A rotating lattice single (RLS) crystal is a unique form of solid, which was fabricated recently as one-dimensional architecture in glass via solid state transformation induced by laser irradiation. In these objects, the lattice rotates gradually and predictably about an axis that lies in the plane of the crystal and is normal to the laser scanning direction. This paper reports on the fabrication of Sb 2 S 3 two-dimensional (2D) RLS crystals on the surface of 16SbI 3 −84Sb 2 S 3 glass, as a model example: individual RLS crystal lines are joined together using "stitching" or "rastering" as two successful protocols. The electron back scattered diffraction mapping and scanning Laue X-ray microdiffraction of the 2D RLS crystals show gradual rotation of lattice comprising of two components, one along the length of each line and another normal to this direction. The former component is determined by the rotation of the first line of the 2D pattern, but the relative contribution of the last component depends on the extent of overlap between two successive lines. By the appropriate choice of initial seed orientation and the direction of scanning, it is possible to control the lattice rotation, and even to reduce it down to ∼5°for a 50 × 50 μm 2 2D pattern of Sb 2 S 3 crystal.

This study explores multiple fields as a mechanism of controlling the orientation of the nucleation process, which is generally believed to be a stochastic process, as observed in the equiaxed grain structure of glass ceramics. Specifically, as a model system, Sb2S3 single crystals are grown on the surface of Sb-S-I chalcogenide glass via laser crystallization. A spatial light modulator is used to configure the beam shape, thermal gradient, and/or polarization of the laser for controlling the orientation of Sb2S3 crystal seeds. We determine that the chemical and thermal gradient can affect the crystal morphology but do not significantly influence the crystal seed orientation. In contrast, the short crystal axis along [010] has a preferential alignment along the direction of polarization and perpendicular to the surface normal. Thus, we conclude that polarization can be used as an effective tool for controlling the nucleation and hence the orientation of Sb2S3 crystals on the surface of Sb-S-I chalcogenide glasses.

Laser heating of chalcogenide glasses has successfully produced rotating lattice single crystals through a solid-solid transformation. To better understand the nature of complex, orientation-dependent lattice rotation, we designed heat profiles of the continuous wave laser by beam shaping, fabricated larger Sb2S3 crystal dots in Sb2S3 glass, and investigated the lattice rotation where the crystal could grow in all radial directions under a circular thermal gradient. The results show that the rate of lattice rotation is highly anisotropic and depends on crystallographic direction. The nature of this rotation is the same in crystals of different orientation relative to the surface. The growth directions that align with the slip planes show the highest rate of rotation and the rotation rate gradually decreases away from this direction. Additionally, the presence of multiple growth directions results in a complicated rotation system. We suggest that the growth front influences the density of dislocations introduced during growth under confinement and thus affects the lattice rotation rate in these crystals.

Single-crystal architectures in glass, formed by a solid-solid transformation via laser heating, are novel solids with a rotating lattice. To understand the process of lattice formation that proceeds via crystal growth, we have observed in situ Sb 2 S 3 crystal formation under X-ray irradiation with simultaneous Laue micro X-ray diffraction (μXRD) pattern collection. By translating the sample with respect to the beam, we form rotating lattice single (RLS) crystal lines with a consistently linear relationship between the rotation angle and distance from nucleation site. The lines begin with a seed crystal, followed by a transition region comprising of sub-grain or very similarly oriented grains, followed by the presence of a rotating lattice single crystal of unrestricted length. The results demonstrate that the primary cause of lattice rotation within RLS crystals is the densification accompanying the glass → crystal transformation, rather than stresses produced from the difference in thermal expansion coefficient of the two phases or paraelectric → ferroelectric transition during cooling to ambient temperature.

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