Primary nucleation control of crystals is central to achieve targeted crystal properties such as purity, size, morphology and polymorphic form. Non-photochemical laser-induced nucleation (NPLIN) from solution has gained attention due to its presumed absence of chemical reactions, non-invasive procedures, spatio-temporal control of the nucleation rate, and the ability to influence the polymorphic form of the crystals. Yet, the existing literature has no general agreement on the underlying mechanism and therefore lacks optimization to be applied at the industrial scale. The objective of this dissertation is to elucidate the dominant mechanism behind the direct interaction of the laser pulse(s) with a slightly supersaturated solution that result in crystallization....