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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) multicrystalline spicules from the solitary tunicate Herdmania momus, with polarization-dependent imaging contrast (PIC)-mapping and scanning and aberration-corrected transmission electron microscopies. The first fully quantitative PIC-mapping data, presented here, measured 0-30° angle spreads between immediately adjacent crystals. Such narrowly distributed crystal orientations demonstrate that crystallinity does not propagate from one crystal to another (0° angle spreads), nor that new crystals with random orientation (90°) 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°. Two observations are cons...

Narrowly Distributed Crystal Orientation in Biomineral Vaterite