Surface relief gratings were spontaneously photoinduced from a collimated Nd:YAG laser beam at 532 nm on thin films of a disperse red 1 functionalized glass-forming compound. Pattern formation was studied by measuring the diffraction intensity of a He-Ne laser probe beam at 633 nm and by atomic force microscopy (AFM). The dependence of pattern formation on both irradiation time and intensity was studied. The gratings could be erased both optically and thermally. The orientation of the gratings is influenced by the polarization of the writing beam, and it is accompanied by strong diffraction of the incident light into the sample plane, thereby providing a way to couple and trap the light into the substrate. Interestingly, photobleaching upon prolonged irradiation yields transparent gratings, and the process is partially reversible upon thermal erasure.

Nucleation and growth of spontaneous surface relief gratings (SSRGs) on a Disperse Red 1 (DR1) glass-forming derivative were investigated. No interference pattern is applied and surface patterning is induced using single-beam irradiation: the gratings are selforganized. Grating growth is assumed to initiate from an interference pattern formed between the incident light beam and waves scattered at grazing angle by surface defects. However, the mechanism is not yet fully understood and there is not a comprehensive explanation of the structure formation process. Herein, the grating formation procedure is studied by monitoring the surface topology of thin films exposed to one writing beam for various periods of time, under both linear and circular polarizations, using AFM. Even in the absence of surface defects on the initial film, irradiation produces light-induced surface defects due to the reorientation and mass movement of the azo molecules. These defects act as seeds for SSRG around which gratings gradually emerge and propagate throughout the sample. To consolidate this hypothesis, the formation of gratings was studied on samples with controlled surface roughness. Pore-shaped defects do not diffract light on top of the sample, and thus have no impact on SSRG growth, while for hill-shaped defects, growth rate decreases sharply with defect sizes larger than the writing beam wavelength. Two other analogous glass-forming azobenzene derivatives were studied, and in all cases, SSRG formation was correlated with the induction of birefringence in the early stages of the irradiation.

Chiral structures and materials interact with light in well-documented ways, but light can also interact with achiral materials to generate chirality by inscribing its asymmetric configuration on photoresponsive materials, such as azobenzene derivatives. While it is thus possible to generate both two-dimensional (2D) and three-dimensional (3D) chirality, 2D chirality is especially attractive because of its non-reciprocity. Herein, 2D chirality is induced on the surface of a glass-forming Disperse Red 1 derivative by irradiation with a single laser beam, yielding crossed spontaneous surface relief gratings with different pitches. Azimuth rotations up to 10° have been observed, and the absence of 3D chirality has been confirmed. This method thus allows generating non-reciprocal planar chiral objects by a simple, single irradiation process on a thin film of a material that can easily be processed over large areas or onto small objects.

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