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Quasi-periodic moiré patterns and their effect on electronic properties of twisted bilayer graphene have been intensely studied. At small twist angle θ, due to atomic reconstruction, the moiré superlattice morphs into a network of narrow domain walls separating micron-scale AB and BA stacking regions. We use scanning probe photocurrent imaging to resolve nanoscale variations of the Seebeck coefficient occurring at these domain walls. The observed features become enhanced in a range of mid-infrared frequencies where the hexagonal boron nitride substrate is optically hyperbolic. Our results illustrate the capabilities of the nano-photocurrent technique for probing nanoscale electronic inhomogeneities in two-dimensional materials., Here, the authors use scanning probe photocurrent imaging to resolve nanoscale variations of the Seebeck coefficient occurring at domain walls separating micron-scale AB and BA stacking regions in twisted bilayer graphene, and observe hyperbolic enhancement of the photocurrent pattern.

Significance Micrometer-sized uniform four-layer (ABCA) rhombohedral graphene is realized by introducing a small twist angle between two bilayers of Bernal graphene. By means of scanning tunneling spectroscopy we observe an extremely sharp van Hove singularity of 3–5-meV half-width and a correlated many-body gap of 9.5 meV at neutrality, thus making small twisted double-bilayer graphene a unique platform to realize electronic correlations in the absence of a moiré potential. Furthermore, ABCA graphene domain walls display tunable topological edge states, of great interest in Floquet engineering., Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene––a simple material that also exhibits a flat electronic band edge but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3–5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.

Dragging of light by moving dielectrics was predicted by Fresnel and verified by Fizeau's celebrated experiments with flowing water. This momentous discovery is among the experimental cornerstones of Einstein's special relativity and is well understood in the context of relativistic kinematics. In contrast, experiments on dragging photons by an electron flow in solids are riddled with inconsistencies and so far eluded agreement with the theory. Here we report on the electron flow dragging surface plasmon polaritons (SPPs): hybrid quasiparticles of infrared photons and electrons in graphene. The drag is visualized directly through infrared nano-imaging of propagating plasmonic waves in the presence of a high-density current. The polaritons in graphene shorten their wavelength when launched against the drifting carriers. Unlike the Fizeau effect for light, the SPP drag by electrical currents defies the simple kinematics interpretation and is linked to the nonlinear electrodynamics of the Dirac electrons in graphene. The observed plasmonic Fizeau drag enables breaking of time-reversal symmetry and reciprocity at infrared frequencies without resorting to magnetic fields or chiral optical pumping., Comment: 11 pages, 3 figures

Moiré superlattices in van der Waals heterostructures have given rise to a number of emergent electronic phenomena due to the interplay between atomic structure and electron correlations. Indeed, electrons in these structures have been recently found to exhibit a number of emergent properties that the individual layers themselves do not exhibit. This includes superconductivity1,2, magnetism3, topological edge states4,5, exciton trapping6 and correlated insulator phases7. However, the lack of a straightforward technique to characterize the local structure of moiré superlattices has thus far impeded progress in the field. In this work we describe a simple, room-temperature, ambient method to visualize real-space moiré superlattices with sub-5-nm spatial resolution in a variety of twisted van der Waals heterostructures including, but not limited to, conducting graphene, insulating boron nitride and semiconducting transition metal dichalcogenides. Our method uses piezoresponse force microscopy, an atomic force microscope modality that locally measures electromechanical surface deformation. We find that all moiré superlattices, regardless of whether the constituent layers have inversion symmetry, exhibit a mechanical response to out-of-plane electric fields. This response is closely tied to flexoelectricity wherein electric polarization and electromechanical response is induced through strain gradients present within moiré superlattices. Therefore, moiré superlattices of two-dimensional materials manifest themselves as an interlinked network of polarized domain walls in a non-polar background matrix., This work is supported by the Programmable Quantum Materials (Pro-QM) programme at Columbia University, an Energy Frontier Research Center established by the Department of Energy (grant no. DE-SC0019443). L.J.M. acknowledges support from the Swiss National Science Foundation (grant no. P400P2_186744). Synthesis of MoSe2 and WSe2 was supported by the National Science Foundation Materials Research Science and Engineering Centers programme through Columbia in the Center for Precision Assembly of Superstratic and Superatomic Solids (DMR-1420634). The Flatiron Institute is a division of the Simons Foundation. C.E.D. acknowledges support from the National Science Foundation under grant no. DMR-1918455. M.S. and K.S. acknowledge the support of the European Research Council under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 724529), Ministerio de Economia, Industria y Competitividad through grant nos. MAT2016-77100-C2-2-P and SEV-2015-0496, and the Generalitat de Catalunya (grant no. 2017SGR 1506). We thank D. Griffin and T. Walsh from Oxford Instruments Asylum Research for confirmation of PFM results.

In this talk I will overview recent efforts to discover, characterize and deploy new forms of quantum matter controllable by light, gating, and nano-mechanical manipulation, effectively programming their properties 1. I will focus on enticing opportunities to investigate novel quantum phenomena using nascent nano-optical methods developed in our group 2, 3.

Two dimensional materials such as graphene and transition metal dichalcogenides (TMDs) are promising for optical modulation, detection, and light emission since their material properties can be tuned on-demand via electrostatic doping. The optical properties of TMDs have been shown to change drastically with doping in the wavelength range near the excitonic resonances. However, little is known about the effect of doping on the optical properties of TMDs away from these resonances, where the material is transparent and therefore could be leveraged in photonic circuits. Here, we probe the electro-optic response of monolayer TMDs at near infrared (NIR) wavelengths (i.e. deep in the transparency regime), by integrating them on silicon nitride (SiN) photonic structures to induce strong light$-$matter interaction with the monolayer. We dope the monolayer to carrier densities of ($7.2 \pm 0.8$) $\times$ $10^{13} \textrm{cm}^{-2}$, by electrically gating the TMD using an ionic liquid. We show strong electro-refractive response in monolayer tungsten disulphide (WS$_2$) at NIR wavelengths by measuring a large change in the real part of refractive index $\Delta$n = $0.53$, with only a minimal change in the imaginary part $\Delta$k = $0.004$. The doping induced phase change ($\Delta$n), compared to the induced absorption ($\Delta$k) measured for WS$_2$ ($\Delta$n/$\Delta$k $\sim 125$), a key metric for photonics, is an order of magnitude higher than the $\Delta$n/$\Delta$k for bulk materials like silicon ($\Delta$n/$\Delta$k $\sim 10$), making it ideal for various photonic applications. We further utilize this strong tunable effect to demonstrate an electrostatically gated SiN-WS$_2$ phase modulator using a WS$_2$-HfO$_2$ (Hafnia)-ITO (Indium Tin Oxide) capacitive configuration, that achieves a phase modulation efficiency (V$_\pi$L) of 0.8 V $\cdot$ cm with a RC limited bandwidth of 0.3 GHz.

Silicon waveguides have enabled large-scale manipulation and processing of near-infrared optical signals on chip. Yet, expanding the bandwidth of guided waves to other frequencies will further increase the functionality of silicon as a photonics platform. Frequency multiplexing by integrating additional architectures is one approach to the problem, but this is challenging to design and integrate within the existing form factor due to scaling with the free-space wavelength. This paper demonstrates that a hexagonal boron nitride (hBN)/silicon hybrid waveguide can simultaneously enable dual-band operation at both mid-infrared (6.5-7.0 µm) and telecom (1.55 µm) frequencies, respectively. The device is realized via the lithography-free transfer of hBN onto a silicon waveguide, maintaining near-infrared operation. In addition, mid-infrared waveguiding of the hyperbolic phonon polaritons (HPhPs) supported in hBN is induced by the index contrast between the silicon waveguide and the surrounding air underneath the hBN, thereby eliminating the need for deleterious etching of the hyperbolic medium. The behavior of HPhP waveguiding in both straight and curved trajectories is validated within an analytical waveguide theoretical framework. This exemplifies a generalizable approach based on integrating hyperbolic media with silicon photonics for realizing frequency multiplexing in on-chip photonic systems.

Author(s): Schalch, Jacob S; Post, Kirk; Duan, Guangwu; Zhao, Xiaoguang; Kim, Young Duck; Hone, James; Fogler, Michael M; Zhang, Xin; Basov, Dmitri N; Averitt, Richard D

Uniaxial materials whose axial and tangential permittivities have opposite signs are referred to as indefinite or hyperbolic media. While hyperbolic responses are normally achieved with metamaterials, hexagonal boron nitride (hBN) naturally possesses this property due to the anisotropic phonons in the mid-infrared. Using scattering-type scanning near-field optical microscopy, we studied polaritonic phenomena in hBN. We performed infrared nano-imaging of highly confined and low-loss hyperbolic phonon polaritons in hBN. The polariton wavelength was shown to be governed by the hBN thickness according to a linear law persisting down to few atomic layers [1]. Additionally, we carried out the modification of hyperbolic response in meta-structures comprised of a mononlayer graphene deposited on hBN [2]. Electrostatic gating of the top graphene layer allows for the modification of wavelength and intensity of hyperbolic phonon polaritons in bulk hBN. The physics of the modification originates from the plasmon-phonon coupling in the hyperbolic medium. Furthermore, we demonstrated the “hyperlens” for subdiffractional focusing and imaging using a slab of hBN [3]. References [1] S. Dai et al., Science, 343, 1125 (2014). [2] S. Dai et al., Nature Nanotechnology, 10, 682 (2015). [3] S. Dai et al., Nature Communications, 6, 6963 (2015).

Black phosphorous, a van der Waals layered semiconductor, is reported to reveal a plasmonic response that can be initiated by photoexcitation with femtosecond pulses.

Nonlinear optical response from a van der Waals interface is modulated and enhanced in twistable boron nitride homostructures., Broken symmetries induce strong even-order nonlinear optical responses in materials and at interfaces. Unlike conventional covalently bonded nonlinear crystals, van der Waals (vdW) heterostructures feature layers that can be stacked at arbitrary angles, giving complete control over the presence or lack of inversion symmetry at a crystal interface. Here, we report highly tunable second harmonic generation (SHG) from nanomechanically rotatable stacks of bulk hexagonal boron nitride (BN) crystals and introduce the term twistoptics to describe studies of optical properties in twistable vdW systems. By suppressing residual bulk effects, we observe SHG intensity modulated by a factor of more than 50, and polarization patterns determined by moiré interface symmetry. Last, we demonstrate greatly enhanced conversion efficiency in vdW vertical superlattice structures with multiple symmetry-broken interfaces. Our study paves the way for compact twistoptics architectures aimed at efficient tunable frequency conversion and demonstrates SHG as a robust probe of buried vdW interfaces.