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Hauptverfasser: Cao, Renkuan, Peng, Fan, Zhang, Yunhan, Sun, Hao, Liu, Ziwei, Xu, Tingyu, Li, Liangbin
Format: Preprint
Veröffentlicht: 2024
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Online-Zugang:https://arxiv.org/abs/2410.13128
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author Cao, Renkuan
Peng, Fan
Zhang, Yunhan
Sun, Hao
Liu, Ziwei
Xu, Tingyu
Li, Liangbin
author_facet Cao, Renkuan
Peng, Fan
Zhang, Yunhan
Sun, Hao
Liu, Ziwei
Xu, Tingyu
Li, Liangbin
contents Non-classical two-step nucleation including preordering and crystal nucleation has been widely proposed to challenge the one-step nucleation framework in diverse materials, while what drives preordering has not been explicitly resolved yet. With molecular dynamics simulation, we find that two-step nucleation occurs in polyethylene, during which preordering precedes through the coupling between intrachain conformation and interchain orientation orders. Unexpectedly, preordering is driven by entropy rather than enthalpy, during which the interchain translational entropy gain compensates for the intrachain conformation entropy loss. This entropy-driven mechanism resolves the longstanding puzzle why flexible polymers with high entropy penalty still show high nucleation rate and opens a new perspective for understanding nucleation of synthetic and bio-polymers with conformation and orientation orders.
format Preprint
id arxiv_https___arxiv_org_abs_2410_13128
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Entropy-Driven Preordering Assists Nucleation in Polyethylene
Cao, Renkuan
Peng, Fan
Zhang, Yunhan
Sun, Hao
Liu, Ziwei
Xu, Tingyu
Li, Liangbin
Soft Condensed Matter
Non-classical two-step nucleation including preordering and crystal nucleation has been widely proposed to challenge the one-step nucleation framework in diverse materials, while what drives preordering has not been explicitly resolved yet. With molecular dynamics simulation, we find that two-step nucleation occurs in polyethylene, during which preordering precedes through the coupling between intrachain conformation and interchain orientation orders. Unexpectedly, preordering is driven by entropy rather than enthalpy, during which the interchain translational entropy gain compensates for the intrachain conformation entropy loss. This entropy-driven mechanism resolves the longstanding puzzle why flexible polymers with high entropy penalty still show high nucleation rate and opens a new perspective for understanding nucleation of synthetic and bio-polymers with conformation and orientation orders.
title Entropy-Driven Preordering Assists Nucleation in Polyethylene
topic Soft Condensed Matter
url https://arxiv.org/abs/2410.13128