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We studied the structural transformations and atomic rearrangements in strontium titanate (SrTiO3) via nanosecond pulsed laser irradiation-induced melting and ultrafast quenching. Using scanning transmission electron microscopy, we determine that the laser-irradiated surface in single-crystalline SrTiO3 transforms into an amorphous phase with an interposing disordered crystalline region between amorphous and ordered phases. The formation of disordered phase is attributed to the rapid recrystallization of SrTiO3 from the melt phase constrained by an epitaxial relation with the pristine region, which eases up on the surface, leading to amorphous phase formation. With electron energy-loss spectroscopic analysis, we confirm the transformation of Ti+4 to Ti+3 due to oxygen vacancy formation as a result of laser irradiation. In the disordered region, the maximum transformation of Ti+4 is observed to be 16.2 ± 0.2%, whereas it is observed to be 20.2 ± 0.2% in the amorphous region. Finally, we deduce that the degree of the disorder increases from atomically disordered to amorphous transition in SrTiO3 under laser-irradiation. The signatures of short-range ordering remain similar, leading to a comparable fingerprint of electronic structure. With these results, this study addresses the gap in understanding the atomic and electronic structure modified by pulsed laser irradiation and functionalizing pristine SrTiO3 for electronic, magnetic, and optical applications.

Understanding the interfaces in heterostructures at an atomic scale is crucial in enabling the possibility to manipulate underlying functional properties in correlated materials. This work presents a detailed study on the atomic structures of heterogeneous interfaces in La0.7Sr0.3MnO3 (LSMO) film grown epitaxially on c-Al2O3 (0001) with a buffer layer of MgO. Using aberration-corrected scanning transmission electron microscopy, we detected nucleation of periodic misfit dislocations at the interfaces of the large misfit systems of LSMO/MgO and MgO/c-Al2O3 following the domain matching epitaxy paradigm. It was experimentally observed that the dislocations terminate with 4/5 lattice planes at the LSMO/MgO interface and with 12/13 lattice planes at the MgO/c-Al2O3 interface. This is consistent with theoretical predictions. Using the atomic-resolution image data analysis approach to generate atomic bond length maps, we investigated the atomic displacement in the LSMO/MgO and MgO/c-Al2O3 systems. Minimal presence of residual strain was shown at the respective interface due to strain relaxation following misfit dislocation formation. Further, based on electron energy-loss spectroscopy analysis, we confirmed an interfacial interdiffusion within two monolayers at both LSMO/MgO and MgO/c-Al2O3 interfaces. In essence, misfit dislocation configurations of the LSMO/MgO/c-Al2O3 system have been thoroughly investigated to understand atomic-scale insights on atomic structure and interfacial chemistry in these large misfit systems.