TY - JOUR
T1 - Competing relaxation channels in continuously polydisperse fluids
T2 - A mode-coupling study
AU - Laudicina, Corentin C.L.
AU - Pihlajamaa, Ilian
AU - Janssen, Liesbeth M.C.
PY - 2023/8
Y1 - 2023/8
N2 - We perform a systematic analysis of continuously polydisperse hard-sphere fluids as a function of the degree of polydispersity within the framework of the mode-coupling theory of the glass transition (MCT). Our results show that a high degree of polydispersity tends to stabilize the liquid phase against vitrification, the magnitude of which depends on the shape of the polydispersity distribution. Furthermore, we report on a separation between the localization lengths of the smallest and largest particles. A diameter-resolved analysis of the intermediate scattering functions reveals that this separation significantly stretches the relaxation patterns, which we quantitatively study by an analysis of the dynamical exponents predicted by the theory. Our observations have strong implications for our understanding of the nature of dynamical heterogeneities and localization lengths in continuously polydisperse systems with hard-core interactions. These results suggest that the dynamics of the smallest particles is of central importance to understand structural relaxation of such systems, already in the mildly supercooled regime where MCT is usually applicable.
AB - We perform a systematic analysis of continuously polydisperse hard-sphere fluids as a function of the degree of polydispersity within the framework of the mode-coupling theory of the glass transition (MCT). Our results show that a high degree of polydispersity tends to stabilize the liquid phase against vitrification, the magnitude of which depends on the shape of the polydispersity distribution. Furthermore, we report on a separation between the localization lengths of the smallest and largest particles. A diameter-resolved analysis of the intermediate scattering functions reveals that this separation significantly stretches the relaxation patterns, which we quantitatively study by an analysis of the dynamical exponents predicted by the theory. Our observations have strong implications for our understanding of the nature of dynamical heterogeneities and localization lengths in continuously polydisperse systems with hard-core interactions. These results suggest that the dynamics of the smallest particles is of central importance to understand structural relaxation of such systems, already in the mildly supercooled regime where MCT is usually applicable.
UR - http://www.scopus.com/inward/record.url?scp=85169291256&partnerID=8YFLogxK
U2 - 10.1103/PhysRevResearch.5.033121
DO - 10.1103/PhysRevResearch.5.033121
M3 - Article
AN - SCOPUS:85169291256
SN - 2643-1564
VL - 5
JO - Physical Review Research
JF - Physical Review Research
IS - 3
M1 - 033121
ER -