The formation of the domain structure in congruent lithium niobate crystals by multiple pulse irradiation using an infrared laser was studied experimentally. The qualitative change of the domain wall shape with an increase of the pulse number was revealed. The chains of isolated nanodomains representing the domain wall traces appeared after each laser pulse irradiation in the samples with an irradiated polar surface covered by an indium–tin oxide layer. This effect allowed extraction of the detailed information about the evolution of the domain wall shape. The domain kinetics under the action of the pyroelectric field has been considered. The mechanism of the self-assembled shape evolution of the moving domain wall as a result of the local wall accelerations and retardations caused by the shape fluctuations (bumps and valleys) was proposed. The experimentally observed formation of the quasi-regular comb-like domain structures with randomly distributed bumps and valleys was confirmed by computer simulation. The discovered effects allowed us to create the stable random and quasi-regular domain structures and open the way for further development of the domain engineering methods.
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