Transport and Spatial Separation of Valley Coherence via Few Layer WS2 Exciton-Polaritons.

The optical response in two-dimensional transition-metal dichalcogenides (2D TMDCs) is dominated by excitons. The lack of spatial inversion symmetry in the hexagonal lattice within each TMDC layer leads to valley-dependent excitonic emission of photoluminescence. Here, we demonstrate experimentally the spatial separation of valley coherent emission into orthogonal directions through self-resonant exciton polaritons of a free-standing three-layer (3L) WS2 waveguide. This was achieved by patterning a photonic crystal consisting of a square array of holes allowing for the far field probing of valley coherence of engendered exciton-polaritons. Furthermore, we report detailed experimental modal characterization of this coupled system in good agreement with theory. Momentum space measurements reveal a degree of valley coherence in the range 30-60%. This work provides a platform for manipulation of valley excitons in coherent light-matter states for potential implementations of valley-coherent optoelectronics.

Directing valley-polarized emission of 3†L WS2 by photonic crystal with directional circular dichroism.

The valley degree of freedom that results from broken inversion symmetry in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) has sparked a lot of interest due to its huge potential in information processing. In this experimental work, to optically address the valley-polarized emission from three-layer (3 L) thick WS2 at room temperature, we employ a SiN photonic crystal slab that has two sets of holes in a square lattice that supports directional circular dichroism engendered by delocalized guided mode resonances. By perturbatively breaking the inversion symmetry of the photonic crystal slab, we can simultaneously manipulate s and p components of the radiating field so that these resonances correspond to circularly polarized emission. The emission of excitons from distinct valleys is coupled into different radiative channels and hence separated in the farfield. This directional exciton emission from selective valleys provides a potential route for valley-polarized light emitters, which lays the groundwork for future valleytronic devices.

High-density transparent graphene arrays for predicting cellular calcium activity at depth from surface potential recordings.

Optically transparent neural microelectrodes have facilitated simultaneous electrophysiological recordings from the brain surface with the optical imaging and stimulation of neural activity. A remaining challenge is to scale down the electrode dimensions to the single-cell size and increase the density to record neural activity with high spatial resolution across large areas to capture nonlinear neural dynamics. Here we developed transparent graphene microelectrodes with ultrasmall openings and a large, transparent recording area without any gold extensions in the field of view with high-density microelectrode arrays up to 256 channels. We used platinum nanoparticles to overcome the quantum capacitance limit of graphene and to scale down the microelectrode diameter to 20 µm. An interlayer-doped double-layer graphene was introduced to prevent open-circuit failures. We conducted multimodal experiments, combining the recordings of cortical potentials of microelectrode arrays with two-photon calcium imaging of the mouse visual cortex. Our results revealed that visually evoked responses are spatially localized for high-frequency bands, particularly for the multiunit activity band. The multiunit activity power was found to be correlated with cellular calcium activity. Leveraging this, we employed dimensionality reduction techniques and neural networks to demonstrate that single-cell and average calcium activities can be decoded from surface potentials recorded by high-density transparent graphene arrays.

MoS2-enabled dual-mode optoelectronic biosensor using a water soluble variant of µ-opioid receptor for opioid peptide detection.

Owing to their unique electrical and optical properties, two-dimensional transition metal dichalcogenides have been extensively studied for their potential applications in biosensing. However, simultaneous utilization of both optical and electrical properties has been overlooked, yet it can offer enhanced accuracy and detection versitility. Here, we demonstrate a dual-mode optoelectronic biosensor based on monolayer molybdenum disulfide (MoS2) capable of producing simultaneous electrical and optical readouts of biomolecular signals. On a single platform, the biosensor exhibits a tunable photonic Fano-type optical resonance while also functioning as a field-effect transistor (FET) based on a optically transparent gate electrode. Furthermore, chemical vapor deposition grown MoS2 provides a clean surface for direct immobilization of a water-soluble variant of the µ-opioid receptor (wsMOR), via a nickel ion-mediated linker chemistry. We utilize a synthetic opioid peptide to show the operation of the electronic and optical sensing modes. The responses of both modes exhibit a similar trend with dynamic ranges of four orders of magnitude and detection limits of <1 nM. Our work explores the potential of a versatile multimodal sensing platform enabled by monolayer MoS2, since the integration of electrical and optical sensors on the same chip can offer flexibility in read-out and improve the accuracy in detection of low concentration targets.

Guiding of visible photons at the ångström thickness limit.

Optical waveguides are vital components of data communication system technologies, but their scaling down to the nanoscale has remained challenging despite advances in nano-optics and nanomaterials. Recently, we theoretically predicted that the ultimate limit of visible photon guiding can be achieved in monolayer-thick transition metal dichalcogenides. Here, we present an experimental demonstration of light guiding in an atomically thick tungsten disulfide membrane patterned as a photonic crystal structure. In this scheme, two-dimensional tungsten disulfide excitonic photoluminescence couples into quasi-guided photonic crystal modes known as resonant-type Wood's anomalies. These modes propagate via total internal reflection with only a small portion of the light diffracted to the far field. Such light guiding at the ultimate limit provides more possibilities to miniaturize optoelectronic devices and to test fundamental physical concepts.

Nitride-Based Microarray Biochips: A New Route of Plasmonic Imaging.

The desire to improve human lives has led to striking development in biosensing technologies. While the ongoing research efforts are mostly dedicated to enhancing speed and sensitivity of the sensor, a third consideration that has become increasingly important is compactness, which is strongly desired in emergency situations and personal health management. Surface plasmon resonance imaging (SPRi) is one of the few techniques that can potentially fulfill all the three goals, considering its multiplexed assay capability. However, miniaturizing SPRi biosensors remains elusive as it entails complicated optical gears. Here, we significantly slim the architecture of SPRi devices by visualizing the varied local density of states around analytes. The unusual detection scheme is realized by building a gain-assisted SPRi with InGaN quantum wells (QWs), where the QW-plasmon coupling efficiency hinges on localized refractive index variation. This new modality abolishes the prism, the polarizer, and the beam-tracking components in the most used Kretschmann configuration without compromising the performances.

Dynamic Photochemical and Optoelectronic Control of Photonic Fano Resonances via Monolayer MoS2 Trions.

Active tunability of photonic resonances is of great interest for various applications such as optical switching and modulation based on optoelectronic materials. Manipulation of charged excitons in atomically thin transition metal dichalcogenides (TMDCs) like monolayer MoS2 offers an unexplored route for diverse functionalities in optoelectronic nanodevices. Here, we experimentally demonstrate the dynamic photochemical and optoelectronic control of the photonic crystal Fano resonances by optical and electrical tuning of monolayer MoS2 refractive index via trions without any chemical treatment. The strong spatial and spectral overlap between the photonic Fano mode and the active MoS2 monolayer enables efficient modulation of the Fano resonance. Our approach offers new directions for potential applications in the development of optical modulators based on emerging 2D direct band gap semiconductors.

Unidirectional Doubly Enhanced MoS2 Emission via Photonic Fano Resonances.

Atomically thin transition metal dichalcogenides like MoS2 monolayers exhibit unique luminescent properties. However, weak quantum yield and low light absorption hinder their practical applications in two-dimensional light emitting devices. Here, we report 1300 times enhancement in photoluminescence emission from a MoS2 monolayer via simultaneous Fano resonances in a dielectric photonic crystal. The spatially extended double Fano resonance scheme allows resonant enhancement of both the MoS2 absorption and emission. We also achieve unidirectional emission within a narrow divergence angle of 5° by engineering the Fano resonance angular dispersion. Our approach provides a new platform for efficient light sources with high directionality based on emerging two-dimensional materials.

Electromechanically reconfigurable CdS nanoplate based nonlinear optical device.

Here, we report experimental demonstration of dynamic control and enhancement of second harmonic generation and two photon excited photoluminescence in CdS nanoplates via an electromechanically reconfigurable Fabry-Perot (FP) microcavity. Microcavity coupled CdS nanoplates can be configured as a single or dual wavelength nonlinear light source by tuning the pump wavelength while the output intensities can be tuned by the on-chip control voltage. Our work realizes a reconfigurable device platform with insight toward advanced optical devices based on semiconductor nanoplates for next generation on-chip tunable light sources, sensors and optomechanical systems.

Optomechanical Enhancement of Doubly Resonant 2D Optical Nonlinearity.

Emerging two-dimensional semiconductor materials possess a giant second order nonlinear response due to excitonic effects while the monolayer thickness of such active materials limits their use in practical nonlinear devices. Here, we report 3300 times optomechanical enhancement of second harmonic generation from a MoS2 monolayer in a doubly resonant on-chip optical cavity. We achieve this by engineering the nonlinear light-matter interaction in a microelectro-mechanical system enabled optical frequency doubling device based on an electrostatically tunable Fabry-Perot microresonator. Our versatile optomechanical approach will pave the way for next generation efficient on-chip tunable light sources, sensors, and systems based on molecularly thin materials.

Wavelength tunable microdisk cavity light source with a chemically enhanced MoS2 emitter.

In this work, we report an integrated narrowband light source based on thin MoS2 emissive material coupled to the high quality factor whispering gallery modes of a microdisk cavity with a spatial notch that enables easy out-coupling of emission while it yields high spatial coherence and a Gaussian intensity distribution. The active light emitting material consists of chemically enhanced bilayer MoS2 flakes with a thin atomic layer deposited SiO2 protective coating that yields 20-times brighter chemically enhanced photoluminescence compared to as-exfoliated monolayers on the microdisk. Quality factors ≈ 1000 are observed as well as a high degree of spatial coherence. We also experimentally achieve effective index tuning of cavity coupled emission over a full free spectral range. The thermal response of this system is also studied. This work provides new insights for nanophotonic light sources with atomically thin active media.

Transparent and flexible low noise graphene electrodes for simultaneous electrophysiology and neuroimaging.

Calcium imaging is a versatile experimental approach capable of resolving single neurons with single-cell spatial resolution in the brain. Electrophysiological recordings provide high temporal, but limited spatial resolution, because of the geometrical inaccessibility of the brain. An approach that integrates the advantages of both techniques could provide new insights into functions of neural circuits. Here, we report a transparent, flexible neural electrode technology based on graphene, which enables simultaneous optical imaging and electrophysiological recording. We demonstrate that hippocampal slices can be imaged through transparent graphene electrodes by both confocal and two-photon microscopy without causing any light-induced artefacts in the electrical recordings. Graphene electrodes record high-frequency bursting activity and slow synaptic potentials that are hard to resolve by multicellular calcium imaging. This transparent electrode technology may pave the way for high spatio-temporal resolution electro-optic mapping of the dynamic neuronal activity.

Optoelectromechanical multimodal biosensor with graphene active region.

A general, overarching theme in nanotechnology is the integration of multiple disparate fields to realize novel or expanded functionalities. Here, we present a graphene enabled, integrated optoelectromechanical device and demonstrate its utility for biomolecular sensing. We experimentally achieve an ultrawide linear dynamic sensing range of 5 orders of magnitude of protein concentration, an improvement over state-of-the-art single mode nanosensors by approximately 2-3 orders of magnitude, while retaining a subpicomolar lowest detection limit. Moreover, the ability to monitor and characterize adsorption events in the full optoelectromechanical space allows for the extraction of key intrinsic parameters of adsorbates and has the potential to extend the capabilities of nanosensors beyond the traditional binary-valued test for a single type of molecule. This could have significant implications for molecular detection applications at variable concentrations, such as early disease detection in biomedical diagnostics.

Plasmonically enhanced thermomechanical detection of infrared radiation.

Nanoplasmonics has been an attractive area of research due to its ability to localize and manipulate freely propagating radiation on the nanometer scale for strong light-matter interactions. Meanwhile, nanomechanics has set records in the sensing of mass, force, and displacement. In this work, we report efficient coupling between infrared radiation and nanomechanical resonators through nanoantenna enhanced thermoplasmonic effects. Using efficient conversion of electromagnetic energy to mechanical energy in this plasmo-thermomechanical platform with a nanoslot plasmonic absorber integrated directly on a nanobeam mechanical resonator, we demonstrate room-temperature detection of nanowatt level power fluctuations in infrared radiation. We expect our approach, which combines nanoplasmonics with nanomechanical resonators, to lead to optically controlled nanomechanical systems enabling unprecedented functionality in biomolecular and toxic gas sensing and on-chip mass spectroscopy.

Graphene-enabled silver nanoantenna sensors.

Silver is the ideal material for plasmonics because of its low loss at optical frequencies but is often replaced by a more lossy metal, gold. This is because of silver's tendency to tarnish and roughen, forming Ag(2)S on its surface, dramatically diminishing optical properties and rendering it unreliable for applications. By passivating the surface of silver nanostructures with monolayer graphene, atmospheric sulfur containing compounds are unable to penetrate the graphene to degrade the surface of the silver. Preventing this sulfidation eliminates the increased material damping and scattering losses originating from the unintentional Ag(2)S layer. Because it is atomically thin, graphene does not interfere with the ability of localized surface plasmons to interact with the environment in sensing applications. Furthermore, after 30 days graphene-passivated silver (Ag-Gr) nanoantennas exhibit a 2600% higher sensitivity over that of bare Ag nanoantennas and 2 orders of magnitude improvement in peak width endurance. By employing graphene in this manner, the excellent optical properties and large spectral range of silver can be functionally utilized in a variety of nanoscale plasmonic devices and applications.

Strongly enhanced molecular fluorescence inside a nanoscale waveguide gap.

We experimentally demonstrate dramatically enhanced light-matter interaction for molecules placed inside the nanometer scale gap of a plasmonic waveguide. We observe spontaneous emission rate enhancements of up to about 60 times due to strong optical localization in two dimensions. This rate enhancement is a nonresonant nature of the plasmonic waveguide under study overcoming the fundamental bandwidth limitation of conventional devices. Moreover, we show that about 85% of molecular emission couples into the waveguide highlighting the dominance of the nanoscale optical mode in competing with quenching processes. Such optics at molecular length scales paves the way toward integrated on-chip photon source, rapid transfer of quantum information, and efficient light extraction for solid-state-lighting devices.

Coherent coupling of multiple transverse modes in quantum cascade lasers.

Quantum cascade lasers are a unique laboratory for studying nonlinear laser dynamics because of their high intracavity intensity, strong intersubband optical nonlinearity, and an unusual combination of relaxation time scales. Here we investigate the nonlinear coupling between the transverse modes of quantum cascade lasers. We present evidence for stable phase coherence of multiple transverse modes over a large range of injection currents. We explain the phase coherence by a four-wave mixing interaction originating from the strong optical nonlinearity of the gain transition. The phase-locking conditions predicted by theory are supported by spectral data and both near- and far-field mode measurements.

Aligned carbon nanotubes as polarization-sensitive, molecular near-field detectors.

Near-field scanning optical microscopes are widely used in imaging of subwavelength features in various material systems and nanostructures. For a variety of applications, polarization-sensitive near-field probes can provide valuable information on the nature and symmetry of the imaged nanoparticles and emitters. Conventional near-field optical microscopy lacks in-plane polarization sensitivity. Here, we use aligned single-wall carbon nanotubes as polarization-sensitive molecular scale probes to image the transverse near-field components of an optical Hertzian dipole antenna. Because of the Raman "antenna effect" in carbon nanotubes, only the near-field components along the nanotube axis are detected. These findings demonstrate that aligned carbon nanotubes can be used as polarization-sensitive near-field detectors.

Optical properties of surface plasmon resonances of coupled metallic nanorods.

We present a systematic study of optical antenna arrays, in which the effects of coupling between the antennas, as well as of the antenna length, on the reflection spectra are investigated and compared. Such arrays can be fabricated on the facet of a fiber, and we propose a photonic device, a plasmonic optical antenna fiber probe, that can potentially be used for in-situ chemical and biological detection and surface-enhanced Raman scattering.

Near-field imaging of quantum cascade laser transverse modes.

We report near field imaging of the transverse lasing modes of quantum cascade lasers. A mid-infrared apertureless near-field scanning optical microscope was used to characterize the modes on the laser facet. A very stable mode pattern corresponding to a TM(00) mode was observed as function of increasing driving current for a narrow active region quantum cascade laser. Higher order modes were observed for devices with a larger active region width-to-wavelength ratio operated in pulsed mode close to threshold. A theoretical model is proposed to explain why specific transverse modes are preferred close to threshold. The model is in good agreement with the experimental results.