Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films

Gentekos, Dillon T.; Jia, Junteng; Tirado, Erika S.; Barteau, Katherine P.; Smilgies, Detlef -M.; DiStasio, Jr., Robert A.; Fors, Brett P.

doi:10.1021/jacs.8b00694

Title: Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films

Journal Article · 09 March 2018 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.8b00694 · OSTI ID:1489032

Gentekos, Dillon T. ^[1]; Jia, Junteng ^[1]; Tirado, Erika S. ^[1];

^[1];

^[1]; DiStasio, Jr., Robert A. ^[1];

^[1]

Cornell Univ., Ithaca, NY (United States)

We report a method for tuning the domain spacing (D_sp) of self-assembled block copolymer thin films of poly(styrene-block-methyl methacrylate) (PS-b-PMMA) over a large range of lamellar periods. By modifying the molecular weight distribution (MWD) shape (including both the breadth and skew) of the PS block via temporal control of polymer chain initiation in anionic polymerization, we observe increases of up to 41% in D_sp for polymers with the same overall molecular weight (M_n ≈ 125 kg mol^–1) without significantly changing the overall morphology or chemical composition of the final material. In conjunction with our experimental efforts, we have utilized concepts from population statistics and least-squares analysis to develop a model for predicting D_sp based on the first three moments of the MWDs. This statistical model reproduces experimental D_sp values with high fidelity (with mean absolute errors of 1.2 nm or 1.8%) and provides novel physical insight into the individual and collective roles played by the MWD moments in determining this property of interest. As a result, this work demonstrates that both MWD breadth and skew have a profound influence over D_sp, thereby providing an experimental and conceptual platform for exploiting MWD shape as a simple and modular handle for fine-tuning D_sp in block copolymer thin films.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1489032

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 13; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 82 works

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Recent progress on polydispersity effects on block copolymer phase behavior Kim, Inho; Li, Sheng Polymer Reviews, Vol. 59, Issue 3 https://doi.org/10.1080/15583724.2019.1579227	journal	April 2019
Precise modulation of molecular weight distribution for structural engineering Tan, Rui; Zhou, Dongdong; Liu, Baolei Chemical Science, Vol. 10, Issue 46 https://doi.org/10.1039/c9sc04736k	journal	January 2019
Deconstructing Oligomer Distributions: Discrete Species and Artificial Distributions De Neve, Jeroen; Haven, Joris J.; Harrisson, Simon Angewandte Chemie International Edition, Vol. 58, Issue 39 https://doi.org/10.1002/anie.201906842	journal	September 2019
Amphiphilic fluorous random copolymer self‐assembly for encapsulation of a fluorinated agrochemical Ko, Jeong Hoon; Bhattacharya, Arvind; Terashima, Takaya Journal of Polymer Science Part A: Polymer Chemistry, Vol. 57, Issue 3 https://doi.org/10.1002/pola.29187	journal	September 2018
Tuning Dispersity by Photoinduced Atom Transfer Radical Polymerisation: Monomodal Distributions with ppm Copper Concentration Whitfield, Richard; Parkatzidis, Kostas; Rolland, Manon Angewandte Chemie, Vol. 131, Issue 38 https://doi.org/10.1002/ange.201906471	journal	August 2019
Deconstructing Oligomer Distributions: Discrete Species and Artificial Distributions De Neve, Jeroen; Haven, Joris J.; Harrisson, Simon Angewandte Chemie, Vol. 131, Issue 39 https://doi.org/10.1002/ange.201906842	journal	July 2019
Investigation of the Locked-Unlocked Mechanism in Living Anionic Polymerization Realized with 1-(Tri-isopropoxymethylsilylphenyl)-1-phenylethylene Liu, Pibo; Ma, Hongwei; Han, Li Angewandte Chemie, Vol. 130, Issue 50 https://doi.org/10.1002/ange.201809857	journal	November 2018
Tailoring polymer dispersity and shape of molecular weight distributions: methods and applications Whitfield, Richard; Truong, Nghia P.; Messmer, Daniel ETH Zurich https://doi.org/10.3929/ethz-b-000370769	text	January 2019
Precise modulation of molecular weight distribution for structural engineering Tan, Rui; Zhou, Dongdong; Liu, Baolei Chemical Science, Vol. 10, Issue 46 https://doi.org/10.1039/c9sc04736k	journal	January 2019

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