High-quality nanocavities through multimodal confinement of hyperbolic polaritons in hexagonal boron nitride.

Compressing light into nanocavities substantially enhances light-matter interactions, which has been a major driver for nanostructured materials research. However, extreme confinement generally comes at the cost of absorption and low resonator quality factors. Here we suggest an alternative optical multimodal confinement mechanism, unlocking the potential of hyperbolic phonon polaritons in isotopically pure hexagonal boron nitride. We produce deep-subwavelength cavities and demonstrate several orders of magnitude improvement in confinement, with estimated Purcell factors exceeding 108 and quality factors in the 50-480 range, values approaching the intrinsic quality factor of hexagonal boron nitride polaritons. Intriguingly, the quality factors we obtain exceed the maximum predicted by impedance-mismatch considerations, indicating that confinement is boosted by higher-order modes. We expect that our multimodal approach to nanoscale polariton manipulation will have far-reaching implications for ultrastrong light-matter interactions, mid-infrared nonlinear optics and nanoscale sensors.

Experimental signatures of the transition from acoustic plasmon to electronic sound in graphene.

Fermi liquids respond differently to perturbations depending on whether their frequency is higher (collisionless regime) or lower (hydrodynamic regime) than the interparticle collision rate. This results in a different phase velocity between the collisionless zero sound and the hydrodynamic first sound. We performed terahertz photocurrent nanoscopy measurements on graphene devices, with a metallic gate close to the graphene layer, to probe the dispersion of propagating acoustic plasmons, the counterpart of sound modes in electronic Fermi liquids. We report the observation of a change in the plasmon phase velocity when the excitation frequency approaches the electron-electron collision rate that is compatible with the transition between the zero and the first sound mode.

Transverse Hypercrystals Formed by Periodically Modulated Phonon Polaritons.

Photonic crystals and metamaterials are two overarching paradigms for manipulating light. By combining these approaches, hypercrystals can be created, which are hyperbolic dispersion metamaterials that undergo periodic modulation and mix photonic-crystal-like aspects with hyperbolic dispersion physics. Despite several attempts, there has been limited experimental realization of hypercrystals due to technical and design constraints. In this work, hypercrystals with nanoscale lattice constants ranging from 25 to 160 nm were created. The Bloch modes of these crystals were then measured directly using scattering near-field microscopy. The dispersion of the Bloch modes was extracted from the frequency dependence of the Bloch modes, revealing a clear switch from positive to negative group velocity. Furthermore, spectral features specific to hypercrystals were observed in the form of sharp density of states peaks, which are a result of intermodal coupling and should not appear in ordinary polaritonic crystals with an equivalent geometry. These findings are in agreement with theoretical predictions that even simple lattices can exhibit a rich hypercrystal bandstructure. This work is of both fundamental and practical interest, providing insight into nanoscale light-matter interactions and the potential to manipulate the optical density of states.

Engineering high quality graphene superlattices via ion milled ultra-thin etching masks.

Nanofabrication research pursues the miniaturization of patterned feature size. In the current state of the art, micron scale areas can be patterned with features down to ~30 nm pitch using electron beam lithography. Here, we demonstrate a nanofabrication technique which allows patterning periodic structures with a pitch down to 16 nm. It is based on focused ion beam milling of suspended membranes, with minimal proximity effects typical to standard electron beam lithography. The membranes are then transferred and used as hard etching masks. We benchmark our technique by electrostatically inducing a superlattice potential in graphene and observe bandstructure modification in electronic transport. Our technique opens the path towards the realization of very short period superlattices in 2D materials, but with the ability to control lattice symmetries and strength. This can pave the way for a versatile solid-state quantum simulator platform and the study of correlated electron phases.

WSe2 as Transparent Top Gate for Infrared Near-Field Microscopy.

Independent control of carrier density and out-of-plane displacement field is essential for accessing novel phenomena in two-dimensional (2D) material heterostructures. While this is achieved with independent top and bottom metallic gate electrodes in transport experiments, it remains a challenge for near-field optical studies as the top electrode interferes with the optical path. Here, we characterize the requirements for a material to be used as the top-gate electrode and demonstrate experimentally that few-layer WSe2 can be used as a transparent, ambipolar top-gate electrode in infrared near-field microscopy. We carry out nanoimaging of plasmons in a bilayer graphene heterostructure tuning the plasmon wavelength using a trilayer WSe2 gate, achieving a density modulation amplitude exceeding 2 × 1012 cm-2. The observed ambipolar gate-voltage response allows us to extract the energy gap of WSe2, yielding a value of 1.05 eV. Our results provide an additional tuning knob to cryogenic near-field experiments on emerging phenomena in 2D materials and moiré heterostructures.

Tunable and giant valley-selective Hall effect in gapped bilayer graphene.

Berry curvature is analogous to magnetic field but in momentum space and is commonly present in materials with nontrivial quantum geometry. It endows Bloch electrons with transverse anomalous velocities to produce Hall-like currents even in the absence of a magnetic field. We report the direct observation of in situ tunable valley-selective Hall effect (VSHE), where inversion symmetry, and thus the geometric phase of electrons, is controllable by an out-of-plane electric field. We use high-quality bilayer graphene with an intrinsic and tunable bandgap, illuminated by circularly polarized midinfrared light, and confirm that the observed Hall voltage arises from an optically induced valley population. Compared with molybdenum disulfide (MoS2), we find orders of magnitude larger VSHE, attributed to the inverse scaling of the Berry curvature with bandgap. By monitoring the valley-selective Hall conductivity, we study the Berry curvature's evolution with bandgap. This in situ manipulation of VSHE paves the way for topological and quantum geometric optoelectronic devices, such as more robust switches and detectors.

Nano-imaging photoresponse in a moiré unit cell of minimally twisted bilayer graphene.

Graphene-based moiré superlattices have recently emerged as a unique class of tuneable solid-state systems that exhibit significant optoelectronic activity. Local probing at length scales of the superlattice should provide deeper insight into the microscopic mechanisms of photoresponse and the exact role of the moiré lattice. Here, we employ a nanoscale probe to study photoresponse within a single moiré unit cell of minimally twisted bilayer graphene. Our measurements reveal a spatially rich photoresponse, whose sign and magnitude are governed by the fine structure of the moiré lattice and its orientation with respect to measurement contacts. This results in a strong directional effect and a striking spatial dependence of the gate-voltage response within the moiré domains. The spatial profile and carrier-density dependence of the measured photocurrent point towards a photo-thermoelectric induced response that is further corroborated by good agreement with numerical simulations. Our work shows sub-diffraction photocurrent spectroscopy is an exceptional tool for uncovering the optoelectronic properties of moiré superlattices.

Graphene-Quantum Dot Hybrid Photodetectors with Low Dark-Current Readout.

Graphene-based photodetectors have shown responsivities up to 108 A/W and photoconductive gains up to 108 electrons per photon. These photodetectors rely on a highly absorbing layer in close proximity to graphene, which induces a shift of the graphene chemical potential upon absorption, hence modifying its channel resistance. However, due to the semimetallic nature of graphene, the readout requires dark currents of hundreds of microamperes up to milliamperes, leading to high power consumption needed for the device operation. Here, we propose a different approach for highly responsive graphene-based photodetectors with orders of magnitude lower dark-current levels. A shift of the graphene chemical potential caused by light absorption in a layer of colloidal quantum dots induces a variation of the current flowing across a metal-insulator-graphene diode structure. Owing to the low density of states of graphene near the neutrality point, the light-induced shift in chemical potential can be relatively large, dramatically changing the amount of current flowing across the insulating barrier and giving rise to an alternative gain mechanism. This readout requires dark currents of hundreds of nanoamperes up to a few microamperes, orders of magnitude lower than that of other graphene-based photodetectors, while keeping responsivities of ∼70 A/W in the infrared, almost 2 orders of magnitude higher than that of established germanium on silicon and indium gallium arsenide infrared photodetectors. This makes the device appealing for applications where high responsivity and low power consumption are required.

Mid- and Long-Wave Infrared Optoelectronics via Intraband Transitions in PbS Colloidal Quantum Dots.

Optical sensing in the mid- and long-wave infrared (MWIR, LWIR) is of paramount importance for a large spectrum of applications including environmental monitoring, gas sensing, hazard detection, food and product manufacturing inspection, and so forth. Yet, such applications to date are served by costly and complex epitaxially grown HgCdTe quantum-well and quantum-dot infrared photodetectors. The possibility of exploiting low-energy intraband transitions make colloidal quantum dots (CQD) an attractive low-cost alternative to expensive low bandgap materials for infrared applications. Unfortunately, fabrication of quantum dots exhibiting intraband absorption is technologically constrained by the requirement of controlled heavy doping, which has limited, so far, MWIR and LWIR CQD detectors to mercury-based materials. Here, we demonstrate intraband absorption and photodetection in heavily doped PbS colloidal quantum dots in the 5-9 µm range, beyond the PbS bulk band gap, with responsivities on the order of 10-4 A/W at 80 K. We have further developed a model based on quantum transport equations to understand the impact of electron population of the conduction band in the performance of intraband photodetectors and offer guidelines toward further performance improvement.

Nonlinear Light Mixing by Graphene Plasmons.

Graphene is known to possess strong optical nonlinearity which turned out to be suitable for creation of efficient saturable absorbers in mode locked fiber lasers. Nonlinear response of graphene can be further enhanced by the presence of graphene plasmons. Here, we report a novel nonlinear effect observed in nanostructured graphene which comes about due to excitation of graphene plasmons. We experimentally detect and theoretically explain enhanced mixing of near-infrared and mid-infrared light in arrays of graphene nanoribbons. Strong compression of light by graphene plasmons implies that the described effect of light mixing is nonlocal in nature and orders of magnitude larger than the conventional local graphene nonlinearity. Both second and third order nonlinear effects were observed in our experiments with the recalculated third-order nonlinearity coefficient reaching values of 4.5 × 10-6 esu. The suggested effect could be used in variety of applications including nonlinear light modulators, light multiplexers, light logic, and sensing devices.