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Zhang, Cheng; Vigil, Daniel L; Sun, Dan; Bates, Morgan W; Loman, Tessa; Murphy, Elizabeth A; Barbon, Stephanie M; Song, Jung-Ah; Yu, Beihang; Fredrickson, Glenn H; Whittaker, Andrew K; Hawker, Craig J; Bates, Christopher M
Journal of the American Chemical Society, 09/2021, Letnik: 143, Številka: 35Journal Article
The hexagonally close-packed (HCP) sphere phase is predicted to be stable across a narrow region of linear block copolymer phase space, but the small free energy difference separating it from face-centered cubic spheres usually results in phase coexistence. Here, we report the discovery of pure HCP spheres in linear block copolymer melts with A = poly(2,2,2-trifluoroethyl acrylate) (“F”) and B = poly(2-dodecyl acrylate) (“2D”) or poly(4-dodecyl acrylate) (“4D”). In 4DF diblocks and F4DF triblocks, the HCP phase emerges across a substantial range of A-block volume fractions (circa f A = 0.25–0.30), and in F4DF, it forms reversibly when subjected to various processing conditions which suggests an equilibrium state. The time scale associated with forming pure HCP upon quenching from a disordered liquid is intermediate to the ordering kinetics of the Frank–Kasper σ and A15 phases. However, unlike σ and A15, HCP nucleates directly from a supercooled liquid or soft solid without proceeding through an intermediate quasicrystal. Self-consistent field theory calculations indicate the stability of HCP is intimately tied to small amounts of molar mass dispersity (Đ); for example, an HCP-forming F4DF sample with f A = 0.27 has an experimentally measured Đ = 1.04. These insights challenge the conventional wisdom that pure HCP is difficult to access in linear block copolymer melts without the use of blending or other complex processing techniques.
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