Structure and energetics of grain boundaries in self-assembled double-gyroid block copolymer networks
Abstract
Grain boundaries (GBs) are ubiquitous defects in crystalline materials, but remain less explored in block copolymer ordered phases. Here, we develop a self-consistent field theory framework to investigate GB structure and energetics in double-gyroid (DG) diblock copolymer networks. Two energy landscapes are obtained for tilt and twist GBs as functions of GB orientations revealing multiple local minima. The lowest-energy GB among the sampled GBs is an asymmetric-tilt network-switching GB ([1̅1̅1] ATNS) rather than the experimentally observed (422) twin boundary (TB) among the sampled GBs. Comparative analyses of tilt ([1̅1̅1], [100] ATNS) and twist ((422) TB, [01̅1̅] TNS) GBs reveal that, unlike enthalpy-dominated hard matter, GB stability in DG networks is entropy-driven. Twist-type GBs generate new nodes and disrupt nodal coplanarity, causing chain-packing frustration and entropy penalties. Although the [100] ATNS does not generate new nodes, its disruption of nodal coplanarity still incurs large entropy penalties. Conversely, the [1̅1̅1] ATNS preserves favorable network connectivity and minimizes conformational constraints, making it the energetically preferred GB.
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BibTeX
@misc{chen2026structure,
title = {{Structure and energetics of grain boundaries in self-assembled double-gyroid block copolymer networks}},
author = {Jing Chen and Aiping Zhu and Dan Wei and An-Chang Shi and Kai Jiang},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2605.26927},
eprint = {2605.26927},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2605.26927},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Structure and energetics of grain boundaries in self-assembled double-gyroid block copolymer networks
AU - Jing Chen
AU - Aiping Zhu
AU - Dan Wei
AU - An-Chang Shi
AU - Kai Jiang
PY - 2026
DA - 2026/10/28
PB - arXiv
DO - 10.48550/arxiv.2605.26927
UR - https://arxiv.org/abs/2605.26927
AB - Grain boundaries (GBs) are ubiquitous defects in crystalline materials, but remain less explored in block copolymer ordered phases. Here, we develop a self-consistent field theory framework to investigate GB structure and energetics in double-gyroid (DG) diblock copolymer networks. Two energy landscapes are obtained for tilt and twist GBs as functions of GB orientations revealing multiple local minima. The lowest-energy GB among the sampled GBs is an asymmetric-tilt network-switching GB ([1̅1̅1] ATNS) rather than the experimentally observed (422) twin boundary (TB) among the sampled GBs. Comparative analyses of tilt ([1̅1̅1], [100] ATNS) and twist ((422) TB, [01̅1̅] TNS) GBs reveal that, unlike enthalpy-dominated hard matter, GB stability in DG networks is entropy-driven. Twist-type GBs generate new nodes and disrupt nodal coplanarity, causing chain-packing frustration and entropy penalties. Although the [100] ATNS does not generate new nodes, its disruption of nodal coplanarity still incurs large entropy penalties. Conversely, the [1̅1̅1] ATNS preserves favorable network connectivity and minimizes conformational constraints, making it the energetically preferred GB.
ER -