Dodecagonal quasicrystalline order in a diblock copolymer melt

Gillard, Timothy M.; Lee, Sangwoo; Bates, Frank S.

doi:10.1073/pnas.1601692113

Title: Dodecagonal quasicrystalline order in a diblock copolymer melt

Journal Article · Tue Apr 26 00:00:00 EDT 2016 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1601692113· OSTI ID:1256354

Gillard, Timothy M. ^[1]; Lee, Sangwoo ^[2]; Bates, Frank S. ^[1]

Univ. of Minnesota, Minneapolis, MN (United States)
Rensselaer Polytechnic Inst., Troy, NY (United States)

We report the discovery of a dodecagonal quasicrystalline state (DDQC) in a sphere (micelle) forming poly(isoprene-b-lactide) (IL) diblock copolymer melt, investigated as a function of time following rapid cooling from above the order–disorder transition temperature (T_ODT = 66 °C) using small-angle X-ray scattering (SAXS) measurements. Between T_ODT and the order–order transition temperature T_OOT = 42 °C, an equilibrium body-centered cubic (BCC) structure forms, whereas below T_OOT the Frank–Kasper σ phase is the stable morphology. At T < 40 °C the supercooled disordered state evolves into a metastable DDQC that transforms with time to the σ phase. The times required to form the DDQC and σ phases are strongly temperature dependent, requiring several hours and about 2 d at 35 °C and more than 10 and 200 d at 25 °C, respectively. Remarkably, the DDQC forms only from the supercooled disordered state, whereas the σ phase grows directly when the BCC phase is cooled below T_OOT and vice versa upon heating. A transition in the rapidly supercooled disordered material, from an ergodic liquid-like arrangement of particles to a nonergodic soft glassy-like solid, occurs below ~40 °C, coincident with the temperature associated with the formation of the DDQC. We speculate that this stiffening reflects the development of particle clusters with local tetrahedral or icosahedral symmetry that seed growth of the temporally transient DDQC state. Here, this work highlights extraordinary opportunities to uncover the origins and stability of aperiodic order in condensed matter using model block polymers.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; 1104368

OSTI ID:: 1256354

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 113, Issue 19; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 128 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
quasicrystals
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block polymers

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