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Title: Examining the role of fluctuations in the early stages of homogenous polymer crystallization with simulation and statistical learning

Abstract

Here, we propose a relationship between the dynamics in the amorphous and crystalline domains during polymer crystallization: the fluctuations of ordering-rate about a material-specific value in the amorphous phase drive those fluctuations associated with the increase in percent crystallinity. This suggests a differential equation that satisfies the three experimentally observed time regimes for the rate of crystal growth. To test this postulated expression, we applied a suite of statistical learning tools to molecular dynamics simulations to extract the relevant phenomenology. This study shows that the proposed relationship holds in the early time regime. It illustrates the effectiveness of soft computing tools in the analysis of coarse-grained simulations in which patterns exist, but may not easily yield to strict quantitative evaluation. This ability assists us in characterizing the critical early time molecular arrangement during the primary nucleation phase of polymer melt crystallization. In addition to supporting the validity of the proposed kinetics expression, the simulations show that (i) the classical nucleation and growth mechanism is active in the early stages of ordering; (ii) the number of nuclei and their masses grow linearly during this early time regime; and (iii) a fixed inter-nuclei distance is established.

Authors:
ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1410618
Report Number(s):
LA-UR-16-23368
Journal ID: ISSN 0021-9606; TRN: US1800138
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 4; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 97 MATHEMATICS AND COMPUTING

Citation Formats

Welch, Jr., Paul Michael. Examining the role of fluctuations in the early stages of homogenous polymer crystallization with simulation and statistical learning. United States: N. p., 2017. Web. doi:10.1063/1.4973346.
Welch, Jr., Paul Michael. Examining the role of fluctuations in the early stages of homogenous polymer crystallization with simulation and statistical learning. United States. doi:10.1063/1.4973346.
Welch, Jr., Paul Michael. Mon . "Examining the role of fluctuations in the early stages of homogenous polymer crystallization with simulation and statistical learning". United States. doi:10.1063/1.4973346. https://www.osti.gov/servlets/purl/1410618.
@article{osti_1410618,
title = {Examining the role of fluctuations in the early stages of homogenous polymer crystallization with simulation and statistical learning},
author = {Welch, Jr., Paul Michael},
abstractNote = {Here, we propose a relationship between the dynamics in the amorphous and crystalline domains during polymer crystallization: the fluctuations of ordering-rate about a material-specific value in the amorphous phase drive those fluctuations associated with the increase in percent crystallinity. This suggests a differential equation that satisfies the three experimentally observed time regimes for the rate of crystal growth. To test this postulated expression, we applied a suite of statistical learning tools to molecular dynamics simulations to extract the relevant phenomenology. This study shows that the proposed relationship holds in the early time regime. It illustrates the effectiveness of soft computing tools in the analysis of coarse-grained simulations in which patterns exist, but may not easily yield to strict quantitative evaluation. This ability assists us in characterizing the critical early time molecular arrangement during the primary nucleation phase of polymer melt crystallization. In addition to supporting the validity of the proposed kinetics expression, the simulations show that (i) the classical nucleation and growth mechanism is active in the early stages of ordering; (ii) the number of nuclei and their masses grow linearly during this early time regime; and (iii) a fixed inter-nuclei distance is established.},
doi = {10.1063/1.4973346},
journal = {Journal of Chemical Physics},
number = 4,
volume = 146,
place = {United States},
year = {Mon Jan 23 00:00:00 EST 2017},
month = {Mon Jan 23 00:00:00 EST 2017}
}

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