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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 lifetimes1–7. 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.Real-space mid-infrared nanoimaging reveals vibrational strong coupling between molecules and propagating phonon polaritons in unstructured, thin hexagonal boron nitride layers, which could provide a platform for testing strong coupling and local control of chemical properties.

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 1 – 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-V 2 O 5 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. The spectral range of long-lived and confined phonon polaritons in a polar van der Waals crystal is shown to be tunable by intercalation of Na atoms, expanding their potential for nanophotonic applications in the mid-infrared domain.

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.

Integrating and manipulating the nano-optoelectronic properties of Van der Waals heterostructures can enable unprecedented platforms for photodetection and sensing. The main challenge of infrared photodetectors is to funnel the light into a small nanoscale active area and efficiently convert it into an electrical signal. Here, we overcome all of those challenges in one device, by efficient coupling of a plasmonic antenna to hyperbolic phonon-polaritons in hexagonal-BN to highly concentrate mid-infrared light into a graphene p n -junction. We balance the interplay of the absorption, electrical and thermal conductivity of graphene via the device geometry. This approach yields remarkable device performance featuring room temperature high sensitivity (NEP of 82 pW / Hz ) and fast rise time of 17 nanoseconds (setup-limited), among others, hence achieving a combination currently not present in the state-of-the-art graphene and commercial mid-infrared detectors. We also develop a multiphysics model that shows very good quantitative agreement with our experimental results and reveals the different contributions to our photoresponse, thus paving the way for further improvement of these types of photodetectors even beyond mid-infrared range. A significant challenge of infrared (IR) photodetectors is to funnel light into a small nanoscale active area and efficiently convert it into an electrical signal. Here, the authors couple a plasmonic antenna to hyperbolic phonon-polaritons in hexagonal-BN to highly concentrate mid-IR light into a graphene pn-junction.

Strong coupling between molecular vibrations and microcavity modes has been demonstrated to modify physical and chemical properties of the molecular material. Here, we study the less explored coupling between lattice vibrations (phonons) and microcavity modes. Embedding thin layers of hexagonal boron nitride (hBN) into classical microcavities, we demonstrate the evolution from weak to ultrastrong phonon-photon coupling when the hBN thickness is increased from a few nanometers to a fully filled cavity. Remarkably, strong coupling is achieved for hBN layers as thin as 10 nm. Further, the ultrastrong coupling in fully filled cavities yields a polariton dispersion matching that of phonon polaritons in bulk hBN, highlighting that the maximum light-matter coupling in microcavities is limited to the coupling strength between photons and the bulk material. Tunable cavity phonon polaritons could become a versatile platform for studying how the coupling strength between photons and phonons may modify the properties of polar crystals. Strong coupling between light and matter can be engineered to influence their properties and behaviour. Here, the authors demonstrate the evolution from weak to ultrastrong coupling of microcavity modes and optical phonons with hexagonal boron nitride layers in a Fabry-Perot resonator.

Two-dimensional (2D) graphene emerged as an outstanding material for plasmonic and photonic applications due to its charge-density tunability, high electron mobility, optical transparency and mechanical flexibility. Recently, novel fabrication processes have realised a three-dimensional (3D) nanoporous configuration of high-quality monolayer graphene which provides a third dimension to this material. In this work, we investigate the optical behaviour of nanoporous graphene by means of terahertz and infrared spectroscopy. We reveal the presence of intrinsic 2D Dirac plasmons in 3D nanoporous graphene disclosing strong plasmonic absorptions tunable from terahertz to mid-infrared via controllable doping level and porosity. In the far-field the spectral width of these absorptions is large enough to cover most of the mid-Infrared fingerprint region with a single plasmon excitation. The enhanced surface area of nanoporous structures combined with their broad band plasmon absorption could pave the way for novel and competitive nanoporous-graphene based plasmonic-sensors. Recently, fabrication processes have realised three-dimensional nanoporous graphene. Here, the authors reveal two-dimensional Dirac plasmons in three-dimensional nanoporous graphene disclosing strong plasmonic absorptions tunable from terahertz to mid-infrared via controllable doping level and porosity.

Phonon polaritons – quasiparticles formed by strong coupling of infrared (IR) light with lattice vibrations in polar materials – can be utilized for surface-enhanced infrared absorption (SEIRA) spectroscopy and even for vibrational strong coupling with nanoscale amounts of molecules. Here, we introduce and demonstrate a compact on-chip phononic SEIRA spectroscopy platform, which is based on an h-BN/graphene/h-BN heterostructure on top of a metal split-gate creating a p-n junction in graphene. The metal split-gate concentrates the incident light and launches hyperbolic phonon polaritons (HPhPs) in the heterostructure, which serves simultaneously as SEIRA substrate and room-temperature infrared detector. When thin organic layers are deposited directly on top of the heterostructure, we observe a photocurrent encoding the layer’s molecular vibrational fingerprint, which is strongly enhanced compared to that observed in standard far-field absorption spectroscopy. A detailed theoretical analysis supports our results, further predicting an additional sensitivity enhancement as the molecular layers approach deep subwavelength scales. Future on-chip integration of infrared light sources such as quantum cascade lasers or even electrical generation of the HPhPs could lead to fully on-chip phononic SEIRA sensors for molecular and gas sensing. Phonon polaritons can be harnessed for SEIRA spectroscopy. Here, the authors demonstrate a compact on-chip phononic SEIRA platform based on a h-BN/graphene/h-BN heterostructure atop a metal split-gate that serves both as a SEIRA substrate and as a room-temperature infrared detector.

Far-field photons can be coupled to acoustic graphene plasmons with near 100% efficiency and used to acquire infrared spectra of thin, subnanometre-layer samples.

The response of electron systems to electrodynamic fields that change rapidly in space is endowed by unique features, including an exquisite spatial nonlocality. This can reveal much about the materials’ electronic structure that is invisible in standard probes that use gradually varying fields. Here, we use graphene plasmons, propagating at extremely slow velocities close to the electron Fermi velocity, to probe the nonlocal response of the graphene electron liquid. The near-field imaging experiments reveal a parameter-free match with the full quantum description of the massless Dirac electron gas, which involves three types of nonlocal quantum effects: single-particle velocity matching, interaction-enhanced Fermi velocity, and interaction-reduced compressibility. Our experimental approach can determine the full spatiotemporal response of an electron system.

A Correction to this paper has been published: https://doi.org/10.1038/s41566-020-00746-y