DNA-mediated assembly of Au bipyramids into anisotropic light emitting kagome superlattices.

Colloidal crystal engineering with DNA allows one to design diverse superlattices with tunable lattice symmetry, composition, and spacing. Most of these structures follow the complementary contact model, maximizing DNA hybridization on building blocks and producing relatively close-packed lattices. Here, low-symmetry kagome superlattices are assembled from DNA-modified gold bipyramids that can engage only in partial DNA surface matching. The bipyramid dimensions and DNA length can be engineered for two different superlattices with rhombohedral unit cells, including one composed of a periodic stacking of kagome lattices. Enabled by the partial facet alignment, the kagome lattices exhibit lattice distortion, bipyramid twisting, and planar chirality. When conjugated with Cy-5 dyes, the kagome lattices serve as cavities with high-density optical states and large Purcell factors along lateral directions, leading to strong dipole radiation along the z axis and facet-dependent light emission. Such complex optical properties make these materials attractive for lasers, displays, and quantum sensing constructs.

Metasurface enabled broadband all optical edge detection in visible frequencies.

Image processing is of fundamental importance for numerous modern technologies. In recent years, due to increasing demand for real-time and continuous data processing, metamaterial and metasurface based all-optical computation techniques emerged as a promising alternative to digital computation. Most of the pioneer research focused on all-optical edge detection as a fundamental step of image processing. Metasurfaces have been shown to enable real time edge detection with low to no power consumption. However, the previous demonstrations were subjected to the several limitations such as need for oblique-incidence, polarization dependence, need for additional polarizers, narrow operation bandwidth, being limited with processing in 1D, operation with coherent light only, and requiring digital post-processing. Here, we propose and experimentally demonstrate 2D isotropic, polarization-independent, broadband edge detection with high transmission efficiency under both coherent and incoherent illumination along the visible frequency range using a metasurface based on Fourier optics principles.

Open-channel metal particle superlattices.

Although tremendous advances have been made in preparing porous crystals from molecular precursors1,2, there are no general ways of designing and making topologically diversified porous colloidal crystals over the 10-1,000 nm length scale. Control over porosity in this size range would enable the tailoring of molecular absorption and storage, separation, chemical sensing, catalytic and optical properties of such materials. Here, a universal approach for synthesizing metallic open-channel superlattices with pores of 10 to 1,000 nm from DNA-modified hollow colloidal nanoparticles (NPs) is reported. By tuning hollow NP geometry and DNA design, one can adjust crystal pore geometry (pore size and shape) and channel topology (the way in which pores are interconnected). The assembly of hollow NPs is driven by edge-to-edge rather than face-to-face DNA-DNA interactions. Two new design rules describing this assembly regime emerge from these studies and are then used to synthesize 12 open-channel superlattices with control over crystal symmetry, channel geometry and topology. The open channels can be selectively occupied by guests of the appropriate size and that are modified with complementary DNA (for example, Au NPs).

Monolayer Plasmonic Nanoframes as Large-Area, Broadband Metasurface Absorbers.

Broadband absorbers are useful ultraviolet protection, energy harvesting, sensing, and thermal imaging. The thinner these structures are, the more device-relevant they become. However, it is difficult to synthesize ultrathin absorbers in a scalable and straightforward manner. A general and straightforward synthetic strategy for preparing ultrathin, broadband metasurface absorbers that do not rely on cumbersome lithographic steps is reported. These materials are prepared through the surface-assembly of plasmonic octahedral nanoframes (NFs) into large-area ordered monolayers via drop-casting with subsequent air-drying at room temperature. This strategy is used to produce three types of ultrathin broadband absorbers with thicknesses of ≈200 nm and different lattice symmetries (loose hexagonal, twisted hexagonal, dense hexagonal), all of which exhibit efficient light absorption (≈90%) across wavelengths ranging from 400-800 nm. Their broadband absorption is attributed to the hollow morphologies of the NFs, the incorporation of a high-loss material (i.e., Pt), and the strong field enhancement resulting from surface assembly. The broadband absorption is found to be polarization-independent and maintained for a wide range of incidence angles (±45°). The ability to design and fabricate broadband metasurface absorbers using this high-throughput surface-based assembly strategy is a significant step toward the large-scale, rapid manufacturing of nanophotonic structures and devices.

Neural networks enabled forward and inverse design of reconfigurable metasurfaces.

Nanophotonics has joined the application areas of deep neural networks (DNNs) in recent years. Various network architectures and learning approaches have been employed to design and simulate nanophotonic structures and devices. Design and simulation of reconfigurable metasurfaces is another promising application area for neural network enabled nanophotonic design. The tunable optical response of these metasurfaces rely on the phase transitions of phase-change materials, which correspond to significant changes in their dielectric permittivity. Consequently, simulation and design of these metasurfaces requires the ability to model a diverse span of optical properties. In this work, to realize forward and inverse design of reconfigurable metasurfaces, we construct forward and inverse networks to model a wide range of optical characteristics covering from lossless dielectric to lossy plasmonic materials. As proof-of-concept demonstrations, we design a Ge2Sb2Te5 (GST) tunable resonator and a VO2 tunable absorber using our forward and inverse networks, respectively.

Highly Efficient Light Absorption of Monolayer Graphene by Quasi-Bound State in the Continuum.

Graphene is an ideal ultrathin material for various optoelectronic devices, but poor light-graphene interaction limits its further applications particularly in the visible (Vis) to near-infrared (NIR) region. Despite tremendous efforts to improve light absorption in graphene, achieving highly efficient light absorption of monolayer graphene within a comparatively simple architecture is still urgently needed. Here, we demonstrate the interesting attribute of bound state in the continuum (BIC) for highly efficient light absorption of graphene by using a simple Si-based photonic crystal slab (PCS) with a slit. Near-perfect absorption of monolayer graphene can be realized due to high confinement of light and near-field enhancement in the Si-based PCS, where BIC turns into quasi-BIC due to the symmetry-breaking of the structure. Theoretical analysis based on the coupled mode theory (CMT) is proposed to evaluate the absorption performances of monolayer graphene integrated with the symmetry-broken PCS, which indicates that high absorption of graphene is feasible at critical coupling based on the destructive interference of transmission light. Moreover, the absorption spectra of the monolayer graphene are stable to the variations of the structural parameters, and the angular tolerances of classical incidence can be effectively improved via full conical incidence. By using the full conical incidence, the angular bandwidths for the peak absorptivity and for the central wavelength of graphene absorption can be enhanced more than five times and 2.92 times, respectively. When the Si-based PCS with graphene is used in refractive index sensors, excellent sensing performances with sensitivity of 604 nm/RIU and figure of merit (FoM) of 151 can be achieved.

Lithography-free IR polarization converters via orthogonal in-plane phonons in α-MoO3 flakes.

Exploiting polaritons in natural vdW materials has been successful in achieving extreme light confinement and low-loss optical devices and enabling simplified device integration. Recently, α-MoO3 has been reported as a semiconducting biaxial vdW material capable of sustaining naturally orthogonal in-plane phonon polariton modes in IR. In this study, we investigate the polarization-dependent optical characteristics of cavities formed using α-MoO3 to extend the degrees of freedom in the design of IR photonic components exploiting the in-plane anisotropy of this material. Polarization-dependent absorption over 80% in a multilayer Fabry-Perot structure with α-MoO3 is reported without the need for nanoscale fabrication on the α-MoO3. We observe coupling between the α-MoO3 optical phonons and the Fabry-Perot cavity resonances. Using cross-polarized reflectance spectroscopy we show that the strong birefringence results in 15% of the total power converted into the orthogonal polarization with respect to incident wave. These findings can open new avenues in the quest for polarization filters and low-loss, integrated planar IR photonics and in dictating polarization control.

Sub-single exciton optical gain threshold in colloidal semiconductor quantum wells with gradient alloy shelling.

Colloidal semiconductor quantum wells have emerged as a promising material platform for use in solution-processable lasers. However, applications relying on their optical gain suffer from nonradiative Auger decay due to multi-excitonic nature of light amplification in II-VI semiconductor nanocrystals. Here, we show sub-single exciton level of optical gain threshold in specially engineered CdSe/CdS@CdZnS core/crown@gradient-alloyed shell quantum wells. This sub-single exciton ensemble-averaged gain threshold of (Ng)≈ 0.84 (per particle) resulting from impeded Auger recombination, along with a large absorption cross-section of quantum wells, enables us to observe the amplified spontaneous emission starting at an ultralow pump fluence of ~ 800 nJ cm-2, at least three-folds better than previously reported values among all colloidal nanocrystals. Finally, using these gradient shelled quantum wells, we demonstrate a vertical cavity surface-emitting laser operating at a low lasing threshold of 7.5 µJ cm-2. These results represent a significant step towards the realization of solution-processable electrically-driven colloidal lasers.

Orientation-Controlled Nonradiative Energy Transfer to Colloidal Nanoplatelets: Engineering Dipole Orientation Factor.

We proposed and showed strongly orientation-controlled Förster resonance energy transfer (FRET) to highly anisotropic CdSe nanoplatelets (NPLs). For this purpose, we developed a liquid-air interface self-assembly technique specific to depositing a complete monolayer of NPLs only in a single desired orientation, either fully stacked (edge-up) or fully nonstacked (face-down), with near-unity surface coverage and across large areas over 20 cm2. These NPL monolayers were employed as acceptors in an energy transfer working model system to pair with CdZnS/ZnS core/shell quantum dots (QDs) as donors. We found the resulting energy transfer from the QDs to be significantly accelerated (by up to 50%) to the edge-up NPL monolayer compared to the face-down one. We revealed that this acceleration of FRET is accounted for by the enhancement of the dipole-dipole interaction factor between a QD-NPL pair (increased from 1/3 to 5/6) as well as the closer packing of NPLs with stacking. Also systematically studying the distance-dependence of FRET between QDs and NPL monolayers via varying their separation (d) with a dielectric spacer, we found out that the FRET rate scales with d-4 regardless of the specific NPL orientation. Our FRET model, which is based on the original Förster theory, computes the FRET efficiencies in excellent agreement with our experimental results and explains well the enhancement of FRET to NPLs with stacking. These findings indicate that the geometrical orientation of NPLs and thereby their dipole interaction strength can be exploited as an additional degree of freedom to control and tune the energy transfer rate.