Search

We report a nanoinfrared (IR) imaging study of the localized plasmon resonance modes of graphene nanoribbons (GNRs) using a scattering-type scanning near-field optical microscope (s-SNOM). By comparing the imaging data of GNRs that are aligned parallel and perpendicular to the in-plane component of the excitation laser field, we observed symmetric and asymmetric plasmonic interference fringes, respectively. Theoretical analysis indicates that the asymmetric fringes are formed due to the interplay between the localized surface plasmon resonance (SPR) mode excited by the GNRs and the propagative surface plasmon polariton (SPP) mode launched by the s-SNOM tip. With rigorous simulations, we reproduce the observed fringe patterns and address quantitatively the role of the s-SNOM tip on both the SPR and SPP modes. Furthermore, we have seen real-space signatures of both the dipole and higher-order SPR modes by varying the ribbon width.

We investigated phonon-polaritons in hexagonal boron nitride - a naturally hyperbolic van der Waals material - by means of the scattering-type scanning near-field optical microscopy. Real-space nanoimages we have obtained detail how the polaritons are launched when the light incident on a thin hexagonal boron nitride slab is scattered by various intrinsic and extrinsic inhomogeneities, including sample edges, metallic nanodisks deposited on its top surface, random defects, and surface impurities. The scanned tip of the near-field microscope is itself a polariton launcher whose efficiency proves to be superior to all the other types of polariton launchers we studied. Our work may inform future development of polaritonic nanodevices as well as fundamental studies of collective modes in van der Waals materials.

We report on a nanoinfrared (IR) imaging study of ultraconfined plasmonic hotspots inside graphene nanobubbles formed in graphene/hexagonal boron nitride (hBN) heterostructures. The volume of these plasmonic hotspots is more than one-million-times smaller than what could be achieved by free-space IR photons, and their real-space distributions are controlled by the sizes and shapes of the nanobubbles. Theoretical analysis indicates that the observed plasmonic hotspots are formed due to a significant increase of the local plasmon wavelength in the nanobubble regions. Such an increase is attributed to the high sensitivity of graphene plasmons to its dielectric environment. Our work presents a novel scheme for plasmonic hotspot formation and sheds light on future applications of graphene nanobubbles for plasmon-enhanced IR spectroscopy.

We report on nano-infrared (IR) imaging studies of confined plasmon modes inside patterned graphene nanoribbons (GNRs) fabricated with high-quality chemical-vapor-deposited (CVD) graphene on Al2O3 substrates. The confined geometry of these ribbons leads to distinct mode patterns and strong field enhancement, both of which evolve systematically with the ribbon width. In addition, spectroscopic nanoimaging in the mid-infrared range 850-1450 cm(-1) allowed us to evaluate the effect of the substrate phonons on the plasmon damping. Furthermore, we observed edge plasmons: peculiar one-dimensional modes propagating strictly along the edges of our patterned graphene nanostructures.

We report experimental signatures of plasmonic effects due to electron tunneling between adjacent graphene layers. At subnanometer separation, such layers can form either a strongly coupled bilayer graphene with a Bernal stacking or a weakly coupled double-layer graphene with a random stacking order. Effects due to interlayer tunneling dominate in the former case but are negligible in the latter. We found through infrared nanoimaging that bilayer graphene supports plasmons with a higher degree of confinement compared to single- and double-layer graphene, a direct consequence of interlayer tunneling. Moreover, we were able to shut off plasmons in bilayer graphene through gating within a wide voltage range. Theoretical modeling indicates that such a plasmon-off region is directly linked to a gapped insulating state of bilayer graphene, yet another implication of interlayer tunneling. Our work uncovers essential plasmonic properties in bilayer graphene and suggests a possibility to achieve novel plasmonic functionalities in graphene few-layers.

In a two-dimensional moiré superlattice, the atomic reconstruction of constituent layers could introduce significant modifications to the lattice symmetry and electronic structure at small twist angles. Here, we employ conductive atomic force microscopy to investigate a twisted trilayer graphene double-moiré superlattice. Two sets of moiré superlattices are observed. At neighboring domains of the large moiré, the current exhibits either 2- or 6-fold rotational symmetry, indicating delicate symmetry breaking beyond the rigid model. Moreover, an anomalous current appears at the "A-A" stacking site of the larger moiré, contradictory to previous observations on twisted bilayer graphene. Both behaviors can be understood by atomic reconstruction, and we also show that the measured current is dominated by the tip-graphene contact resistance that maps the local work function qualitatively. Our results reveal new insights of atomic reconstruction in novel moiré superlattices and opportunities for manipulating exotic quantum states on the basis of twisted van der Waals heterostructures.

Emerging twistronics based on van der Waals (vdWs) materials has attracted great interest in condensed matter physics. Recently, more neoteric three-dimensional (3D) architectures with interlayer twist are realized in germanium sulfide (GeS) crystals. Here, we further demonstrate a convenient way for tailoring the twist rate of helical GeS crystals via tuning of the growth temperature. Under higher growth temperatures, the twist angles between successive nanoplates of the GeS mesowires (MWs) are statistically smaller, which can be understood by the dynamics of the catalyst during the growth. Moreover, we fabricate self-assembled helical heterostructures by introducing germanium selenide (GeSe) onto helical GeS crystals via edge epitaxy. Besides the helical architecture, the moiré superlattices at the twisted interfaces are also inherited. Compared with GeS MWs, helical GeSe/GeS heterostructures exhibit improved electrical conductivity and photoresponse. These results manifest new opportunities in future electronics and optoelectronics by harnessing 3D twistronics based on vdWs materials.

In recent years, novel materials supporting in-plane anisotropic polaritons have attracted a great deal of research interest due to their capability of shaping nanoscale field distributions and controlling nanophotonic energy flows. Here we report a nano-optical imaging study of waveguide exciton polaritons (EPs) in tin sulfide (SnS) in the near-infrared (near-IR) region using scattering-type scanning near-field optical microscopy (s-SNOM). With s-SNOM, we mapped in real space the propagative EPs in SnS, which show sensitive dependence on the excitation energy and sample thickness. Moreover, we found that both the polariton wavelength and propagation length are anisotropic in the sample plane. In particular, in a narrow spectral range from 1.32 to 1.44 eV, the EPs demonstrate quasi-one-dimensional propagation, which is rarely seen in natural polaritonic materials. A further analysis indicates that the observed polariton anisotropy originates from the different optical band gaps and exciton binding energies along the two principal crystal axes of SnS.

van der Waals (vdW) magnets have emerged as a tunable platform for exploring a variety of layer-dependent magnetic phenomena. Here we probe the thickness-dependent magnetism of vanadium triiodide (VI 3 ), a material known as a layered ferromagnetic Mott insulator in its bulk form, using magnetic circular dichroism microscopy. Robust ferromagnetism is observed in all thin layers, down to the monolayer limit with large coercive fields. In contrast to known vdW magnets, the Curie temperature shows an anomalous increase as the layer number decreases, reaching a maximum of 60 K in monolayers. Second harmonic generation measurements reveal broken inversion symmetry in exfoliated flakes, down to trilayers. This observation demonstrates that the exfoliated flakes take a layer stacking arrangement that differed from the inversion-symmetric parent bulk counterpart. Our results suggest a coupling effect between magnetic and structural degrees of freedom in VI 3 and its potential for engineering layer and twist angle-dependent magnetic phenomena.

MnBi 2 Te 4 , a van der Waals magnet, is an emergent platform for exploring Chern insulator physics. Its layered antiferromagnetic order was predicted to enable even-odd layer number dependent topological states. Furthermore, it becomes a Chern insulator when all spins are aligned by an applied magnetic field. However, the evolution of the bulk electronic structure as the magnetic state is continuously tuned and its dependence on layer number remains unexplored. Here, employing multimodal probes, we establish one-to-one correspondence between bulk electronic structure, magnetic state, topological order, and layer thickness in atomically thin MnBi 2 Te 4 devices. As the magnetic state is tuned through the canted magnetic phase, we observe a band crossing, i.e., the closing and reopening of the bulk band gap, corresponding to the concurrent topological phase transition in both even- and odd-layer-number devices. Our findings shed new light on the interplay between band topology and magnetic order in this newly discovered topological magnet.

We characterized plasmon propagation in graphene on thin films of the high-κ dielectric PbZr0.3Ti0.7O3 (PZT). Significant modulation (up to ±75%) of the plasmon wavelength was achieved with application of ultrasmall voltages (< ±1 V) across PZT. Analysis of the observed plasmonic fringes at the graphene edge indicates that carriers in graphene on PZT behave as noninteracting Dirac Fermions approximated by a semiclassical Drude response, which may be attributed to strong dielectric screening at the graphene/PZT interface. Additionally, significant plasmon scattering occurs at the grain boundaries of PZT from topographic and/or polarization induced graphene conductivity variation in the interior of graphene, reducing the overall plasmon propagation length. Lastly, through application of 2 V across PZT, we demonstrate the capability to persistently modify the plasmonic response of graphene through transient voltage application.

We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump-probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1-2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 μJ/cm(2), much smaller than fluences of ∼ 1-10 mJ/cm(2) previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 μm fiber laser. Thus, InAs--a common semiconductor with favorable plasmonic properties such as a low effective mass--has the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies.

Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ∼ 20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO2 at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 fs time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances.

We report on infrared (IR) nanoscopy of 2D plasmon excitations of Dirac fermions in graphene. This is achieved by confining mid-IR radiation at the apex of a nanoscale tip: an approach yielding 2 orders of magnitude increase in the value of in-plane component of incident wavevector q compared to free space propagation. At these high wavevectors, the Dirac plasmon is found to dramatically enhance the near-field interaction with mid-IR surface phonons of SiO(2) substrate. Our data augmented by detailed modeling establish graphene as a new medium supporting plasmonic effects that can be controlled by gate voltage.