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Polaritons allow for strong light-matter coupling and for highly sensitive analysis of (bio)chemical substances and processes. Nanoimaging of the polaritons' evanescent fields is critically important for experimental mode identification and field confinement studies. Here we describe two setups for polariton nanoimaging and spectroscopy in liquid. We first demonstrate the mapping of localized plasmon polaritons in metal antennas with a transflection infrared scattering-type scanning near-field optical microscope (s-SNOM), where the tip acts as a near-field scattering probe. We then demonstrate a total internal reflection (TIR)-based setup, where the tip is both launching and probing ultraconfined polaritons in van der Waals materials (here phonon polaritons in hexagonal boron nitride flakes), laying the foundation for s-SNOM-based polariton interferometry in liquid. Our results promise manifold applications, for example, in situ studies of strong coupling between polaritons and molecular vibrations or chemical reactions at the bare or functionalized surfaces of polaritonic materials.

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.

Plasmon polaritons in topological insulators attract attention from a fundamental perspective and for potential THz photonic applications. Although polaritons have been observed by THz far-field spectroscopy on topological insulator microstructures, real-space imaging of propagating THz polaritons has been elusive so far. Here, we show spectroscopic THz near-field images of thin Bi2Se3 layers (prototypical topological insulators) revealing polaritons with up to 12 times increased momenta as compared to photons of the same energy and decay times of about 0.48 ps, yet short propagation lengths. From the images we determine and analyze the polariton dispersion, showing that the polaritons can be explained by the coupling of THz radiation to various combinations of Dirac and massive carriers at the Bi2Se3 surfaces, massive bulk carriers and optical phonons. Our work provides critical insights into the nature of THz polaritons in topological insulators and establishes instrumentation and methodology for imaging of THz polaritons.

Plasmon polaritons in topological insulators attract attention from a fundamental perspective and for potential THz photonic applications. Although polaritons have been observed by THz far-field spectroscopy on topological insulator microstructures, real-space imaging of propagating THz polaritons has been elusive so far. Here, we show spectroscopic THz near-field images of thin Bi

Refraction between isotropic media is characterized by light bending towards the normal to the boundary when passing from a low- to a high-refractive-index medium. However, refraction between anisotropic media is a more exotic phenomenon which remains barely investigated, particularly at the nanoscale. Here, we visualize and comprehensively study the general case of refraction of electromagnetic waves between two strongly anisotropic (hyperbolic) media, and we do it with the use of nanoscale-confined polaritons in a natural medium: α-MoO3. The refracted polaritons exhibit non-intuitive directions of propagation as they traverse planar nanoprisms, enabling to unveil an exotic optical effect: bending-free refraction. Furthermore, we develop an in-plane refractive hyperlens, yielding foci as small as λp/6, being λp the polariton wavelength (λ0/50 compared to the wavelength of free-space light). Our results set the grounds for planar nano-optics in strongly anisotropic media, with potential for effective control of the flow of energy at the nanoscale., G.Á.-P. and J.T.-G. acknowledge support through the Severo Ochoa Program from the Government of the Principality of Asturias (nos. PA-20-PF-BP19-053 and PA-18-PF-BP17-126, respectively). S.X. acknowledges the support from Independent Research Fund Denmark (Project No. 9041-00333B). B.C. acknowledges the support from VILLUM FONDEN (No. 00027987). The Center for Nanostructured Graphene is sponsored by the Danish National Research Foundation (Project No. DNRF103.) K.V.V. and V.S.V. gratefully acknowledge the financial support from the Ministry of Science and Higher Education of the Russian Federation (Agreement No. 075-15-2021-606). J.M.-S. acknowledges financial support through the Ramón y Cajal Program from the Government of Spain (RYC2018-026196-I). A.Y.N. and J.I.M. acknowledge the Spanish Ministry of Science, Innovation and Universities (national projects MAT201788358-C3-3-R and PID2019-104604RB/AEI/10.13039/501100011033). R.H. acknowledges financial support from the Spanish Ministry of Science, Innovation and Universities (national project RTI2018-094830-B-100 and the project MDM-2016-0618 of the Marie de Maeztu Units of Excellence Program) and the Basque Government (grant No. IT1164-19). A.Y.N. also acknowledges the Basque Department of Education (grant no. PIBA-2020-1-0014). 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).

Large optical anisotropy observed in a broad spectral range is of paramount importance for efficient light manipulation in countless devices. Although a giant anisotropy has been recently observed in the mid-infrared wavelength range, for visible and near-infrared spectral intervals, the problem remains acute with the highest reported birefringence values of 0.8 in BaTiS3 and h-BN crystals. This issue inspired an intensive search for giant optical anisotropy among natural and artificial materials. Here, we demonstrate that layered transition metal dichalcogenides (TMDCs) provide an answer to this quest owing to their fundamental differences between intralayer strong covalent bonding and weak interlayer van der Waals interaction. To do this, we made correlative far- and near-field characterizations validated by first-principle calculations that reveal a huge birefringence of 1.5 in the infrared and 3 in the visible light for MoS2. Our findings demonstrate that this remarkable anisotropy allows for tackling the diffraction limit enabling an avenue for on-chip next-generation photonics., We gratefully acknowledge financial support from the Ministry of Science and Higher Education of the Russian Federation (No. 0714-2020-0002) and the Russian Foundation for Basic Research (20-07-00475, 18-29-02089 and 20-07-00840). A.Y.N. acknowledges the Spanish Ministry of Science, Innovation and Universities (national project no. MAT201788358-C3-3-R) and the Basque Department of Education (grant PIBA-2020-1-0014). P.A-G. and J.D. acknowledge financial support from the European Research Council under Starting Grant 715496, 2DNANOPTICA. A.N.G., V.G.K. and K.S.N. acknowledges support from EU Graphene Flagship Core 3 (881603). K.S.N. also acknowledges support from EU Flagship Program 2D-SIPC Quantum Technology, European Research Council Synergy Grant Hetero2D, the Royal Society, EPSRC grants EP/N010345/1, EP/P026850/1, EP/S030719/1.

Phonon polaritons—light coupled to lattice vibrations—in polar van der Waals crystals are promising candidates for controlling the flow of energy on the nanoscale due to their strong field confinement, anisotropic propagation and ultra-long lifetime in the picosecond range1,2,3,4,5. However, the lack of tunability of their narrow and material-specific spectral range—the Reststrahlen band—severely limits their technological implementation. Here, we demonstrate that intercalation of Na atoms in the van der Waals semiconductor α-V2O5 enables a broad spectral shift of Reststrahlen bands, and that the phonon polaritons excited show ultra-low losses (lifetime of 4 ± 1 ps), similar to phonon polaritons in a non-intercalated crystal (lifetime of 6 ± 1 ps). We expect our intercalation method to be applicable to other van der Waals crystals, opening the door for the use of phonon polaritons in broad spectral bands in the mid-infrared domain., J.T.-G. and G.Á.-P. acknowledge support through the Severo Ochoa Program from the Government of the Principality of Asturias (nos. PA-18-PF-BP17-126 and PA-20-PF-BP19-053, respectively). J.M.-S. acknowledges finantial support from the Clarín Programme from the Government of the Principality of Asturias and a Marie Curie-COFUND grant (PA-18-ACB17-29) and the Ramón y Cajal Program from the Government of Spain (RYC2018-026196-I). K.C., X.P.A.G., H.V. and M.H.B. acknowledge the Air Force Office of Scientific Research (AFOSR) grant no. FA 9550-18-1-0030 for funding support. I.E. acknowledges financial support from the Spanish Ministry of Economy and Competitiveness (grant no. FIS2016-76617-P). A.Y.N. acknowledges the Spanish Ministry of Science, Innovation and Universities (national project no. MAT2017-88358-C3-3-R) and the Basque Government (grant no. IT1164-19). Q.B. acknowledges the support from Australian Research Council (grant nos. FT150100450, IH150100006 and CE170100039). R.H. acknowledges support from the Spanish Ministry of Economy, Industry, and Competitiveness (national project RTI2018-094830-B-100 and the Project MDM-2016-0618 of the María de Maeztu Units of Excellence Program) and the Basque Goverment (grant no. IT1164-19). P.A.-G. acknowledges support from the European Research Council under starting grant no. 715496, 2DNANOPTICA.

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.

Phonon polaritons in van der Waals materials can strongly enhance light–matter interactions at mid-infrared frequencies, owing to their extreme field confinement and long lifetimes1,2,3,4,5,6,7. Phonon polaritons thus bear potential for vibrational strong coupling with molecules. Although the onset of vibrational strong coupling was observed spectroscopically with phonon-polariton nanoresonators8, no experiments have resolved vibrational strong coupling in real space and with propagating modes. Here we demonstrate by nanoimaging that vibrational strong coupling can be achieved between propagating phonon polaritons in thin van der Waals crystals (hexagonal boron nitride) and molecular vibrations in adjacent thin molecular layers. We performed near-field polariton interferometry, showing that vibrational strong coupling leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict vibrational strong coupling for nanometre-thin molecular layers and phonon polaritons in few-layer van der Waals materials, which could make propagating phonon polaritons a promising platform for ultrasensitive on-chip spectroscopy and strong-coupling experiments., We acknowledge financial support from 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), the Basque Government (grant numbers IT1164-19 and PIBA-2020-1-0014) and the European Union’s Horizon 2020 research and innovation programme under the Graphene Flagship (grant agreement numbers 785219 and 881603, GrapheneCore2 and GrapheneCore3). F. Calavelle acknowledges support from the European Union H2020 under the Marie Skłodowska-Curie Actions (766025-QuESTech). J.T.-G. acknowledges support through the Severo Ochoa Program from the Government of the Principality of Asturias (number PA-18-PF-BP17-126). P.A.-G. acknowledges support from the European Research Council under starting grant number 715496, 2DNANOPTICA. 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 biaxial van der Waals semiconductor α-phase molybdenum trioxide (α-MoO

Phonon polaritons-light coupled to lattice vibrations-in polar van der Waals crystals are promising candidates for controlling the flow of energy on the nanoscale due to their strong field confinement, anisotropic propagation and ultra-long lifetime in the picosecond range

We experimentally study the gate-tunable terahertz plasmon resonance in large area grating-coupled CVD graphene. Despite moderate carrier mobility in CVD graphene (~103 cm2/V/s), the resonance is clearly distinguishable above the Drude absorption background in the 5-10 THz range. The optical scattering time governing the quality factor of plasmon resonance appears to be well above the dc relaxation time. We confirm this relation by simultaneous THz transmission and field-effect measurements. We also show that the presence of the grating coupler in close proximity to graphene modifies the plasmon spectra. The plasmon field becomes tightly bound below the metal stripes, while the frequency depends on the stripe length but not by grating period.

In present study, we introduce graphene field-effect transistors (G-FET) fabricated on silicon - silicon dioxide wafers and analyse their properties. Electric and photoelectric effects in these devices were experimentally observed and discussed. We demonstrate that the understanding of the processes occurring in the substrate is of high importance not only for the development of all types of photodetectors based on field-effect transistors, but also could be used for the designing of devices with novel functionalities.

We develop a theory of electron tunneling accompanied by carrier-carrier scattering in graphene - insulator - graphene heterostructures. Due to the dynamic screening of Coulomb interaction, the scattering-aided tunneling is resonantly enhanced if the transferred energy and momentum correspond to those of surface plasmons. We reveal the possible experimental manifestations of such plasmon-assisted tunneling in current-voltage curves and plasmon emission spectra of graphene-based tunnel junctions. We find that inelastic current and plasmon emission rates have sharp peaks at voltages providing equal energies, momenta and group velocities of plasmons and interlayer single-particle excitations. The strength of this resonance, which we call plasmaronic resonance, is limited by interlayer twist and plasmon lifetime. The onset of plasmon-assisted tunneling can be also marked by a cusp in the junction $I(V)$-curve at low temperatures, and the threshold voltage for such tunneling weakly depends on carrier density and persists in the presence of interlayer twist.

The biaxial van der Waals semiconductor α‐phase molybdenum trioxide (α‐MoO3) 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‐MoO3 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‐MoO3, 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‐MoO3 are provided., G.Á-P. and J.T.-G. acknowledge support through the Severo Ochoa Program from the I of the Principality of Asturias (grants No. PA-20-PF-BP19-053 and PA-18-PF-BP17-126, respectively). I.E. acknowledges support from the Spanish Ministry of Economy and Competitiveness (FIS2016-76617-P). J.M.-S. acknowledges support through a Clarín Marie Curie-COFUND grant from the Government of the Principality of Asturias and the EU (PA18-ACB17-29), and the Ramón y Cajal Program (RYC2018-026196-I) from the Government of Spain. Q. B. acknowledges support from Australian Research Council (ARC, FT150100450, IH150100006 and CE170100039). J.D.C. was supported by the National Science Foundation (U.S.A.) under grant number U0048926. A.Y.N. acknowledges the Spanish Ministry of Science, Innovation and Universities (national project MAT2017-88358-C3-3-R) and Basque Government (grant No. IT1164-19). P.A-G. acknowledges support from the European Research Council under Starting Grant 715496, 2DNANOPTICA.