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Phonon polaritons (PhPs) in van der Waals (vdW) crystal slabs enable nanoscale infrared light manipulation. Specifically, periodically structured vdW slabs behave as polaritonic crystals (vdW-PCs), where the polaritons form Bloch modes. Because the polariton wavelengths are smaller than that of light, conventional far-field spectroscopy does not allow for a complete characterization of vdW-PCs or for revealing their band structure. Here, we perform hyperspectral infrared nanoimaging and analysis of PhPs in a vdW-PC slab made of h-BN. We demonstrate that infrared spectra recorded at individual spatial positions within the unit cell of the vdW-PC can be associated with its band structure and local density of photonic states (LDOS). We thus introduce hyperspectral infrared nanoimaging as a tool for the comprehensive analysis of polaritonic crystals, which could find applications in the reconstruction of complex polaritonic dispersion surfaces in momentum-frequency space or for exploring exotic electromagnetic modes in topological photonic structures., A.Y.N., L.M.-M., and S.G.R. acknowledge the Spanish Ministry of Science, Innovation and Universities (grant MAT201788358-C3.) A.Y.N. acknowledges the Basque Department of Education (grant PIBA-2020-1-0014). P.A.-G. acknowledges support from the European Research Council under starting grant no. 715496, 2DNANOPTICA and from the Spanish Ministry of Science and Innovation (State Plan for Scientific and Technical Research and Innovation grant number PID2019-111156GB-I00). R.H., F.C., and L.E.H. acknowledge the Spanish Ministry of Science, Innovation and Universities (national projects MAT2017-88358-C3, RTI2018-094830-B-100, RTI2018-094861-B-100, and the project MDM-2016-0618 of the Maria de Maeztu Units of Excellence Program). A.Y.N. and R.H. acknowledge funding from the Basque Government (grant no. IT1164-19).

Hexagonal boron nitride (hBN) hosts long-lived phonon polaritons, yielding a strong mid-infrared (mid-IR) electric field enhancement and concentration on the nanometer scale. It is thus a promising material for highly sensitive mid-IR sensing and spectroscopy. In addition, hBN possesses high chemical and thermal stability as well as mechanical durability, making it suitable for operation in demanding environments. In this work, we demonstrate a mid-IR CO2 gas sensor exploiting phonon polariton (PhP) modes in hBN nanoresonators functionalized by a thin CO2-adsorbing polyethylenimine (PEI) layer. We find that the PhP resonance shifts to lower frequency, weakens, and broadens for increasing CO2 concentrations, which are related to the change of the permittivity of PEI upon CO2 adsorption. Moreover, the PhP resonance exhibits a high signal-to-noise ratio even for small ribbon arrays of 30 × 30 μm2. Our results show the potential of hBN nanoresonators to become a novel platform for miniaturized phonon-enhanced SEIRA gas sensors., The research leading to these results has received funding from the H2020 Programme under Grant Agreement No. 881603 (Graphene Flagship). This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant Agreement No. 754510. This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant Agreement No. 665884. This work was partially funded by CEX2019-000910-S [MICINN/AEI/10.13039/501100011033] and Project TUNA-SURF (PID2019-106892RB-I00), Fundació Cellex, Fundació Mir-Puig, and Generalitat de Catalunya through CERCA. We acknowledge financial support from the Spanish Ministry of Science, Innovation and Universities (RTI2018-094830-B-100 and the Project MDM-2016-0618 of the Maria de Maeztu Units of Excellence Program) and the Basque Government (Grant Number IT1164-19). We acknowledge the Ministry of Science, Innovation and Universities through the ‘Maria de Maezt’ Programme for Units of Excellence in R&D (CEX2018-000805-M). Further, support from the Materials Engineering and Processing program of the National Science Foundation, Award Number CMMI 1538127 for h-BN crystal growth is greatly appreciated. The hBN crystals growth is also supported by an Office of Naval Research Award No. N00014-20-1-2474. I.D. acknowledges the Basque Government (Grant No. PRE_2019_2_0164). We acknowledge Project PID2020-115221GB-C41 financed by MCIN/AEI/10.13039/501100011033 and Aragon Government through Project Q-MAD.

Optical nanoantennas are of great importance for photonic devices and spectroscopy due to their capability of squeezing light at the nanoscale and enhancing light–matter interactions. Among them, nanoantennas made of polar crystals supporting phonon polaritons (phononic nanoantennas) exhibit the highest quality factors. This is due to the low optical losses inherent in these materials, which, however, hinder the spectral tuning of the nanoantennas due to their dielectric nature. Here, active and passive tuning of ultranarrow resonances in phononic nanoantennas is realized over a wide spectral range (≈35 cm−1, being the resonance linewidth ≈9 cm−1), monitored by near-field nanoscopy. To do that, the local environment of a single nanoantenna made of hexagonal boron nitride is modified by placing it on different polar substrates, such as quartz and 4H-silicon carbide, or covering it with layers of a high-refractive-index van der Waals crystal (WSe2). Importantly, active tuning of the nanoantenna polaritonic resonances is demonstrated by placing it on top of a gated graphene monolayer in which the Fermi energy is varied. This work presents the realization of tunable polaritonic nanoantennas with ultranarrow resonances, which can find applications in active nanooptics and (bio)sensing., J.M.-S. acknowledges financial support from the Ramón y Cajal Program of the Government of Spain and FSE (Grant No. RYC2018-026196-I) and the Spanish Ministry of Science and Innovation (State Plan for Scientific and Technical Research and Innovation Grant Number PID2019-110308GA-I00). P.A.-G. acknowledges support from the European Research Council under starting Grant No. 715496, 2DNANOPTICA, and the Spanish Ministry of Science and Innovation (State Plan for Scientific and Technical Research and Innovation Grant Number PID2019-111156GB-I00). G.Á.-P. and J.T.-G. acknowledge support through the Severo Ochoa Program from the Government of the Principality of Asturias (Grant nos. PA20-PF-BP19-053 and PA-18-PF-BP17-126, respectively). A.Y.N. acknowledges the Spanish Ministry of Science and Innovation (Grant Nos. MAT201788358-C3-3-R and PID2020-115221GB-C42) and the Basque Department of Education (Grant No. PIBA-2020-1-0014) J.H.E. acknowledges support for h-BN crystal growth from the National Science Foundation, Award Number CMMI-1538127. R.H. acknowledges financial support from the Spanish Ministry of Science, Innovation and Universities (National Project Grant No. RTI2018-094830-B-100 and the Project Grant No. MDM-2016-0618 of the Marie de Maeztu Units of Excellence Program), the Basque Government (Grant No. IT1164-19), and the European Union's Horizon 2020 research and innovation programme under the Graphene Flagship (Grant Agreement Numbers 785219 and 881603, GrapheneCore2 and GrapheneCore3). I.D. acknowledges the Basque Government (Grant No. PRE_2019_2_0164). Work at MIT was partly supported through AFOSR Grant No. FA9550-16-1-0382, through the NSF QII-TAQS program (Grant No. 1936263), and the Gordon and Betty Moore Foundation EPiQS Initiative through Grant No. GBMF9643 to P.J.-H.

In the talk, we will present our recent work on mid-IR gas sensing using highly confined surface modes in graphene and hBN nanoresonators. We have used ultrathin functional coatings to selectively concentrate the target gas molecules in proximity of the 2D nanostructures, just like recognition elements are used in biosensors. As a proof of concept we have demonstrated CO2 sensing using graphene nanoribbons coated with a 10nm polyethylenimine chemisorber. We will discuss the different sensing mechanisms that can be leveraged (e.g. plasmon tuning via polymer-induced chemical doping) and the possibility to extend this platform to other 2D materials like hBN.

Patterning a hyperbolic metasurface Structured metasurfaces potentially enable the control of the propagation direction of excitations on the material's surface. However, the high losses associated with the materials used to date has led to relatively short lifetimes for the excitations. Li et al. patterned a subwavelength grating into a layer of hexagonal boron nitride (hBN) and found that the lifetime and propagation length of the excitations could be much longer. Direct imaging of the polariton excitations illustrates that hBN can be a viable platform for nanophotonic circuits. Science , this issue p. 892

Van der Waals (vdW) materials host a variety of polaritons, which make them an emerging material platform for manipulating light at the nanoscale. Due to the layered structure of vdW materials, the polaritons can exhibit a hyperbolic dispersion and propagate as nanoscale-confined volume modes in thin flakes. On the other hand, surface-confined modes can be found at the flake edges. Surprisingly, the guiding of these modes in ribbons-representing typical linear waveguide structures-is widely unexplored. Here, a detailed study of hyperbolic phonon polaritons propagating in hexagonal boron nitride ribbons is reported. Employing infrared nanoimaging, a variety of modes are observed. Particularly, the fundamental volume waveguide mode that exhibits a cutoff width is identified, which, interestingly, can be lowered by reducing the waveguide thickness. Further, hybridization of the surface modes and their evolution with varying frequency and waveguide width are observed. Most importantly, it is demonstrated that the symmetrically hybridized surface mode does not exhibit a cutoff width, and thus enables linear waveguiding of the polaritons in arbitrarily narrow ribbons. The experimental data, supported by simulations, establish a solid basis for the understanding of hyperbolic polaritons in linear waveguides, which is of critical importance for their application in future photonic devices.

Polaritons – coupled excitations of photons and dipolar matter excitations – can propagate along anisotropic metasurfaces with either hyperbolic or elliptical dispersion. At the transition from hyperbolic to elliptical dispersion (corresponding to a topological transition), various intriguing phenomena are found, such as an enhancement of the photonic density of states, polariton canalization and hyperlensing. Here, we investigate theoretically and experimentally the topological transition, the polaritonic coupling and the strong nonlocal response in a uniaxial infrared-phononic metasurface, a grating of hexagonal boron nitride (hBN) nanoribbons. By hyperspectral infrared nanoimaging, we observe a synthetic transverse optical phonon resonance (strong collective near-field coupling of the nanoribbons) in the middle of the hBN Reststrahlen band, yielding a topological transition from hyperbolic to elliptical dispersion. We further visualize and characterize the spatial evolution of a deeply subwavelength canalization mode near the transition frequency, which is a collimated polariton that is the basis for hyperlensing and diffraction-less propagation., Nature Communications, 11 (1), ISSN:2041-1723

Nanofocusing of light offers new technological opportunities for the delivery and manipulation of electromagnetic fields at sub-diffraction limited length scales. Here, we show that hyperbolic phonon polarity,HPP, modes in the mid infrared as supported by a hexagonal boron nitride, h-BN, slab can be nanofocused (i.e. both field enhanced and wavelength compressed) by propagation along a vertical taper. Via numerical simulations, we demonstrate that field enhancement factors of 90, for steep tapers, and wavelength compression of more than an order of magnitude for adiabatic tapers, can be expected. Employing scatteringtype scanning near field optical microscopy ,s SNOM, we provide for the first time proof of principle experimental evidence of a significant HPP wavelength compression. We expect these functionalities to provide diverse applications, from biosensing and non-linear optics to optical circuitry., Comment: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Photonics, copyright \c{opyright} American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see: https://pubs.acs.org/doi/abs/10.1021/acsphotonics.6b00186

Launching and manipulation of polaritons in van der Waals materials offers novel opportunities for field-enhanced molecular spectroscopy and photodetection, among other applications. Particularly, the highly confined hyperbolic phonon polaritons (HPhPs) in h-BN slabs attract growing interest for their capability of guiding light at the nanoscale. An efficient coupling between free space photons and HPhPs is, however, hampered by their large momentum mismatch. Here, we show —by far-field infrared spectroscopy, infrared nanoimaging and numerical simulations— that resonant metallic antennas can efficiently launch HPhPs in thin h-BN slabs. Despite the strong hybridization of HPhPs in the h-BN slab and Fabry-Pérot plasmonic resonances in the metal antenna, the efficiency of launching propagating HPhPs in h-BN by resonant antennas exceeds significantly that of the non-resonant ones. Our results provide fundamental insights into the launching of HPhPs in thin polar slabs by resonant plasmonic antennas, which will be crucial for phonon-polariton based nanophotonic devices., The authors acknowledge financial support from the European Commission under the Graphene Flagship (GrapheneCore2), the Spanish Ministry of Science, Innovation and Universities (national projects MAT2017-88358-C3, MAT2015-65159-R, MAT2015-65525-R, RTI2018-094830-B-100, RTI2018-094861-B-100, and the project MDM-2016-0618 of the Marie de Maeztu Units of Excellence Program) the Marie Sklodowska-Curie individual fellowship (SGPCM-705960), the Basque Government (PhD fellowship PRE 2018 2 0253), and the project PIC201660E046 from CSIC. M.M.W. acknowledges support from the Konrad-Adenauer-Stiftung. P.A.G. acknowledges support from the European Research Council under Starting Grant 715496, 2DNANOPTICA.

Photonic crystals (PCs) are periodically patterned dielectrics providing opportunities to shape and slow down the light for processing of optical signals, lasing and spontaneous emission control. Unit cells of conventional PCs are comparable to the wavelength of light and are not suitable for subwavelength scale applications. We engineer a nanoscale hole array in a van der Waals material (h-BN) supporting ultra-confined phonon polaritons (PhPs)—atomic lattice vibrations coupled to electromagnetic fields. Such a hole array represents a polaritonic crystal for mid-infrared frequencies having a unit cell volume of 10−5λ30 (with λ0 being the free-space wavelength), where PhPs form ultra-confined Bloch modes with a remarkably flat dispersion band. The latter leads to both angle- and polarization-independent sharp Bragg resonances, as verified by far-field spectroscopy and near-field optical microscopy. Our findings could lead to novel miniaturized angle- and polarization-independent infrared narrow-band couplers, absorbers and thermal emitters based on van der Waals materials and other thin polar materials., The authors acknowledge financial support from the European Commission under the Graphene Flagship (GrapheneCore2), the Spanish Ministry of Economy and Competitiveness (national projects MAT2017-88358-C3,MAT 2015-65159-R, MAT2014-53432-C5, FIS2014-60195-JIN), the Basque government (PhD fellowship PRE-2016-1-0150) and the European Research Council under the starting grants SPINTROS (Grant no. 257654) and 2DNANOPTICA (Grant no. 715496).

Metallic split ring resonators have achieved broad interest in the field of metamaterials and light matter interaction in general. We present split ring resonators fabricated from the van-der Waals material Boron Nitride and designed to operate in the reststrahlen band arround 1400 cm−1. We observe two distinct modes in far field transmission spectra exhibiting high quality factors of 55 and 88. Simulations allow to identify the lowest mode as an LC-mode for which the displacement current is provided by the phononinc material instead of electrons as in metallic counterparts.

Trabajo presentado al Microscopy & Microanalysis Meeting, celebrado en Baltimore (USA) del 5 al 9 de agosto de 2018., AK acknowledges Thermo Fisher Scientific and the Czechoslovak Microscopic Society scholarship for young researchers.

Enhanced light-matter interactions are the basis of surface-enhanced infrared absorption (SEIRA) spectroscopy, and conventionally rely on plasmonic materials and their capability to focus light to nanoscale spot sizes. Phonon polariton nanoresonators made of polar crystals could represent an interesting alternative, since they exhibit large quality factors, which go far beyond those of their plasmonic counterparts. The recent emergence of van der Waals crystals enables the fabrication of high-quality nanophotonic resonators based on phonon polaritons, as reported for the prototypical infrared-phononic material hexagonal boron nitride (h-BN). In this work we use, for the first time, phonon-polariton-resonant h-BN ribbons for SEIRA spectroscopy of small amounts of organic molecules in Fourier transform infrared spectroscopy. Strikingly, the interaction between phonon polaritons and molecular vibrations reaches experimentally the onset of the strong coupling regime, while numerical simulations predict that vibrational strong coupling can be fully achieved. Phonon polariton nanoresonators thus could become a viable platform for sensing, local control of chemical reactivity and infrared quantum cavity optics experiments., We also acknowledge support from the European Commission under the Graphene Flagship (GrapheneCore1, Grant no. 696656), the Marie SklodowskaCurie individual fellowship (SGPCM-705960), the Spanish Ministry of Economy and Competitiveness (Maria de Maetzu Units of Excellence Programme MDM-2016-0618 and national projects FIS2014-60195-JIN, MAT2014-53432- C5-4-R, MAT2015-65525-R, MAT2015-65159-R, FIS2016-80174-P, MAT2017- 88358-C3-3-R), the Basque government (PhD fellowship PRE-2016-1-0150, PRE-2016-2-0025), the Department of Industry of the Basque Government (ELKARTEK project MICRO4FA), the Regional Council of Gipuzkoa (project no. 100/16) and the ERC starting grant 715496, 2DNANOPTICA.

Polaritons in layered materials—including van der Waals materials—exhibit hyperbolic dispersion and strong field confinement, which makes them highly attractive for applications including optical nanofocusing, sensing and control of spontaneous emission. Here we report a near-field study of polaritonic Fabry–Perot resonances in linear antennas made of a hyperbolic material. Specifically, we study hyperbolic phonon–polaritons in rectangular waveguide antennas made of hexagonal boron nitride (h-BN, a prototypical van der Waals crystal). Infrared nanospectroscopy and nanoimaging experiments reveal sharp resonances with large quality factors around 100, exhibiting atypical modal near-field patterns that have no analogue in conventional linear antennas. By performing a detailed mode analysis, we can assign the antenna resonances to a single waveguide mode originating from the hybridization of hyperbolic surface phonon–polaritons (Dyakonov polaritons) that propagate along the edges of the h-BN waveguide. Our work establishes the basis for the understanding and design of linear waveguides, resonators, sensors and metasurface elements based on hyperbolic materials and metamaterials., Here, the authors report a near-field study of hyperbolic phonon polaritons in linear antennas made of hexagonal boron nitride. Infrared nanospectroscopy and nanoimaging experiments reveal sharp Fabry-Perot resonances with large quality factors, exhibiting atypical modal behaviour.

yperbolic polaritons in van der Waals materials recently attract a lot of attention, owing to their strong electromagnetic field confinement, ultraslow group velocities and long lifetimes. Typically, volume confined hyperbolic polaritons (HPs) are studied. Here we show the first near-field optical images of hyperbolic surface polarities, HSPs, which are confined and guided at the edges of thin flakes of a vdW material. To that end, we applied scattering-type scanning near-field optical microscopy (s-SNOM) for launching and real-space nanoimaging of hyperbolic surface phonon polariton modes on a hexagonal boron nitride, h-BN, flake. Our imaging data reveal that the fundamental HSP mode exhibits stronger field confinement, smaller group velocities and nearly identical lifetimes, as compared to the fundamental HP mode of the same h-BN flake. Our experimental data, corroborated by theory, establish a solid basis for future studies and applications of HPs and HSPs in vdW materials., This document is the Accepted Manuscript version of a Published Work that appeared in final form in Nano Letters, copyright \c{opyright} American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see: https://pubs.acs.org/doi/abs/10.1021/acs.nanolett.6b03920

Phonon-polaritons, mixed excitations of light coupled to lattice vibrations (phonons), are emerging as a powerful platform for nanophotonic applications. This is because of their ability to concentrate light into extreme sub-wavelength scales and because of their longer phonon lifetimes compared to their plasmonic counterparts. In this work, the infrared properties of phonon-polaritonic nanoresonators made of monoisotopic 10B hexagonal boron nitride (h-BN) are explored, a material with increased phonon-polariton lifetimes compared to naturally abundant h-BN due to reduced photon scattering from randomly distributed isotopes. An average relative improvement of 50% of the quality factor of monoisotopic h-BN nanoresonators is obtained with respect to nanoresonators made of naturally abundant h-BN, allowing for the sensing of nanometric-thick films of molecules through both surface-enhanced absorption spectroscopy and refractive index sensing. Further, even strong coupling between molecular vibrations and the phonon-polariton resonance in monoisotopic h-BN ribbons can be achieved., The authors acknowledge funding from the Graphene Flagship (Core2 and Core3), the Spanish Ministry of Science and Innovation (projects MDM-2016-0618 of the Maria de Maeztu Units of Excellence Programme and national projects (RTI2018-094830-B-100, RTI2018-094861-B-100, and PID2019-107432GB-I00)), and the Basque Government (project GIU18/202, Ekartek project KK-2018/00001, IT1164-19, and PhD fellowships PRE_2018_2_0253 and PRE_2017_2_0052). The h-BN crystal growth was supported by the National Science Foundation, grant CMMI 1538127 and the II-VI Foundation.