Structured light – electromagnetic waves with a strong spatial inhomogeneity of amplitude, phase, and polarization – has occupied far-reaching positions in both optical research and applications. Terahertz (THz) waves, due to recent innovations in photonics and nanotechnology, became so robust that it was not only implemented in a wide variety of applications such as communications, spectroscopic analysis, and non-destructive imaging, but also served as a low-cost and easily implementable experimental platform for novel concept illustration. In this work, we show that structured nonparaxial THz light in the form of Airy, Bessel, and Gaussian beams can be generated in a compact way using exclusively silicon diffractive optics prepared by femtosecond laser ablation technology. The accelerating nature of the generated structured light is demonstrated via THz imaging of objects partially obscured by an opaque beam block. Unlike conventional paraxial approaches, when a combination of a lens and a cubic phase (or amplitude) mask creates a nondiffracting Airy beam, we demonstrate simultaneous lensless nonparaxial THz Airy beam generation and its application in imaging system. Images of single objects, imaging with a controllable placed obstacle, and imaging of stacked graphene layers are presented, revealing hence potential of the approach to inspect quality of 2D materials. Structured nonparaxial THz illumination is investigated both theoretically and experimentally with appropriate extensive benchmarks. The structured THz illumination consistently outperforms the conventional one in resolution and contrast, thus opening new frontiers of structured light applications in imaging and inverse scattering problems, as it enables sophisticated estimates of optical properties of the investigated structures.

The design and synthesis of new stimuli-responsive hydrogen-bonding monomers that display a diversity of self-assembly pathways is of central importance in supramolecular chemistry. Here we describe the aggregation properties of a simple, intrinsically C₂-symmetric enantiopure bicyclic cavity compound bearing a terminally unsubstituted ureidopyrimidinone fragment fused with a pyrrole moiety in different solvents and in the absence and presence of C₆₀ and C₇₀ guests. The tetrameric cyclic aggregate is selectively obtained in chlorinated solvents, where only part of the available hydrogen bonding sites are utilized, whereas in toluene or upon addition of C₇₀ guests, further aggregation into tubular supramolecular polymers is achieved. The open-end cyclic assemblies rearrange into a closed-shell capsule upon introduction of C₆₀ with an accompanied symmetry breaking of the monomer. Our study demonstrates that a C₆₀ switch can be used to simultaneously control the topology and occupancy of tubular assemblies resulting from the aggregation of small monomers.

A femto- and picosecond laser assisted periodic nanostructuring of hydrogenated amorphous silicon (a-Si:H) is demonstrated. The grating structure with the subwavelength modulation of refractive index shows form birefringence (Δn ≈ −0.6) which is two orders of magnitude higher than commonly observed in uniaxial crystals and femtosecond laser nanostructured silica glass. The laser-induced giant birefringence and dichroism in a-Si:H film introduce extra dimensions to the polarization sensitive laser writing with applications that include data storage, security marking, and flat optics.