While
self-actuation and motility are habitual for humans and nonsessile
animals, they are hardly intuitive for simple, lifeless, homogeneous
objects. Among mechanically responsive materials, the few accidentally
discovered examples of crystals that when heated suddenly jump, propelling
themselves to distances that can reach thousands of times their own
size in less than 1 ms, provide the most impressive display of the
conversion of heat into mechanical work. Such thermosalient
crystals are biomimetic, nonpolymeric self-actuators par
excellence. Yet, due to the exclusivity and incongruity of the phenomenon,
as well as because of the unavailability of ready analytical methodology
for its characterization, the reasons behind this colossal self-actuation
remain unexplained. Aimed at unraveling the mechanistic aspects of
the related processes, herein we establish the first systematic assessment
of the interplay among the thermodynamic, kinematic, structural, and
macroscopic factors driving the thermosalient phenomenon. The collective
results are consistent with a latent but very rapid anisotropic unit
cell deformation in a two-stage process that ultimately results in
crystal explosion, separation of debris, or crystal reshaping. The
structural perturbations point to a mechanism similar to phase transitions
of the martensitic family