Nonlinear Nano-Imaging of Interlayer Coupling in 2D Graphene-Semiconductor Heterostructures.

The emergent electronic, spin, and other quantum properties of 2D heterostructures of graphene and transition metal dichalcogenides are controlled by the underlying interlayer coupling and associated charge and energy transfer dynamics. However, these processes are sensitive to interlayer distance and crystallographic orientation, which are in turn affected by defects, grain boundaries, or other nanoscale heterogeneities. This obfuscates the distinction between interlayer charge and energy transfer. Here, nanoscale imaging in coherent four-wave mixing (FWM) and incoherent two-photon photoluminescence (2PPL) is combined with a tip distance-dependent coupled rate equation model to resolve the underlying intra- and inter-layer dynamics while avoiding the influence of structural heterogeneities in mono- to multi-layer graphene/WSe2 heterostructures. With selective insertion of hBN spacer layers, it is shown that energy, as opposed to charge transfer, dominates the interlayer-coupled optical response. From the distinct nano-FWM and -2PPL tip-sample distance-dependent modification of interlayer and intralayer relaxation by tip-induced enhancement and quenching, an interlayer energy transfer time of τ ET ≈ ( 0 . 35 - 0.15 + 0.65 ) $\tau _{\rm ET} \approx (0.35^{+0.65}_{-0.15})$  ps consistent with recent reports is derived. As a local probe technique, this approach highlights the ability to determine intrinsic sample properties even in the presence of large sample heterogeneity.

Gate-Tuning Hybrid Polaritons in Twisted α-MoO3/Graphene Heterostructures.

Modulating anisotropic phonon polaritons (PhPs) can open new avenues in infrared nanophotonics. Promising PhP dispersion engineering through polariton hybridization has been demonstrated by coupling gated graphene to single-layer α-MoO3. However, the mechanism underlying the gate-dependent modulation of hybridization has remained elusive. Here, using IR nanospectroscopic imaging, we demonstrate active modulation of the optical response function, quantified in measurements of gate dependence of wavelength, amplitude, and dissipation rate of the hybrid plasmon-phonon polaritons (HPPPs) in both single-layer and twisted bilayer α-MoO3/graphene heterostructures. Intriguingly, while graphene doping leads to a monotonic increase in HPPP wavelength, amplitude and dissipation rate show transition from an initially anticorrelated decrease to a correlated increase. We attribute this behavior to the intricate interplay of gate-dependent components of the HPPP complex momentum. Our results provide the foundation for active polariton control of integrated α-MoO3 nanophotonics devices.