Microcavity phonon polaritons from the weak to the ultrastrong phonon-photon coupling regime.

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.

Plasmonic antenna coupling to hyperbolic phonon-polaritons for sensitive and fast mid-infrared photodetection with graphene.

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 pn-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[Formula: see text]) 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.

Broad spectral tuning of ultra-low-loss polaritons in a van der Waals crystal by intercalation.

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 range1-5. 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.

Substrate Matters: Surface-Polariton Enhanced Infrared Nanospectroscopy of Molecular Vibrations.

Infrared nanospectroscopy based on Fourier transform infrared near-field spectroscopy (nano-FTIR) is an emerging nanoanalytical tool with large application potential for label-free mapping and identification of organic and inorganic materials with nanoscale spatial resolution. However, the detection of thin molecular layers and nanostructures on standard substrates is still challenged by weak signals. Here, we demonstrate a significant enhancement of nano-FTIR signals of a thin organic layer by exploiting polariton-resonant tip-substrate coupling and surface polariton illumination of the probing tip. When the molecular vibration matches the tip-substrate resonance, we achieve up to nearly one order of magnitude signal enhancement on a phonon-polaritonic quartz (c-SiO2) substrate, as compared to nano-FTIR spectra obtained on metal (Au) substrates, and up to two orders of magnitude when compared to the standard infrared spectroscopy substrate CaF2. Our results will be of critical importance for boosting nano-FTIR spectroscopy toward the routine detection of monolayers and single molecules.

Fast and Sensitive Terahertz Detection Using an Antenna-Integrated Graphene pn Junction.

Although the detection of light at terahertz (THz) frequencies is important for a large range of applications, current detectors typically have several disadvantages in terms of sensitivity, speed, operating temperature, and spectral range. Here, we use graphene as a photoactive material to overcome all of these limitations in one device. We introduce a novel detector for terahertz radiation that exploits the photothermoelectric (PTE) effect, based on a design that employs a dual-gated, dipolar antenna with a gap of ∼100 nm. This narrow-gap antenna simultaneously creates a pn junction in a graphene channel located above the antenna and strongly concentrates the incoming radiation at this pn junction, where the photoresponse is created. We demonstrate that this novel detector has an excellent sensitivity, with a noise-equivalent power of 80 pW/[Formula: see text] at room temperature, a response time below 30 ns (setup-limited), a high dynamic range (linear power dependence over more than 3 orders of magnitude) and broadband operation (measured range 1.8-4.2 THz, antenna-limited), which fulfills a combination that is currently missing in the state-of-the-art detectors. Importantly, on the basis of the agreement we obtained between experiment, analytical model, and numerical simulations, we have reached a solid understanding of how the PTE effect gives rise to a THz-induced photoresponse, which is very valuable for further detector optimization.

Boron nitride nanoresonators for phonon-enhanced molecular vibrational spectroscopy at the strong coupling limit.

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.

Tuning quantum nonlocal effects in graphene plasmonics.

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.

Terahertz and mid-infrared plasmons in three-dimensional nanoporous graphene.

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.

Topologically protected Dirac plasmons and their evolution across the quantum phase transition in a (Bi(1-x)In(x))2Se3 topological insulator.

A 3D Topological Insulator (TI) is an intrinsically stratified electronic material characterized by an insulating bulk and Dirac free electrons at the interface with vacuum or another dielectric. In this paper, we investigate, through terahertz (THz) spectroscopy, the plasmon excitation of Dirac electrons on thin films of (Bi1-xInx)2Se3 TI patterned in the form of a micro-ribbon array, across a Quantum Phase Transition (QPT) from the topological to a trivial insulating phase. The latter is achieved by In doping onto the Bi-site and is characterized by massive electrons at the surface. While the plasmon frequency is nearly independent of In content, the plasmon width undergoes a sudden broadening across the QPT, perfectly mirroring the single particle (free electron) behavior as measured on the same films. This strongly suggests that the topological protection from backscattering characterizing Dirac electrons in the topological phase extends also to their plasmon excitations.