Search

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 -MoO 3 and heterostructures of α -MoO 3 and β -Ga 2 O 3 . 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., (© 2024. The Author(s).)

Objectives: To explore the incidence of adverse childhood experiences (ACEs) in breast cancer survivors and potential associations with long-term treatment-related sequelae., Sample & Setting: English-speaking breast cancer survivors three or more years from diagnosis with complete treatment response (N = 120) were recruited prior to scheduled survivorship clinic visits., Methods & Variables: Participants in this cross-sectional observational feasibility study rated anxiety, depression, fatigue, sleep disturbance, cognitive issues, resilience, and ACEs (experienced prior to age 18 years). Blood samples were analyzed for inflammatory and epigenetic biomarkers., Results: ACEs assessment was feasible. Higher ACE scores correlated with greater fatigue, anxiety, and depression, and with lower cognitive function (p < 0.05). Resilience was positively associated with cognitive function and negatively associated with fatigue, anxiety, and depression., Implications for Nursing: There is evidence for the impact of ACEs on long-term treatment-related sequelae in women with breast cancer. Oncology nurses should consider incorporating ACEs assessment into the workflow for women receiving survivorship care.

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, infrared-visible sum-frequency spectro-microscopy is introduced 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. The technique is employed to image hybridization and strong coupling of localized and propagating surface phonon polaritons in a metasurface of SiC micropillars. Spectro-microscopy allows to measure the polariton dispersion simultaneously in momentum space by angle-dependent resonance imaging, and in real space by polariton interferometry. Notably, it is possible to directly image how strong coupling affects the spatial localization of polaritons, inaccessible with conventional spectroscopic techniques. The formation of edge states is observed at excitation frequencies where strong coupling prevents polariton propagation into the metasurface. The technique 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., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

In heterostructures made from polar materials, e.g., AlN-GaN-AlN, the nonequivalence of the two interfaces is long recognized as a critical aspect of their electronic properties; in that, they host different 2D carrier gases. Interfaces play an important role in the vibrational properties of materials, where interface states enhance thermal conductivity and can generate unique infrared-optical activity. The nonequivalence of the corresponding interface atomic vibrations, however, is not investigated so far due to a lack of experimental techniques with both high spatial and high spectral resolution. Herein, the nonequivalence of AlN-(Al 0.65 Ga 0.35 )N and (Al 0.65 Ga 0.35 )N-AlN interface vibrations is experimentally demonstrated using monochromated electron energy-loss spectroscopy in the scanning transmission electron microscope (STEM-EELS) and density-functional-theory (DFT) calculations are employed to gain insights in the physical origins of observations. It is demonstrated that STEM-EELS possesses sensitivity to the displacement vector of the vibrational modes as well as the frequency, which is as critical to understanding vibrations as polarization in optical spectroscopies. The combination enables direct mapping of the nonequivalent interface phonons between materials with different phonon polarizations. The results demonstrate the capacity to carefully assess the vibrational properties of complex heterostructures where interface states dominate the functional properties., (© 2024 Wiley‐VCH GmbH.)

Polariton 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-MoO 3 , by combining α-MoO 3 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 LiV 2 O 5 . In addition to canalization, PhPs in LiV 2 O 5 exhibit strong field confinement ( 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., (© 2024. The Author(s).)

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.

Polar dielectrics are key materials of interest for infrared (IR) nanophotonic applications due to their ability to host phonon-polaritons that allow for low-loss, subdiffractional control of light. The properties of phonon-polaritons are limited by the characteristics of optical phonons, which are nominally fixed for most "bulk" materials. Superlattices composed of alternating atomically thin materials offer control over crystal anisotropy through changes in composition, optical phonon confinement, and the emergence of new modes. In particular, the modified optical phonons in superlattices offer the potential for so-called crystalline hybrids whose IR properties cannot be described as a simple mixture of the bulk constituents. To date, however, studies have primarily focused on identifying the presence of new or modified optical phonon modes rather than assessing their impact on the IR response. This study focuses on assessing the impact of confined optical phonon modes on the hybrid IR dielectric function in superlattices of GaSb and AlSb. Using a combination of first principles theory, Raman, FTIR, and spectroscopic ellipsometry, the hybrid dielectric function is found to track the confinement of optical phonons, leading to optical phonon spectral shifts of up to 20 cm -1 . These results provide an alternative pathway toward designer IR optical materials., (© 2023 Wiley-VCH GmbH.)

Hyperbolic phonon polaritons (HPhPs) can be supported in materials where the real parts of their permittivities along different directions are opposite in sign. HPhPs offer confinements of long-wavelength light to deeply subdiffractional scales, while the evanescent field allows for interactions with substrates, enabling the tuning of HPhPs by altering the underlying materials. Yet, conventionally used noble metal and dielectric substrates restrict the tunability of this approach. To overcome this challenge, here we show that doped semiconductor substrates, e.g., InAs and CdO, enable a significant tuning effect and dynamic modulations. We elucidated HPhP tuning with the InAs plasma frequency in the near-field, with a maximum difference of 8.3 times. Moreover, the system can be dynamically modulated by photo-injecting carriers into the InAs substrate, leading to a wavevector change of ~20%. Overall, the demonstrated hBN/doped semiconductor platform offers significant improvements towards manipulating HPhPs, and potential for engineered and modulated polaritonic systems., (© 2023. The Author(s).)

Surface waves can lead to intriguing transport phenomena. In particular, surface phonon polaritons (SPhPs), which result from coupling between infrared light and optical phonons, have been predicted to contribute to heat conduction along polar thin films and nanowires 1 . However, experimental efforts so far suggest only very limited SPhP contributions 2-5 . Through systematic measurements of thermal transport along the same 3C-SiC nanowires with and without a gold coating on the end(s) that serves to launch SPhPs, here we show that thermally excited SPhPs can substantially enhance the thermal conductivity of the uncoated portion of these wires. The extracted pre-decay SPhP thermal conductance is more than two orders of magnitude higher than the Landauer limit predicted on the basis of equilibrium Bose-Einstein distributions. We attribute the notable SPhP conductance to the efficient launching of non-equilibrium SPhPs from the gold-coated portion into the uncoated SiC nanowires, which is strongly supported by the observation that the SPhP-mediated thermal conductivity is proportional to the length of the gold coating(s). The reported discoveries open the door for modulating energy transport in solids by introducing SPhPs, which can effectively counteract the classical size effect in many technologically important films and improve the design of solid-state devices., (© 2023. The Author(s), under exclusive licence to Springer Nature Limited.)

Intercalation is the process of inserting chemical species into the heterointerfaces of two-dimensional (2D) layered materials. While much research has focused on the intercalation of metals and small gas molecules into graphene, the intercalation of larger molecules through the basal plane of graphene remains challenging. In this work, we present a new mechanism for intercalating large molecules through monolayer graphene to form confined oxide materials at the graphene-substrate heterointerface. We investigate the intercalation of phosphorus pentoxide (P 2 O 5 ) molecules directly from the vapor phase and confirm the formation of confined P 2 O 5 at the graphene-substrate heterointerface using various techniques. Density functional theory (DFT) corroborates the experimental results and reveals the intercalation mechanism, whereby P 2 O 5 dissociates into small fragments catalyzed by defects in the graphene that then permeates through lattice defects and reacts at the heterointerface to form P 2 O 5 . This process can also be used to form new confined metal phosphates (e.g., 2D InPO 4 ). While the focus of this study is on P 2 O 5 intercalation, the possibility of intercalation from predissociated molecules catalyzed by defects in graphene may exist for other types of molecules as well. This in-depth study advances our understanding of intercalation routes of large molecules via the basal plane of graphene as well as heterointerface chemical reactions leading to the formation of distinctive confined complex oxide compounds.

Techniques are well established for the control of nanoparticle shape and size in colloidal synthesis, but very little is understood about precursor interactions and their effects on the resultant crystalline phase. Here we show that oleate, a surface stabilizing ligand that is ubiquitous in nanocrystal synthesis, plays a large role in the mechanism of phase selection of various metal sulfide nanoparticles when thiourea is used as the sulfur source. Gas and solid-phase FTIR, 13 C, and 1 H NMR studies revealed that oleate and thiourea interact to produce oleamide which promotes the isomeric shift of thiourea into ammonium thiocyanate, a less reactive sulfur reagent. Because of these sulfur sequestering reactions, sulfur deficient and metastable nanoparticles are produced, a trend seen across four different metals: copper, iron, nickel, and cobalt. At low carboxylate concentrations, powder XRD indicated that the following phases formed: covellite (CuS); vaesite (NiS 2 ); smythite (FeS 1.3 ), greigite (FeS 1.3 ), marcasite (FeS 2 ) and pyrite (FeS 2 ); and cattierite (CoS 2 ). At high sodium oleate concentration, these phases formed: digenite (CuS 0.55 ), nickel sulfide (NiS), pyrrhotite (FeS 1.1 ), and jaipurite (CoS).

Structural anisotropy in crystals is crucial for controlling light propagation, particularly in the infrared spectral regime where optical frequencies overlap with crystalline lattice resonances, enabling light-matter coupled quasiparticles called phonon polaritons (PhPs). Exploring PhPs in anisotropic materials like hBN and MoO 3 has led to advancements in light confinement and manipulation. In a recent study, PhPs in the monoclinic crystal β-Ga 2 O 3 (bGO) were shown to exhibit strongly asymmetric propagation with a frequency dispersive optical axis. Here, using scanning near-field optical microscopy (s-SNOM), we directly image the symmetry-broken propagation of hyperbolic shear polaritons in bGO. Further, we demonstrate the control and enhancement of shear-induced propagation asymmetry by varying the incident laser orientation and polariton momentum using different sizes of nano-antennas. Finally, we observe significant rotation of the hyperbola axis by changing the frequency of incident light. Our findings lay the groundwork for the widespread utilization and implementation of polaritons in low-symmetry crystals., (© 2023. Springer Nature Limited.)

The coupled interactions among the fundamental carriers of charge, heat, and electromagnetic fields at interfaces and boundaries give rise to energetic processes that enable a wide array of technologies. The energy transduction among these coupled carriers results in thermal dissipation at these surfaces, often quantified by the thermal boundary resistance, thus driving the functionalities of the modern nanotechnologies that are continuing to provide transformational benefits in computing, communication, health care, clean energy, power recycling, sensing, and manufacturing, to name a few. It is the purpose of this Review to summarize recent works that have been reported on ultrafast and nanoscale energy transduction and heat transfer mechanisms across interfaces when different thermal carriers couple near or across interfaces. We review coupled heat transfer mechanisms at interfaces of solids, liquids, gasses, and plasmas that drive the resulting interfacial heat transfer and temperature gradients due to energy and momentum coupling among various combinations of electrons, vibrons, photons, polaritons (plasmon polaritons and phonon polaritons), and molecules. These interfacial thermal transport processes with coupled energy carriers involve relatively recent research, and thus, several opportunities exist to further develop these nascent fields, which we comment on throughout the course of this Review.

Highly anisotropic materials show great promise for spatial control and the manipulation of polaritons. In-plane hyperbolic phonon polaritons (HPhPs) supported by α-phase molybdenum trioxide (MoO 3 ) allow for wave propagation with a high directionality due to the hyperbola-shaped isofrequency contour (IFC). However, the IFC prohibits propagations along the [001] axis, hindering information or energy flow. Here, we illustrate a novel approach to manipulating the HPhP propagation direction. We experimentally demonstrate that geometrical confinement in the [100] axis can guide HPhPs along the forbidden direction with phase velocity becoming negative. We further developed an analytical model to provide insights into this transition. Moreover, as the guided HPhPs are formed in-plane, modal profiles were directly imaged to further expand our understanding of the formation of HPhPs. Our work reveals a possibility for manipulating HPhPs and paves the way for promising applications in metamaterials, nanophotonics, and quantum optics based on natural van der Waals materials.

Hyperbolic phonon polaritons (HPhPs) are stimulated by coupling infrared (IR) photons with the polar lattice vibrations. Such HPhPs offer low-loss, highly confined light propagation at subwavelength scales with out-of-plane or in-plane hyperbolic wavefronts. For HPhPs, while a hyperbolic dispersion implies multiple propagating modes with a distribution of wavevectors at a given frequency, so far it has been challenging to experimentally launch and probe the higher-order modes that offer stronger wavelength compression, especially for in-plane HPhPs. In this work, the experimental observation of higher-order in-plane HPhP modes stimulated on a 3C-SiC nanowire (NW)/α-MoO 3 heterostructure is reported where leveraging both the low-dimensionality and low-loss nature of the polar NWs, higher-order HPhPs modes within 2D α-MoO 3 crystal are launched by the 1D 3C-SiC NW. The launching mechanism is further studied and the requirements for efficiently launching of such higher-order modes are determined. In addition, by altering the geometric orientation between the 3C-SiC NW and α-MoO 3 crystal, the manipulation of higher-order HPhP dispersions as a method of tuning is demonstrated. This work illustrates an extremely anisotropic low dimensional heterostructure platform to confine and configure electromagnetic waves at the deep-subwavelength scales for a range of IR applications including sensing, nano-imaging, and on-chip photonics., (© 2023 Wiley-VCH GmbH.)

One of the main bottlenecks in the development of terahertz (THz) and long-wave infrared (LWIR) technologies is the limited intrinsic response of traditional materials. Hyperbolic phonon polaritons (HPhPs) of van der Waals semiconductors couple strongly with THz and LWIR radiation. However, the mismatch of photon - polariton momentum makes far-field excitation of HPhPs challenging. Here, we propose an In-Plane Hyperbolic Polariton Tuner that is based on patterning van der Waals semiconductors, here α-MoO 3 , into ribbon arrays. We demonstrate that such tuners respond directly to far-field excitation and give rise to LWIR and THz resonances with high quality factors up to 300, which are strongly dependent on in-plane hyperbolic polariton of the patterned α-MoO 3 . We further show that with this tuner, intensity regulation of reflected and transmitted electromagnetic waves, as well as their wavelength and polarization selection can be achieved. Our results can help the development of THz and LWIR miniaturized devices., (© 2023. The Author(s).)

Wavelength-selective absorbers (WS-absorbers) are of interest for various applications, including chemical sensing and light sources. Lithography-free fabrication of WS-absorbers can be realized via Tamm plasmon polaritons (TPPs) supported by distributed Bragg reflectors (DBRs) on plasmonic materials. While multifrequency and nearly arbitrary spectra can be realized with TPPs via inverse design algorithms, demanding and thick DBRs are required for high quality-factors (Q-factors) and/or multiband TPP-absorbers, increasing the cost and reducing fabrication error tolerance. Here, high Q-factor multiband absorption with limited DBR layers (3 layers) is experimentally demonstrated by Tamm hybrid polaritons (THPs) formed by coupling TPPs and Tamm phonon polaritons when modal frequencies are overlapped. Compared to the TPP component, the Q-factors of THPs are improved twofold, and the angular broadening is also reduced twofold, facilitating applications where narrow-band and nondispersive WS-absorbers are needed. Moreover, an open-source algorithm is developed to inversely design THP-absorbers consisting of anisotropic media and exemplify that the modal frequencies can be assigned to desirable positions. Furthermore, it is demonstrated that inversely designed THP-absorbers can realize same spectral resonances with fewer DBR layers than a TPP-absorber, thus reducing the fabrication complexity and enabling more cost-effective, lithography-free, wafer-scale WS-absorberss for applications such as free-space communications and gas sensing., (© 2023 Wiley-VCH GmbH.)

Various optical crystals possess permittivity components of opposite signs along different principal directions in the mid-infrared regime, exhibiting exotic anisotropic phonon resonances. Such materials with hyperbolic polaritons-hybrid light-matter quasiparticles with open isofrequency contours-feature large-momenta optical modes and wave confinement that make them promising for nanophotonic on-chip technologies. So far, hyperbolic polaritons have been observed and characterized in crystals with high symmetry including hexagonal (boron nitride), trigonal (calcite) and orthorhombic (α-MoO 3 or α-V 2 O 5 ) crystals, where they obey certain propagation patterns. However, lower-symmetry materials such as monoclinic crystals were recently demonstrated to offer richer opportunities for polaritonic phenomena. Here, using scanning near-field optical microscopy, we report the direct real-space nanoscale imaging of symmetry-broken hyperbolic phonon polaritons in monoclinic CdWO 4 crystals, and showcase inherently asymmetric polariton excitation and propagation associated with the nanoscale shear phenomena. We also introduce a quantitative theoretical model to describe these polaritons that leads to schemes to enhance crystal asymmetry via the damping loss of phonon modes. Ultimately, our findings show that polaritonic nanophotonics is attainable using natural materials with low symmetry, favouring a versatile and general way to manipulate light at the nanoscale., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

Dielectric metasurfaces governed by bound states in the continuum (BIC) are actively investigated for achieving high-quality factors and strong electromagnetic field enhancements. Traditional approaches reported for tuning the performance of quasi-BIC metasurfaces include tuning the resonator size, period, and structure symmetry. Here we propose and experimentally demonstrate an alternative approach through engineering slots within a zigzag array of elliptical silicon resonators. Through analytical theory, three-dimensional electromagnetic modeling, and infrared spectroscopy, we systematically investigate the spectral responses and field distributions of the slotted metasurface in the mid-IR. Our results show that by introducing slots, the electric field intensity enhancement near the apex and the quality factor of the quasi-BIC resonance are increased by a factor of 2.1 and 3.3, respectively, in comparison to the metasurface without slots. Furthermore, the slotted metasurface also provides extra regions of electromagnetic enhancement and confinement, which holds enormous potential in particle trapping, sensing, and emission enhancement.

Optical metasurfaces offer a compact platform for manipulation of the amplitude, phase, and polarization state of light. Independent control over these properties, however, is hindered by the symmetric transmission matrix associated with single-layer metasurfaces. Here, we utilize multilayer birefringent meta-optics to realize high-efficiency, independent control over the amplitude, phase, and polarization state of light. High-efficiency control is enabled by redistributing the wavefront between cascaded metasurfaces, while end-to-end inverse design is used to realize independent complex-valued functions for orthogonal polarization states. Based on this platform, we demonstrate spatial mode division multiplexing, optical mode conversion, and universal vectorial holograms, all with diffraction efficiencies over 80%. This meta-optic platform expands the design space of flat optics and could lead to advances in optical communications, quantum entanglement, and information encryption.

The lattice symmetry of a crystal is one of the most important factors in determining its physical properties. Particularly, low-symmetry crystals offer powerful opportunities to control light propagation, polarization and phase 1-4 . Materials featuring extreme optical anisotropy can support a hyperbolic response, enabling coupled light-matter interactions, also known as polaritons, with highly directional propagation and compression of light to deeply sub-wavelength scales 5 . Here we show that monoclinic crystals can support hyperbolic shear polaritons, a new polariton class arising in the mid-infrared to far-infrared due to shear phenomena in the dielectric response. This feature emerges in materials in which the dielectric tensor cannot be diagonalized, that is, in low-symmetry monoclinic and triclinic crystals in which several oscillators with non-orthogonal relative orientations contribute to the optical response 6,7 . Hyperbolic shear polaritons complement previous observations of hyperbolic phonon polaritons in orthorhombic 1,3,4 and hexagonal 8,9 crystal systems, unveiling new features, such as the continuous evolution of their propagation direction with frequency, tilted wavefronts and asymmetric responses. The interplay between diagonal loss and off-diagonal shear phenomena in the dielectric response of these materials has implications for new forms of non-Hermitian and topological photonic states. We anticipate that our results will motivate new directions for polariton physics in low-symmetry materials, which include geological minerals 10 , many common oxides 11 and organic crystals 12 , greatly expanding the material base and extending design opportunities for compact photonic devices., (© 2022. The Author(s).)

Localized surface phonon polaritons (LSPhPs) can be implemented to engineer light-matter interactions through nanoscale patterning for a range of midinfrared application spaces. However, the polar material systems studied to date have mainly focused on simple designs featuring a single element in the periodic unit cell. Increasing the complexity of the unit cell can serve to modify the resonant near-fields and intra- and inter-unit-cell coupling as well as to dictate spectral tuning in the far-field. In this work, we exploit more complicated unit-cell structures to realize LSPhP modes with additional degrees of design freedom, which are largely unexplored. Collectively excited LSPhP modes with distinctly symmetric and antisymmetric near-fields are supported in these subarray designs, which are based on nanopillars that are scaled by the number of subarray elements to ensure a constant unit-cell size. Moreover, we observe an anomalous mode-matching of the collective symmetric mode in our fabricated subarrays that is robust to changing numbers of pillars within the subarrays as well as to defects intentionally introduced in the form of missing pillars. This work therefore illustrates the hierarchical design of tailored LSPhP resonances and modal near-field profiles simultaneously for a variety of IR applications such as surface-enhanced spectroscopies and biochemical sensing.

As the length scales of materials decrease, the heterogeneities associated with interfaces become almost as important as the surrounding materials. This has led to extensive studies of emergent electronic and magnetic interface properties in superlattices 1-9 . However, the interfacial vibrations that affect the phonon-mediated properties, such as thermal conductivity 10,11 , are measured using macroscopic techniques that lack spatial resolution. Although it is accepted that intrinsic phonons change near boundaries 12,13 , the physical mechanisms and length scales through which interfacial effects influence materials remain unclear. Here we demonstrate the localized vibrational response of interfaces in strontium titanate-calcium titanate superlattices by combining advanced scanning transmission electron microscopy imaging and spectroscopy, density functional theory calculations and ultrafast optical spectroscopy. Structurally diffuse interfaces that bridge the bounding materials are observed and this local structure creates phonon modes that determine the global response of the superlattice once the spacing of the interfaces approaches the phonon spatial extent. Our results provide direct visualization of the progression of the local atomic structure and interface vibrations as they come to determine the vibrational response of an entire superlattice. Direct observation of such local atomic and vibrational phenomena demonstrates that their spatial extent needs to be quantified to understand macroscopic behaviour. Tailoring interfaces, and knowing their local vibrational response, provides a means of pursuing designer solids with emergent infrared and thermal responses., (© 2022. The Author(s).)

Wavelength-selective thermal emitters (WS-EMs) are of interest due to the lack of cost-effective, narrow-band sources in the mid- to long-wave infrared. WS-EMs can be realized via Tamm plasmon polaritons (TPPs) supported by distributed Bragg reflectors on metals. However, the design of multiple resonances is challenging as numerous structural parameters must be optimized simultaneously. Here we use stochastic gradient descent to optimize TPP emitters (TPP-EMs) composed of an aperiodic distributed Bragg reflector deposited on doped cadmium oxide (CdO) film, where layer thicknesses and carrier density are inversely designed. The combination of the aperiodic distributed Bragg reflector with the designable plasma frequency of CdO enables multiple TPP-EM modes to be simultaneously designed with arbitrary spectral control not accessible with metal-based TPPs. Using this approach, we experimentally demonstrated and numerically proposed TPP-EMs exhibiting single or multiple emission bands with designable frequencies, line-widths and amplitudes. This thereby enables lithography-free, wafer-scale WS-EMs that are complementary metal-oxide-semiconductor compatible for applications such as free-space communications and gas sensing., (© 2021. The Author(s), under exclusive licence to Springer Nature Limited.)

The hyperbolic phonon polaritons supported in hexagonal boron nitride (hBN) with long scattering lifetimes are advantageous for applications such as super-resolution imaging via hyperlensing. Yet, hyperlens imaging is challenging for distinguishing individual and closely spaced objects and for correlating the complicated hyperlens fields with the structure of an unknown object underneath. Here, we make significant strides to overcome each of these challenges. First, we demonstrate that monoisotopic h 11 BN provides significant improvements in spatial resolution, experimentally resolving structures as small as 44 nm and those with sub 25 nm spacings at 6.76 μm free-space wavelength. We also present an image reconstruction algorithm that provides a structurally accurate, visual representation of the embedded objects from the complex hyperlens field. Further, we offer additional insights into optimizing hyperlens performance on the basis of material properties, with an eye toward realizing far-field imaging modalities. Thus, our results significantly advance label-free, high-resolution, spectrally selective hyperlens imaging and image reconstruction methodologies.

The mid-infrared (MIR) is an exciting spectral range that also hosts useful molecular vibrational fingerprints. There is a growing interest in nanophotonics operating in this spectral range, and recent advances in plasmonic research are aimed at enhancing MIR infrared nanophotonics. In particular, the design of hybrid plasmonic metasurfaces has emerged as a promising route to realize novel MIR applications. Here we demonstrate a hybrid nanostructure combining graphene and silicon carbide to extend the spectral phonon response of silicon carbide and enable absorption and field enhancement of the MIR photon via the excitation and hybridization of surface plasmon polaritons and surface phonon polaritons. We combine experimental methods and finite element simulations to demonstrate enhanced absorption of MIR photons and the broadening of the spectral resonance of graphene-coated silicon carbide nanowires. We also indicate subwavelength confinement of the MIR photons within a thin oxide layer a few nanometers thick, sandwiched between the graphene and silicon carbide. This intermediate shell layer is characteristically obtained using our graphitization approach and acts as a coupling medium between the core and outer shell of the nanowires.

Hyperbolic phonon polaritons (HPhPs) enable strong confinements, low losses, and intrinsic beam steering capabilities determined by the refractive index anisotropy-providing opportunities from hyperlensing to flat optics and other applications. Here, two scanning-probe techniques, photothermal induced resonance (PTIR) and scattering-type scanning near-field optical microscopy (s-SNOM), are used to map infrared ( 6.4 - 7.4 μ m ) HPhPs in large (up to 120 × 250 μ m 2 near-monoisotopic > 99 % B 10 ) hexagonal boron nitride (hBN) flakes. Wide ( ≈ 40 μ m ) PTIR and s-SNOM scans on such large flakes avoid interference from polaritons launched from different asperities (edges, folds, surface defects, etc.) and together with Fourier analyses 0.05 μ m - 1 resolution) enable precise measurements of HPhP lifetimes (up to ≈ 4.2 p s and propagation lengths (up to ≈ 25 and ≈ 17 μ m for the first- and second-order branches, respectively). With respect to naturally abundant hBN, we report an eightfold improved, record-high (for hBN) propagating figure of merit (i.e., with both high confinement and long lifetime) in ≈ 99 % B 10 hBN, achieving, finally, theoretically predicted values. We show that wide near-field scans critically enable accurate estimates of the polaritons' lifetimes and propagation lengths and that the incidence angle of light, with respect to both the sample plane and the flake edge, needs to be considered to extract correctly the dispersion relation from the near-field polaritons maps. Overall, the measurements and data analyses employed here elucidate details pertaining to polaritons' propagation in isotopically enriched hBN and pave the way for developing high-performance HPhP-based devices., Competing Interests: The authors have no conflicts to disclose.

Natural hyperbolic materials with dielectric permittivities of opposite signs along different principal axes can confine long-wavelength electromagnetic waves down to the nanoscale, well below the diffraction limit. Confined electromagnetic waves coupled to phonons in hyperbolic dielectrics including hexagonal boron nitride (hBN) and α-MoO 3 are referred to as hyperbolic phonon polaritons (HPPs). HPP dissipation at ambient conditions is substantial, and its fundamental limits remain unexplored. Here, we exploit cryogenic nanoinfrared imaging to investigate propagating HPPs in isotopically pure hBN and naturally abundant α-MoO 3 crystals. Close to liquid-nitrogen temperatures, losses for HPPs in isotopic hBN drop significantly, resulting in propagation lengths in excess of 8 μm, with lifetimes exceeding 5 ps, thereby surpassing prior reports on such highly confined polaritonic modes. Our nanoscale, temperature-dependent imaging reveals the relevance of acoustic phonons in HPP damping and will be instrumental in mitigating such losses for miniaturized mid-infrared technologies operating at liquid-nitrogen temperatures.

Silicon waveguides have enabled large-scale manipulation and processing of near-infrared optical signals on chip. Yet, expanding the bandwidth of guided waves to other frequencies will further increase the functionality of silicon as a photonics platform. Frequency multiplexing by integrating additional architectures is one approach to the problem, but this is challenging to design and integrate within the existing form factor due to scaling with the free-space wavelength. This paper demonstrates that a hexagonal boron nitride (hBN)/silicon hybrid waveguide can simultaneously enable dual-band operation at both mid-infrared (6.5-7.0 µm) and telecom (1.55 µm) frequencies, respectively. The device is realized via the lithography-free transfer of hBN onto a silicon waveguide, maintaining near-infrared operation. In addition, mid-infrared waveguiding of the hyperbolic phonon polaritons (HPhPs) supported in hBN is induced by the index contrast between the silicon waveguide and the surrounding air underneath the hBN, thereby eliminating the need for deleterious etching of the hyperbolic medium. The behavior of HPhP waveguiding in both straight and curved trajectories is validated within an analytical waveguide theoretical framework. This exemplifies a generalizable approach based on integrating hyperbolic media with silicon photonics for realizing frequency multiplexing in on-chip photonic systems., (© 2021 Wiley-VCH GmbH.)

Strong coupling between optical modes can be implemented into nanophotonic design to modify the energy-momentum dispersion relation. This approach offers potential avenues for tuning the thermal emission frequency, line width, polarization, and spatial coherence. Here, we employ three-mode strong coupling between propagating and localized surface phonon polaritons, with zone-folded longitudinal optic phonons within periodic arrays of 4H-SiC nanopillars. Energy exchange, mode evolution, and coupling strength between the three polariton branches are explored experimentally and theoretically. The influence of strong coupling upon the angle-dependent thermal emission was directly measured, providing excellent agreement with theory. We demonstrate a 5-fold improvement in the spatial coherence and 3-fold enhancement of the quality factor of the polaritonic modes, with these hybrid modes also exhibiting a mixed character that could enable opportunities to realize electrically driven emission. Our results show that polariton-phonon strong coupling enables thermal emitters, which meet the requirements for a host of IR applications in a simple, lightweight, narrow-band, and yet bright emitter.

Light-matter interactions that induce charge and energy transfer across interfaces form the foundation for photocatalysis 1,2 , energy harvesting 3 and photodetection 4 , among other technologies. One of the most common mechanisms associated with these processes relies on carrier injection. However, the exact role of the energy transport associated with this hot-electron injection remains unclear. Plasmon-assisted photocatalytic efficiencies can improve when intermediate insulation layers are used to inhibit the charge transfer 5,6 or when off-resonance excitations are employed 7 , which suggests that additional energy transport and thermal effects could play an explicit role even if the charge transfer is inhibited 8 . This provides an additional interfacial mechanism for the catalytic and plasmonic enhancement at interfaces that moves beyond the traditionally assumed physical charge injection 9-12 . In this work, we report on a series of ultrafast plasmonic measurements that provide a direct measure of electronic distributions, both spatially and temporally, after the optical excitation of a metal/semiconductor heterostructure. We explicitly demonstrate that in cases of strong non-equilibrium, a novel energy transduction mechanism arises at the metal/semiconductor interface. We find that hot electrons in the metal contact transfer their energy to pre-existing free electrons in the semiconductor, without an equivalent spatiotemporal transfer of charge. Further, we demonstrate that this ballistic thermal injection mechanism can be utilized as a unique means to modulate plasmonic interactions. These experimental results are well-supported by both rigorous multilayer optical modelling and first-principle ab initio calculations.

Exploiting polaritons in natural vdW materials has been successful in achieving extreme light confinement and low-loss optical devices and enabling simplified device integration. Recently, α-MoO 3 has been reported as a semiconducting biaxial vdW material capable of sustaining naturally orthogonal in-plane phonon polariton modes in IR. In this study, we investigate the polarization-dependent optical characteristics of cavities formed using α-MoO 3 to extend the degrees of freedom in the design of IR photonic components exploiting the in-plane anisotropy of this material. Polarization-dependent absorption over 80% in a multilayer Fabry-Perot structure with α-MoO 3 is reported without the need for nanoscale fabrication on the α-MoO 3 . We observe coupling between the α-MoO 3 optical phonons and the Fabry-Perot cavity resonances. Using cross-polarized reflectance spectroscopy we show that the strong birefringence results in 15% of the total power converted into the orthogonal polarization with respect to incident wave. These findings can open new avenues in the quest for polarization filters and low-loss, integrated planar IR photonics and in dictating polarization control.

Polaritons in two-dimensional materials provide extreme light confinement that is difficult to achieve with metal plasmonics. However, such tight confinement inevitably increases optical losses through various damping channels. Here we demonstrate that hyperbolic phonon polaritons in hexagonal boron nitride can overcome this fundamental trade-off. Among two observed polariton modes, featuring a symmetric and antisymmetric charge distribution, the latter exhibits lower optical losses and tighter polariton confinement. Far-field excitation and detection of this high-momenta mode become possible with our resonator design that can boost the coupling efficiency via virtual polariton modes with image charges that we dub 'image polaritons'. Using these image polaritons, we experimentally observe a record-high effective index of up to 132 and quality factors as high as 501. Further, our phenomenological theory suggests an important role of hyperbolic surface scattering in the damping process of hyperbolic phonon polaritons.

The biaxial van der Waals semiconductor α-phase molybdenum trioxide (α-MoO 3 ) has recently received significant attention due to its ability to support highly anisotropic phonon polaritons (PhPs)-infrared (IR) light coupled to lattice vibrations-offering an unprecedented platform for controlling the flow of energy at the nanoscale. However, to fully exploit the extraordinary IR response of this material, an accurate dielectric function is required. Here, the accurate IR dielectric function of α-MoO 3 is reported by modeling far-field polarized IR reflectance spectra acquired on a single thick flake of this material. Unique to this work, the far-field model is refined by contrasting the experimental dispersion and damping of PhPs, revealed by polariton interferometry using scattering-type scanning near-field optical microscopy (s-SNOM) on thin flakes of α-MoO 3 , with analytical and transfer-matrix calculations, as well as full-wave simulations. Through these correlative efforts, exceptional quantitative agreement is attained to both far- and near-field properties for multiple flakes, thus providing strong verification of the accuracy of this model, while offering a novel approach to extracting dielectric functions of nanomaterials. In addition, by employing density functional theory (DFT), insights into the various vibrational states dictating the dielectric function model and the intriguing optical properties of α-MoO 3 are provided., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

There are a broad range of applications for narrowband long-wave infrared (LWIR) sources, especially within the 8-12 μm atmospheric window. These include infrared beacons, free-space communications, spectroscopy, and potentially on-chip photonics. Unfortunately, commercial light-emitting diode (LED) sources are not available within the LWIR, leaving only gas-phase and quantum cascade lasers, which exhibit low wall-plug efficiencies and in many cases require large footprints, precluding their use for many applications. Recent advances in nanophotonics have demonstrated the potential for tailoring thermal emission into an LED-like response, featuring narrowband, polarized thermal emitters. In this work, we demonstrate that such nanophotonic IR emitting metamaterials (NIREMs), featuring near-unity absorption, can serve as LWIR sources with effectively no net power consumption, enabling their operation entirely by waste heat from conventional electronics. Using experimental emissivity spectra from a SiC NIREM device in concert with a thermodynamic compact model, we verify this feasibility for two test cases: a NIREM device driven by waste heat from a CPU heat sink and one operating using a low-power resistive heater for elevated temperature operation. To validate these calculations, we experimentally determine the temperature-dependent NIREM irradiance and the angular radiation pattern. We purport that these results provide a first proof-of-concept for waste heat-driven thermal emitters potentially employable in a variety of infrared application spaces., Competing Interests: The authors declare no competing financial interest., (Copyright © 2020 American Chemical Society.)

The anisotropy of hexagonal boron nitride (hBN) gives rise to hyperbolic phonon-polaritons (HPhPs), notable for their volumetric frequency-dependent propagation and strong confinement. For frustum (truncated nanocone) structures, theory predicts five, high-order HPhPs, sets, but only one set was observed previously with far-field reflectance and scattering-type scanning near-field optical microscopy. In contrast, the photothermal induced resonance (PTIR) technique has recently permitted sampling of the full HPhP dispersion and observing such elusive predicted modes; however, the mechanism underlying PTIR sensitivity to these weakly-scattering modes, while critical to their understanding, has not yet been clarified. Here, by comparing conventional contact- and newly developed tapping-mode PTIR, we show that the PTIR sensitivity to those weakly-scattering, high-Q (up to ≈280) modes is, contrary to a previous hypothesis, unrelated to the probe operation (contact or tapping) and is instead linked to PTIR ability to detect tip-launched dark, volumetrically-confined polaritons, rather than nanostructure-launched HPhPs modes observed by other techniques. Furthermore, we show that in contrast with plasmons and surface phonon-polaritons, whose Q -factors and optical cross-sections are typically degraded by the proximity of other nanostructures, the high- Q HPhP resonances are preserved even in high-density hBN frustum arrays, which is useful in sensing and quantum emission applications.

Hyperbolic phonon polaritons (HPhPs) are generated when infrared photons couple to polar optic phonons in anisotropic media, confining long-wavelength light to nanoscale volumes. However, to realize the full potential of HPhPs for infrared optics, it is crucial to understand propagation and loss mechanisms on substrates suitable for applications from waveguiding to infrared sensing. We employ scattering-type scanning near-field optical microscopy (s-SNOM) and nano-Fourier transform infrared (FTIR) spectroscopy, in concert with analytical and numerical calculations, to elucidate HPhP characteristics as a function of the complex substrate dielectric function. We consider propagation on suspended, dielectric and metallic substrates to demonstrate that the thickness-normalized wavevector can be reduced by a factor of 25 simply by changing the substrate from dielectric to metallic behavior. Moreover, by incorporating the imaginary contribution to the dielectric function in lossy materials, the wavevector can be dynamically controlled by small local variations in loss or carrier density. Counterintuitively, higher-order HPhP modes are shown to exhibit the same change in the polariton wavevector as the fundamental mode, despite the drastic differences in the evanescent ranges of these polaritons. However, because polariton refraction is dictated by the fractional change in the wavevector, this still results in significant differences in polariton refraction and reduced sensitivity to substrate-induced losses for the higher-order HPhPs. Such effects may therefore be used to spatially separate hyperbolic modes of different orders and for index-based sensing schemes. Our results advance our understanding of fundamental hyperbolic polariton excitations and their potential for on-chip photonics and planar metasurface optics.