We present the results of broadband dielectric spectroscopy of GaMo4S8,
a lacunar spinel system that recently was shown to exhibit non-canonical,
orbitally-driven ferroelectricity. Our study reveals complex relaxation
dynamics of this multiferroic material, both above and below its Jahn-Teller
transition at TJT=47 K. Above TJT, two types of
coupled dipolar-orbital dynamics seem to compete: relaxations within
cluster-like regions with short-range polar order like in relaxor
ferroelectrics and critical fluctuations of only weakly interacting dipoles,
the latter resembling the typical dynamics of order-disorder type
ferroelectrics. Below the Jahn-Teller transition, the onset of orbital order
drives the system into long-range ferroelectric order and dipolar dynamics
within the ferroelectric domains is observed. The coupled dipolar and orbital
relaxation behavior of GaMo4S8 above the Jahn-Teller transition markedly
differs from that of the skyrmion host GaV4S8, which seems to be linked
to differences in the structural distortions of the two systems on the
unit-cell level.Comment: 6 pages, 3 figures + Supplemental Material (2 pages, 2 figures