Cornucopia of Nanoscale Ordered Phases in Sphere-Forming Tetrablock Terpolymers

Chanpuriya, Siddharth; Kim, Kyungtae; Zhang, Jingwen; Lee, Sangwoo; Arora, Akash; Dorfman, Kevin D.; Delaney, Kris T.; Fredrickson, Glenn H.; Bates, Frank S.

doi:10.1021/acsnano.6b00495

Title: Cornucopia of Nanoscale Ordered Phases in Sphere-Forming Tetrablock Terpolymers

Journal Article · Thu Apr 07 00:00:00 EDT 2016 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.6b00495· OSTI ID:1255285

Chanpuriya, Siddharth ^[1]; Kim, Kyungtae ^[1]; Zhang, Jingwen ^[1]; Lee, Sangwoo ^[2]; Arora, Akash ^[1]; Dorfman, Kevin D. ^[1]; Delaney, Kris T. ^[3]; Fredrickson, Glenn H. ^[3]; Bates, Frank S. ^[1]

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

In this paper, we report the phase behavior of a series of poly(styrene)-b-poly(isoprene)-b-poly(styrene)'-b-poly(ethylene oxide) (SIS'O) tetrablock terpolymers. This study was motivated by self-consistent field theory (SCFT) calculations that anticipate a rich array of sphere-forming morphologies with variations in the molecular symmetry parameter τ = N_S/(N_S + N_S'), where N is the block degree of polymerization and the volume fraction of O is less than about 0.22. Eight SIS'O samples, with τ ranging from 0.21 to 0.73, were synthesized and investigated using small-angle X-ray scattering and transmission electron microscopy, yielding evidence of nine different spherical phases: hexagonal, FCC, HCP, BCC, rhombohedral (tentative), liquid-like packing, dodecagonal quasicrystal, and Frank–Kasper σ and A15 phases. At temperatures close to the order–disorder transition, these tetrablocks behave as pseudo-[SIS']-O diblocks and form equilibrium morphologies mediated by facile chain exchange between micelles. Transition from equilibrium to nonequilibrium behavior occurs at a temperature (T_erg) several tens of degrees below the order–disorder transition temperature, speculated to be coincident with the loss of ergodicity, as chain exchange is arrested due to increased segregation strength between the core (O) and corona (SIS') blocks. Nonequilibrium ordered structures form when T < T_erg; these are interpreted using SCFT calculations to elucidate the free energy landscape driving ordering in the S and I block matrix. These experiments demonstrate a profound dependence on phase stability with variations in τ and temperature, providing insights into the formation of ordered phase symmetry in this class of asymmetric multiblock polymers.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); E.I. DuPont de Nemours & Co.; The Dow Chemical Company; Northwestern University; USDOE Office of Science (SC)

Grant/Contract Number:: DMR-1333669; DMR-1332842; AC02-06CH11357

OSTI ID:: 1255285

Journal Information:: ACS Nano, Vol. 10, Issue 5; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 86 works

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