Glass Transition and Structure of Organic Polymers from All-Atom Molecular Simulations
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22340%2F23%3A43927917" target="_blank" >RIV/60461373:22340/23:43927917 - isvavai.cz</a>
Result on the web
<a href="https://pubs.acs.org/doi/10.1021/acs.iecr.3c03038" target="_blank" >https://pubs.acs.org/doi/10.1021/acs.iecr.3c03038</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acs.iecr.3c03038" target="_blank" >10.1021/acs.iecr.3c03038</a>
Alternative languages
Result language
angličtina
Original language name
Glass Transition and Structure of Organic Polymers from All-Atom Molecular Simulations
Original language description
Molecular dynamics simulations of polymer samples with all-atom resolution provide important insight into the relationship between the atom-level structure and macroscopic properties of polymers. The computational setup of molecular simulations in such a case deserves to be validated, paying attention not to overlook various aspects or inferior settings or postprocessing analyses that have the potential to distort the simulation outcome or at least to make the simulated ensemble too incompatible with its experimental counterparts, such as their polydispersity, initial conformation, or thermal history of the samples. The accuracy of the simulation results obtained from existing all-atom nonpolarizable force fields for three selected polymers is independently benchmarked with respect to the polymer densities and glass transition temperatures. Errors of structural or thermodynamic properties arising due to insufficient sample equilibration or inadequate simulation setup are quantified. Special attention is paid to the selection of reference literature data for polymer systems that are well characterized and as similar as possible to the computationally treated samples. Very different performances of predictions of the glass transition temperatures occur among the individual target polymers, with both their sampling uncertainty and errors from reference experimental data ranging from acceptable below 10 K to highly unsatisfactory 100 K in individual cases. The accuracy of the predicted glass transition temperature is found to be higher for polymers exhibiting faster internal dynamics and distinct trend shifts between the glass and the liquid. On the contrary, when the glass transition occurs gradually over a wider temperature range, it becomes very difficult to capture the adequate transition temperature within molecular simulations, regardless of the evaluation protocol used. Bulk density proves to be the most reliable observable for subsequent trend shift analyses, which typically yield similar results regardless of performing equilibrium or nonequilibrium simulations and adopting the bilinear or hyperbolic regression analyses. © 2023 The Authors. Published by American Chemical Society.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
<a href="/en/project/GM23-05476M" target="_blank" >GM23-05476M: Making ab initio modelling possible for disordered molecular semi-conductive materials</a><br>
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)
Others
Publication year
2023
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
ISSN
0888-5885
e-ISSN
1520-5045
Volume of the periodical
62
Issue of the periodical within the volume
49
Country of publishing house
US - UNITED STATES
Number of pages
12
Pages from-to
21437-21448
UT code for WoS article
001126781200001
EID of the result in the Scopus database
2-s2.0-85179618031