内老化数周。观察到的可逆性窗口的光学模拟与拉曼光谱的淬火熔体和Tg循环玻璃是相同的IP中的玻璃组合物，但不同的IP外的组合物。摩尔体积的变化，显示三个制度的行为与全球最低的IP和一个显着的增加以外的阶段。干的和均匀的硫族化物玻璃的固有的物理行为可以急剧变化的弹性和化学相变附近的组成，表明网络玻璃的物理需要均匀的样品，可能是远比迄今为止认识到的更有趣。
英文摘要：
A Raman profiling method is used to monitor growth of GexSe100-x melts and reveals a two step process of homogenization. Resulting homogeneous glasses show the non-reversing enthalpy at Tg, ΔHnr(x), to show a square-well like variation with x, with a rigidity transition near xc(1) = 19.5(5)% and stress transition near xc(2) = 26.0(5)%) representing the boundaries of the rigid but stress-free Intermediate Phase (IP). The square-well like variation of ΔHnr(x) develops sloping walls, a triangular shape and eventually disappears in glasses having an increasing heterogeneity. The ΔHnr term ages over weeks outside the IP but not inside the IP. An optical analogue of the reversibility window is observed with Raman spectra of as-quenched melts and Tg cycled glasses being the same for glass compositions in the IP but different for compositions outside the IP. Variations of Molar volumes, display three regimes of behavior with a global minimum in the IP and a pronounced increase outside that phase. The intrinsic physical behavior of dry and homogeneous chalcogenides glasses can vary sharply with composition near elastic and chemical phase transitions, showing that the physics of network glasses requires homogeneous samples, and may be far more interesting than hitherto recognized.
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