We analyze dynamical heterogeneities in a simulated “bead-spring” model of a nonentangled, supercooled polymer melt. We explore the importance of chain connectivity on the spatially heterogeneous motion of the monomers. We find that when monomers move, they tend to follow each other in one-dimensional paths, forming strings as previously reported in atomic liquids and colloidal suspensions. The mean string length is largest at a time close to the peak time of the mean cluster size of mobile monomers. This maximum string length increases, roughly in an exponential fashion, on cooling toward the critical temperature of the mode-coupling theory, but generally remains small, although large strings involving ten or more monomers are observed. An important contribution to this replacement comes from directly bonded neighbors in the chain. However, mobility is not concentrated along the backbone of the chains. Thus, a relaxation mechanism in which neighboring mobile monomers along the chain move predominantly along the backbone of the chains, seems unlikely for the system studied.
Skip Nav Destination
Article navigation
8 September 2003
Research Article|
August 21 2003
Polymer-specific effects of bulk relaxation and stringlike correlated motion in the dynamics of a supercooled polymer melt
M. Aichele;
M. Aichele
Institut Charles Sadron, 6 rue Boussingault, 67083 Strasbourg, France
Institut für Physik, Johannes Gutenberg-Universität, 55099 Mainz, Germany
Search for other works by this author on:
Y. Gebremichael;
Y. Gebremichael
Department of Chemical Engineering, University of Michigan, Ann Arbor, Michigan 48109
and Chemical Physics Program, Institute for Physical Sciences and Technology, University of Maryland, College Park, Maryland 20742
Search for other works by this author on:
F. W. Starr;
F. W. Starr
Center for Theoretical and Computational Materials Science and Polymers Division, National Institute of Standards and Technology, Gaithersburg, Maryland 20899
Search for other works by this author on:
J. Baschnagel;
J. Baschnagel
Institut Charles Sadron, 6 rue Boussingault, 67083 Strasbourg, France
Search for other works by this author on:
S. C. Glotzer
S. C. Glotzer
Departments of Chemical Engineering and Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109
Search for other works by this author on:
J. Chem. Phys. 119, 5290–5304 (2003)
Article history
Received:
April 15 2003
Accepted:
June 11 2003
Connected Content
Citation
M. Aichele, Y. Gebremichael, F. W. Starr, J. Baschnagel, S. C. Glotzer; Polymer-specific effects of bulk relaxation and stringlike correlated motion in the dynamics of a supercooled polymer melt. J. Chem. Phys. 8 September 2003; 119 (10): 5290–5304. https://doi.org/10.1063/1.1597473
Download citation file:
Sign in
Don't already have an account? Register
Sign In
You could not be signed in. Please check your credentials and make sure you have an active account and try again.
Sign in via your Institution
Sign in via your InstitutionPay-Per-View Access
$40.00