The control of pulsed-laser-induced deposition was studied with the case of ZnO crystallization in a hydrothermal reaction. Crystal orientation, morphologies, and growth rate were observed to vary under different pulsed-laser irradiation conditions. Different energy barriers during nucleation and crystal growth processes were determined by stepped changes of input energy levels of a pulsed laser with the corresponding observations of the states of the material. Therefore, by precisely adjusting the pulsed-laser energy that overcomes a particular energy barrier, ZnO crystals with desired orientation and morphology could be obtained on a seedless substrate in a catalyst-free environment. Crystals varied in morphologies showed different behavior in laser-induced growth, and growth rates were orders of magnitude higher than those of other hydrothermal reactions. By analyzing crystal growth characteristics in the reaction/diffusion-limited region, a set of guidelines were defined to tune the dimensions of ZnO crystals. Laser-induced crystal growth will benefit nanomanufacturing by providing a practical tool to tune the morphology of nanomaterials in a precise and effective manner, and it will bring deeper insight into the thermodynamic and kinetic mechanisms in hydrothermal reactions.
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