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Low symmetry crystals have recently emerged as a platform for exploring novel light-matter interactions in the form of hyperbolic shear polaritons. These excitations exhibit unique optical properties such as frequency-dispersive optical axes and asymmetric light propagation and energy dissipation, which arise from the presence of non-orthogonal resonances. However, only non-vdW materials have been demonstrated to support hyperbolic shear polaritons, limiting their exotic properties and potential applications. Here we introduce for the first time novel shear phenomena in low symmetry crystal thin films by demonstrating the existence of elliptical and canalized shear phonon polaritons in gypsum, an exfoliable monoclinic sulphate mineral. Our results unveil a topological transition from hyperbolic shear to elliptical shear polaritons, passing through a canalization regime with strong field confinement. Importantly, we observe a significant slowdown of group velocity, reaching values as low as 0.0005c, highlighting the potential of gypsum for "slow light" applications and extreme light-matter interaction control. These findings expand the application scope of low-symmetry crystals with the benefits that an exfoliable material provides, such as stronger field confinement, tunability, and versatility for its incorporation in complex photonic devices that might unlock new optical phenomena at the nanoscale.

Strong coupling of molecules to vacuum fields has been widely reported to lead to modified chemical properties such as reaction rates. However, some recent attempts to reproduce infrared strong coupling results have not been successful, suggesting that factors other than strong coupling may sometimes be involved. Here we re-examine the first of these vacuum-modified chemistry experiments in which changes to a molecular photoisomerisation process in the UV-vis spectral range were attributed to strong coupling of the molecules to visible light. We observed significant variations in photoisomerisation rates consistent with the original work; however, we found no evidence that these changes need to be attributed to strong coupling. Instead, we suggest that the photoisomerisation rates involved are most strongly influenced by the absorption of ultraviolet radiation in the cavity. Our results indicate that care must be taken to rule out non-polaritonic effects before invoking strong coupling to explain any changes of chemical properties arising in cavity-based experiments., Comment: 33 pages, 17 figures

We report on the single-step fabrication of homogeneous and highly ordered Laser Induced Periodic Surface Structures (LIPSS) over large areas on Au nanolayers, that can be used for plasmonic sensing. A comprehensive study on LIPSS formation on 32 nm Au film upon double, 170 fs pulse irradiation, unveiled the key importance of interpulse delay as the determining factor behind the homogeneity of laser induced structures and confirmed that highly ordered, functional LIPSS occur solely upon double pulse irradiation. In particular, the impact of pulse overlap, fluence and interpulse delay reveals that homogeneous LIPSS formation is optimized within a specific interpulse delay range. At the same time, examination of nanoscale features of the structures points out a significant differentiation of the LIPSS formation characteristics between single and double pulse irradiation. Theoretical investigation complements experimental results providing insights on the structure formation mechanism. Ellipsometric measurements validate that such structures exhibit characteristic plasmon resonances that can be exploited for sensing applications. The presented data demonstrate a novel functionality of LIPSS, while providing strong evidence of the capabilities of femtosecond double pulse irradiation as a valuable and low-cost tool for the precise fabrication of highly ordered structures.

Geometric phase optical elements made of space-variant anisotropic media customarily find their optimal operating conditions when the half-wave retardance condition is fulfilled, which allows imparting polarization-dependent changes to an incident wavefront. In practice, intrinsic limitations of man-made manufacturing process or the finite spectrum of the light source lead to a deviation from the ideal behavior. This implies the implementation of strategies to compensate for the associated efficiency losses. Here we report on how the intrinsic tunable features of self-engineered liquid crystal topological defects can be used to enhance the rejection capabilities of spectrally adaptive vector vortex coronagraphs. We also discuss the extent of which current models enable to design efficient devices.

Atomically thin transition metal dichalcogenides (TMDCs) present a promising platform for numerous photonic applications due to excitonic spectral features, possibility to tune their constants by external gating, doping, or light, and mechanical stability. Utilization of such materials for sensing or optical modulation purposes would require a clever optical design, as by itself the 2D materials can offer only a small optical phase delay - consequence of the atomic thickness. To address this issue, we combine films of 2D semiconductors which exhibit excitonic lines with the Fabry-Perot resonators of the standard commercial SiO$_2$/Si substrate, in order to realize topological phase singularities in reflection. Around these singularities, reflection spectra demonstrate rapid phase changes while the structure behaves as a perfect absorber. Furthermore, we demonstrate that such topological phase singularities are ubiquitous for the entire class of atomically thin TMDCs and other high-refractive-index materials, making it a powerful tool for phase engineering in flat optics. As a practical demonstration, we employ PdSe$_2$ topological phase singularities for a refractive index sensor and demonstrate its superior phase sensitivity compared to typical surface plasmon resonance sensors.

Large optical anisotropy observed in a broad spectral range is of paramount importance for efficient light manipulation in countless devices. Although a giant anisotropy was recently observed in the mid-infrared wavelength range, for visible and near-infrared spectral intervals, the problem remains acute with the highest reported birefringence values of 0.8 in BaTiS3 and h-BN crystals. This inspired an intensive search for giant optical anisotropy among natural and artificial materials. Here, we demonstrate that layered transition metal dichalcogenides (TMDCs) provide an answer to this quest owing to their fundamental differences between intralayer strong covalent bonding and weak interlayer van der Walls interaction. To do this, we carried out a correlative far- and near-field characterization validated by first-principle calculations that reveals an unprecedented birefringence of 1.5 in the infrared and 3 in the visible light for MoS2. Our findings demonstrate that this outstanding anisotropy allows for tackling the diffraction limit enabling an avenue for on-chip next-generation photonics., Comment: 20 pages, 5 figures

In this work, we present a simple method for the direct retrieval of the effective permittivity and permeability of a bulk semi-infinite metamaterial from variable-angle spectroscopic ellipsometry measurements. Starting from the well-known Fresnel equations, we derive an analytical expression in which unknown coefficients are fitted to the experimental data using a linear regression model. The effective permittivity and permeability are then determined by solving a simple system and the correct solution is selected based on physical criteria. As an example, the method is applied to the case of a self-assembled metamaterial exhibiting strong isotropic optical magnetism., Comment: 11 pages, 5 figures

Water splitting is unanimously recognized as environment friendly, potentially low cost and renewable energy solution based on the future hydrogen economy. Especially appealing is photo-catalytic water splitting whereby a suitably chosen catalyst dramatically improves efficiency of the hydrogen production driven by direct sunlight and allows it to happen even at zero driving potential. Here, we suggest a new class of stable photo-catalysts and the corresponding principle for catalytic water splitting in which infrared and visible light play the main role in producing the photocurrent and hydrogen. The new class of catalysts based on ionic binary metals with layered graphite-like structures which effectively absorb visible and infrared light facilitating the reaction of water splitting, suppress the inverse reaction of ion recombination by separating ions due to internal electric fields existing near alternating layers, provide the sites for ion trapping of both polarities, and finally deliver the electrons and holes required to generate hydrogen and oxygen gases. As an example, we demonstrate conversion efficiency of 27 percent at bias voltage bias 0.5 V for magnesium di-boride working as a catalyst for photo-induced water splitting. We discuss its advantages over some existing materials and propose the underlying mechanism of photo-catalytic water splitting by binary layered metals.

Optical properties of ferromagnetic half-metallic full-Heusler Co$_{2}$FeGe alloy are investigated experimentally and theoretically. Co$_{2}$FeGe thin films were obtained by DC magnetron sputtering and show the saturation magnetization at $T$=10 K of $m\approx$5.6 $\mu_{B}$/f.u., close to the value predicted by the Slater-Pauling rule. First-principles calculations of the electronic structure and the dielectric tensor are performed using the full-potential linearized-augmented-plane-wave method in the generalized gradient (GGA) and GGA+U approximations. The measured interband optical conductivity spectrum for the alloy exhibits a strong absorption band in the 1 - 4 eV energy range with pronounced fine structure, which agrees well with the calculated half-metallic spectrum of the system, suggesting a near perfect spin-polarization in the material., Comment: 6 pages, 9 figures