Jihoon Kyhm

Multiphoton polymerization (MPP) offers a mask‐less and full three‐dimensional accessibility for photonic integrated circuits (PICs). However, conventional free‐space‐based MPP suffers from poor stability, reconfigurability and process efficiency due to bulky components and complex free‐space alignment. Furthermore, it is typically restricted to linear passive devices constraining the functional scope of PICs. We demonstrate nonlinear polymer waveguides incorporating homogeneously dispersed nonlinear nanomaterials through an all‐fiber‐configured MPP process. Control of the target voxel is achieved by managing in‐line chromatic dispersion along with optimizing the design of lensed optical fibers employed. The nanomaterials, upconversion nanoparticles (UCNPs), simultaneously enable cascaded multiphoton absorption with a telecommunication‐wavelength photon source, and introduce nonlinear saturable absorption allowing the devices to operate in an ultrafast regime. An 880 µm‐long waveguide with a few‐micrometer‐scale cross section is fabricated. The nonlinearity of the resultant UCNP‐dispersed waveguide is verified by demonstrating a mode‐locked fiber ring laser that generates 746 fs pulses at a 1.49 MHz repetition rate. The all‐fiber MPP process provides a compact platform for localized fabrication of nanomaterial‐incorporated nonlinear polymer waveguides.

Multicolor tunable upconversion nanoparticles (UCNPs) have garnered attention owing to their diverse applications such as displays, imaging, and security. Typically, achieving multicolor emission from UCNPs requires complicated core/multishell nanostructures comprising a core with at least five shells. Here, we propose a strategy to achieve bright and orthogonal red (R), green (G), and blue (B) upconversion (UC) luminescence without synthesizing complicated core/quintuple-shell or core/sextuple-shell nanostructures. For achieving bright and orthogonal RGB triprimary color UC luminescence, orthogonal bicolor-emitting core/shell-structured UCNPs are synthesized and blended. Orthogonal RB, RG, and GB luminescence are achieved through photon blocking. The combination of two orthogonal bicolor-emitting UCNPs exhibits pure RGB UC luminescence and full-color tunability via manipulation of excitation laser conditions. Furthermore, we present color displays achieved with transparent UCNP-polymer composites utilizing three distinct near-infrared light wavelengths, implying that the proposed strategy for attaining RGB UC luminescence may facilitate advancements in the development of full-color volumetric displays.

High‐performance chiroptical synaptic phototransistors are successfully demonstrated using heterojunctions composed of a self‐assembled nanohelix of a π‐conjugated molecule and a metal oxide semiconductor. To impart strong chiroptical activity to the device, a diketopyrrolopyrrole‐based π‐conjugated molecule decorated with chiral glutamic acid is newly synthesized; this molecule is capable of supramolecular self‐assembly through noncovalent intermolecular interactions. In particular, nanohelix formed by intertwinded fibers with strong and stable chiroptical activity in a solid‐film state are obtained through hydrogen‐bonding‐driven, gelation‐assisted self‐assembly. Phototransistors based on interfacial charge transfer at the heterojunction from the chiroptical nanohelix to the metal oxide semiconductor show excellent chiroptical detection with a high photocurrent dissymmetry factor of 1.97 and a high photoresponsivity of 218 A W⁻¹. The chiroptical phototransistor demonstrates photonic synapse‐like, time‐dependent photocurrent generation, along with persistent photoconductivity, which is attributed to the interfacial charge trapping. Through the advantage of synaptic functionality, a trained convolutional neural network successfully recognizes noise‐reduced circularly polarized images of handwritten alphabetic characters with better than 89.7% accuracy.

Herein, we demonstrate video-rate color three-dimensional (3D) volumetric displays using elemental-migration-assisted full-color-tunable upconversion nanoparticles (UCNPs). In the heavily doped NaErF₄:Tm-based core@multishell UCNPs, erbium migration was observed. By tailoring this migration through adjustment of the intermediate shell thickness between the core and the sensitizer-doped second shell, red-green orthogonal upconversion luminescence (UCL) was achieved. Furthermore, highly efficient red-green-blue orthogonal UCL and full-color tunability were achieved in the UCNPs through a combination of elemental-migration-assisted color tuning and selective photon blocking. Finally, 3D volumetric displays were fabricated using a UCNP-polydimethylsiloxane composite. More specifically, 3D color images were created and motion pictures based on the expansion, rotation, and up/down movement of the displayed images were realized in the display matrix. Overall, our study provides new insights into upconversion color tuning and the achievement of motion pictures in the UCNP-polydimethylsiloxane composite is expected to accelerate the further development of solid-state full-color 3D volumetric displays.

Chiral perovskites have emerged as promising candidates for polarization-sensing materials. Despite their excellent chiroptical properties, the nature of their multiple-quantum-well structures is a critical hurdle for polarization-based and spintronic applications. Furthermore, as the origin of chiroptical activity in chiral perovskites is still illusive, the strategy for simultaneously enhancing the chiroptical activity and charge transport has not yet been reported. Here, we demonstrated that incorporating a Lewis base into the lattice can effectively tune the chiroptical response and electrical properties of chiral perovskites. Through solid-state nuclear magnetic resonance spectroscopic measurements and theoretical calculations, it was demonstrated that the material property manipulation resulted from the change in the time-averaged structure induced by the Lewis base. Finally, as a preliminary proof of concept, a vertical-type circularly polarized light photodetector based on chiral perovskites was developed, exhibiting an outstanding performance with a distinguishability of 0.27 and a responsivity of 0.43 A W^-1.

Chiral perovskites are being extensively studied as a promising candidate for spintronic- and polarization-based optoelectronic devices due to their interesting spin-polarization properties. However, the origin of chiroptical activity in chiral perovskites is still unknown, as the chirality transfer mechanism has been rarely explored. Here, through the nano-confined growth of chiral perovskites (MBA₂PbI_4(1-x)Br_4x), we verified that the asymmetric hydrogen-bonding interaction between chiral molecular spacers and the inorganic framework plays a key role in promoting the chiroptical activity of chiral perovskites. Based on this understanding, we observed remarkable asymmetry behavior (absorption dissymmetry of 2.0 × 10⁻³ and anisotropy factor of photoluminescence of 6.4 × 10⁻² for left- and right-handed circularly polarized light) in nanoconfined chiral perovskites even at room temperature. Our findings suggest that electronic interactions between building blocks should be considered when interpreting the chirality transfer phenomena and designing hybrid materials for future spintronic and polarization-based devices.

Polarization-sensitive photodetection has attracted considerable attention as an emerging technology for future optoelectronic applications such as three-dimensional (3D) imaging, quantum optics, and encryption. However, traditional photodetectors based on Si or III–V InGaAs semiconductors cannot directly detect polarized light without additional optical components. Herein, we demonstrate a self-powered linear-polarization-sensitive near-infrared (NIR) photodetector using a two-dimensional WSe₂/ReSe₂ van der Waals heterostructure. The WSe₂/ReSe₂ heterojunction photodiode with semivertical geometry exhibits excellent performance: an ideality factor of 1.67, a broad spectral photoresponse of 405–980 nm with a significant photovoltaic effect, outstanding linearity with a linear dynamic range wider than 100 dB, and rapid photoswitching behavior with a cutoff frequency up to 100 kHz. Strongly polarized excitonic transitions around the band edge in ReSe₂ lead to significant 980 nm NIR linear-polarization-dependent photocurrent. This linear polarization sensitivity remains stable even after exposure to air for longer than five months. Furthermore, by leveraging the NIR (980 nm)-selective linear polarization detection of this photodiode under photovoltaic operation, we demonstrate digital incoherent holographic 3D imaging.

Here, excitation orthogonalized red/green/blue upconversion luminescence (UCL)-based full-color tunable rare-earth (RE) ion-doped upconversion nanophosphors (UCNPs) are reported. The LiREF₄-based core/sextuple-shell (C/6S) UCNPs are synthesized, and they consist of a blue-emitting core, green-emitting inner shell, and red-emitting outer shell, with inert intermediate and outermost shells. The synthesized C/6S UCNPs emit blue, green, and red light under 980, 800, and 1532 nm, respectively. Importantly, by combining incident near-infrared (NIR) light with various wavelengths (800, 980, and 1532 nm), full-color UCL including blue, cyan, green, yellow, orange, red, purple, and white UCL is achieved from the single C/6S UCNP composition. The color gamut obtained from the C/6S UCNPs shows 101.6% of the sRGB standard color gamut. Furthermore, transparent C/6S UCNP-polydimethylsiloxane (PDMS) composite is prepared. Full-color display realized in the transparent C/6S UCNP-PDMS composite indicates the feasibility of constructing the C/6S UCNP-based three-dimensional volumetric displays with wide color gamut.