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Hyperbolic phonon polaritons (HPhPs) can be supported in highly anisotropic materials, where the real parts of their permittivities along different directions are opposite in sign as a result of spectrally offset optical phonons. Compared to surface polaritons, HPhPs offer further confinement of long-wavelength light to deeply subdiffractional scales, and volume propagation that enables control of the polariton wavevector by changing the underlying medium. This allows for greater control of polaritonic resonators and near-field polariton propagation without deleterious etching of hyperbolic materials. Yet, conventionally used noble metal and dielectric substrates restrict the tunability of this approach, leaving most of the wavevector inaccessible. To overcome this challenge, we demonstrate that using doped semiconductors, e.g., InAs and CdO, can enable near-continuous tuning and access to both the maximum and minimum wavevectors (~8.3 times experimentally demonstrated). We further elucidate HPhP tuning with the plasma frequency of an InAs substrate, which features a significant wavevector discontinuity and modal order transition when the substrate permittivity crosses -1 in the Reststrahlen band. Around the transition point, the HPhP system is sensitive to perturbations, e.g., the working frequency, InAs plasma frequency and superstrate, thus it is suitable for sensing and modulation applications. We also illustrate that the hBN/InAs platform allows for active modulation at picosecond timescales by photo-injecting carriers into the InAs substrate, demonstrating a dynamic wavevector change of ~20%. Overall, the demonstrated hBN/doped semiconductor platform offers significant improvements towards manipulating HPhPs, and enormous potential for engineered and modulated polaritonic systems for applications in on-chip photonics and planar metasurface optics.

Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional (2D) electron systems subject to strong magnetic fields are expected to exhibit quantized Hall conductivity, chiral edge currents, and distinctive collective modes referred to as magnetoplasmons and magnetoexcitons. Generating these propagating collective modes in charge-neutral samples and imaging them at their native nanometer length scales have thus far been experimentally elusive tasks. In this study, we visualize propagating magenetoexction polaritons at their native length scales and report their magnetic-field-tunable dispersions in near-charge-neutral graphene. Imaging of these collective modes and their associated opto-electrical responses at the sample edges is enabled by innovations to our cryogenic near-field optical microscope that allows us to nano-image the optical responses of 2D materials in magnetic fields up to 7 Tesla. This novel nano-magneto-optics approach represents a new paradigm for exploring and manipulating magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

We investigate transient nanotextured heterogeneity in vanadium dioxide (VO2) thin films during a light-induced insulator-to-metal transition (IMT). Time-resolved scanning near-field optical microscopy (Tr-SNOM) is used to study VO2 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. The observed contrast is associated with inequivalent twin domain structures. Upon thermal or optical initiation of the IMT, coexisting metallic and insulating regions are observed. Correlations between the transient and steady-state nano-optical textures reveal that heterogeneous nucleation is partially anchored to twin domain interfaces and grain boundaries. Ultrafast nanoscopic dynamics enable quantification of the growth rate and bound the nucleation rate. Finally, we deterministically anchor photoinduced nucleation to predefined nanoscopic regions by locally enhancing the electric field of pump radiation using nanoantennas and monitor the on-demand emergent metallicity in space and time.

Deep learning (DL) is an emerging analysis tool across the sciences and engineering. Encouraged by the successes of DL in revealing quantitative trends in massive imaging data, we applied this approach to nanoscale deeply subdiffractional images of propagating polaritonic waves in complex materials. Utilizing the convolutional neural network (CNN), we developed a practical protocol for the rapid regression of images that quantifies the wavelength and the quality factor of polaritonic waves. Using simulated near-field images as training data, the CNN can be made to simultaneously extract polaritonic characteristics and material parameters in a time scale that is at least 3 orders of magnitude faster than common fitting/processing procedures. The CNN-based analysis was validated by examining the experimental near-field images of charge-transfer plasmon polaritons at graphene/α-RuCl

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.

In twisted bilayers of semiconducting transition metal dichalcogenides (TMDs), a combination of structural rippling and electronic coupling gives rise to periodic moir\'e potentials that can confine charged and neutral excitations. Here, we report experimental measurements of the structure and spectroscopic properties of twisted bilayers of WSe2 and MoSe2 in the H-stacking configuration using scanning tunneling microscopy (STM). Our experiments reveal that the moir\'e potential in these bilayers at small angles is unexpectedly large, reaching values of above 300 meV for the valence band and 150 meV for the conduction band - an order of magnitude larger than theoretical estimates based on interlayer coupling alone. We further demonstrate that the moir\'e potential is a non-monotonic function of moir\'e wavelength, reaching a maximum at around a 13nm moir\'e period. This non-monotonicity coincides with a drastic change in the structure of the moir\'e pattern from a continuous variation of stacking order at small moir\'e wavelengths to a one-dimensional soliton dominated structure at large moir\'e wavelengths. We show that the in-plane structure of the moir\'e pattern is captured well by a continuous mechanical relaxation model, and find that the moir\'e structure and internal strain rather than the interlayer coupling is the dominant factor in determining the moir\'e potential. Our results demonstrate the potential of using precision moir\'e structures to create deeply trapped carriers or excitations for quantum electronics and optoelectronics.

Chiral Weyl fermions with linear energy-momentum dispersion in the bulk accompanied by Fermi-arc states on the surfaces prompt a host of enticing optical effects. While new Weyl semimetal materials keep emerging, the available optical probes are limited. In particular, isolating bulk and surface electrodynamics in Weyl conductors remains a challenge. We devised an approach to the problem based on near-field photocurrent imaging at the nanoscale and applied this technique to a prototypical Weyl semimetal TaIrTe(4). As a first step, we visualized nano-photocurrent patterns in real space and demonstrated their connection to bulk nonlinear conductivity tensors through extensive modeling augmented with density functional theory calculations. Notably, our nanoscale probe gives access to not only the in-plane but also the out-of-plane electric fields so that it is feasible to interrogate all allowed nonlinear tensors including those that remained dormant in conventional far-field optics. Surface- and bulk-related nonlinear contributions are distinguished through their “symmetry fingerprints” in the photocurrent maps. Robust photocurrents also appear at mirror-symmetry breaking edges of TaIrTe(4) single crystals that we assign to nonlinear conductivity tensors forbidden in the bulk. Nano-photocurrent spectroscopy at the boundary reveals a strong resonance structure absent in the interior of the sample, providing evidence for elusive surface states.

The scattering-type scanning near-field optical microscope (s-SNOM) has emerged as a powerful tool for resolving nanoscale inhomogeneities in laterally heterogeneous samples. However, most analytical models used to predict the scattering near-field signals are assuming homogenous landscapes (bulk materials), resulting in inconsistencies when applied to samples with more complex configurations. In this work, we combine the point-dipole model (PDM) to the finite-element method (FEM) to account for the lateral and vertical heterogeneities while keeping the computation time manageable. Full images, spectra, or hyperspectral line profiles can be simulated by calculating the self-consistent dipole radiation demodulated at higher harmonics of the tip oscillation, mimicking real experimental procedures. Using this formalism, we clarify several important yet puzzling experimental observations in near-field images on samples with rich typography and complex material compositions, heterostructures of two-dimensional material flakes, and plasmonic antennas. The developed method serves as a basis for future investigations of nano-systems with nontrivial topography.

Dirac fermions with highly dispersive linear bands1–3 are usually considered weakly correlated due to the relatively large bandwidths (W) compared to Coulomb interactions (U). With the discovery of nodal-line semimetals, the notion of the Dirac point has been extended to lines and loops in momentum space. The anisotropy associated with nodal-line structure gives rise to greatly reduced kinetic energy along the line. However, experimental evidence for the anticipated enhanced correlations in nodal-line semimetals is sparse. Here, we report on prominent correlation effects in a nodal-line semimetal compound, ZrSiSe, through a combination of optical spectroscopy and density functional theory calculations. We observed two fundamental spectroscopic hallmarks of electronic correlations: strong reduction (1/3) of the free-carrier Drude weight and also the Fermi velocity compared to predictions of density functional band theory. The renormalization of Fermi velocity can be further controlled with an external magnetic field. ZrSiSe therefore offers the rare opportunity to investigate correlation-driven physics in a Dirac system. What happens to topological materials when their electrons are strongly interacting is an open question. Shao and others demonstrate that ZrSiSe is a material that can address this as it has a topological band structure and non-trivial correlations.

Author(s): Chen, X; Yao, Z; Xu, S; McLeod, AS; Gilbert Corder, SN; Zhao, Y; Tsuneto, M; Bechtel, HA; Martin, MC; Carr, GL; Fogler, MM; Stanciu, SG; Basov, DN; Liu, M | Abstract: The underlying physics behind an experimental observation often lacks a simple analytical description. This is especially the case for scanning probe microscopy techniques, where the interaction between the probe and the sample is nontrivial. Realistic modeling to include the exact details of the probe is widely acknowledged as a challenge. Due to various complexity constraints, the probe is often only approximated in a simplified geometry, leading to a source for modeling inconsistencies. On the other hand, a well-trained artificial neural network based on real data can grasp the hidden correlation between the signal and the sample properties, circumventing the explicit probe modeling process. In this work we show that, via a combination of model calculation and experimental data acquisition, a physics-infused hybrid neural network can predict the probe-sample interaction in the widely used scattering-type scanning near-field optical microscope. This hybrid network provides a long-sought solution for accurate extraction of material properties from tip-specific raw data. The methodology can be extended to other scanning probe microscopy techniques as well as other data-oriented physical problems in general.

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.

We demonstrate the creation of permanent, localized strain structures in hBN with a phonon-resonant femtosecond laser at 7.3 µm. We spatially resolve the strain profile of the resulting micron-scale bubbles using Raman and AFM measurements.

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

We theoretically study the low energy electromagnetic response of BCS type superconductors focusing on propagating collective modes that are observable with THz near field optics. The interesting frequency and momentum range is $\omega < 2\Delta$ and $q < 1/\xi$ where $\Delta$ is the gap and $\xi$ is the coherence length. We show that it is possible to observe the superfluid plasmons, amplitude (Higgs) modes, Bardasis-Schrieffer modes and Carlson-Goldman modes using THz near field technique, although none of these modes couple linearly to far field radiation. Coupling of THz near field radiation to the amplitude mode requires particle-hole symmetry breaking while coupling to the Bardasis-Schrieffer mode does not and is typically stronger. For parameters appropriate to layered superconductors of current interest, the Carlson-Goldman mode appears in the near field reflection coefficient as a weak feature in the sub-THz frequency range. In a system of two superconducting layers with nanometer scale separation, an acoustic phase mode appears as the antisymmetric density fluctuation mode of the system. This mode produces well defined resonance peaks in the near-field THz response and has strong anticrossings with the Bardasis-Schrieffer and amplitude modes, enhancing their response. In a slab consisting of many layers of quasi-two dimensional superconductors, realized for example in samples of high T$_c$ cuprate compounds, many branches of propagating Josephson plasmon modes are found to couple to the THz near field radiation., Comment: 12 pages, 7 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.

Conventional optical components are limited to size-scales much larger than the wavelength of light, as changes to the amplitude, phase and polarization of the electromagnetic fields are accrued gradually along an optical path. However, advances in nanophotonics have produced ultrathin, so-called “flat” optical components that beget abrupt changes in these properties over distances significantly shorter than the free space wavelength. While high optical losses still plague many approaches, phonon polariton materials have demonstrated long lifetimes for localized modes in comparison to plasmon-polariton based nanophotonics. Our work predicts a further 14-fold increase in the optic phonon lifetime and we experimentally report a ~3-fold improvement through isotopic enrichment of hexagonal boron nitride (hBN). We establish commensurate increases in the phonon polariton propagation length via direct imaging of polaritonic standing waves by means of infrared nano-optics. Our results provide the foundation for a materials-growth-directed approach towards realizing the loss control necessary for the development of phonon polariton based nanophotonic devices.

Hexagonal boron nitride (hBN) is a natural hyperbolic material that supports both volume-confined hyperbolic polaritons (HPs) and sidewall-confined hyperbolic surface polaritons (HSPs). In this work, we demonstrate efficient excitation, control and steering of HSPs in hBN through engineering the geometry and orientation of hBN sidewalls. By combining infrared (IR) nano-imaging and numerical simulations, we investigate the reflection, transmission and scattering of HSPs at the hBN corners with various apex angles. We show that the sidewall-confined nature of HSPs enables a high degree of control over their propagation by designing the geometry of hBN nanostructures.

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

For hyperbolic materials, we numerically recover the full near field of a radiating antenna from one component of its far-field intensity. The phase-retrieval-like algorithm leverages anisotropy and the HM coupling of propagating and evanescent modes.

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).

van der Waals (vdW) crystals consist of individual atomic planes coupled by vdW interaction, similar to graphene monolayers in bulk graphite. We investigated van der Waals heterostructures assembled from atomically thin layers of graphene and hexagonal boron nitride (hBN). We launched, detected and imaged plasmonic, phonon polaritonic and hybrid plasmon-phonon polariton waves in a setting of an antenna based nano-infrared apparatus. Hyperbolic phonon polaritons in hBN enabled sub-diffractional focusing in infrared frequencies. Because electronic, plasmonic and phonon polaritonic properties in van der Waals heterstructures are intertwined, gate voltage and/or details of layer assembly enable efficient control of nano-photonic effects.

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