Wandering principal optical axes in van der Waals triclinic materials.

Nature is abundant in material platforms with anisotropic permittivities arising from symmetry reduction that feature a variety of extraordinary optical effects. Principal optical axes are essential characteristics for these effects that define light-matter interaction. Their orientation - an orthogonal Cartesian basis that diagonalizes the permittivity tensor, is often assumed stationary. Here, we show that the low-symmetry triclinic crystalline structure of van der Waals rhenium disulfide and rhenium diselenide is characterized by wandering principal optical axes in the space-wavelength domain with above π/2 degree of rotation for in-plane components. In turn, this leads to wavelength-switchable propagation directions of their waveguide modes. The physical origin of wandering principal optical axes is explained using a multi-exciton phenomenological model and ab initio calculations. We envision that the wandering principal optical axes of the investigated low-symmetry triclinic van der Waals crystals offer a platform for unexplored anisotropic phenomena and nanophotonic applications.

Exploring van der Waals materials with high anisotropy: geometrical and optical approaches.

The emergence of van der Waals (vdW) materials resulted in the discovery of their high optical, mechanical, and electronic anisotropic properties, immediately enabling countless novel phenomena and applications. Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials. Furthermore, the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches. Here, we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization. Using our approach, we found As2S3 as a highly anisotropic vdW material. It demonstrates high in-plane optical anisotropy that is ~20% larger than for rutile and over two times as large as calcite, high refractive index, and transparency in the visible range, overcoming the century-long record set by rutile. Given these benefits, As2S3 opens a pathway towards next-generation nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry-Pérot optical phase accumulations. Hence, our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties.

Broadband optical properties of Ti3C2 MXene revisited.

The exceptional optical, electrical, and mechanical capabilities of layered transition metal carbides, nitrides, and carbonitrides, called MXenes, revolutionized materials science. Among them, Ti3C2 received the most attention owing to the developed synthesis and processing methods, high conductivity, and pronounced plasmonic response. The latter, however, remains controversial with the open question of whether the peak around 800 nm has plasmonic or interband transition origin. To address this issue, we combine spectroscopic ellipsometry and transmittance results with first-principle computations. Their combination reveals that although Ti3C2 is a metal, its optical response becomes plasmonic (Re ε < 0) above 1415 nm, in contrast to the previous understanding. In addition to fundamental significance, this dual dielectric/plasmonic optical response opens a path for theranostic applications, as we demonstrated on the example of Ti3C2 nanospheres. Thus, our study revisits broadband (300-3300 nm) optical constants of Ti3C2 and broadens its application scope in photonics.

van der Waals Materials for Overcoming Fundamental Limitations in Photonic Integrated Circuitry.

With the advance of on-chip nanophotonics, there is a high demand for high-refractive-index and low-loss materials. Currently, this technology is dominated by silicon, but van der Waals (vdW) materials with a high refractive index can offer a very advanced alternative. Still, up to now, it was not clear if the optical anisotropy perpendicular to the layers might be a hindering factor for the development of vdW nanophotonics. Here, we studied WS2-based waveguides in terms of their optical properties and, particularly, in terms of possible crosstalk distance. Surprisingly, we discovered that the low refractive index in the direction perpendicular to the atomic layers improves the characteristics of such devices, mainly due to expanding the range of parameters at which single-mode propagation can be achieved. Thus, using anisotropic materials offers new opportunities and novel control knobs when designing nanophotonic devices.

Broadband Optical Properties of Bi2Se3.

Materials with high optical constants are of paramount importance for efficient light manipulation in nanophotonics applications. Recent advances in materials science have revealed that van der Waals (vdW) materials have large optical responses owing to strong in-plane covalent bonding and weak out-of-plane vdW interactions. However, the optical constants of vdW materials depend on numerous factors, e.g., synthesis and transfer method. Here, we demonstrate that in a broad spectral range (290-3300 nm) the refractive index n and the extinction coefficient k of Bi2Se3 are almost independent of synthesis technology, with only a ~10% difference in n and k between synthesis approaches, unlike other vdW materials, such as MoS2, which has a ~60% difference between synthesis approaches. As a practical demonstration, we showed, using the examples of biosensors and therapeutic nanoparticles, that this slight difference in optical constants results in reproducible efficiency in Bi2Se3-based photonic devices.

Giant and Tunable Excitonic Optical Anisotropy in Single-Crystal Halide Perovskites.

During the last years, giant optical anisotropy has demonstrated its paramount importance for light manipulation. In spite of recent advances in the field, the achievement of continuous tunability of optical anisotropy remains an outstanding challenge. Here, we present a solution to the problem through the chemical alteration of halogen atoms in single-crystal halide perovskites. As a result, we manage to continually modify the optical anisotropy by 0.14. We also discover that the halide perovskite can demonstrate optical anisotropy up to 0.6 in the visible range─the largest value among non-van der Waals materials. Moreover, our results reveal that this anisotropy could be in-plane and out-of-plane depending on perovskite shape─rectangular and square. As a practical demonstration, we have created perovskite anisotropic nanowaveguides and shown a significant impact of anisotropy on high-order guiding modes. These findings pave the way for halide perovskites as a next-generation platform for tunable anisotropic photonics.

Sr-Doped Superionic Hydrogen Glass: Synthesis and Properties of SrH22.

Recently, several research groups announced reaching the point of metallization of hydrogen above 400 GPa. Despite notable progress, detecting superconductivity in compressed hydrogen remains an unsolved problem. Following the mainstream of extensive investigations of compressed metal polyhydrides, here small doping of molecular hydrogen by strontium is demonstrated to lead to a dramatic reduction in the metallization pressure to ≈200 GPa. Studying the high-pressure chemistry of the Sr-H system, the formation of several new phases is observed: C2/m-Sr3 H13 , pseudocubic SrH6 , SrH9 with cubic F 4 ¯ 3 m $F\bar{4}3m$ -Sr sublattice, and pseudo tetragonal superionic P1-SrH22 , the metal hydride with the highest hydrogen content (96 at%) discovered so far. High diffusion coefficients of hydrogen in the latter phase DH  = 0.2-2.1 × 10-9 m2 s-1 indicate an amorphous state of the H-sublattice, whereas the strontium sublattice remains solid. Unlike Ca and Y, strontium forms molecular semiconducting polyhydrides, whereas calcium and yttrium polyhydrides are high-TC superconductors with an atomic H sublattice. The discovered SrH22 , a kind of hydrogen sponge, opens a new class of materials with ultrahigh content of hydrogen.

Topological phase singularities in atomically thin high-refractive-index materials.

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 SiO2/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 PdSe2 topological phase singularities for a refractive index sensor and demonstrate its superior phase sensitivity compared to typical surface plasmon resonance sensors.

Broadband Optical Properties of Atomically Thin PtS2 and PtSe2.

Noble transition metal dichalcogenides (TMDCs) such as PtS2 and PtSe2 show significant potential in a wide range of optoelectronic and photonic applications. Noble TMDCs, unlike standard TMDCs such as MoS2 and WS2, operate in the ultrawide spectral range from ultraviolet to mid-infrared wavelengths; however, their properties remain largely unexplored. Here, we measured the broadband (245-3300 nm) optical constants of ultrathin PtS2 and PtSe2 films to eliminate this gap and provide a foundation for optoelectronic device simulation. We discovered their broadband absorption and high refractive index both theoretically and experimentally. Based on first-principle calculations, we also predicted their giant out-of-plane optical anisotropy for monocrystals. As a practical illustration of the obtained optical properties, we demonstrated surface plasmon resonance biosensors with PtS2 or PtSe2 functional layers, which dramatically improves sensor sensitivity by 60 and 30%, respectively.

Broadband Optical Constants and Nonlinear Properties of SnS2 and SnSe2.

SnS2 and SnSe2 have recently been shown to have a wide range of applications in photonic and optoelectronic devices. However, because of incomplete knowledge about their optical characteristics, the use of SnS2 and SnSe2 in optical engineering remains challenging. Here, we addressed this problem by establishing SnS2 and SnSe2 linear and nonlinear optical properties in the broad (300-3300 nm) spectral range. Coupled with the first-principle calculations, our experimental study unveiled the full dielectric tensor of SnS2 and SnSe2. Furthermore, we established that SnS2 is a promising material for visible high refractive index nanophotonics. Meanwhile, SnSe2 demonstrates a stronger nonlinear response compared with SnS2. Our results create a solid ground for current and next-generation SnS2- and SnSe2-based devices.