Chiral electroluminescence from thin-film perovskite metacavities.

Chiral light sources realized in ultracompact device platforms are highly desirable for various applications. Among active media used for thin-film emission devices, lead-halide perovskites have been extensively studied for photoluminescence due to their exceptional properties. However, up to date, there have been no demonstrations of chiral electroluminescence with a substantial degree of circular polarization (DCP) based on perovskite materials, being critical for the development of practical devices. Here, we propose a concept of chiral light sources based on a thin-film perovskite metacavity and experimentally demonstrate chiral electroluminescence with a peak DCP approaching 0.38. We design a metacavity created by a metal and a dielectric metasurface supporting photonic eigenstates with a close-to-maximum chiral response. Chiral cavity modes facilitate asymmetric electroluminescence of pairs of left and right circularly polarized waves propagating in the opposite oblique directions. The proposed ultracompact light sources are especially advantageous for many applications requiring chiral light beams of both helicities.

Topological Control of 2D Perovskite Emission in the Strong Coupling Regime.

Momentum space topology can be exploited to manipulate radiation in real space. Here we demonstrate topological control of 2D perovskite emission in the strong coupling regime via polaritonic bound states in the continuum (BICs). Topological polarization singularities (polarization vortices and circularly polarized eigenstates) are observed at room temperature by measuring the Stokes parameters of photoluminescence in momentum space. Particularly, in symmetry-broken structures, a very large degree of circular polarization (DCP) of ∼0.835 is achieved in the perovskite emission, which is the largest in perovskite materials to our knowledge. In the strong coupling regime, lower polariton modes shift to the low-loss spectral region, resulting in strong emission enhancement and large DCP. Our reciprocity analysis reveals that DCP is limited by material absorption at the emission wavelength. Polaritonic BICs based on 2D perovskite materials combine unique topological features with exceptional material properties and may become a promising platform for active nanophotonic devices.

Circularly Polarized Emission from Organic-Inorganic Hybrid Perovskites via Chiral Fano Resonances.

Organic-inorganic hybrid perovskites hold great potential for various optoelectronic devices with exceptional properties. Although the direct generation of circularly polarized emission from perovskites would enable various compact devices, achieving a large degree of circular polarization (DCP) at room temperature still remains challenging. Herein, we demonstrate that DCP can be strongly enhanced at the narrow mode position of chiral Fano resonances. In our design, a perovskite film is spin-coated on a symmetry-broken structure with a relatively large feature size. A large DCP of more than 0.5 is achieved at room temperature without the direct patterning of the perovskite layer. Reciprocity calculation reveals that chiral field enhancement enables the emission of opposite helicity to couple into counter-propagating slab modes and leads to a large DCP. Our design is very general and scalable. Our work may lead to circularly polarized light sources based on various perovskite materials.

Multicolor 4D printing of shape-memory polymers for light-induced selective heating and remote actuation.

Four-dimensional (4D) printing can add active and responsive functions to three-dimensional (3D) printed objects in response to various external stimuli. Light, among others, has a unique advantage of remotely controlling structural changes to obtain predesigned shapes. In this study, we demonstrate multicolor 4D printing of shape-memory polymers (SMPs). Using color-dependent selective light absorption and heating in multicolor SMP composites, we realize remote actuation with light illumination. We experimentally investigate the temperature changes in colored SMPs and observe a clear difference between the different colors. We also present simulations and analytical calculations to theoretically model the structural variations in multicolor composites. Finally, we consider a multicolor hinged structure and demonstrate the multistep actuation by changing the color of light and duration of illumination. 4D printing can allow complex, multicolor geometries with predesigned responses. Moreover, SMPs can be reused multiple times for thermal actuation by simply conducting thermomechanical programming again. Therefore, 4D printing of multicolor SMP composites have unique merits for light-induced structural changes. Our study indicates that multicolor 4D printing of SMPs are promising for various structural changes and remote actuation.

Enhancement of sub-bandgap light absorption in perovskite semiconductor films via critical coupling.

Light absorption in semiconductors is a fundamental problem that has broad impact on a wide range of fields. However, it is intrinsically limited by the bandgap energy of the semiconductor. Herein, we study the enhancement of sub-bandgap light absorption in inorganic-organic hybrid perovskite semiconductor films via critical coupling. This is achieved at large incidence angles by balancing radiative and nonradiative decay rates in a planar multilayer structure. We found that a very small loss in the semiconductor layer can result in substantial light absorption. This simple but general method can be used to enhance the optical and optoelectronic responses of semiconductors below the bandgap energy.

Femtosecond laser irradiation of molecular excitonic films for nanophotonic response control and large-area patterning.

Molecular excitonic films such as J-aggregate thin films can show an optically metallic response in the visible region and can be considered as alternative materials for plasmonics. However, there was no direct, top-down method to modify the optical response over a large area. Here, we demonstrate the femtosecond (fs) laser processing of J-aggregate films on the centimeter scale. With proper laser conditions, optically metallic films (Re[ε] < 0) were modified to dielectric ones (Re[ε] > 0) with large changes in optical responses. We performed various optical spectrum measurements to investigate the effect of fs-laser irradiation. Our results demonstrate that the strong modification of the optical response can be induced over a large area by fs-laser processing and this can be useful for novel nanophotonic studies.