Advanced Optical Materials最新文献

E. N. Gerasimova, V. V. Yaroshenko, L. V. Mikhailova, et al.: Thermally Induced Mechanical Switching of the Second-Harmonic Generation in pNIPAM Hydrogels-Linked Resonant Au and Si Nanoparticles. Adv. Optical Mater. 10, 2201375 (2022). https://doi.org/10.1002/adom.202201375

Following the publication of our article [Adv. Optical Mater. 2022, 10, 2201375], a query was raised concerning the Energy-Dispersive X-ray (EDX) spectroscopy data in Figure S11 of the Supporting Information. In response, the authors conducted new EDX analyses in 2025 on newly prepared samples, replicating the experimental protocols of the original study. The new data, presented in the corrected Figure S11 below, confirm the presence of silicon (Si) in the pNIPAM@Si system and both silicon (Si) and gold (Au) in the pNIPAM@Si@Au system, thereby validating the original findings.

The authors are therefore replacing the original Figure S11 in the Supporting Information with the new Figure S11 below, which is based on the verification experiments conducted in 2025.

Figure S11. EDX spectra of pNIPAM@Si and pNIPAM@Si@Au. Titanium peaks originate from the titanium foil. All spectra were also smoothed (represented by the orange lines in the graphs). The original, unsmoothed spectra are shown as grey lines.

The authors apologize for any confusion this may have caused and state that the scientific conclusions of the original article are unaffected.

The development of high-performance nonlinear optical (NLO) materials is crucial for advancing photoelectric devices, particularly optical nonlinear activation units in optical neural networks (ONNs), yet it remains a significant challenge. In this work, it is demonstrated that electrostatic doping offers a versatile strategy to enhance the NLO performance of two-dimensional materials, with promising implications for ONN applications. As a proof of concept, we employed proton (H⁺) intercalation to dope SnS₂. Spectroscopic characterizations, including Raman, X-ray photoelectron spectroscopy, and electron paramagnetic resonance, confirm successful electrostatic doping with negligible lattice expansion or defect generation. The doped SnS₂ exhibits enhanced saturable absorption (SA), two-photon absorption (2PA), or three-photon absorption (3PA) under femtosecond laser excitation across a broad wavelength range (515–1550 nm). The enhancement in SA is attributed to increased electron population in the conduction band that strengthens the Pauli blocking effect, while the improvements in 2PA and 3PA arise from the internal electric field generated by intercalated H⁺ ions within the van der Waals gaps and accumulated electrons in SnS₂. The application potential of H⁺-intercalated SnS₂ is further validated in a modeled ONN, where it achieves digit recognition accuracy comparable to that of conventional electronic activation functions.

Photocatalytic hydrogen generation offers a promising route for sustainable energy by emulating natural photosynthesis. However, translating promising lab-scale efficiencies into practical, scalable systems remains a formidable challenge. The efficiency of these scaled systems typically fall below 1%, significantly below their small-scale benchmarks. Despite extensive exploration of technical and mechanistic factors, one parameter remains overlooked: the dissolved inert gas, primarily argon. Argon is routinely used in lab setups but omitted in practical-scale system, creating exceptionally high gas-to-catalyst molar ratios given low catalyst weight loadings. Here, it is demonstrated that high gas-to-catalyst molar ratios actively modulates exciton dynamics by activating triplet-mediated pathways such as reverse intersystem crossing (RISC) and thermally activated delay fluorescence. For example, in the molecular photocatalyst acridine, a high molar ratio stabilizes triplet excitons and enables RISC to the protonated state within 100 ps. As a result, the hydrogen evolution rate is enhanced by two orders of magnitude compared to conditions with a smaller ratio. Analogous gas-dependent modulation of exciton dynamics is also observed in carbon nitride, highlighting the general relevance of gas–exciton interactions. The findings identify the gas-to-catalyst molar ratio as an overlooked yet crucial barrier to achieving high-efficiency, scalable photocatalytic systems.

Plasmonic hydrogen sensors have enabled hydrogen detection below parts-per-million (ppm) range by boosting the sensitivity using localized surface plasmonic resonant (LSPR) structures. However, the intrinsic optical losses of Palladium (Pd), the primary plasmonic metal used for hydrogen detection, result in a low quality (Q) factor LSPR, which fundamentally hinders further improvement. In this work, a hybrid plasmonic metasurface is proposed that couples Pd-based LSPR structure with an Au film supporting surface plasmon polariton mode (Au-SPP). The coupled near-perfect absorber resonance yields a spectrally narrow, high Q response that retains strong sensitivity to hydrogen while improving resonance localization. Numerical analysis shows that, under shot-noise-limited conditions, the limit of detection (LoD) can be improved by over threefold compared to the state-of-the-art designs. This hybrid plasmonic coupled-mode metasurface thus presents a promising pathway to achieve parts-per-billion-level (ppb-level) hydrogen detection with enhanced spectral precision and robustness.

J-aggregates are promising organic materials for nanophotonic applications due to their excitonic properties and ability to support surface exciton polaritons at room temperature, providing a robust platform for nanoscale light manipulation. Colloidal J-aggregate nanoparticles have demonstrated unique benefits such as easy integration into devices and combination with other materials, and enhanced surface-to-volume ratios. Herein, the one-step synthesis of colloidal J-aggregate flakes is reported in water based on electrostatic interaction of cyanine molecules (TDBC) and oppositely charged polyelectrolytes (polydiallyldimethylammonium chloride, PDDA). These flakes exhibit colloidal stability maintaining the J-aggregate conformation even in solvents that favoured their monomeric state. The characterization of the colloidal J-aggregate flakes reveals no significant monomer contribution and, more importantly, their capability to support surface exciton polaritons at room temperature (for first time). This is further confirmed at single-particle level by observing an angular-independent Reststrahlen band near the excitonic resonance. In addition, the colloidal flakes exhibit a strong scattering component that broadens the extinction band and redshifts the photoluminescence, indicating that the colloidal architecture influences the optical response. These findings introduce a versatile colloidal system, extendable to other cyanine dyes, for constructing excitonic nanostructures tailored for advanced photonic applications.

The precise design of organic multifunctional dyes provides a powerful platform for tailoring optical properties. This study presents a comprehensive analysis of a novel family of pyrazolone-based dyes, comprising five structural isomers and derivatives, synthesized with high purity and verified through multiple spectroscopic and chromatographic techniques. Their fundamental photophysical properties are investigated via absorption and fluorescence spectroscopy, revealing distinct spectral characteristics influenced by structural variations. Nonlinear optical (NLO) behavior is confirmed through 2^nd harmonic generation (SHG; χ⁽²⁾ ranging from 0.07 to 3.20 pm V⁻¹ across various derivatives and experimental conditions) and 3^rd harmonic generation (χ⁽³⁾ ranging from 3.01 to 5.41 × 10⁻²² m² V⁻²) measurements in thin-film systems, with polarization-dependent SHG analysis using Maker fringes. Furthermore, all-optical switching is demonstrated via the optical Kerr effect, revealing molecular-structure-dependent photoinduced birefringence kinetics, magnitudes (Δn from 0.32 × 10⁻⁴ up to 1.31 × 10⁻⁴ for all derivatives, with n₂ for the 4-ClPYR compound reaching 2.62 × 10⁻⁸ m² W⁻¹), and ultrafast responsivity up to 1 kHz signal modulation. To gain deeper insight into their electronic properties, TD-DFT calculations are performed. The results highlight the exceptional tunability of these materials across multiple spectroscopic dimensions, underscoring their potential for next-generation photonic and optoelectronic applications.

Achieving high loading, uniformly dispersed scintillators in polymer matrices remains challenging for flexible X-ray detectors. Herein, a large-area NaLuF₄:Tb@WPU scintillator film (48 × 20 cm²) is reported that synergistically integrates solution-processed NaLuF₄:Tb scintillators with waterborne polyurethane (WPU), enabling a record-high 90.4 wt% loading with uniform dispersion. Optimized interfacial compatibility ensures outstanding operational durability with 99.5% radioluminescence intensity retention and <0.5% permanent bending deformation after 2000 bending cycles. The X-ray scintillator film demonstrates a low detection limit of 20.9 nGy_air s⁻¹ alongside environmental, thermal, and radiation stability. Crucially, it highlights high-resolution thermally-stimulated luminescence X-ray imaging (29.0 lp mm⁻¹) with minimal geometric distortion (<1.1%) on curved surfaces, overcoming parallax artifacts in rigid detection. This work establishes a novel flexible platform unifying high sensitivity and spatial resolution for medical/industrial X-ray imaging.

Stress–strain responsiveness and visualization materials have considerable potential for information encryption, environmental sensing, and flexible optoelectronics. However, there still remain challenges in molecular design and understanding the intrinsic mechanism. Herein, two novel luminogens are designed and synthesized. They simultaneously exhibited TADF and RTP emissions in plastic polyvinyl chloride (PVC) and elastic styrene-isoprene-styrene block copolymer (SIS) doping matrices, accompanied by time-dependent afterglow from blue to green. The high-contrast stretchable and stress–strain responsiveness and visualization behaviors are achieved for the two luminogens in PVC and SIS matrices. Noteworthy, 1% AN-CN@PVC and 1% AN-NH₂@PVC films showed continuously decreasing RTP intensity and lifetime, as well as increased RTP-to-TADF intensity ratio with the increase of elongation, with the lowest strain detection limits of 13.19% and 5.84% in turn. This work not only obtained new long-lived TADF and RTP materials, achieved multi-color dynamic afterglow, strain detection and visualization, advanced anti-counterfeiting, and high-contrast stretchable behaviors, but also can be expected to provide more inspirations and possibilities for using TADF and RTP materials in a more cutting-edge field, as well as theoretical guidance and experimental supports for further molecular designs.

Although 2D semiconductors with excellent electronic and optical properties are considered as strong candidates for next-generation photodetectors, the sphotoelectric conversion efficiency of present ultrathin 2D semiconductor is still lower than expected owing to their weak optical absorption. Here, a high responsivity photodetector based on MoTe₂ ultrathin film (5.7 nm) is proposed, which is surface modified by CsPbBr₃ quantum dots (QDs) as an absorbent layer. Compared with pristine MoTe₂ devices, the responsivity of the MoTe₂/CsPbBr₃ photodetector is up to 42.7 A W⁻¹ at 0.2 V, and the enhancement ratio reaches 5400 times. Furthermore, the process of ligand exchange partially replaces the long organic chains with PF₆⁻ ions, enabling the MoTe₂/PF₆-CsPbBr₃ photodetector to achieve a responsivity of up to 165.8 A W⁻¹ at 0.2 V. Due to the reduction in the recombination of photogenerated electron–hole pairs, the responsivity of the MoTe₂/PF₆-CsPbBr₃ photodetector is 2 × 10⁴ times higher than that of pristine MoTe₂ devices. Additionally, thanks to the excellent charge transfer capability of ionic ligands, the response time of the MoTe₂/PF₆-CsPbBr₃ photodetector accelerates from 11.1 to 1.58 s. This work paves a new way for the further development of high-performance, low-cost, and energy-efficient photodetectors by using QDs modified ultrathin 2D materials.

The integrated control of transmitted and reflected electromagnetic (EM) waves plays a pivotal role in information processing and security. However, due to the complexity of antenna designs, most existing devices are limited to half-space wave manipulation to ensure high-quality transmission characteristics. Achieving dynamic and integrated control of full-space waves remains a significant challenge, especially at the same aperture in high-frequency applications. This paper introduces a novel liquid crystal (LC) transmission-reflection integrated programmable metasurface (LC-TRIPM). Based on the birefringence effect of LC, each meta-atom can be 1bit coded to modulate the phase of both transmitted and reflected EM waves, allowing full-space manipulation in both the near- and far-fields. Dual-layer LC structure is employed to enable the LC-TRIPM to operate in transmission, reflection, and simultaneous transmission-reflection modes at 94 GHz. Both simulation and experimental results demonstrate the reliable capability of the proposed LC-TRIPM in transmission-reflection integrated control. Full-space far-field beam scanning and near-field dynamic focusing can all be realized by using the proposed LC-TRIPM. This work not only offers a new strategy for integrated full-space EM wave control but also contributes to the development of multifunctional intelligent metasurface technology.