Terahertz third harmonic generation in c-axis La1.85_{1.85}Sr0.15_{0.15}CuO4_4

Terahertz nonlinear optics is a viable method to interrogate collective phenomena in quantum materials spanning ferroelectrics, charge-density waves, and superconductivity. In superconductors this includes the Higgs amplitude and Josephson phase modes. We have investigated the nonlinear c-axis response of optimally doped La$_{1.85}$Sr$_{0.15}$CuO$_4$ using high-field THz time domain spectroscopy (THz-TDS) at field strengths up to $\sim$80 kV/cm. With increasing field, we observe a distinct red-shift of the Josephson plasma edge and enhanced reflectivity (above the plasma edge) arising from third harmonic generation. The non-monotonic temperature dependent response is consistent with nonlinear drive of the Josephson Plasma Mode (JPM) as verified with comparison to theoretical expectations. Our results add to the understanding that, using THz light, the JPM (in addition to the Higgs mode) provides a route to interrogate and control superconducting properties

Tunable magnetic domains in ferrimagnetic MnSb2_2Te4_4

Highly tunable properties make Mn(Bi,Sb)$_2$Te$_4$ a rich playground for exploring the interplay between band topology and magnetism: On one end, MnBi$_2$Te$_4$ is an antiferromagnetic topological insulator, while the magnetic structure of MnSb$_2$Te$_4$ (MST) can be tuned between antiferromagnetic and ferrimagnetic. Motivated to control electronic properties through real-space magnetic textures, we use magnetic force microscopy (MFM) to image the domains of ferrimagnetic MST. We find that magnetic field tunes between stripe and bubble domain morphologies, raising the possibility of topological spin textures. Moreover, we combine in situ transport with domain manipulation and imaging to both write MST device properties and directly measure the scaling of the Hall response with domain area. This work demonstrates measurement of the local anomalous Hall response using MFM, and opens the door to reconfigurable domain-based devices in the M(B,S)T family

Internal strain tunes electronic correlations on the nanoscale

Da die Strukturen innerhalb von Festkörpern am Phasenübergang von Metallen zu Isolatoren meist kleiner sind als die Wellenlänge des Lichts, kann man sie nicht mit einem normalen Mikroskop beobachten. Daher nutzten die Stuttgarter Physiker ein Nahfeld-Mikroskop. Bei diesem macht man sich zunutze, dass eine atomar dünne Spitze ganz knapp über dem Material Licht streut und tiefe Blicke in die lokalen elek­tronischen Eigenschaften gibt. So konnten die Wissenschaftler auch an einem molekularen Kristall den Metall-Isolator-Phasenübergang untersuchen, der dort bei -138 Grad Celsius (136 K) auftritt. Es wurden scharfe Grenzen zwischen metallischen und isolierenden Gebieten beobachtet, was zweifelsfrei einen Phasenübergang erster Ordnung nachgeweist, der durch elektronische Wechselwirkungen getrieben wird. Zudem entsteht ein charakteristisches ("Zebra-") Streifenmuster als Folge mechanischer Verspannungen im Kristall. Dies liefert wichtige Erkenntnisse, welch wichtigen Einfluss die mechanische Integrität einer chemisch reinen Probe auf die makroskopisch gemessenen physikalischen Eigenschaften haben kann

Towards compact phase-matched and waveguided nonlinear optics in atomically layered semiconductors

Nonlinear frequency conversion provides essential tools for light generation, photon entanglement, and manipulation. Transition metal dichalcogenides (TMDs) possess huge nonlinear susceptibilities and 3R-stacked TMD crystals further combine broken inversion symmetry and aligned layering, representing ideal candidates to boost the nonlinear optical gain with minimal footprint. Here, we report on the efficient frequency conversion of 3R-MoS2, revealing the evolution of its exceptional second-order nonlinear processes along the ordinary (in-plane) and extraordinary (out-of-plane) directions. By measuring second harmonic generation (SHG) of 3R-MoS2 with various thickness - from monolayer (~0.65 nm) to bulk (~1 {\mu}m) - we present the first measurement of the in-plane SHG coherence length (~530 nm) at 1520 nm and achieve record nonlinear optical enhancement from a van der Waals material, >10^4 stronger than a monolayer. It is found that 3R-MoS2 slabs exhibit similar conversion efficiencies of lithium niobate, but within propagation lengths >100-fold shorter at telecom wavelengths. Furthermore, along the extraordinary axis, we achieve broadly tunable SHG from 3R-MoS2 in a waveguide geometry, revealing the coherence length in such structure for the first time. We characterize the full refractive index spectrum and quantify both birefringence components in anisotropic 3R-MoS2 crystals with near-field nano-imaging. Empowered with these data we assess the intrinsic limits of the conversion efficiency and nonlinear optical processes in 3R-MoS2 attainable in waveguide geometries. Our analysis highlights the potential of 3R-stacked TMDs for integrated photonics, providing critical parameters for designing highly efficient on-chip nonlinear optical devices including periodically poled structures, resonators, compact optical parametric oscillators and amplifiers, and optical quantum circuits

Nanometer-Scale Lateral p–n Junctions in Graphene/α-RuCl3 Heterostructures

[EN] The ability to create nanometer-scale lateral p-n junctions is essential for the next generation of two-dimensional (2D) devices. Using the charge-transfer heterostructure graphene/alpha-RuCl3, we realize nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multipronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy (s-SNOM) to simultaneously probe the electronic and optical responses of nanobubble p-n junctions. Our STM/STS results reveal that p-n junctions with a band offset of 0.6 eV can be achieved with widths of 3 nm, giving rise to electric fields of order 108 V/m. Concurrent s-SNOM measurements validate a point-scatterer formalism for modeling the interaction of surface plasmon polaritons (SPPs) with nanobubbles. Ab initio density functional theory (DFT) calculations corroborate our experimental data and reveal the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for generating p-n nanojunctions in 2D materials.Research at Columbia University was supported as part of the Energy Frontier Research Center on Programmable Quantum Materials funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No DE-SC0019443. Plasmonic nano-imaging at Columbia University was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No DE-SC0018426. J.Z. and A.R. were supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence “Advanced Imaging of Matter” (AIM) EXC 2056-390715994, funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under RTG 2247, Grupos Consolidados (IT1249-19), and SFB925 “Light induced dynamics and control of correlated quantum systems”. J.Z. and A.R. would like to acknowledge Nicolas Tancogne-Dejean and Lede Xian for fruitful discussions and also acknowledge support by the Max Planck Institute-New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. J.Z. acknowledges funding received from the European Union Horizon 2020 research and innovation programme under Marie Skłodowska-Curie Grant Agreement 886291 (PeSD-NeSL). STM support was provided by the National Science Foundation via Grant DMR-2004691. C.R.-V. acknowledges funding from the European Union Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement 844271. D.G.M. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF9069. J.Q.Y. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. S.E.N. acknowledges support from the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Division of Scientific User Facilities. Work at University of Tennessee was supported by NSF Grant 180896

Dual-gated graphene devices for near-field nano-imaging

Graphene-based heterostructures display a variety of phenomena that are strongly tunable by electrostatic local gates. Monolayer graphene (MLG) exhibits tunable surface plasmon polaritons, as revealed by scanning nano-infrared experiments. In bilayer graphene (BLG), an electronic gap is induced by a perpendicular displacement field. Gapped BLG is predicted to display unusual effects such as plasmon amplification and domain wall plasmons with significantly larger lifetime than MLG. Furthermore, a variety of correlated electronic phases highly sensitive to displacement fields have been observed in twisted graphene structures. However, applying perpendicular displacement fields in nano-infrared experiments has only recently become possible (Ref. 1). In this work, we fully characterize two approaches to realizing nano-optics compatible top-gates: bilayer $\text{MoS}_2$ and MLG. We perform nano-infrared imaging on both types of structures and evaluate their strengths and weaknesses. Our work paves the way for comprehensive near-field experiments of correlated phenomena and plasmonic effects in graphene-based heterostructures