TY - JOUR
T1 - Morphometric Approach to Many-Body Correlations in Hard Spheres
AU - Robinson, Joshua
AU - Turci, Francesco
AU - Roth, Roland
AU - Royall, Cp
PY - 2019/2/14
Y1 - 2019/2/14
N2 - We model the thermodynamics of local structures within the hard sphere liquid at arbitrary volume fractions through the morphometric calculation of n-body correlations. We calculate absolute free energies of local geometric motifs in excellent quantitative agreement with molecular dynamics simulations across the liquid and supercooled liquid regimes. We find a bimodality in the density library of states where five-fold symmetric structures appear lower in free energy than four-fold symmetric structures, and from a single reaction path predict an Arrhenius-like scaling of local relaxation dynamics. The method provides a new route to assess changes in the free energy landscape at volume fractions dynamically inaccessible to conventional techniques.
AB - We model the thermodynamics of local structures within the hard sphere liquid at arbitrary volume fractions through the morphometric calculation of n-body correlations. We calculate absolute free energies of local geometric motifs in excellent quantitative agreement with molecular dynamics simulations across the liquid and supercooled liquid regimes. We find a bimodality in the density library of states where five-fold symmetric structures appear lower in free energy than four-fold symmetric structures, and from a single reaction path predict an Arrhenius-like scaling of local relaxation dynamics. The method provides a new route to assess changes in the free energy landscape at volume fractions dynamically inaccessible to conventional techniques.
U2 - 10.1103/PhysRevLett.122.068004
DO - 10.1103/PhysRevLett.122.068004
M3 - Letter
VL - 122
JO - Physical Review Letters
JF - Physical Review Letters
SN - 0031-9007
IS - 6
M1 - 068004
ER -