Hyperbolic phonon polaritons - hybridized modes arising from the ultrastrong coupling of infrared light to strongly anisotropic lattice vibrations in uniaxial or biaxial polar crystals - enable to confine light to the nanoscale with low losses and high directionality. In even lower symmetry materials, such as monoclinic β $\beta$ -Ga2O3 (bGO), hyperbolic shear polaritons (HShPs) further enhance the directionality. Yet, HShPs are intrinsically supported only within narrow frequency ranges defined by the phonon frequencies of the host material. Here, we report spectral tuning of HShPs in bGO by isotopic substitution. Employing near-field optical microscopy to image HShPs in 18O bGO films homoepitaxially grown on a 16O bGO substrate, we demonstrate a spectral redshift of ∼ $\sim$ 40 cm-1 for the 18O bGO, compared to 16O bGO. The technique allows for direct observation and a model-free estimation of the spectral shift driven by isotopic substitution without the need for knowledge of the dielectric tensor. Complementary far-field measurements and ab initio calculations - in good agreement with the near-field data - confirm the effectiveness of this estimation. This multifaceted study demonstrates a significant isotopic substitution induced spectral tuning of HShPs into a previously inaccessible frequency range, creating new avenues for technological applications of such highly directional polaritons.

Textiles provide a valuable source of information regarding past cultures and their artistic practices. Understanding ancient textiles requires identifying the raw materials used, since the origin of dyes and fibers may be from plants or animals, with the specific species used varying based on geography, trade routes and cultural significance. A selection of nine Chancay textile fragments attributed to 800-1200 CE were studied with liquid chromatography mass spectrometry (LC-MS) and direct analysis in real time mass spectrometry (DART-MS) to identify the chemical compounds in extracts of natural dyes used to create green, blue, red, yellow and black colors. From the identified molecular markers, the green colors involved the overdyeing of indigo and flavonoid dyes, the blue colors were achieved using an indigo dye, the yellows came from a flavonoid dye, the reds from anthraquinone dyes of both plant and animal origin, and the black from a mixture of flavonoid, anthraquinone and indigo dyes. A subset of the textiles was identified as containing proteinaceous fibers based on ATR-FTIR. These textiles were further studied using a mass spectrometry-based proteomics approach to identify the species used, with the peptide sequences measured confirming the presence of South American camelids, most likely llama or alpaca.

Low-symmetry crystals have emerged as a platform for exploring unique light-matter interactions in the form of hyperbolic shear polaritons. These excitations exhibit unique properties such as frequency-dispersive optical axes and asymmetric light propagation and energy dissipation. However, only non-vdW materials have been demonstrated to support hyperbolic shear polaritons, limiting their exotic properties and potential applications. Here, we introduce shear phenomena in low symmetry crystals by demonstrating 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. We observe a notable slowdown of group velocity, reaching values as low as 0.0005c. 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.

Thermal transport across solid-solid interfaces is vital for advanced electronic and photonic applications, yet conventional conduction pathways often restrict performance. In polar crystals, hybridized vibrational modes called phonon polaritons offer a promising avenue to overcome the limitations of intrinsic phonon heat conduction. Here our work demonstrates that volume-confined hyperbolic phonon polariton (HPhP) modes can transfer energy across solid-solid interfaces at rates far exceeding phonon-phonon conduction. Using pump-probe thermoreflectance with a mid-infrared, tunable probe pulse with subpicosecond resolution, we remotely and selectively observe HPhP modes in hexagonal boron nitride (hBN) via broadband radiative heating from a gold source. Our measurements ascertain that hot electrons impinging at the interface radiate directly into the HPhPs of hBN in the near field, bypassing the phonon-phonon transport pathway. Such polaritonic coupling enables thermal transport speeds in solids orders of magnitude faster than possible through diffusive phonon processes. We thereby showcase a pronounced thermal transport enhancement across the gold-hBN interface via phonon-polariton coupling, advancing the limits of interfacial heat transfer.

Metal-based thermal metasurfaces exhibit stable spectral characteristics under temperature fluctuations, in contrast to more traditional gray- and near black-bodies, as well as some dielectric metasurfaces, whose emission spectra shift with changing temperatures. However, they often suffer from limited quality (Q) factors due to significant non-radiative ohmic losses. In this study, we address the challenge of achieving high emissivity and Q-factors in metal-based thermal emitters. By leveraging the coupling between a magnetic dipole resonance and two bound-state-in-continuum (BIC) resonances to achieve electromagnetically induced absorption (EIA) in an asymmetric metallic ring structure, we design a metal-based thermal metasurface with a near-unity emissivity (0.96) and a Q factor as high as 320 per simulations. Experimental validation yields an emissivity of 0.82 and a Q factor of 202, representing an approximately five-fold improvement in the experimentally measured Q factor compared to the state-of-the-art metal-based thermal metasurfaces. Our work offers a promising approach for developing efficient, narrow-band, directional thermal emitters with stable emission spectra across a wide temperature range.

In-plane Hyperbolic Phonon polaritons (HPhPs) are quasiparticles formed via coupling of photons and optical phonons in in-plane hyperbolic materials and offer unique applications in sensing, thermal emitters and high resolution imaging. However, the large momentum mismatch between photons and these in-plane HPhPs has restricted their technological potential as most experimental demonstration rely on sophisticated and expensive near field detection schemes. In this work, using the example of $\alpha-$MoO$_3$, we demonstrate that by constructing photonic hypercrystals of this material, one can not only excite these in-plane HPhPs in the far field but also tune the far field response via twisting the hypercrystal lattice with respect the lattice of $\alpha-$MoO$_3$. Our findings will pave the way for the development of practical in-plane HPhP devices as well as provide access to new fundamental physics of such materials via conventional and well developed far field measurement techniques.

Extended defects in wide-bandgap semiconductors have been widely investigated using techniques providing either spectroscopic or microscopic information. Nano-Fourier transform infrared spectroscopy (nano-FTIR) is a nondestructive characterization method combining FTIR with nanoscale spatial resolution (∼20 nm) and topographic information. Here, we demonstrate the capability of nano-FTIR for the characterization of extended defects in semiconductors by investigating an in-grown stacking fault (IGSF) present in a 4H-SiC epitaxial layer. We observe a local spectral shift of the mid-infrared near-field response, consistent with the identification of the defect stacking order as 3C-SiC (cubic) from comparative simulations based on the finite dipole model (FDM). This 3C-SiC IGSF contrasts with the more typical 8H-SiC IGSFs reported previously and is exemplary in showing that nanoscale spectroscopy with nano-FTIR can provide new insights into the properties of extended defects, the understanding of which is crucial for mitigating deleterious effects of such defects in alternative semiconductor materials and devices.

The vast repository of van der Waals (vdW) materials supporting polaritons offers numerous possibilities to tailor electromagnetic waves at the nanoscale. The development of twistoptics-the modulation of the optical properties by twisting stacks of vdW materials-enables directional propagation of phonon polaritons (PhPs) along a single spatial direction, known as canalization. Here we demonstrate a complementary type of directional propagation of polaritons by reporting the visualization of unidirectional ray polaritons (URPs). They arise naturally in twisted hyperbolic stacks with very different thicknesses of their constituents, demonstrated for homostructures of α -MoO3 and heterostructures of α -MoO3 and β -Ga2O3. Importantly, their ray-like propagation, characterized by large momenta and constant phase, is tunable by both the twist angle and the illumination frequency. Apart from their fundamental importance, our findings introduce twisted asymmetric stacks as efficient platforms for nanoscale directional polariton propagation, opening the door for applications in nanoimaging, (bio)-sensing, or polaritonic thermal management.

This report demonstrates tunable carrier densities in CdO thin films through local ion irradiation, providing lateral control of mid-IR optical properties. Ion-solid interactions produce donor-like defects that boost electron concentrations from the practical minimum of 2.5 x 10(19) cm(-3) to a maximum of 2.5 x 10(20) cm(-3) by metered ion exposure. This range is achieved using He, N, Ar, or Au ions at 1-2.8 MeV; when normalized by displacements per atom, all ion species produce comparable results. Since CdO is well-described by the Drude model, irradiation-tuned carrier densities directly alter the infrared dielectric function, and in turn, mid-infrared optical properties. Further, it is demonstrated that by combining irradiation with traditional lithography, CdO films expose to ions in the presence of 3-mu m thick, patterned photoresist exhibit lateral carrier density profiles with approximate to 400-nm resolution. Scanning near-field optical microscopy reveals sharp optical interfaces with almost no companion contrast in surface morphology, microstructure, or crystallinity. Finally, CdO lateral homostructures supporting surface plasmon polaritons (SPPs) are demonstrated whose dispersion relation can be tuned through periodic patterning in a monolithic platform by simple nanofabrication. Numerical simulations show these polaritons result from strong coupling between excitations at CdO plasma frequencies and SPPs supported by the platinum substrate.

Notwithstanding its relevance to many applications in sensing, security, and communications, electrical generation of narrow-band mid-infrared light remains highly challenging. Unlike in the ultraviolet or visible spectral regions few materials possess direct electronic transitions in the mid-infrared and most that do are created through complex band-engineering schemes. An alternative mechanism, independent of dipole active material transitions, relies instead on energy lost to the polar lattice through the Coulomb interaction. Longitudinal phonons radiated in this way can be spectrally tuned through the engineering of polar nanostructures and coupled to localized optical modes in the material, allowing them to radiate mid-infrared photons into the far-field. A recent theoretical work explored this process providing for the first time an indication of its technological relevance when compared to standard thermal emitters. In order to do so it nevertheless used an equilibrium model of the electron gas, making this model difficult to inform the design of an optimal device to experimentally observe the effect. The present paper removes this limitation, describing the electron gas using a rigorous, self-consistent, non-equilibrium Green's function model, accounting for variations in material properties across the device, and electron-electron interactions. Although the instability of the Schrodinger-Poisson iteration limits our studies to the low-bias regime, our results demonstrate emission rates comparable to that of room-temperature thermal emission despite such low biases. These results provide a pathway to design a confirmatory experiment of this new emission channel, that could power a new generation of mid-infrared optoelectronic devices.

AbstractPolariton canalization is characterized by intrinsic collimation of energy flow along a single crystalline axis. This optical phenomenon has been experimentally demonstrated at the nanoscale by stacking and twisting van der Waals (vdW) layers of α-MoO3, by combining α-MoO3 and graphene, or by fabricating an h-BN metasurface. However, these material platforms have significant drawbacks, such as complex fabrication and high optical losses in the case of metasurfaces. Ideally, it would be possible to canalize polaritons “naturally” in a single pristine layer. Here, we theoretically predict and experimentally demonstrate naturally canalized phonon polaritons (PhPs) in a single thin layer of the vdW crystal LiV2O5. In addition to canalization, PhPs in LiV2O5 exhibit strong field confinement ($${{{{{{\boldsymbol{\lambda }}}}}}}_{{{{{{\bf{p}}}}}}} \sim \frac{{{{{{{\boldsymbol{\lambda }}}}}}}_{{{{{{\bf{0}}}}}}}}{{{{{{\bf{27}}}}}}}$$ λ p ~ λ 0 27 ), slow group velocity (0.0015c), and ultra-low losses (lifetimes of 2 ps). Our findings are promising for the implementation of low-loss optical nanodevices where strongly directional light propagation is needed, such as waveguides or optical routers.

Wavelength-selective thermal emitters (WS-EMs) hold considerable appeal due to the scarcity of cost-effective, narrow-band sources in the mid-to-long-wave infrared spectrum. WS-EMs achieved via dielectric materials typically exhibit thermal emission peaks with high quality factors (Q factors), but their optical responses are prone to temperature fluctuations. Metallic EMs, on the other hand, show negligible drifts with temperature changes, but their Q factors usually hover around 10. In this study, we introduce and experimentally verify an EM grounded in plasmonic quasi-bound states in the continuum (BICs) within a mirror-coupled system. Our design numerically delivers an ultra-narrowband single peak with a Q factor of approximately 64 and near-unity absorptance that can be freely tuned within an expansive band of more than 10 µm. By introducing air slots symmetrically, the Q factor can be further augmented to around 100. Multipolar analysis and phase diagrams are presented to elucidate the operational principle. Importantly, our infrared spectral measurements affirm the remarkable resilience of our designs’ resonance frequency in the face of temperature fluctuations over 300°C. Additionally, we develop an effective impedance model based on the optical nanoantenna theory to understand how further tuning of the emission properties is achieved through precise engineering of the slot. This research thus heralds the potential of applying plasmonic quasi-BICs in designing ultra-narrowband, temperature-stable thermal emitters in the mid-infrared. Moreover, such a concept may be adaptable to other frequency ranges, such as near-infrared, terahertz, and gigahertz.

Hexagonal boron nitride (hBN), also known as white graphite, is a transparent layered crystal with a wide bandgap. Its crystal structure resembles graphite, featuring layers composed of honeycomb lattices held together through van der Waals forces. The layered crystal structure of hBN facilitates exfoliation into thinner flakes and makes it highly anisotropic in in-plane and out-of-plane directions. Unlike graphite, hBN is both insulating and transparent, making it an ideal material for isolating devices from the environment and acting as a waveguide. As a result, hBN has found extensive applications in optical devices, electronic devices, and quantum photonic devices. This comprehensive tutorial aims to provide readers with a thorough understanding of hBN, covering its synthesis, lattice and spectroscopic characterization, and various applications in optoelectronic and quantum photonic devices. This tutorial is designed for both readers without prior experience in hBN and those with expertise in specific fields seeking to understand its relevance and connections to others.

It has been well-accepted that heat conduction in solids is mainly mediated by electrons and phonons. Recently, there has been a strong emerging interest in the contribution of various polaritons, quasi-particles resulting from the coupling between electromagnetic waves and different excitations in solids, to heat conduction. Traditionally, the polaritonic effect on conduction has been largely neglected because of the low number density of polaritons. However, it has been recently predicted and experimentally confirmed that polaritons could play significant roles in heat conduction in polar nanostructures. Since the transport characteristics of polaritons are very different from those of electrons and phonons, polariton-mediated heat conduction provides new opportunities for manipulating heat flow in solid-state devices for more efficient heat dissipation or energy conversion. In view of the rapid growth of polariton-mediated heat conduction, especially by phonon polaritons, here we review the recent progress in this field and provide perspectives for challenges and opportunities.

Cultural heritage artifacts present a distinct set of challenges when it comes to characterizing the material composition of extracted samples. Whatever samples are removed must be small to preserve the integrity of the artwork, and ideally, applied techniques should be nondestructive to allow samples to be saved for future use. Unfortunately, most nondestructive optical detection schemes are constrained to spatial resolutions set by the diffraction limit of light. Since many material-specific properties used for identification are dependent upon molecular vibrations and conductivity, this implies the need for spectral analysis in the infrared. The long wavelengths associated with infrared light can make it difficult to definitively identify materials when the sample composition varies at the length scales of nanometers. Nano-FTIR provides a unique solution whereby scattering-type scanning near-field optical microscopy is combined with a broadband illumination source for FTIR-like detection with subdiffraction spatial resolution (similar to 20 nm). The nondestructive nature of the technique makes it optimally suited to characterize art conservation samples while minimizing sample extraction by allowing individual samples to be characterized by multiple complementary techniques. In this work, the capabilities of nano-FTIR are evaluated in the study of surface coatings sampled from African wood sculptures, where the submicrometer scale of some of the layers makes the composition of the cross sections difficult to interpret using other established techniques. We show that the functional groups corresponding to different classes of organic coatings and inorganic pigments can be assigned based on point spectra, indicating that nano-FTIR holds great promise for the field of art conservation.

Anisotropic planar polaritons - hybrid electromagnetic modes mediated by phonons, plasmons, or excitons - in biaxial two-dimensional (2D) van der Waals crystals have attracted significant attention due to their fundamental physics and potential nanophotonic applications. In this Perspective, we review the properties of planar hyperbolic polaritons and the variety of methods that can be used to experimentally tune them. We argue that such natural, planar hyperbolic media should be fairly common in biaxial and uniaxial 2D and 1D van der Waals crystals, and identify the untapped opportunities they could enable for functional (i.e. ferromagnetic, ferroelectric, and piezoelectric) polaritons. Lastly, we provide our perspectives on the technological applications of such planar hyperbolic polaritons.

Phonon polaritons enable waveguiding and localization of infrared light with extreme confinement and low losses. The spatial propagation and spectral resonances of such polaritons are usually probed with complementary techniques such as near-field optical microscopy and far-field reflection spectroscopy. Here, we introduce infrared-visible sum-frequency spectro-microscopy as a tool for spectroscopic imaging of phonon polaritons. The technique simultaneously provides sub-wavelength spatial resolution and highly-resolved spectral resonance information. This is implemented by resonantly exciting polaritons using a tunable infrared laser and wide-field microscopic detection of the upconverted light. We employ this technique to image hybridization and strong coupling of localized and propagating surface phonon polaritons in metasurfaces of SiC micropillars. Spectro-microscopy allows us to measure the polariton dispersion simultaneously in momentum space by angle-dependent resonance imaging, and in real space by polariton interferometry. Notably, we directly visualize how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. We further observe the formation of edge states at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. Our approach is applicable to the wide range of polaritonic materials with broken inversion symmetry and can be used as a fast and non-perturbative tool to image polariton hybridization and propagation.

In heterostructures made from polar materials, e.g., AlN-GaN-AlN, the non-equivalence of the two interfaces has long been recognized as a critical aspect of their electronic properties, in that they host different two-dimensional carrier gasses. Interfaces play as important a role in the vibrational properties of materials, where interface states enhance thermal conductivity and can generate unique infrared-optical activity. The non-equivalence of the corresponding interface atomic vibrations, however, has not been investigated so far due to a lack of experimental techniques with both high spatial and high spectral resolution. Herein we experimentally demonstrate the non-equivalence of AlN-(Al0.65Ga0.35)N and (Al0.65Ga0.35)N-AlN interface vibrations using monochromated electron energy-loss spectroscopy in the scanning transmission electron micro-scope (STEM-EELS) and employ density-functional-theory (DFT) calculations to gain insights in the origins of observations. We demonstrate that STEM-EELS possesses sensitivity to the dis-placement vector of the vibrational modes as well as the frequency, which enables direct mapping of the non-equivalent interface phonons between materials with different phonon polarizations in the interface direction. The physical origin of the non-equivalent interface behavior is then unraveled by understanding the localization and anisotropy of phonon displacements using DFT calculations. The results demonstrate the capacity to carefully assess the vibrational properties of com-plex heterostructures where interface states dominate the functional properties.