Dual-Band Coupling of Phonon and Surface Plasmon Polaritons with Vibrational and Electronic Excitations in Molecules.

Strong coupling (SC) between light and matter excitations bears intriguing potential for manipulating material properties. Typically, SC has been achieved between mid-infrared (mid-IR) light and molecular vibrations or between visible light and excitons. However, simultaneously achieving SC in both frequency bands remains unexplored. Here, we introduce polaritonic nanoresonators (formed by h-BN layers on Al ribbons) hosting surface plasmon polaritons (SPPs) at visible frequencies and phonon polaritons (PhPs) at mid-IR frequencies, which simultaneously couple to excitons and molecular vibrations in an adjacent layer of CoPc molecules, respectively. Employing near-field optical nanoscopy, we demonstrate the colocalization of near fields at both visible and mid-IR frequencies. Far-field transmission spectroscopy of the nanoresonator structure covered with a layer of CoPc molecules shows clear mode splittings in both frequency ranges, revealing simultaneous SPP-exciton and PhP-vibron coupling. Dual-band SC may offer potential for manipulating coupling between exciton and molecular vibration in future optoelectronics, nanophotonics, and quantum information applications.

Tailoring Photoluminescence by Strain-Engineering in Layered Perovskite Flakes.

Strain is an effective strategy to modulate the optoelectronic properties of 2D materials, but it has been almost unexplored in layered hybrid organic-inorganic metal halide perovskites (HOIPs) due to their complex band structure and mechanical properties. Here, we investigate the temperature-dependent microphotoluminescence (PL) of 2D (C6H5CH2CH2NH3)2Cs3Pb4Br13 HOIP subject to biaxial strain induced by a SiO2 ring platform on which flakes are placed by viscoelastic stamping. At 80 K, we found that a strain of <1% can change the PL emission from a single peak (unstrained) to three well-resolved peaks. Supported by micro-Raman spectroscopy, we show that the thermomechanically generated strain modulates the bandgap due to changes in the octahedral tilting and lattice expansion. Mechanical simulations demonstrate the coexistence of tensile and compressive strain along the flake. The observed PL peaks add an interesting feature to the rich phenomenology of photoluminescence in 2D HOIPs, which can be exploited in tailored sensing and optoelectronic devices.

Coherent Phononics of van der Waals Layers on Nanogratings.

Strain engineering can be used to control the physical properties of two-dimensional van der Waals (2D-vdW) crystals. Coherent phonons, which carry dynamical strain, could push strain engineering to control classical and quantum phenomena in the unexplored picosecond temporal and nanometer spatial regimes. This intriguing approach requires the use of coherent GHz and sub-THz 2D phonons. Here, we report on nanostructures that combine nanometer thick vdW layers and nanogratings. Using an ultrafast pump-probe technique, we generate and detect in-plane coherent phonons with frequency up to 40 GHz and hybrid flexural phonons with frequency up to 10 GHz. The latter arises from the periodic modulation of the elastic coupling of the vdW layer at the grooves and ridges of the nanograting. This creates a new type of a tailorable 2D periodic phononic nanoobject, a flexural phononic crystal, offering exciting prospects for the ultrafast manipulation of states in 2D materials in emerging quantum technologies.

Near- and Far-Field Observation of Phonon Polaritons in Wafer-Scale Multilayer Hexagonal Boron Nitride Prepared by Chemical Vapor Deposition.

Polaritons in layered materials (LMs) are a promising platform to manipulate and control light at the nanometer scale. Thus, the observation of polaritons in wafer-scale LMs is critically important for the development of industrially relevant nanophotonics and optoelectronics applications. In this work, phonon polaritons (PhPs) in wafer-scale multilayer hexagonal boron nitride (hBN) grown by chemical vapor deposition are reported. By infrared nanoimaging, the PhPs are visualized, and PhP lifetimes of ≈0.6 ps are measured, comparable to that of micromechanically exfoliated multilayer hBN. Further, PhP nanoresonators are demonstrated. Their quality factors of ≈50 are about 0.7 times that of state-of-the-art devices based on exfoliated hBN. These results can enable PhP-based surface-enhanced infrared spectroscopy (e.g., for gas sensing) and infrared photodetector applications.

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.