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Abstract The electronic and optical properties of 2D transition metal dichalcogenides are dominated by strong excitonic resonances. Exciton dynamics plays a critical role in the functionality and performance of many miniaturized 2D optoelectronic devices; however, the measurement of nanoscale excitonic behaviors remains challenging. Here, a near‐field transient nanoscopy is reported to probe exciton dynamics beyond the diffraction limit. Exciton recombination and exciton–exciton annihilation processes in monolayer and bilayer MoS₂are studied as the proof‐of‐concept demonstration. Moreover, with the capability to access local sites, intriguing exciton dynamics near the monolayer‐bilayer interface and at the MoS₂nano‐wrinkles are resolved. Such nanoscale resolution highlights the potential of this transient nanoscopy for fundamental investigation of exciton physics and further optimization of functional devices. 

Abstract Element isotopes are characterized by distinct atomic masses and nuclear spins, which can significantly influence material properties. Notably, however, isotopes in natural materials are homogenously distributed in space. Here, we propose a method to configure material properties by repositioning isotopes in engineered van der Waals (vdW) isotopic heterostructures. We showcase the properties of hexagonal boron nitride (hBN) isotopic heterostructures in engineering confined photon-lattice waves—hyperbolic phonon polaritons. By varying the composition, stacking order, and thicknesses of h¹⁰BN and h¹¹BN building blocks, hyperbolic phonon polaritons can be engineered into a variety of energy-momentum dispersions. These confined and tailored polaritons are promising for various nanophotonic and thermal functionalities. Due to the universality and importance of isotopes, our vdW isotope heterostructuring method can be applied to engineer the properties of a broad range of materials. 

The mid‐infrared with a characteristic wavelength of 3–20 μm is important for a wealth of technologies. In particular, mid‐infrared spectroscopy can reveal material composition and structure information by fingerprinting chemical bonds’ infrared resonances. Despite these merits, state‐of‐the‐art mid‐infrared techniques are spatially limited above tens of micrometers due to the fundamental diffraction law. Herein, recent progress in the scanning probe nanoscale infrared characterization of biochemical materials and natural specimens beyond this spatial limitation is reviewed. By leveraging the strong tip–sample local interactions, scanning probe nano‐infrared methods probe nanoscale optical and mechanical responses to disclose material composition, heterogeneity, orientation, fine structure, and phase transitions at unprecedented length scales. These advances, therefore, revolutionize the understanding of a broad range of biochemical and natural materials and offer new material manipulation and engineering opportunities close to the ultimate length scales of fundamental physical, chemical, and biological processes. 

Polar van der Waals (vdW) crystals, composed of atomic layers held together by vdW forces, can host phonon polaritons—quasiparticles arising from the interaction between photons in free-space light and lattice vibrations in polar materials. These crystals offer advantages such as easy fabrication, low Ohmic loss, and optical confinement. Recently, hexagonal boron nitride (hBN), known for having hyperbolicity in the mid-infrared range, has been used to explore multiple modes with high optical confinement. This opens possibilities for practical polaritonic nanodevices with subdiffractional resolution. However, polariton waves still face exposure to the surrounding environment, leading to significant energy losses. In this work, we propose a simple approach to inducing a hyperbolic phonon polariton (HPhP) waveguide in hBN by incorporating a low dielectric medium, ZrS2. The low dielectric medium serves a dual purpose—it acts as a pathway for polariton propagation, while inducing high optical confinement. We establish the criteria for the HPhP waveguide in vdW heterostructures with various thicknesses of ZrS2 through scattering-type scanning near-field optical microscopy (s-SNOM) and by conducting numerical electromagnetic simulations. Our work presents a feasible and straightforward method for developing practical nanophotonic devices with low optical loss and high confinement, with potential applications such as energy transfer, nano-optical integrated circuits, light trapping, etc. 

Charge transfer is a fundamental interface process that can be harnessed for light detection, photovoltaics, and photosynthesis. Recently, charge transfer was exploited in nanophotonics to alter plasmon polaritons by involving additional non-polaritonic materials to activate the charge transfer. Yet, direct charge transfer between polaritonic materials has not been demonstrated. We report the direct charge transfer in pure polaritonic van der Waals (vdW) heterostructures of α-MoO3/graphene. We extracted the Fermi energy of 0.6 eV for graphene by infrared nano-imaging of charge transfer hyperbolic polaritons in the vdW heterostructure. This unusually high Fermi energy is attributed to the charge transfer between graphene and α-MoO3. Moreover, we have observed charge transfer hyperbolic polaritons in multiple energy–momentum dispersion branches with a wavelength elongation of up to 150%. With the support from the density functional theory calculation, we find that the charge transfer between graphene and α-MoO3, absent in mechanically assembled vdW heterostructures, is attributed to the relatively pristine heterointerface preserved in the epitaxially grown vdW heterostructure. The direct charge transfer and charge transfer hyperbolic polaritons demonstrated in our work hold great promise for developing nano-optical circuits, computational devices, communication systems, and light and energy manipulation devices. 

The wave nature of light sets a fundamental diffraction limit that challenges confinement and control of light in nanoscale structures with dimensions significantly smaller than the wavelength. Here, we study light–matter interaction in van der Waals MoS₂nanophotonic devices. We show that light can be coupled and guided in structures with dimensions as small as ≃λ/16 (∼60nm at 1000 nm excitation wavelength), while offering unprecedented optical field confinement. This deep subwavelength optical field confinement is achieved by exploiting strong lightwave dispersion in MoS₂. We further study the performance of a range of nanophotonic integrated devices via far- and near-field measurements. Our near-field measurements reveal detailed imaging of excitation, evolution, and guidance of fields in nanostructured MoS₂, whereas our far-field study examines light excitation and coupling to highly confined integrated photonics. Nanophotonics at a fraction of a wavelength demonstrated here could dramatically reduce the size of integrated photonic devices and opto-electronic circuits with potential applications in optical information science and engineering.