We investigate the strongly correlated ion dynamics and the degree of
coupling achievable in the evolution of freely expanding ultracold neutral
plasmas. We demonstrate that the ionic Coulomb coupling parameter Γi increases considerably in later stages of the expansion, reaching the
strongly coupled regime despite the well-known initial drop of Γi
to order unity due to disorder-induced heating. Furthermore, we formulate a
suitable measure of correlation and show th at Γi calculated from
the ionic temperature and density reflects the degree of order in the system if
it is sufficiently close to a quasisteady state. At later times, however, the
expansion of the plasma cloud becomes faster than the relaxation of
correlations, and the system does not reach thermodynamic equilibrium anymore