Phase change materials for nano-polaritonics: a case study of hBN/VO2 heterostructures
S. Dai, J. Zhang, Q. Ma, S. Kittiwatanakul, A. S. McLeod, X. Chen, S. N. Gilbert Corder, K. Watanabe, T. Taniguchi, J. Lu, Q. Dai, P. Jarillo-Herrero, M. K. Liu, D. N. Basov
Polaritonic excitation and control in van der Waals (vdW) materials exhibit superior merits than conventional materials and thus hold new promise for exploring light matter interactions. In this work, we created vdW heterostructures combining hexagonal boron nitride (hBN) and a representative phase change material - vanadium dioxide (VO2). Using infrared nano-spectroscopy and nano-imaging, we demonstrated the dynamic tunability of hyperbolic phonon polaritons in hBN/VO2 heterostructures by temperature control in a precise and reversible fashion. The dynamic tuning of the polaritons stems from the change of local dielectric properties of the VO2 sublayer through insulator to metal transition by the temperature control. The high susceptibility of polaritons to electronic phase transitions opens possibilities for applications of vdW materials in combination with correlated phase change materials.
Ultrafast Nano-Imaging and Optical Control of Hyperbolic Phonon Polaritons at hBN/WS$_2$ Heterojunctions
Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Department of Physics and Electronics, Graduate School of Engineering, Osaka Metropolitan University（大阪公立大学工学研究科物理电子学专业）；The Graduate University for Advanced Studies, SOKENDAI（日本高级研究院）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所物质结构纳米构造研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国立材料研究所电子光学材料研究中心）；Fritz-Haber-Institut der Max-Planck-Gesellschaft（马克斯·普朗克学会弗里茨·哈伯研究所）
Probing Azimuthal Anatomy of Hyperbolic Whispering Gallery Modes in hBN
University of Notre Dame（圣母大学）；Cornell University（康奈尔大学）；Korea University（高丽大学）；Kansas State University（堪萨斯州立大学）；National Institute for Materials Science（国立材料研究所）；Bar-Ilan University（巴伊兰大学）
Uniaxial materials whose axial and tangential permittivities have opposite signs are referred to as indefinite or hyperbolic media. In such materials light propagation is unusual, leading to novel and often non-intuitive optical phenomena. Here we report infrared nano-imaging experiments demonstrating that crystals of hexagonal boron nitride (hBN), a natural mid-infrared hyperbolic material, can act as a "hyper-focusing lens" and as a multi-mode waveguide. The lensing is manifested by subdiffractional focusing of phonon-polaritons launched by metallic disks underneath the hBN crystal. The wave…
We present a new fabrication method of graphene spin-valve devices which yields enhanced spin and charge transport properties by improving both the electrode-to-graphene and graphene-to-substrate interface. First, we prepare Co/MgO spin injection electrodes onto Si$^{++}$/SiO$_2$. Thereafter, we mechanically transfer a graphene-hBN heterostructure onto the prepatterned electrodes. We show that room temperature spin transport in single-, bi- and trilayer graphene devices exhibit nanosecond spin lifetimes with spin diffusion lengths reaching 10$μ$m combined with carrier mobilities exceeding 20,0…
Extreme confinement of electromagnetic energy by phonon polaritons holds the promise of strong and new forms of control over the dynamics of matter. To bring such control to the atomic-scale limit, it is important to consider phonon polaritons in two-dimensional (2D) systems. Recent studies have pointed out that in 2D, splitting between longitudinal and transverse optical (LO and TO) phonons is absent at the $Γ$ point, even for polar materials. Does this lack of LO--TO splitting imply the absence of a phonon polariton in polar monolayers? Here, we derive a first-principles expression for the c…
In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride (hBN), low-loss infrared-active phonon-polaritons exhibit hyperbolic behavior for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transitio…
Artificial semiconductor heterostructures played a pivotal role in modern electronic and photonic technologies, providing a highly effective mean for the manipulation and control of carriers, from the visible to the Terahertz (THz) frequency range. Despite the exceptional versatility, they commonly require challenging epitaxial growth procedures due to the need of clean and abrupt interfaces, which proved to be a major obstacle for the realization of room-temperature (RT), high-efficiency devices, like source, detectors or modulators, especially in the far-infrared. Two-dimensional (2D) layere…
Ferromagnetic contacts are widely used to inject spin polarized currents into non-magnetic materials such as semiconductors or 2-dimensional materials like graphene. In these systems, oxidation of the ferromagnetic materials poses an intrinsic limitation on device performance. Here we investigate the role of ex-situ transferred chemical vapour deposited hexagonal boron nitride (hBN) as an oxidation barrier for nanostructured cobalt and permalloy electrodes. The chemical state of the ferromagnets was investigated using X-ray photoemission electron microscopy owing to its high sensitivity and la…
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 effective 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 contro…
The integrated inplane growth of two dimensional materials with similar lattices, but distinct electrical properties, could provide a promising route to achieve integrated circuitry of atomic thickness. However, fabrication of edge specific GNR in the lattice of hBN still remains an enormous challenge for present approaches. Here we developed a two step growth method and successfully achieved sub 5 nm wide zigzag and armchair GNRs embedded in hBN, respectively. Further transport measurements reveal that the sub 7 nm wide zigzag GNRs exhibit openings of the band gap inversely proportional to th…
We use confocal Raman microscopy and modified vector analysis methods to investigate the nanoscale origin of strain and carrier concentration in exfoliated graphene-hexagonal boron nitride (hBN) heterostructures on silicon dioxide (SiO2). Two types of heterostructures are studied: graphene on SiO2 partially coved by hBN, and graphene fully encapsulated between two hBN flakes. We extend the vector analysis methods to produce spatial maps of the strain and doping variation across the heterostructures. This allows us to visualise and directly quantify the much-speculated effect of the environment…
Semiconductor InSb nanosheet/hexagonal boron nitride (hBN)/graphite trilayers are fabricated, and single- and double-gate devices made from the trilayers are realized and characterized. The InSb nanosheets employed in the trilayer devices are epitaxially grown, free-standing, zincblende crystals and are in micrometer lateral sizes. The hBN and graphite flakes are obtained by exfoliation. Each trilayer is made by successively stacking an InSb nanosheet on an hBN flake and on a graphite flake using a home-made alignment stacking/transfer setup. The fabricated single- and double-gate devices are …
Hexagonal boron nitride (hBN) is the supporting substrate of choice for two-dimensional material devices because it is atomically flat and chemically inert. However, due to the small size of mechanically exfoliated hBN flakes, electronic structure studies of 2D materials supported by hBN using angle-resolved photoemission spectroscopy (ARPES) are challenging. Here we investigate the electronic band structure of a Bernal-stacked bilayer graphene sheet on a hexagonal boron nitride (BLG/hBN) flake using nanospot ARPES (nanoARPES). By fitting high-resolution energy vs. momentum electronic band spe…
The inherent crystal anisotropy of hexagonal boron nitride (hBN) sustains naturally hyperbolic phonon polaritons, i.e. polaritons that can propagate with very large wavevectors within the material volume, thereby enabling optical confinement to exceedingly small dimensions. Indeed, previous research has shown that nanometer-scale truncated nanocone hBN cavities, with deep subwavelength dimensions, support three-dimensionally confined optical modes in the mid-infrared. Due to optical selection rules, only a few of many such modes predicted theoretically have been observed experimentally via far…
We study the radiative heat flux between two nanoparticles in close vicinity to the natural hyperbolic material hBN with its optical axis oriented parallel to the interface. We show that the heat flux between the nanoparticles can be efficiently modulated when rotating the nanoparticles due to the coupling to the highly directional hyperbolic surface modes in hBN. Finally, we discuss the thickness and distance dependence of this effect.
Phonon polaritons are quasiparticles resulting from strong coupling of photons with optical phonons. Excitation and control of these quasiparticles in 2D materials offer the opportunity to confine and transport light at the nanoscale. Here, we image the phonon polariton (PhP) spectral response in thin hexagonal boron nitride (hBN) crystals as a representative 2D material using amplitude- and phase-resolved near-field interferometry with broadband mid-IR synchrotron radiation. The large spectral bandwidth enables the simultaneous measurement of both out-of-plane (780 cm-1) and in-plane (1370 cm…
Quadrupole topological insulator is a symmetry-protected higher-order topological phase with intriguing topology of Wannier bands, which, however, has not yet been realized in plasmonic metamaterials. Here, we propose a lattice of plasmon-polaritonic nanocavities which can realize quadrupole topological insulators by exploiting the geometry-dependent sign-reversal of the couplings between the daisy-like nanocavities. The designed system exhibits various topological and trivial phases as characterized by the nested Wannier bands and the topological quadrupole moment which can be controlled by t…
The hyperbolic phonon-polaritons within the Reststrahlen band of hBN are of great interest for applications in nanophotonics as they are capable of propagating light signals with low losses over large distances. However, due to the phononic nature of the polaritons in hBN, amplitude modulation of its signal proves to be difficult and has been underexplored. In this paper, we propose theoretically a broadband efficient amplitude modulator for hyperbolic rays in hBN operating in the frequency range between 1450 cm$^{-1}$ and 1550 cm$^{-1}$. The modulating region comprises a few tens of nanometer…
Recent discoveries have shown that when two layers of van der Waals (vdW) materials are superimposed with a relative twist angle between their respective in-plane principal axes, the electronic properties of the coupled system can be dramatically altered. Here, we demonstrate that a similar concept can be extended to the optics realm, particularly to propagating polaritons, hybrid light-matter interactions. To do this, we fabricate stacks composed of two twisted slabs of a polar vdW crystal (MoO3) supporting low-loss anisotropic phonon polaritons (PhPs), and image the propagation of the latter…
Enhanced light-matter interaction at the nanoscale is pivotal in the foundation of nonlinear optics, quantum optics, and nanophotonics, which are essential for a vast range of applications including single-photon sources, nanolasers, and nanosensors. In this context, the combination of strongly confined polaritons and low-loss nanocavities provides a promising way to enhance light-matter interaction, thus giving rise to a high density of optical states, as quantified by the so-called Purcell factor - the ratio of the decay rate of an optical quantum emitter to its value in free space. Here, we…
Two-dimensional (2D) materials occupy noteworthy place in nanophotonics providing for subwavelength light confinement and optical phenomena dissimilar to those of their bulk counterparts. In the mid-infrared, graphene-based heterostructures and van der Waals crystals of hexagonal boron nitride (hBN) overwhelmingly concentrate the attention by exhibiting real-space nano-optics from plasmons, phonon-polaritons and hybrid plasmon phonon-polaritons quasiparticles. Here we present the mid-infrared nanophotonics of talc, a natural atomically flat layered material, and graphene-talc (G-talc) heterost…
We investigated emission and propagation of polaritons in a two dimensional van der Waals material hexagonal boron nitride (hBN). Our specific emphasis in this work is on hyperbolic phonon polariton emission that we investigated by means of scattering-type scanning near-field optical microscopy. Real-space nano-images detail how the polaritons are launched in several common arrangements including: light scattering by the edges of the crystal, metallic nanostructures deposited on the surface of hBN crystals, as well as random defects and impurities. Notably, the scanned tip of the near-field mi…
Light-matter interaction in two-dimension photonic materials allows for confinement and control of free-space radiation on sub-wavelength scales. Most notably, the van der Waals heterostructure obtained by stacking graphene (G) and hexagonal Boron Nitride (hBN) can provide for hybrid hyperbolic plasmon phonon-polaritons (HP3). Here, we present a polariton diode effect and low-bias control of HP3 modes confined in G-hBN. Using broadband infrared synchrotron radiation coupled to a scattering-type near-field optical microscope, we launch HP3 waves over both hBN Reststrahlen bands and observe the …
We perform extensive first-principles calculations for heterostructures composed of monolayer graphene and hexagonal boron nitride (hBN). Employing a symmetry-derived minimal tight-binding model, we extract orbital and spin-orbit coupling (SOC) parameters for graphene on hBN, as well as for hBN encapsulated graphene. Our calculations show that the parameters depend on the specific stacking configuration of graphene on hBN. We also perform an interlayer distance study for the different graphene/hBN stacks to find the corresponding lowest energy distances. For very large interlayer distances, on…
The large oscillator strength of excitons in transition metal dichalcogenide layers facilitates the formation of exciton-polariton resonances for monolayers and van-der-Waals heterostructures embedded in optical microcavities. Here, we show, that locally changing the number of layers in a WSe2/hBN/WSe2 van-der-Waals heterostructure embedded in a monolithic, high-quality-factor cavity gives rise to a local variation of the coupling strength. This effect yields a polaritonic stair case potential, which we demonstrate at room temperature. Our result paves the way towards engineering local polarit…
Layered materials can be assembled vertically to fabricate a new class of van der Waals (VDW) heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/boron nitride (MoSe$_2$/hBN) quantum wells (QWs) in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe$_2$ excitons and cavity photons, evidenced from a clear anticrossing between the neutra…
Nanostructured superlattices are promising materials for novel electronic devices due to their adjustable physical properties. Periodic superlattices facilitate coherent phonon thermal transport due to constructive wave interference at the boundaries between the materials. However, it is possible to induce a crossover from coherent to incoherent transport regimes by adjusting the superlattice period. We have recently observed such crossover in periodic graphene-boron nitride nanoribbons as the length of individual domains was increased. In general, transport properties are dominated by transla…
Complementary metal oxide semiconductor (CMOS) logic circuits at the ultimate scaling limit place the utmost demands on the properties of all materials involved. The requirements for semiconductors are well explored and could possibly be satisfied by a number of layered two-dimensional (2D) materials, like for example transition-metal dichalcogenides or black phosphorus. The requirements for the gate insulator are arguably even more challenging and difficult to meet. In particular the combination of insulator to semiconductor which forms the central element of the metal oxide semiconductor fie…
We report experimental and computational studies of thermal transport properties in hexagonal boron nitride (hBN) encapsulated molybdenum disulfide (MoS2) structure using refined optothermal Raman techniques, and reveal very high interfacial thermal conductance between hBN and MoS2. By studying the Raman shift of hBN and MoS2 in suspended and substrate-supported thin films under varying laser power and temperature, we calibrate lateral (in-plane) thermal conductivity of hBN and MoS2 and the vertical interfacial thermal conductance in the hBN/MoS2/hBN heterostructure as well as the interfaces b…
Nanopores in 2D materials are highly desirable for DNA sequencing, yet achieving single-stranded DNA (ssDNA) transport through them is challenging. Using density functional theory calculations and molecular dynamics simulations we show that ssDNA transport through a pore in monolayer hexagonal boron nitride (hBN) is marked by a basic nanomechanical conflict. It arises from the notably inhomogeneous flexural rigidity of ssDNA and causes high friction $\textit{via}$ transient DNA desorption costs exacerbated by solvation effects. For a similarly sized pore in bilayer hBN, its self-passivated ato…
Encapsulating graphene in hexagonal Boron Nitride has several advantages: the highest mobilities reported to date are achieved in this way, and precise nanostructuring of graphene becomes feasible through the protective hBN layers. Nevertheless, subtle effects may arise due to the differing lattice constants of graphene and hBN, and due to the twist angle between the graphene and hBN lattices. Here, we use a recently developed model which allows us to perform band structure and magnetotransport calculations of such structures, and show that with a proper account of the moiré physics an excelle…
Controlling light-matter interactions in solid-state systems has motivated intense research to produce bosonic quasi-particles known as exciton-polaritons, which requires strong coupling between excitons and cavity photons. Ultra-low threshold coherent light emitters can be achieved through lasing from exciton-polariton condensates, but this generally requires sophisticated device structures and cryogenic temperatures. Polaritonic nanolasers operating at room temperature lie on the crucial path of related research, not only for the exploration of polariton physics at the nanoscale but also for…
Hybrid halide perovskites are now considered as low-cost materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining low-cost devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of the 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton-photon coupling with 3D bromide hybrid perovskite. Cavity polaritons ar…
We develop a quantum theory of plasmon polaritons in chains of metallic nanoparticles, describing both near- and far-field interparticle distances, by including plasmon-photon Umklapp processes. Taking into account the retardation effects of the long-range dipole-dipole interaction between the nanoparticles, which are induced by the coupling of the plasmonic degrees of freedom to the photonic continuum, we reveal the polaritonic nature of the normal modes of the system. We compute the dispersion relation and radiative linewidth, as well as the group velocities of the eigenmodes, and compare ou…
Scattering-type scanning near-field optical microscopy (s-SNOM) is instrumental in exploring polaritonic behaviors of two-dimensional (2D) materials at the nanoscale. A sharp s-SNOM tip couples momenta into 2D materials through phase matching to excite phonon polaritons, which manifest as nanoscale interference fringes in raster images. However, s-SNOM lacks the ability to detect the progression of near-field property along the perpendicular axis to the surface. Here, we perform near-field analysis of a micro-disk and a reflective edge made of isotopically pure hexagonal boron nitride (h-11BN)…
Unlike the electrical conductance that can be widely modulated within the same material even in deep nanoscale devices, tuning the thermal conductance within a single material system or nanostructure is extremely challenging and requires a large-scale device. This prohibits the realization of robust ON/OFF states in switching the flow of thermal currents. Here, we present the theory of a thermal switch based on resonant coupling of three photonic resonators, in analogy to the field-effect electronic transistor composed of a source, gate, and drain. As a material platform, we capitalize on the …
Hexagonal boron nitride (hBN) is a wide bandgap van der Waals material that has recently emerged as promising platform for quantum photonics experiments. In this work we study the formation and localization of narrowband quantum emitters in large flakes (up to tens of microns wide) of hBN. The emitters can be activated in as-grown hBN by electron irradiation or high temperature annealing, and the emitter formation probability can be increased by ion implantation or focused laser irradiation of the as-grown material. Interestingly, we show that the emitters are always localized at edges of the …
The field of 2D materials-based nanophotonics has been growing at a rapid pace, triggered by the ability to design nanophotonic systems with in situ control, unprecedented degrees of freedom, and to build material heterostructures from bottom up with atomic precision. A wide palette of polaritonic classes have been identified, comprising ultra confined optical fields, even approaching characteristic length scales of a single atom. These advances have been a real boost for the emerging field of quantum nanophotonics, where the quantum mechanical nature of the electrons and-or polaritons and the…
Nanostructuring allows altering of the electronic and photonic properties of two-dimensional (2D) materials. The efficiency, flexibility, and convenience of top-down lithography processes are however compromised by nm-scale edge roughness and resolution variability issues, which especially affects the performance of 2D materials. Here we study how dry anisotropic etching of multilayer 2D materials with sulfur hexafluoride (SF6) may overcome some of these issues, showing results for hexagonal boron nitride (hBN), tungsten disulfide (WS2), tungsten diselenide (WSe2), molybdenum disulfide (MoS2),…
Spin defects in hexagonal Boron Nitride (hBN) attract increasing interest for quantum technology since they represent optically-addressable qubits in a van der Waals material. In particular, negatively-charged boron vacancy centers (${V_B}^-$) in hBN have shown promise as sensors of temperature, pressure, and static magnetic fields. However, the short spin coherence time of this defect currently limits its scope for quantum technology. Here, we apply dynamical decoupling techniques to suppress magnetic noise and extend the spin coherence time by nearly two orders of magnitude, approaching the …
