Abstract
The formation of needle-shaped calcium oxalate crystals called raphides is unique to plants, in which related matrix proteins control crystallization of raphides at biomacromolecule–mineral interfaces with convoluted internal structure and complex morphology. However, investigations for understanding intermediate structures and the underlying mechanisms of raphide biomineralization have been lacking. We present a more detailed single-raphide composition by nanoscale secondary ion mass spectrometry (NanoSIMS) mapping to reveal the presence of individual organic fibers embedded inside raphides. This is in situ observed by imaging demineralization of individual raphides using atomic force microscopy (AFM) to unveil the template-mediated organized aggregation of calcium oxalate nanoparticles via a nonclassical particle-based pathway; internal structures are analyzed using high-resolution transmission electron microscopy (HRTEM) to demonstrate the multistep phase transformation by beam-induced coarsening throu...
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