  Biominerals formed by animals provide skeletal support, and many other
functions. They were previously shown to grow by aggregation of amorphous
nanoparticles, but never to grow ion-by-ion from solution, which is a common
growth mechanism for abiotic crystals. We analyze vaterite CaCO3 multi
crystalline spicules from the solitary tunicate Herdmania momus, with
Polarization dependent Imaging Contrast PIC mapping, scanning and aberration
corrected transmission electron microscopies. The first fully quantitative PIC
mapping data, presented here, measured 0{\deg} 30{\deg} angle spreads between
immediately adjacent crystals. Such narrowly distributed crystal orientations
demonstrate that crystallinity does not propagate from one crystal to another
0{\deg} angle spreads, nor that new crystals with random orientation 90{\deg}
nucleate. There are no organic layers at the interface between crystals, hence
a new, unknown growth mechanism must be invoked, with crystal nucleation
constrained within 30{\deg}. Two observations are consistent with crystal
growth from solution: vaterite microcrystals express crystal faces, and are
smooth at the nanoscale after cryo fracture. The observation of 30{\deg} angle
spreads, lack of interfacial organic layers, and smooth fracture figures
broadens the range of known biomineralization mechanisms and may inspire novel
synthetic crystal growth strategies. Spherulitic growth from solution is one
possible mechanism consistent with all these observations.
