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            Optical metasurfaces provide solutions to label-free biochemical sensing by localizing light resonantly beyond the diffraction limit, thereby selectively enhancing light–matter interactions for improved analytical performance. However, high-Qresonances in metasurfaces are usually achieved in the reflection mode, which impedes metasurface integration into compact imaging systems. Here, we demonstrate a metasurface platform for advanced biochemical sensing based on the physics of the bound states in the continuum (BIC) and electromagnetically induced transparency (EIT) modes, which arise when two interfering resonances from a periodic pattern of tilted elliptic holes overlap both spectrally and spatially, creating a narrow transparency window in the mid-infrared spectrum. We experimentally measure these resonant peaks observed in transmission mode (Q∼734 atλ∼8.8µm) in free-standing silicon membranes and confirm their tunability through geometric scaling. We also demonstrate the strong coupling of the BIC-EIT modes with a thinly coated PMMA film on the metasurface, characterized by a large Rabi splitting (32cm−1) and biosensing of protein monolayers in transmission mode. Our new photonic platform can facilitate the integration of metasurface biochemical sensors into compact and monolithic optical systems while being compatible with scalable manufacturing, thereby clearing the way for on-site biochemical sensing in everyday applications.more » « less
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            Abstract BaTiS3, a quasi-1D complex chalcogenide, has gathered considerable scientific and technological interest due to its giant optical anisotropy and electronic phase transitions. However, the synthesis of high-quality BaTiS3crystals, particularly those featuring crystal sizes of millimeters or larger, remains a challenge. Here, we investigate the growth of BaTiS3crystals utilizing a molten salt flux of either potassium iodide, or a mixture of barium chloride and barium iodide. The crystals obtained through this method exhibit a substantial increase in volume compared to those synthesized via the chemical vapor transport method, while preserving their intrinsic optical and electronic properties. Our flux growth method provides a promising route toward the production of high-quality, large-scale single crystals of BaTiS3, which will greatly facilitate advanced characterizations of BaTiS3and its practical applications that require large crystal dimensions. Additionally, our approach offers an alternative synthetic route for other emerging complex chalcogenides. Graphical Abstractmore » « less
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            We found that temperature-dependent infrared spectroscopy measurements (i.e., reflectance or transmittance) using a Fourier-transform spectrometer can have substantial errors, especially for elevated sample temperatures and collection using an objective lens. These errors can arise as a result of partial detector saturation due to thermal emission from the measured sample reaching the detector, resulting in nonphysical apparent reduction of reflectance or transmittance with increasing sample temperature. Here, we demonstrate that these temperature-dependent errors can be corrected by implementing several levels of optical attenuation that enable convergence testing of the measured reflectance or transmittance as the thermal-emission signal is reduced, or by applying correction factors that can be inferred by looking at the spectral regions where the sample is not expected to have a substantial temperature dependence.more » « less
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            null (Ed.)Abstract Optical bottle beams can be used to trap atoms and small low-index particles. We introduce a figure of merit (FoM) for optical bottle beams, specifically in the context of optical traps, and use it to compare optical bottle-beam traps obtained by three different methods. Using this FoM and an optimization algorithm, we identified the optical bottle-beam traps based on a Gaussian beam illuminating a metasurface that are superior in terms of power efficiency than existing approaches. We numerically demonstrate a silicon metasurface for creating an optical bottle-beam trap.more » « less
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            Low-dimensional materials with chain-like (one-dimensional) or layered (two-dimensional) structures are of significant interest due to their anisotropic electrical, optical, and thermal properties. One material with a chain-like structure, BaTiS3 (BTS), was recently shown to possess giant in-plane optical anisotropy and glass-like thermal conductivity. To understand the origin of these effects, it is necessary to fully characterize the optical, thermal, and electronic anisotropy of BTS. To this end, BTS crystals with different orientations (a- and c-axis orientations) were grown by chemical vapor transport. X-ray absorption spectroscopy was used to characterize the local structure and electronic anisotropy of BTS. Fourier transform infrared reflection/transmission spectra show a large in-plane optical anisotropy in the a-oriented crystals, while the c-axis oriented crystals were nearly isotropic in-plane. BTS platelet crystals are promising uniaxial materials for infrared optics with their optic axis parallel to the c-axis. The thermal conductivity measurements revealed a thermal anisotropy of ∼4.5 between the c- and a-axis. Time-domain Brillouin scattering showed that the longitudinal sound speed along the two axes is nearly the same, suggesting that the thermal anisotropy is a result of different phonon scattering rates.more » « less
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            Abstract Polarimetric infrared (IR) detection bolsters IR thermography by leveraging the polarization of light. Optical anisotropy, i.e., birefringence and dichroism, can be leveraged to achieve polarimetric detection. Recently, giant optical anisotropy is discovered in quasi‐1D narrow‐bandgap hexagonal perovskite sulfides, A1+xTiS3, specifically BaTiS3and Sr9/8TiS3. In these materials, the critical role of atomic‐scale structure modulations in the unconventional electrical, optical, and thermal properties raises the broader question of the nature of other materials that belong to this family. To address this issue, for the first time, high‐quality single crystals of a largely unexplored member of the A1+xTiX3(X = S, Se) family, BaTiSe3are synthesized. Single‐crystal X‐ray diffraction determined the room‐temperature structure with theP31cspace group, which is a superstructure of the earlier reportedP63/mmcstructure. The crystal structure of BaTiSe3features antiparallelc‐axis displacements similar to but of lower symmetry than BaTiS3, verified by the polarization dependent Raman spectroscopy. Fourier transform infrared (FTIR) spectroscopy is used to characterize the optical anisotropy of BaTiSe3, whose refractive index along the ordinary (E⊥c) and extraordinary (E‖c) optical axes is quantitatively determined by combining ellipsometry studies with FTIR. With a giant birefringence Δn∼ 0.9, BaTiSe3emerges as a new candidate for miniaturized birefringent optics for mid‐wave infrared to long‐wave infrared imaging.more » « less
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            Abstract It is shown that structural disorder—in the form of anisotropic, picoscale atomic displacements—modulates the refractive index tensor and results in the giant optical anisotropy observed in BaTiS3, a quasi‐1D hexagonal chalcogenide. Single‐crystal X‐ray diffraction studies reveal the presence of antipolar displacements of Ti atoms within adjacent TiS6chains along thec‐axis, and threefold degenerate Ti displacements in thea–bplane.47/49Ti solid‐state NMR provides additional evidence for those Ti displacements in the form of a three‐horned NMR lineshape resulting from a low symmetry local environment around Ti atoms. Scanning transmission electron microscopy is used to directly observe the globally disordered Tia–bplane displacements and find them to be ordered locally over a few unit cells. First‐principles calculations show that the Tia–bplane displacements selectively reduce the refractive index along theab‐plane, while having minimal impact on the refractive index along the chain direction, thus resulting in a giant enhancement in the optical anisotropy. By showing a strong connection between structural disorder with picoscale displacements and the optical response in BaTiS3, this study opens a pathway for designing optical materials with high refractive index and functionalities such as large optical anisotropy and nonlinearity.more » « less
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            Abstract Materials with large birefringence (Δn, wherenis the refractive index) are sought after for polarization control (e.g., in wave plates, polarizing beam splitters, etc.), nonlinear optics, micromanipulation, and as a platform for unconventional light–matter coupling, such as hyperbolic phonon polaritons. Layered 2D materials can feature some of the largest optical anisotropy; however, their use in most optical systems is limited because their optical axis is out of the plane of the layers and the layers are weakly attached. This work demonstrates that a bulk crystal with subtle periodic modulations in its structure—Sr9/8TiS3—is transparent and positive‐uniaxial, with extraordinary indexne= 4.5 and ordinary indexno= 2.4 in the mid‐ to far‐infrared. The excess Sr, compared to stoichiometric SrTiS3, results in the formation of TiS6trigonal‐prismatic units that break the chains of face‐sharing TiS6octahedra in SrTiS3into periodic blocks of five TiS6octahedral units. The additional electrons introduced by the excess Sr form highly oriented electron clouds, which selectively boost the extraordinary indexneand result in record birefringence (Δn> 2.1 with low loss). The connection between subtle structural modulations and large changes in refractive index suggests new categories of anisotropic materials and also tunable optical materials with large refractive‐index modulation.more » « less
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            Abstract Thermal emission is the radiation of electromagnetic waves from hot objects. The promise of thermal‐emission engineering for applications in energy harvesting, radiative cooling, and thermal camouflage has recently led to renewed research interest in this topic. However, accurate and precise measurements of thermal emission in a laboratory setting can be challenging in part due to the presence of background emission from the surrounding environment and the measurement instrument itself. This problem is especially acute for thermal emitters that have unconventional temperature dependence, operate at low temperatures, or are out of equilibrium. In this paper, general procedures are described, recommended, and demonstrated for thermal‐emission measurements that can accommodate such unconventional thermal emitters.more » « less
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