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Temperature Gradients Induced Phase Separation in a Miscible Polymer Solution.

Temperature inhomogeneity is common in nature and technology —yet physical studies of the origins of phase transitions and the resulting morphologies generally concern systems whose temperature is constant everywhere, the contrary situation being viewed as too applied. Indeed, temperature gradients have interesting applications. They can be exploited for controlled crystal growth in zone refining of metals and semiconductors [1], can underly a rich physics of convection [2], and can generate chemical differentiation in an otherwise homogeneous geological mantle [3]. This issue also pertains to a more general intellectual problem, to understand the structure and phase behavior of mixtures when the thermodynamic variables are inhomogeneous [4 ‐ 12]. We report below a connection between temperature inhomogeneity and the actual occurrence of a phase transition above the thermodynamic coexistence temperature. Phase separation induced by temperature gradients has previously been observed when one portion of a sample is below the critical temperature and another portion above it [7,8], but, to our knowledge, not previously when the entire sample is above this temperature, with the possible exception of the cryptic allusion by Lesher and Walker to certain “failed experiments” with geological magmas [13]. Reasons are given to expect such behavior to be especially common for macromolecular mixtures in the vicinity of phase transitions. The experiments show that small temperature gradi