Erratum: Phonon-Mediated Interlayer Conductance in Twisted Graphene Bilayers [Phys. Rev. Lett. 109, 236604 (2012)].

This corrects the article DOI: 10.1103/PhysRevLett.109.236604.

Planar hyperbolic polaritons in 2D van der Waals materials.

Anisotropic planar polaritons - hybrid electromagnetic modes mediated by phonons, plasmons, or excitons - in biaxial two-dimensional (2D) van der Waals crystals have attracted significant attention due to their fundamental physics and potential nanophotonic applications. In this Perspective, we review the properties of planar hyperbolic polaritons and the variety of methods that can be used to experimentally tune them. We argue that such natural, planar hyperbolic media should be fairly common in biaxial and uniaxial 2D and 1D van der Waals crystals, and identify the untapped opportunities they could enable for functional (i.e. ferromagnetic, ferroelectric, and piezoelectric) polaritons. Lastly, we provide our perspectives on the technological applications of such planar hyperbolic polaritons.

Twisted Two-Dimensional Material Stacks for Polarization Optics.

The ability to control the light polarization state is critically important for diverse applications in information processing, telecommunications, and spectroscopy. Here, we propose that a stack of anisotropic van der Waals materials can facilitate the building of optical elements with Jones matrices of unitary, Hermitian, non-normal, singular, degenerate, and defective classes. We show that the twisted stack with electrostatic control can function as arbitrary-birefringent wave-plate or arbitrary polarizer with tunable degree of non-normality, which in turn give access to plethora of polarization transformers including rotators, pseudorotators, symmetric and ambidextrous polarizers. Moreover, we discuss an electrostatic-reconfigurable stack which can be tuned to operate as four different polarizers and be used for Stokes polarimetry.

Nanophotonic biosensors harnessing van der Waals materials.

Low-dimensional van der Waals (vdW) materials can harness tightly confined polaritonic waves to deliver unique advantages for nanophotonic biosensing. The reduced dimensionality of vdW materials, as in the case of two-dimensional graphene, can greatly enhance plasmonic field confinement, boosting sensitivity and efficiency compared to conventional nanophotonic devices that rely on surface plasmon resonance in metallic films. Furthermore, the reduction of dielectric screening in vdW materials enables electrostatic tunability of different polariton modes, including plasmons, excitons, and phonons. One-dimensional vdW materials, particularly single-walled carbon nanotubes, possess unique form factors with confined excitons to enable single-molecule detection as well as in vivo biosensing. We discuss basic sensing principles based on vdW materials, followed by technological challenges such as surface chemistry, integration, and toxicity. Finally, we highlight progress in harnessing vdW materials to demonstrate new sensing functionalities that are difficult to perform with conventional metal/dielectric sensors.

Image polaritons in boron nitride for extreme polariton confinement with low losses.

Polaritons in two-dimensional materials provide extreme light confinement that is difficult to achieve with metal plasmonics. However, such tight confinement inevitably increases optical losses through various damping channels. Here we demonstrate that hyperbolic phonon polaritons in hexagonal boron nitride can overcome this fundamental trade-off. Among two observed polariton modes, featuring a symmetric and antisymmetric charge distribution, the latter exhibits lower optical losses and tighter polariton confinement. Far-field excitation and detection of this high-momenta mode become possible with our resonator design that can boost the coupling efficiency via virtual polariton modes with image charges that we dub 'image polaritons'. Using these image polaritons, we experimentally observe a record-high effective index of up to 132 and quality factors as high as 501. Further, our phenomenological theory suggests an important role of hyperbolic surface scattering in the damping process of hyperbolic phonon polaritons.

Graphene acoustic plasmon resonator for ultrasensitive infrared spectroscopy.

One of the fundamental hurdles in plasmonics is the trade-off between electromagnetic field confinement and the coupling efficiency with free-space light, a consequence of the large momentum mismatch between the excitation source and plasmonic modes. Acoustic plasmons in graphene, in particular, have an extreme level of field confinement, as well as an extreme momentum mismatch. Here, we show that this fundamental compromise can be overcome and demonstrate a graphene acoustic plasmon resonator with nearly perfect absorption (94%) of incident mid-infrared light. This high efficiency is achieved by utilizing a two-stage coupling scheme: free-space light coupled to conventional graphene plasmons, which then couple to ultraconfined acoustic plasmons. To realize this scheme, we transfer unpatterned large-area graphene onto template-stripped ultraflat metal ribbons. A monolithically integrated optical spacer and a reflector further boost the enhancement. We show that graphene acoustic plasmons allow ultrasensitive measurements of absorption bands and surface phonon modes in ångström-thick protein and SiO2 layers, respectively. Our acoustic plasmon resonator platform is scalable and can harness the ultimate level of light-matter interactions for potential applications including spectroscopy, sensing, metasurfaces and optoelectronics.

Intrinsically ultrastrong plasmon-exciton interactions in crystallized films of carbon nanotubes.

In cavity quantum electrodynamics, optical emitters that are strongly coupled to cavities give rise to polaritons with characteristics of both the emitters and the cavity excitations. We show that carbon nanotubes can be crystallized into chip-scale, two-dimensionally ordered films and that this material enables intrinsically ultrastrong emitter-cavity interactions: Rather than interacting with external cavities, nanotube excitons couple to the near-infrared plasmon resonances of the nanotubes themselves. Our polycrystalline nanotube films have a hexagonal crystal structure, ∼25-nm domains, and a 1.74-nm lattice constant. With this extremely high nanotube density and nearly ideal plasmon-exciton spatial overlap, plasmon-exciton coupling strengths reach 0.5 eV, which is 75% of the bare exciton energy and a near record for room-temperature ultrastrong coupling. Crystallized nanotube films represent a milestone in nanomaterials assembly and provide a compelling foundation for high-ampacity conductors, low-power optical switches, and tunable optical antennas.

Graphene-enabled and directed nanomaterial placement from solution for large-scale device integration.

Directed placement of solution-based nanomaterials at predefined locations with nanoscale precision limits bottom-up integration in semiconductor process technology. We report a method for electric-field-assisted placement of nanomaterials from solution by means of large-scale graphene layers featuring nanoscale deposition sites. The structured graphene layers are prepared via either transfer or synthesis on standard substrates, and then are removed once nanomaterial deposition is completed, yielding material assemblies with nanoscale resolution that cover surface areas >1 mm2. In order to demonstrate the broad applicability, we have assembled representative zero-dimensional, one-dimensional, and two-dimensional semiconductors at predefined substrate locations and integrated them into nanoelectronic devices. Ultimately, this method opens a route to bottom-up integration of nanomaterials for industry-scale applications.

Nanomaterial-Based Plasmon-Enhanced Infrared Spectroscopy.

Surface-enhanced infrared absorption (SEIRA) has attracted increasing attention due to the potential of infrared spectroscopy in applications such as molecular trace sensing of solids, polymers, and proteins, specifically fueled by recent substantial developments in infrared plasmonic materials and engineered nanostructures. Here, the significant progress achieved in the past decades is reviewed, along with the current state of the art of SEIRA. In particular, the plasmonic properties of a variety of nanomaterials are discussed (e.g., metals, semiconductors, and graphene) along with their use in the design of efficient SEIRA configurations. To conclude, perspectives on potential applications, including single-molecule detection and in vivo bioassays, are presented.

Strong and Broadly Tunable Plasmon Resonances in Thick Films of Aligned Carbon Nanotubes.

Low-dimensional plasmonic materials can function as high quality terahertz and infrared antennas at deep subwavelength scales. Despite these antennas' strong coupling to electromagnetic fields, there is a pressing need to further strengthen their absorption. We address this problem by fabricating thick films of aligned, uniformly sized semiconducting carbon nanotubes and showing that their plasmon resonances are strong, narrow, and broadly tunable. With thicknesses ranging from 25 to 250 nm, our films exhibit peak attenuation reaching 70%, ensemble quality factors reaching 9, and electrostatically tunable peak frequencies by a factor of 2.3. Excellent nanotube alignment leads to the attenuation being 99% linearly polarized along the nanotube axis. Increasing the film thickness blueshifts the plasmon resonators down to peak wavelengths as low as 1.4 µm, a new near-infrared regime in which they can both overlap the S11 nanotube exciton energy and access the technologically important infrared telecom band.

Coherent Plasmon and Phonon-Plasmon Resonances in Carbon Nanotubes.

Carbon nanotubes provide a rare access point into the plasmon physics of one-dimensional electronic systems. By assembling purified nanotubes into uniformly sized arrays, we show that they support coherent plasmon resonances, that these plasmons couple to nanotube and substrate phonons, and that the resulting phonon-plasmon resonances have quality factors as high as 10. Because nanotube plasmons intensely strengthen electromagnetic fields and light-matter interactions, they provide a compelling platform for surface-enhanced spectroscopy and tunable optical devices at deep-subwavelength scales.

A Platform for Analysis of Nanoscale Liquids with an Array of Sensor Devices Based on Two-Dimensional Material.

Analysis of nanoscale liquids, including wetting and flow phenomena, is a scientific challenge with far reaching implications for industrial technologies. We report the conception, development, and application of an integrated platform for the experimental characterization of liquids at the nanometer scale. The platform combines the functionalities of a two-dimensional electronic array of sensor devices with in situ application of highly sensitive optical microspectroscopy and atomic force microscopy. We demonstrate the performance capabilities of the platform with an embodiment based on an array of optically transparent graphene sensors. The application of electronic and optical sensing in the platform allows for differentiating between liquids electronically, for determining a liquid's molecular fingerprint, and for monitoring surface wetting dynamics in real time. In order to explore the platform's sensitivity limits, we record topographies and optical spectra of individual, spatially isolated sessile oil emulsion droplets having volumes of less than ten attoliters. The results demonstrate that integrated measurement functionalities based on two-dimensional materials have the potential to push lab-on-chip based analysis from the microscale to the nanoscale.

Polaritons in layered two-dimensional materials.

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, low-loss infrared-active phonon-polaritons exhibit hyperbolic behaviour for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transition metal dichalcogenides, reduced screening in the 2D limit leads to optically prominent excitons with large binding energy, with these polaritonic modes having been recently observed with scanning near-field optical microscopy. Here, we review recent progress in state-of-the-art experiments, and survey the vast library of polaritonic modes in 2D materials, their optical spectral properties, figures of merit and application space. Taken together, the emerging field of 2D material polaritonics and their hybrids provide enticing avenues for manipulating light-matter interactions across the visible, infrared to terahertz spectral ranges, with new optical control beyond what can be achieved using traditional bulk materials.

Power Dissipation and Electrical Breakdown in Black Phosphorus.

We report operating temperatures and heating coefficients measured in a multilayer black phosphorus device as a function of injected electrical power. By combining micro-Raman spectroscopy and electrical transport measurements, we have observed a linear temperature increase up to 600 K at a power dissipation rate of 0.896 K µm(3)/mW. By further increasing the bias voltage, we determined the threshold power and temperature for electrical breakdown and analyzed the fracture in the black phosphorus layer that caused the device failure by means of scanning electron microscopy and atomic force microscopy. The results will benefit the research and development of electronics and optoelectronics based on novel two-dimensional materials.

Tunable Light-Matter Interaction and the Role of Hyperbolicity in Graphene-hBN System.

Hexagonal boron nitride (hBN) is a natural hyperbolic material, which can also accommodate highly dispersive surface phonon-polariton modes. In this paper, we examine theoretically the mid-infrared optical properties of graphene-hBN heterostructures derived from their coupled plasmon-phonon modes. We find that the graphene plasmon couples differently with the phonons of the two Reststrahlen bands, owing to their different hyperbolicity. This also leads to distinctively different interaction between an external quantum emitter and the plasmon-phonon modes in the two bands, leading to substantial modification of its spectrum. The coupling to graphene plasmons allows for additional gate tunability in the Purcell factor and narrow dips in its emission spectra.

Plasmon-plasmon hybridization and bandwidth enhancement in nanostructured graphene.

Graphene plasmonic structures with long-range layering periodicity are presented. Resonance energy scaling with the number of graphene layers involved in plasmonic excitation allows these structures to support multiple plasmonic modes that couple and hybridize due to their physical proximity. Hybridized states exhibit bandwidth enhancements of 100-200% compared to unhybridized modes, and resonance energies deviate from what is usually observed in coupled plasmonic systems. Origins of this behavior are discussed, and experimental observations are computationally modeled. This work is a precursor and template for the study of plasmonic hybridization in other two-dimensional material systems with layering periodicity.

Hot spot dynamics in carbon nanotube array devices.

We report on the dynamics of spatial temperature distributions in aligned semiconducting carbon nanotube array devices with submicrometer channel lengths. By using high-resolution optical microscopy in combination with electrical transport measurements, we observe under steady state bias conditions the emergence of time-variable, local temperature maxima with dimensions below 300 nm, and temperatures above 400 K. On the basis of time domain cross-correlation analysis, we investigate how the intensity fluctuations of the thermal radiation patterns are correlated with the overall device current. The analysis reveals the interdependence of electrical current fluctuations and time-variable hot spot formation that limits the overall device performance and, ultimately, may cause device degradation. The findings have implications for the future development of carbon nanotube-based technologies.

Black phosphorus photodetector for multispectral, high-resolution imaging.

Black phosphorus is a layered semiconductor that is intensely researched in view of applications in optoelectronics. In this letter, we investigate a multilayer black phosphorus photodetector that is capable of acquiring high-contrast (V > 0.9) images both in the visible (λVIS = 532 nm) as well as in the infrared (λIR = 1550 nm) spectral regime. In a first step, by using photocurrent microscopy, we map the active area of the device and we characterize responsivity and gain. In a second step, by deploying the black phosphorus device as a point-like detector in a confocal microsope setup, we acquire diffraction-limited optical images with submicron resolution. The results demonstrate the usefulness of black phosphorus as an optoelectronic material for hyperspectral imaging applications.

Plasmons and screening in monolayer and multilayer black phosphorus.

Black phosphorus exhibits a high degree of band anisotropy. However, we find that its in-plane static screening remains relatively isotropic for momenta relevant to elastic long-range scattering processes. On the other hand, the collective electronic excitations in the system exhibit a strong anisotropy. Band nonparabolicity, due to interband couplings, leads to a plasmon frequency which scales as nß, where n is the carrier concentration, and ß<1/2. Screening and charge distribution in the out-of-plane direction are also studied using a nonlinear Thomas-Fermi model.

Substrate-sensitive mid-infrared photoresponse in graphene.

We report mid-infrared photocurrent spectra of graphene nanoribbon arrays on SiO2 dielectrics showing dual signatures of the substrate interaction. First, hybrid polaritonic modes of graphene plasmons and dielectric surface polar phonons produce a thermal photocurrent in graphene with spectral features that are tunable by gate voltage, nanoribbon width, and light polarization. Second, phonon polaritons associated with the substrate are excited, which indirectly heat up the graphene, leading to a graphene photocurrent with fixed spectral features. Models for other commonly used substrates show that the responsivity of graphene infrared photodetectors can be tailored to specific mid-IR frequency bands by the choice of the substrate.