  The high efficiency of lead organo-metal-halide perovskite solar cells has
raised many questions about the role of the methylammonium (MA) molecules in
the Pb-I framework. Experiments indicate that the MA molecules are able to
'freely' spin around at room temperature even though they carry an intrinsic
dipole moment. We have performed large supercell (2592 atoms) finite
temperature ab-initio molecular dynamics calculations to study the correlation
between the molecules in the framework. An underlying long range
anti-ferroelectric ordering of the molecular dipoles is observed. The dynamical
correlation between neighboring molecules shows a maximum around room
temperature in the mid-temperature phase. In this phase, the rotations are slow
enough to (partially) couple to neighbors via the Pb-I cage. This results in a
collective motion of neighboring molecules in which the cage acts as the
mediator. At lower and higher temperatures the motions are less correlated.
