Thickness-Dependent Cross-Plane Thermal Conductivity Measurements of Exfoliated Hexagonal Boron Nitride.

Submicrometer-thick layers of hexagonal boron nitride (hBN) exhibit high in-plane thermal conductivity and useful optical properties, and serve as dielectric encapsulation layers with low electrostatic inhomogeneity for graphene devices. Despite the promising applications of hBN as a heat spreader, the thickness dependence of its cross-plane thermal conductivity is not known, and the cross-plane phonon mean free paths (MFPs) have not been measured. We measure the cross-plane thermal conductivity of hBN flakes exfoliated from bulk crystals. We find that submicrometer thick flakes exhibit thermal conductivities up to 8.1 ± 0.5 W m-1 K-1 at 295 K, which exceeds previously reported bulk values by more than 60%. Surprisingly, the average phonon mean free path is found to be several hundred nanometers at room temperature, a factor of 5 larger than previous predictions. When planar twist interfaces are introduced into the crystal by mechanically stacking multiple thin flakes, the cross-plane thermal conductivity of the stack is found to be a factor of 7 below that of individual flakes with similar total thickness, thus providing strong evidence that phonon scattering at twist boundaries limits the maximum phonon MFPs. These results have important implications for hBN integration in nanoelectronics and improve our understanding of thermal transport in two-dimensional materials.

Imaging the breaking of electrostatic dams in graphene for ballistic and viscous fluids.

The charge carriers in a material can, under special circumstances, behave as a viscous fluid. In this work, we investigated such behavior by using scanning tunneling potentiometry to probe the nanometer-scale flow of electron fluids in graphene as they pass through channels defined by smooth and tunable in-plane p-n junction barriers. We observed that as the sample temperature and channel widths are increased, the electron fluid flow undergoes a Knudsen-to-Gurzhi transition from the ballistic to the viscous regime characterized by a channel conductance that exceeds the ballistic limit, as well as suppressed charge accumulation against the barriers. Our results are well modeled by finite element simulations of two-dimensional viscous current flow, and they illustrate how Fermi liquid flow evolves with carrier density, channel width, and temperature.

Full 2π tunable phase modulation using avoided crossing of resonances.

Active metasurfaces have been proposed as one attractive means of achieving high-resolution spatiotemporal control of optical wavefronts, having applications such as LIDAR and dynamic holography. However, achieving full, dynamic phase control has been elusive in metasurfaces. In this paper, we unveil an electrically tunable metasurface design strategy that operates near the avoided crossing of two resonances, one a spectrally narrow, over-coupled resonance and the other with a high resonance frequency tunability. This strategy displays an unprecedented upper limit of 4π range of dynamic phase modulation with no significant variations in optical amplitude, by enhancing the phase tunability through utilizing two coupled resonances. A proof-of-concept metasurface is justified analytically and verified numerically in an experimentally accessible platform using quasi-bound states in the continuum and graphene plasmon resonances, with results showing a 3π phase modulation capacity with a uniform reflection amplitude of ~0.65.

Measuring and Tuning the Potential Landscape of Electrostatically Defined Quantum Dots in Graphene.

We use Kelvin probe force microscopy (KPFM) to probe the carrier-dependent potential of an electrostatically defined quantum dot (QD) in a graphene/hexagonal boron nitride (hBN) heterostructure. We show that gate-dependent measurements enable a calibration scheme that corrects for uncertainty inherent in typical KPFM measurements and accurately reconstructs the potential well profile. Our measurements reveal how the well changes with carrier concentration, which we associate with the nonlinear dependence of graphene's work function on carrier density. These changes shift the energy levels of quasi-bound states in the QD which we can measure via scanning tunneling spectroscopy (STS). We show that the experimentally extracted energy levels closely compare with wave functions calculated from the reconstructed KPFM data. This methodology, where KPFM and STS data are simultaneously acquired from 2D materials, allows the quasiparticle response to an electrostatic potential to be determined in a self-consistent way.

Mid-infrared radiative emission from bright hot plasmons in graphene.

Carrier excitation and decay processes in graphene are of broad interest since relaxation pathways that are not present in conventional materials are enabled by a gapless Dirac electronic band structure. Here, we report that a previously unobserved decay pathway-hot plasmon emission-results in Fermi-level-dependent mid-infrared emission in graphene. Our observations of non-thermal contributions to Fermi-level-dependent radiation are an experimental demonstration of hot plasmon emission arising from a photo-inverted carrier distribution in graphene achieved via ultrafast optical excitation. Our calculations indicate that the reported plasmon emission process can be several orders of magnitude brighter than Planckian emission mechanisms in the mid-infrared spectral range. Both the use of gold nanodisks to promote scattering and localized plasmon excitation and polarization-dependent excitation measurements provide further evidence for bright hot plasmon emission. These findings define an approach for future work on ultrafast and ultrabright graphene emission processes and mid-infrared light source applications.

Emerging photonic architectures in two-dimensional opto-electronics.

The isolation of thermodynamically stable, free standing materials with single to few atom thicknesses has brought about a revolution in materials science, condensed matter physics and device engineering for opto-electronic applications. These two dimensional (2D) materials cover a broad range of electronic properties ranging from zero-band gap, semi-metallic graphene to wide band gap semiconductors in sulfides and selenides of Mo and W to metallic behavior in Ti, Nb and Ta sulfides and selenides. This permits their potential application in opto-electronic devices from terahertz frequencies up to the ultraviolet portion of the spectrum. However, their atomically thin nature poses fundamental challenges in driving efficient light-matter interactions. A range of strategies have been explored from the area of photonics and resonant optics that enhance the coupling and interaction of light with atomically thin layers to overcome this challenge. By comparing and contrasting critical advantages of integrating nanophotonic elements with 2D materials, this review highlights the challenges and advantages of such opto-electronic devices.

Electronically Tunable Perfect Absorption in Graphene.

The demand for dynamically tunable light modulation in flat optics applications has grown in recent years. Graphene nanostructures have been extensively studied as means of creating large effective index tunability, motivated by theoretical predictions of the potential for unity absorption in resonantly excited graphene nanostructures. However, the poor radiative coupling to graphene plasmonic nanoresonators and low graphene carrier mobilities from imperfections in processed graphene samples have led to low modulation depths in experimental attempts at creating tunable absorption in graphene devices. Here we demonstrate electronically tunable perfect absorption in graphene, covering less than 10% of the surface area, by incorporating multiscale nanophotonic structures composed of a low-permittivity substrate and subwavelength noble metal plasmonic antennas to enhance the radiative coupling to deep subwavelength graphene nanoresonators. To design the structures, we devised a graphical method based on effective surface admittance, elucidating the origin of perfect absorption arising from critical coupling between radiation and graphene plasmonic modes. Experimental measurements reveal 96.9% absorption in the graphene plasmonic nanostructure at 1389 cm-1, with an on/off modulation efficiency of 95.9% in reflection.

Experimental Demonstration of >230° Phase Modulation in Gate-Tunable Graphene-Gold Reconfigurable Mid-Infrared Metasurfaces.

Metasurfaces offer significant potential to control far-field light propagation through the engineering of the amplitude, polarization, and phase at an interface. We report here the phase modulation of an electronically reconfigurable metasurface and demonstrate its utility for mid-infrared beam steering. Using a gate-tunable graphene-gold resonator geometry, we demonstrate highly tunable reflected phase at multiple wavelengths and show up to 237° phase modulation range at an operating wavelength of 8.50 µm. We observe a smooth monotonic modulation of phase with applied voltage from 0° to 206° at a wavelength of 8.70 µm. Based on these experimental data, we demonstrate with antenna array calculations an average beam steering efficiency of 23% for reflected light for angles up to 30° for this range of phases, confirming the suitability of this geometry for reconfigurable mid-infrared beam steering devices. By incorporating all nonidealities of the device into the antenna array calculations including absorption losses which could be mitigated, 1% absolute efficiency is achievable up to 30°.

Gate-Variable Mid-Infrared Optical Transitions in a (Bi1-xSbx)2Te3 Topological Insulator.

We report mid-infrared spectroscopy measurements of ultrathin, electrostatically gated (Bi1-xSbx)2Te3 topological insulator films in which we observe several percent modulation of transmittance and reflectance as gating shifts the Fermi level. Infrared transmittance measurements of gated films were enabled by use of an epitaxial lift-off method for large-area transfer of topological insulator films from infrared-absorbing SrTiO3 growth substrates to thermal oxidized silicon substrates. We combine these optical experiments with transport measurements and angle-resolved photoemission spectroscopy to identify the observed spectral modulation as a gate-driven transfer of spectral weight between both bulk and 2D topological surface channels and interband and intraband channels. We develop a model for the complex permittivity of gated (Bi1-xSbx)2Te3 and find a good match to our experimental data. These results open the path for layered topological insulator materials as a new candidate for tunable, ultrathin infrared optics and highlight the possibility of switching topological optoelectronic phenomena between bulk and spin-polarized surface regimes.

Electronically tunable extraordinary optical transmission in graphene plasmonic ribbons coupled to subwavelength metallic slit arrays.

Subwavelength metallic slit arrays have been shown to exhibit extraordinary optical transmission, whereby tunnelling surface plasmonic waves constructively interfere to create large forward light propagation. The intricate balancing needed for this interference to occur allows for resonant transmission to be highly sensitive to changes in the environment. Here we demonstrate that extraordinary optical transmission resonance can be coupled to electrostatically tunable graphene plasmonic ribbons to create electrostatic modulation of mid-infrared light. Absorption in graphene plasmonic ribbons situated inside metallic slits can efficiently block the coupling channel for resonant transmission, leading to a suppression of transmission. Full-wave simulations predict a transmission modulation of 95.7% via this mechanism. Experimental measurements reveal a modulation efficiency of 28.6% in transmission at 1,397 cm(-1), corresponding to a 2.67-fold improvement over transmission without a metallic slit array. This work paves the way for enhancing light modulation in graphene plasmonics by employing noble metal plasmonic structures.

Electronic modulation of infrared radiation in graphene plasmonic resonators.

All matter at finite temperatures emits electromagnetic radiation due to the thermally induced motion of particles and quasiparticles. Dynamic control of this radiation could enable the design of novel infrared sources; however, the spectral characteristics of the radiated power are dictated by the electromagnetic energy density and emissivity, which are ordinarily fixed properties of the material and temperature. Here we experimentally demonstrate tunable electronic control of blackbody emission from graphene plasmonic resonators on a silicon nitride substrate. It is shown that the graphene resonators produce antenna-coupled blackbody radiation, which manifests as narrow spectral emission peaks in the mid-infrared. By continuously varying the nanoresonator carrier density, the frequency and intensity of these spectral features can be modulated via an electrostatic gate. This work opens the door for future devices that may control blackbody radiation at timescales beyond the limits of conventional thermo-optic modulation.

The influence of water on the optical properties of single-layer molybdenum disulfide.

Adsorbed molecules can significantly affect the properties of atomically thin materials. Physisorbed water plays a significant role in altering the optoelectronic properties of single-layer MoS2 , one such 2D film. Here the distinct quenching effect of adsorbed water on the photoluminescence of single-layer MoS2 is demonstrated through scanning-probe and optical microscopy.

Hybrid surface-phonon-plasmon polariton modes in graphene/monolayer h-BN heterostructures.

Infrared transmission measurements reveal the hybridization of graphene plasmons and the phonons in a monolayer hexagonal boron nitride (h-BN) sheet. Frequency-wavevector dispersion relations of the electromagnetically coupled graphene plasmon/h-BN phonon modes are derived from measurement of nanoresonators with widths varying from 30 to 300 nm. It is shown that the graphene plasmon mode is split into two distinct optical modes that display an anticrossing behavior near the energy of the h-BN optical phonon at 1370 cm(-1). We explain this behavior as a classical electromagnetic strong-coupling with the highly confined near fields of the graphene plasmons allowing for hybridization with the phonons of the atomically thin h-BN layer to create two clearly separated new surface-phonon-plasmon-polariton (SPPP) modes.

Highly confined tunable mid-infrared plasmonics in graphene nanoresonators.

Single-layer graphene has been shown to have intriguing prospects as a plasmonic material, as modes having plasmon wavelengths ~20 times smaller than free space (λp ~ λ0/20) have been observed in the 2-6 THz range, and active graphene plasmonic devices operating in that regime have been explored. However there is great interest in understanding the properties of graphene plasmons across the infrared spectrum, especially at energies exceeding the graphene optical phonon energy. We use infrared microscopy to observe the modes of tunable plasmonic graphene nanoresonator arrays as small as 15 nm. We map the wavevector-dependent dispersion relations for graphene plasmons at mid-infrared energies from measurements of resonant frequency changes with nanoresonator width. By tuning resonator width and charge density, we probe graphene plasmons with λp ≤ λ0/100 and plasmon resonances as high as 310 meV (2500 cm(-1)) for 15 nm nanoresonators. Electromagnetic calculations suggest that the confined plasmonic modes have a local density of optical states more than 10(6) larger than free space and thus could strongly increase light-matter interactions at infrared energies.

Observing atomic collapse resonances in artificial nuclei on graphene.

Relativistic quantum mechanics predicts that when the charge of a superheavy atomic nucleus surpasses a certain threshold, the resulting strong Coulomb field causes an unusual atomic collapse state; this state exhibits an electron wave function component that falls toward the nucleus, as well as a positron component that escapes to infinity. In graphene, where charge carriers behave as massless relativistic particles, it has been predicted that highly charged impurities should exhibit resonances corresponding to these atomic collapse states. We have observed the formation of such resonances around artificial nuclei (clusters of charged calcium dimers) fabricated on gated graphene devices via atomic manipulation with a scanning tunneling microscope. The energy and spatial dependence of the atomic collapse state measured with scanning tunneling microscopy revealed unexpected behavior when occupied by electrons.

Local electronic properties of graphene on a BN substrate via scanning tunneling microscopy.

The use of boron nitride (BN) as a substrate for graphene nanodevices has attracted much interest since the recent report that BN greatly improves the mobility of charge carriers in graphene compared to standard SiO(2) substrates. We have explored the local microscopic properties of graphene on a BN substrate using scanning tunneling microscopy. We find that BN substrates result in extraordinarily flat graphene layers that display microscopic Moiré patterns arising from the relative orientation of the graphene and BN lattices. Gate-dependent dI/dV spectra of graphene on BN exhibit spectroscopic features that are sharper than those obtained for graphene on SiO(2). We observe a significant reduction in local microscopic charge inhomogeneity for graphene on BN compared to graphene on SiO(2).

Observation of carrier-density-dependent many-body effects in graphene via tunneling spectroscopy.

We find the scanning tunneling spectra of backgated graphene monolayers to be significantly altered by many-body excitations. Experimental features in the spectra arising from electron-plasmon interactions show carrier density dependence, distinguishing them from density-independent electron-phonon features. Using a straightforward model, we are able to calculate theoretical tunneling spectra that agree well with our data, providing insight into the effects of many-body interactions on the lifetime of graphene quasiparticles.

Single-molecule charge transfer and bonding at an organic/inorganic interface: tetracyanoethylene on noble metals.

We have studied the structural and electronic properties of tetracyanoethylene (TCNE) molecules on different noble-metal surfaces using scanning tunneling spectroscopy and density functional theory. Striking differences are observed in the TCNE behavior on Au, Ag, and Cu substrates in the submonolayer limit. We explain our findings by a combination of charge-transfer and lattice-matching properties for TCNE across substrates that results in a strong variation of molecule-molecule and molecule-substrate interactions. These results have significant implications for future organic/inorganic nanoscopic devices incorporating molecule-based magnetism.