Dielectric Engineering for Manipulating Exciton Transport in Semiconductor Monolayers.

The dielectric screening from the disordered media surrounding atomically thin transition metal dichalcogenides (TMDs) monolayers modifies the effective defect energy levels and thereby the transport and energy dynamics of excitons. In this work, we study this effect in WSe2 monolayers for different combinations of surrounding dielectric media. Specifically, we study the source of the anomalous diffusion of excitons in the WSe2 monolayer and attribute the anomaly to the modification of the energy distribution of defect states in different disordered dielectric environments. We use this insight to manipulate exciton transport by engineering the dielectric environment using a graphene/hexagonal boron nitride (h-BN) moiré superlattice. Finally, we observe that the effect of dielectric disorder is even more significant at high excitation fluences, contributing to the nonequilibrium phonon drag effect. These results provide an important step toward achieving control over the exciton energy transport for next-generation opto-excitonic devices.

Optomechanical and photothermal interactions in suspended photonic crystal membranes.

We present here an optomechanical system fabricated with novel stress management techniques that allow us to suspend an ultrathin defect-free silicon photonic-crystal membrane above a Silicon-on-Insulator (SOI) substrate with a gap that is tunable to below 200 nm. Our devices are able to generate strong attractive and repulsive optical forces over a large surface area with simple in- and out- coupling and feature the strongest repulsive optomechanical coupling in any geometry to date (gOM/2π ≈65 GHz/nm). The interplay between the optomechanical and photo-thermal-mechanical dynamics is explored, and the latter is used to achieve cooling and amplification of the mechanical mode, demonstrating that our platform is well-suited for potential applications in low-power mass, force, and refractive-index sensing as well as optomechanical accelerometry.

Single particle detection in CMOS compatible photonic crystal nanobeam cavities.

We report the label-free detection of single particles using photonic crystal nanobeam cavities fabricated in silicon-on-insulator platform, and embedded inside microfluidic channels fabricated in poly-dimethylsiloxane (PDMS). Our system operates in the telecommunication wavelength band, thus leveraging the widely available, robust and tunable telecom laser sources. Using this approach, we demonstrated the detection of polystyrene nanoparticles with dimensions down to 12.5nm in radius. Furthermore, binding events of a single streptavidin molecule have been observed.

Enhanced Exciton Drift Transport through Suppressed Diffusion in One-Dimensional Guides.

Drift-diffusion dynamics is investigated in a one-dimensional (1D) exciton guide at room temperature. Spatial engineering of the exciton energy in a WSe2 monolayer is achieved using local strain to confine and direct exciton transport. An unexpected and massive deviation from the Einstein relation is observed and correlated to exciton capture by defects. We find that the capture reduces exciton temperature and diffusion so much that drift transport visibility improves to 38% as excitons traverse asymmetrically over regions with occupied defect states. Based on measurements over multiple potential gradients, we estimate the exciton mobility to be 169 ± 39 cm2/(eV s) at room temperature. Experiments at elevated exciton densities reveal that the exciton drift velocity monotonically increases with exciton density, unlike exciton mobility, due to contributions from nonequilibrium many-body effects.

Submicrometer-wide amorphous and polycrystalline anatase TiO2 waveguides for microphotonic devices.

We demonstrate amorphous and polycrystalline anatase TiO(2) thin films and submicrometer-wide waveguides with promising optical properties for microphotonic devices. We deposit both amorphous and polycrystalline anatase TiO(2) using reactive sputtering and define waveguides using electron-beam lithography and reactive ion etching. For the amorphous TiO(2), we obtain propagation losses of 0.12 ± 0.02 dB/mm at 633 nm and 0.04 ± 0.01 dB/mm at 1550 nm in thin films and 2.6 ± 0.5 dB/mm at 633 nm and 0.4 ± 0.2 dB/mm at 1550 nm in waveguides. Using single-mode amorphous TiO(2) waveguides, we characterize microphotonic features including microbends and optical couplers. We show transmission of 780-nm light through microbends having radii down to 2 µm and variable signal splitting in microphotonic couplers with coupling lengths of 10 µm.

Integrated TiO2 resonators for visible photonics.

We demonstrate waveguide-coupled titanium dioxide (TiO(2) racetrack resonators with loaded quality factors of 2.2×10(4) for the visible wavelengths. The structures were fabricated in sputtered TiO(2) thin films on oxidized silicon substrates using standard top-down nanofabrication techniques, and passively probed in transmission measurements using a tunable red laser.

Torsional periodic lattice distortions and diffraction of twisted 2D materials.

Twisted 2D materials form complex moiré structures that spontaneously reduce symmetry through picoscale deformation within a mesoscale lattice. We show twisted 2D materials contain a torsional displacement field comprised of three transverse periodic lattice distortions (PLD). The torsional PLD amplitude provides a single order parameter that concisely describes the structural complexity of twisted bilayer moirés. Moreover, the structure and amplitude of a torsional periodic lattice distortion is quantifiable using rudimentary electron diffraction methods sensitive to reciprocal space. In twisted bilayer graphene, the torsional PLD begins to form at angles below 3.89° and the amplitude reaches 8 pm around the magic angle of 1. 1°. At extremely low twist angles (e.g. below 0.25°) the amplitude increases and additional PLD harmonics arise to expand Bernal stacked domains separated by well defined solitonic boundaries. The torsional distortion field in twisted bilayer graphene is analytically described and has an upper bound of 22.6 pm. Similar torsional distortions are observed in twisted WS2, CrI3, and WSe2/MoSe2.

Two-dimensional charge order stabilized in clean polytype heterostructures.

Compelling evidence suggests distinct correlated electron behavior may exist only in clean 2D materials such as 1T-TaS2. Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers disrupts correlation-driven quantum behavior. Here we demonstrate a route to realizing fragile 2D quantum states through endotaxial polytype engineering of van der Waals materials. The true isolation of 2D charge density waves (CDWs) between metallic layers stabilizes commensurate long-range order and lifts the coupling between neighboring CDW layers to restore mirror symmetries via interlayer CDW twinning. The twinned-commensurate charge density wave (tC-CDW) reported herein has a single metal-insulator phase transition at ~350 K as measured structurally and electronically. Fast in-situ transmission electron microscopy and scanned nanobeam diffraction map the formation of tC-CDWs. This work introduces endotaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication.

Fabrication and characterization of high-quality-factor silicon nitride nanobeam cavities.

We present the fabrication and characterization of high-quality-factor (Q) Si3N4 photonic crystal nanobeam cavities at visible wavelengths for coupling to nitrogen-vacancy centers in a cavity QED system. Confocal microphotoluminescence analysis of the nanobeam cavities demonstrates quality factors up to Q ~ 55,000, which are limited by the resolution of our grating spectrometer. This is a 1-order-of-magnitude improvement over previous SiNx cavities at this important wavelength range. We also demonstrate coarse tuning of cavity resonances across 600-700 nm by lithographically scaling the size of fabricated devices.

Piezoelectric Modulation of Excitonic Properties in Monolayer WSe2 under Strong Dielectric Screening.

We investigate the interaction of excitons in monolayer WSe2 with the piezoelectric field of surface acoustic wave (SAW) at room temperature using photoluminescence (PL) spectroscopy and report a large in-plane exciton polarizability of 8.43 ± 0.18 × 10-6 Dm/V. Such large polarizability arises due to the strong dielectric screening from the piezoelectric substrate. In addition, we show that the exciton-piezoelectric field interaction and population distribution between neutral excitons and trions can be optically manipulated by controlling the field screening using photogenerated free carriers. Finally, we model the broadening of the exciton PL line width and report that the interaction is dominated by type-II band edge modulation, because of the in-plane electric field in the system. The results help understand the interaction of excitons in monolayer transition-metal dichalcogenides that will aid in controlled manipulation of excitonic properties for applications in sensing, detection, and on-chip communication.

Waveguiding properties of perylene microcrystals synthesized by retarding the growth along the π-stack direction.

Selective, hard to realize growth retardation of the π-stacking direction over the edge-packing direction has been achieved in perylene microcrystals using an aryl amphiphile. The perylene microcrystals grow predominantly along the edge-packing direction resulting in novel and hitherto unknown perylene square rods. The rods show exciton-polariton waveguiding along the rod axis even though it corresponds to pure edge-packing of the molecules, which is unprecedented in organic microcrystals.

Neutralizing Defect States in MoS2 Monolayers.

We report a method to neutralize the mid-gap defect states in MoS2 monolayers using laser soaking of an organic/transition metal oxide (TMO) blend thin film. The treated MoS2 monolayer shows negligible emission from defect states as compared to the as-exfoliated MoS2, accompanied by a photoluminescence quantum yield improvement from 0.018 to 4.5% at excitation power densities of 10 W/cm2. The effectiveness of the method toward defect neutralization is governed by the polaron pair generated at the organic/TMO interface, the diffusion of free electrons, and the subsequent formation of TMO radicals at the MoS2 monolayer. The treated monolayers are stable in air, vacuum, and acetone environments, potentially enabling the fabrication of defect-free optoelectronic devices based on 2D materials and 2D/organic heterojunctions.

Interlayer Exciton Transport in MoSe2/WSe2 Heterostructures.

A moiré superlattice formed by stacking two lattice mismatched transition metal dichalcogenide monolayers, functions as a diffusion barrier that affects the energy transport and dynamics of interlayer excitons (electron and hole spatially concentrated in different monolayers). In this work, we experimentally quantify the diffusion barrier experienced by interlayer excitons in hexagonal boron nitride-encapsulated molybdenum diselenide/tungsten diselenide (MoSe2/WSe2) heterostructures with different twist angles. We observe the localization of interlayer excitons at low temperature and the temperature-activated diffusivity as a function of twist angle and hence attribute it to the deep periodic potentials arising from the moiré superlattice. We further support the observations with theoretical calculations, Monte Carlo simulations, and a three-level model that represents the exciton dynamics at various temperatures.

Programmable photonic crystal nanobeam cavities.

We present dynamically reconfigurable photonic crystal nanobeam cavities, operating at ~1550 nm, that can be continuously and reversibly tuned over a 9.5 nm wavelength range. The devices are formed by two coupled nanobeam cavities, and the tuning is achieved by varying the lateral gap between the nanobeams. An electrostatic force, obtained by applying bias voltages directly to the nanobeams, is used to control the spacing between the nanobeams, which in turn results in tuning of the cavity resonance. The observed tuning trends were confirmed through simulations that modeled the electrostatic actuation as well as the optical resonances in our reconfigurable geometries.

Energy Transport of Hybrid Charge-Transfer Excitons.

We investigate the energy transport in an organic-inorganic hybrid platform formed between semiconductors that support stable room-temperature excitons. We find that following photoexcitation, fast-moving hot hybrid charge-transfer excitons (HCTEs) are formed in about 36 ps via scattering with optical phonons at the interface between j-aggregates of organic dye and inorganic monolayer MoS2. Once the energy falls below the optical phonon energy, the excess kinetic energy is relaxed slowly via acoustic phonon scattering, resulting in energy transport that is dominated by fast-moving hot HCTEs that transition into cold HCTEs in about 110 ps. We model the exciton-phonon interactions using Fröhlich and deformation potential theory and attribute the prolonged transport of hot HCTEs to phonon bottleneck. We find that the measured diffusivity of HCTEs in both hot and cold regions of transport was higher than the diffusivity of MoS2 A exciton and verify these results by conducting the experiments with different excitation energies. This work not only provides significant insight into the initial energy transport of HCTEs at organic-inorganic hybrid interfaces but also contributes to the formulation of a complete physical picture of the energy dynamics in hybrid materials, which are poised to advance applications in energy conversion and optoelectronic devices.

Efficient Energy Transfer across Organic-2D Inorganic Heterointerfaces.

Combining organic and inorganic semiconductors enables us to integrate complementary advantages of each material system into a single hybrid material platform. Here, we report a study on the energy transport across a hybrid interface consisting of j-aggregates of organic dye and monolayer molybdenum disulfide (MoS2). The excellent overlap between the photoluminescence spectra of j-aggregates and the absorption of MoS2 B-exciton enables the material system to be used to study Förster resonance energy transfer (FRET) across the hybrid interface. We report a short Förster radius of 1.88 nm for the hybrid system. We achieve this by fabricating photodetectors based on the hybrid organic-inorganic interface that combine the high absorption of organics with the high-charge mobility of inorganics. Concomitantly, the hybrid photodetectors show nearly 93 ± 5% enhancement of photoresponsivity in the excitonic spectral overlap regime due to efficient energy transfer (ET) from j-aggregate to MoS2. This work not only provides valuable insight into the ET mechanism across such hybrid organic-inorganic interfaces but also demonstrates the feasibility of the platform for designing efficient energy conversion and optoelectronic devices.

Surface plasmon polariton laser based on a metallic trench Fabry-Perot resonator.

Recent years have witnessed a growing interest in the development of small-footprint lasers for potential applications in small-volume sensing and on-chip optical communications. Surface plasmons-electromagnetic modes evanescently confined to metal-dielectric interfaces-offer an effective route to achieving lasing at nanometer-scale dimensions when resonantly amplified in contact with a gain medium. We achieve narrow-linewidth visible-frequency lasing at room temperature by leveraging surface plasmons propagating in an open Fabry-Perot cavity formed by a flat metal surface coated with a subwavelength-thick layer of optically pumped gain medium and orthogonally bound by a pair of flat metal sidewalls. We show how the lasing threshold and linewidth can be lowered by incorporating a low-profile tapered grating on the cavity floor to couple the excitation beam into a pump surface plasmon polariton providing a strong modal overlap with the gain medium. Low-perturbation transmission-configuration sampling of the lasing plasmon mode is achieved via an evanescently coupled recessed nanoslit, opening the way to high-figure of merit refractive index sensing of analytes interacting with the open metallic trench.

Ultracompact low-threshold organic laser.

We report an ultracompact low-threshold laser with an Alq3:DCM host:guest molecular organic thin film gain layer. The device uses a photonic crystal nanobeam cavity which provides a high quality factor to mode volume (Q/V) ratio and increased spontaneous emission factor along with a small footprint. Lasing is observed with a threshold of 4.2 µJ/cm(2) when pumped by femtosecond pulses of λ = 400 nm wavelength light. We also model the dynamics of the laser and show good agreement with the experimental data. The inherent waveguide geometry of the structure enables easy on-chip integration with potential applications in biochemical sensing, inertial sensors, and data communication.

Visualization of exciton transport in ordered and disordered molecular solids.

Transport of nanoscale energy in the form of excitons is at the core of photosynthesis and the operation of a wide range of nanostructured optoelectronic devices such as solar cells, light-emitting diodes and excitonic transistors. Of particular importance is the relationship between exciton transport and nanoscale disorder, the defining characteristic of molecular and nanostructured materials. Here we report a spatial, temporal and spectral visualization of exciton transport in molecular crystals and disordered thin films. Using tetracene as an archetype molecular crystal, the imaging reveals that exciton transport occurs by random walk diffusion, with a transition to subdiffusion as excitons become trapped. By controlling the morphology of the thin film, we show that this transition to subdiffusive transport occurs at earlier times as disorder is increased. Our findings demonstrate that the mechanism of exciton transport depends strongly on the nanoscale morphology, which has wide implications for the design of excitonic materials and devices.

All optical reconfiguration of optomechanical filters.

Reconfigurable optical filters are of great importance for applications in optical communication and information processing. Of particular interest are tuning techniques that take advantage of mechanical deformation of the devices, as they offer wider tuning range. Here we demonstrate reconfiguration of coupled photonic crystal nanobeam cavities by using optical gradient force induced mechanical actuation. Propagating waveguide modes that exist over a wide wavelength range are used to actuate the structures and control the resonance of localized cavity modes. Using this all-optical approach, more than 18 linewidths of tuning range is demonstrated. Using an on-chip temperature self-referencing method, we determine that 20% of the total tuning was due to optomechanical reconfiguration and the rest due to thermo-optic effects. By operating the device at frequencies higher than the thermal cutoff, we show high-speed operation dominated by just optomechanical effects. Independent control of mechanical and optical resonances of our structures is also demonstrated.