Spatiotemporal imaging of nonlinear optics in van der Waals waveguides.

Van der Waals (vdW) semiconductors have emerged as promising platforms for efficient nonlinear optical conversion, including harmonic and entangled photon generation. Although major efforts are devoted to integrating vdW materials in nanoscale waveguides for miniaturization, the realization of efficient, phase-matched conversion in these platforms remains challenging. Here, to address this challenge, we report a far-field ultrafast imaging method to track the propagation of both fundamental and harmonic waves within vdW waveguides with femtosecond and sub-50 nanometre spatiotemporal precision.

Electronic interactions in Dirac fluids visualized by nano-terahertz spacetime interference of electron-photon quasiparticles.

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here, we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering.

Quenched Excitons in WSe/α-RuCl Heterostructures Revealed by Multimessenger Nanoscopy.

We investigate heterostructures composed of monolayer WSe stacked on α-RuCl using a combination of Terahertz (THz) and infrared (IR) nanospectroscopy and imaging, scanning tunneling spectroscopy (STS), and photoluminescence (PL). Our observations reveal itinerant carriers in the heterostructure prompted by charge transfer across the WSe/α-RuCl interface. Local STS measurements show the Fermi level is shifted to the valence band edge of WSe which is consistent with p-type doping and verified by density functional theory (DFT) calculations.

Ambipolar charge-transfer graphene plasmonic cavities.

Plasmon polaritons in van der Waals materials hold promise for various photonics applications. The deterministic imprinting of spatial patterns of high carrier density in plasmonic cavities and nanoscale circuitry can enable the realization of advanced nonlinear nanophotonic and strong light-matter interaction platforms. Here we demonstrate an oxidation-activated charge transfer strategy to program ambipolar low-loss graphene plasmonic structures.

Infrared plasmons propagate through a hyperbolic nodal metal.

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nanoscale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors, and artificial metamaterials.

Nanoscale Femtosecond Dynamics of Mott Insulator (CaSr)RuO.

CaRuO is a transition-metal oxide that exhibits a Mott insulator-metal transition (IMT) concurrent with a symmetry-preserving Jahn-Teller distortion (JT) at 350 K. The coincidence of these two transitions demonstrates a high level of coupling between the electronic and structural degrees of freedom in CaRuO. Using spectroscopic measurements with nanoscale spatial resolution, we interrogate the interplay of the JT and IMT through the temperature-driven transition.

Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides.

Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse control knobs, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task.

Nanotextured Dynamics of a Light-Induced Phase Transition in VO.

We investigate transient nanotextured heterogeneity in vanadium dioxide (VO) thin films during a light-induced insulator-to-metal transition (IMT). Time-resolved scanning near-field optical microscopy (Tr-SNOM) is used to study VO across a wide parameter space of infrared frequencies, picosecond time scales, and elevated steady-state temperatures with nanoscale spatial resolution. Room temperature, steady-state, phonon enhanced nano-optical contrast reveals preexisting "hidden" disorder.

Quantitative Nanoinfrared Spectroscopy of Anisotropic van der Waals Materials.

Anisotropic dielectric tensors of uniaxial van der Waals (vdW) materials are difficult to investigate at infrared frequencies. The small dimensions of high-quality exfoliated crystals prevent the use of diffraction-limited spectroscopies. Near-field microscopes coupled to broadband lasers can function as Fourier transform infrared spectrometers with nanometric spatial resolution (nano-FTIR).

Femtosecond exciton dynamics in WSe optical waveguides.

Van-der Waals (vdW) atomically layered crystals can act as optical waveguides over a broad range of the electromagnetic spectrum ranging from Terahertz to visible. Unlike common Si-based waveguides, vdW semiconductors host strong excitonic resonances that may be controlled using non-thermal stimuli including electrostatic gating and photoexcitation. Here, we utilize waveguide modes to examine photo-induced changes of excitons in the prototypical vdW semiconductor, WSe, prompted by femtosecond light pulses.

Nano-photocurrent Mapping of Local Electronic Structure in Twisted Bilayer Graphene.

We report a combined nano-photocurrent and infrared nanoscopy study of twisted bilayer graphene (TBG) enabling access to the local electronic phenomena at length scales as short as 20 nm. We show that the photocurrent changes sign at carrier densities tracking the local superlattice density of states of TBG. We use this property to identify domains of varying local twist angle by local photothermoelectric effect.

Nanoscale electrodynamics of strongly correlated quantum materials.

Electronic, magnetic, and structural phase inhomogeneities are ubiquitous in strongly correlated quantum materials. The characteristic length scales of the phase inhomogeneities can range from atomic to mesoscopic, depending on their microscopic origins as well as various sample dependent factors. Therefore, progress with the understanding of correlated phenomena critically depends on the experimental techniques suitable to provide appropriate spatial resolution.

Nonlinear terahertz metamaterials via field-enhanced carrier dynamics in GaAs.

We demonstrate nonlinear metamaterial split ring resonators (SRRs) on GaAs at terahertz frequencies. For SRRs on doped GaAs films, incident terahertz radiation with peak fields of ~20-160 kV/cm drives intervalley scattering. This reduces the carrier mobility and enhances the SRR LC response due to a conductivity decrease in the doped thin film.

Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial.

Electron-electron interactions can render an otherwise conducting material insulating, with the insulator-metal phase transition in correlated-electron materials being the canonical macroscopic manifestation of the competition between charge-carrier itinerancy and localization. The transition can arise from underlying microscopic interactions among the charge, lattice, orbital and spin degrees of freedom, the complexity of which leads to multiple phase-transition pathways. For example, in many transition metal oxides, the insulator-metal transition has been achieved with external stimuli, including temperature, light, electric field, mechanical strain or magnetic field.