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Title: Molecular pathways for defect annihilation in directed self-assembly.

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [2];  [3];  [4];  [5];  [4];  [6];  [7];  [3];  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States); Chonnam National Univ., Gwangju (Korea)
  2. Cornell Univ., Ithaca, NY (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)
  4. Univ. of Chicago, IL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
  6. Georg-August Univ., Gottingen (Germany); Fudan Univ., Shanghai (China)
  7. Georg-August Univ., Gottingen (Germany)

Over the last few years, the directed self-assembly of block copolymers by surface patterns has transitioned from academic curiosity to viable contender for commercial fabrication of next-generation nanocircuits by lithography. Recently, it has become apparent that kinetics, and not only thermodynamics, plays a key role for the ability of a polymeric material to self-assemble into a perfect, defect-free ordered state. Perfection, in this context, implies not more than one defect, with characteristic dimensions on the order of 5 nm, over a sample area as large as 100 cm2. In this work, we identify the key pathways and the corresponding free-energy barriers for eliminating defects, and we demonstrate that an extraordinarily large thermodynamic driving force is not necessarily sufficient for their removal. By adopting a concerted computational and experimental approach, we explain the molecular origins of these barriers, how they depend on material characteristics, and we propose strategies designed to over-come them. The validity of our conclusions for industrially-relevant patterning processes is established by relying on instruments and assembly lines that are only available at state-of-the-art fabrication facilities and, through this confluence of fundamental and applied research, we are able to discern the evolution of morphology at the smallest relevant length scales - a handful of nanometers -, and present a view of defect annihilation in directed self-assembly at an unprecedented level of detail.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1237606
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 112; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 97 works
Citation information provided by
Web of Science

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Cited By (18)

Molecular Modeling of EUV Photoresist Revealing the Effect of Chain Conformation on Line-Edge Roughness Formation journal November 2019
Controlling Self-Assembly in Gyroid Terpolymer Films By Solvent Vapor Annealing. text January 2018
Ionic conductivity and counterion condensation in nanoconfined polycation and polyanion brushes prepared from block copolymer templates journal January 2019
Three-dimensional line edge roughness in pre- and post-dry etch line and space patterns of block copolymer lithography journal January 2020
Janus Graft Block Copolymers: Design of a Polymer Architecture for Independently Tuned Nanostructures and Polymer Properties journal May 2018
Protracted Colored Noise Dynamics Applied to Linear Polymer Systems journal January 2018
Shear-solvo defect annihilation of diblock copolymer thin films over a large area journal June 2019
Janus Graft Block Copolymers: Design of a Polymer Architecture for Independently Tuned Nanostructures and Polymer Properties journal May 2018
Influence of the long-range ordering of gold-coated Si nanowires on SERS journal July 2018
Thermal scanning probe lithography for the directed self-assembly of block copolymers journal April 2017
New frontiers for the materials genome initiative journal April 2019
Dissipative particle dynamics for directed self-assembly of block copolymers journal October 2019
Kinetics of pattern formation in symmetric diblock copolymer melts journal May 2018
Controlling Self-Assembly in Gyroid Terpolymer Films By Solvent Vapor Annealing journal September 2018
Ordering kinetics of lamella-forming block copolymers under the guidance of various external fields studied by dynamic self-consistent field theory journal January 2017
High aspect ratio nanotubes assembled from macrocyclic iminium salts journal August 2018
Nano-confinement of block copolymers in high accuracy topographical guiding patterns: modelling the emergence of defectivity due to incommensurability journal January 2018
Dissipative Particle Dynamics for Directed Self-Assembly of Block Copolymers text January 2019

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