Light-Science & Applications
·
2026
·Vol. 15
·期 1
·360
·
IF 24
Xu Yanming,Liu Yi,Yu Chao,Xu Jinlong,Huang Wenqi,Mo Weichu,Xu Canhua,Sun Zhihua,Huang Yantang,Cao Xun,Xie Zhenda,Lu Ruifeng
Directly full-color frequency-upconversion under high-order multiphoton absorption (MPA) nonlinearities in NIR-III (1550–1870 nm) and NIR-IV (2100–2300 nm) windows is highly desirable for advanced photonics and bioimaging. However, it has remained beyond the reach of current materials due to their inherently weak high-order MPA. Here, we demonstrate that, driven by Bloch oscillations of excitonic dipoles after nonlinear polarization, giant multiphoton nonlinearities can be achieved in layered hybrid perovskites to enable full-color upconversion in NIR-III/IV windows. The MPA cross-section values of the designed three Ruddlesden-Popper perovskites are found to be several orders of magnitude larger than those of the reported MPA materials. These advancements facilitate versatile applications previously inaccessible in NIR-III/IV windows, including full-color upconversion displays and multicolor information encryption. Our work highlights the prospect of efficient high-order MPA and opens avenues for investigating excitonic quantum dynamics in high-order nonlinear optics.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Yongjing Deng,Xiaodong Zhao,Ning Ding,Yong Yang,Yongkang Zhu,Mengzhu Wang,Shujuan Liu,Yun Ma,Qiang Zhao
Zero-dimensional (0D) organic–inorganic hybrid metal halides are promising phosphors, yet their wide bandgaps typically require ultraviolet excitation, limiting compatibility with commercial blue light-emitting diode (LED) chips. Here, we present an aggregate-engineering strategy to unlock blue-light excitability in 0D copper(I) iodides by modulating the aggregation architecture of Cu–I motifs within a fixed phosphonium-cation framework. Two homologous compounds, (C26H24OP)2Cu2I4 and (C26H24OP)2Cu4I6, were selectively synthesized through simple stoichiometric regulation. Increasing the nuclearity from a dimer to a tetramer strengthens cuprophilic interactions, narrows the optical bandgap from 2.98 to 2.61 eV, and markedly broadens the excitation window into the blue region. Density functional theory calculations further support the aggregation-induced bandgap narrowing by revealing increased inorganic contributions at the band edges in the tetramer. Notably, the tetramer achieves a high thermal stability and moisture tolerance. Finally, a single-component white LED (WLED) based on the tetramer and a 450 nm chip delivers high-quality white light, and a proof of concept for visible light communication enables high-fidelity audio transmission. This work establishes aggregate engineering as an effective design principle for bridging 0D hybrid halides with practical blue-chip pumping and integrated lighting communication platforms.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Jin-Wang Liu,Zhe-Kun Xu,Tian Gan,Zhong-Xia Wang
Organic–inorganic hybrid ABX3-type ferroelectric materials with their structural versatility hold broad application prospects in optoelectronics, data storage, sensing, and other advanced fields. Despite chemical strategies targeting organic motifs that have proven effective for the rational design of novel hybrid molecular ferroelectrics, studies on halogen substitution receiving dual regulation of structure and symmetry in an edge-shared ABX3 hybrid ferroelectrics remain scarce. Herein, we synthesized a new one-dimensional ABX3 hybrid ferroelectric DMEIM-CdCl3 (DMEIM = N-(iodomethyl)-N,N-dimethylethylamine) by employing a halogen substitution strategy. This approach precisely tuned the crystal space group of the parent compound (centrosymmetric Pbca) to the ferroelectric Cc space group. Structurally, DMEIM-CdCl3 features one-dimensional [CdCl5]−n pyramidal chains composed of edge-shared CdCl5 hexahedra, deviating from the conventional ABX3 framework built from face- or corner-sharing polyhedra. DMEIM-CdCl3 undergoes a characteristic ferroelectric phase transition above room temperature (Tc = 379 K) with an Aizu notation of 2/mFm. This work offers insights into expanding the family of hybrid ferroelectric materials through rational chemical design.
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Advanced Optical Materials
·
2025
·
IF 7.2
Yu Cai,Yunqing Li,Renyan Zhang,Changqing Shen,Yunxia Zhou,Xiong Li,Xiangang Luo
Dynamic manipulation of terahertz waves is crucial for advancing rapidly evolving terahertz technologies. Recently, intercalation in 2D materials has emerged as a powerful strategy for tuning their physical and chemical properties, enhancing their potential for terahertz modulation applications. However, the terahertz-band response during intercalation and the underlying optical response mechanisms remain poorly understood. Herein, the tunable terahertz properties of the reduced graphene oxide films are investigated via ionic liquid intercalation and elucidate the associated terahertz response mechanism. The free charge carriers transport characteristics during the intercalation process are extracted using Drude–Smith model. The mechanism behind the terahertz response primarily stems from the intercalation of ionic liquid into the reduced graphene oxide films, resulting in an increase in the number of free carriers responding to terahertz waves. These results provide valuable insights for graphene-based tunable terahertz wave control and open a route toward exploring the intercalation mechanism in 2D materials.
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ACS Photonics
·
2025
·
IF 6.7
Ying Lv,Yi Wei,Shengting Zhu,Jinming Hu,Min Gu,Yinan Zhang
Laser direct writing functional optical materials enable high-resolution and optically thin computer-generated holograms with a wide range of applications. However, the traditional material system limits the development of holography technology due to the small refractive index modulation, high optical loss, and complicated preparation process. Perovskite has emerged as competitive candidates because of their superiority in high refractive index, flexible bandgap tunability, and low-cost preparation. Here, we report giant refractive index modulation of perovskites by femtosecond laser direct writing (FsLDW) for applications in holograms and holographic neural networks (HNNs). The interaction mechanism between the femtosecond laser and perovskites is also investigated. Under the precise control of FsLDW, the organic phenylethylamine (PEA) functional groups are reduced, leading to giant refractive index modulation from 0.15 to 1.05 at the broad wavelength range of 519–900 nm, along with geometric thickness reduction. Phase-modulated perovskite holograms and HNNs composed of cascaded holographic plates are demonstrated, greatly expanding the possibilities of perovskite applications in the field of all-optical information encoding.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Huiying Yan,Youpeng Ding,Shumin Lin,Jialiang Li,Yanan Zhao,Zewen Lin,Jinmeng Zhang,Jie Bai,Xiaolan Hu,Hua Bai
Structural energy storage devices, capable of storing energy while simultaneously bearing mechanical loads, are gaining significant interest in aerospace, electric vehicles, and portable electronics. However, the commonly used carbon fiber fabric current collector/reinforcement occupies a disproportionately large share of the device’s mass and volume, thereby limiting the overall energy density of the device. In this paper, we present a device architecture in which an integrated graphene/conducting polymer composite film is used to replace the conventional carbon fiber fabrics to serve as both the current collector and mechanical reinforcement in structural supercapacitors. Owing to the high specific capacitance of the composite film, the new devices exhibit a high specific capacitance of 62.5 mF cm–2 and energy density of 6.1 μW h cm–2 at a current density of 0.2 mA cm–2, corresponding to volumetric energy density of 0.14 mW h cm–3, and gravimetric energy density of 31.2 mW h kg–1. Those values far surpass those of the counterparts using carbon fiber fabrics. To further enhance load-bearing and energy storage performance, multilayer devices are developed. A seven-layer device demonstrated a flexural strength of 19.0 MPa and, through series-parallel connections of internal electrodes, achieved a large working voltage of 4.5 V, or a high specific capacitance of 161.1 mF cm–2 and energy density of 14 μW h cm–2. This work demonstrates the potential of graphene composite film electrodes in structural energy storage applications and provides a new pathway toward achieving high-performance structural energy storage devices.
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ACS Photonics
·
2025
·
IF 6.7
Yingming Wang,Lingyan Xu,Lu Liang,Zhentao Qin,Shuai Han,Chongqi Liu,Lixiang Lian,Wei Zheng,Yanyan Lei,Qinzeng Hu,Tao Wang,Wanqi Jie
Achieving real-time, high-sensitivity radiation detection with stability and precision remains a critical challenge in medical diagnostics and radiation therapy. Here, we report the development of MDABCO-NH4(BF4)3 single crystals (SCs), a metal-free perovskite material with exceptional performance for both X-ray and charged particle detection. Large-scale MDABCO-NH4(BF4)3 SCs (15 × 13 × 5 mm3) were synthesized via a simple low-temperature solution method, achieving superior crystallinity with a full width at half-maximum (fwhm) of 0.0061°. The MDABCO-NH4(BF4)3 detectors exhibit high resistivity (1.31 × 1012 Ω·cm), low trap density (1.09 × 109 cm–3), and excellent charge transport properties ((μτ)h = 3.15 × 10–5 cm2·V–1). For α-particle detection, the MDABCO-NH4(BF4)3 detectors achieve a high energy resolution of 35.0% at 5.49 MeV and a fast response time of 5 ms, demonstrating single-particle sensitivity. For X-ray detection, MDABCO-NH4(BF4)3 detectors exhibit high sensitivity (13,529 μC·Gyabs–1·cm–2) and an ultralow detection limit (17.1 nGyair·s–1), significantly lower than the 5.5 μGyair·s–1 standard for active personal dosimeters used in regular medical diagnostics. The combination of superior charge transport properties with stability and high signal-to-noise ratio establishes MDABCO-NH4(BF4)3 SCs as a versatile material for real-time radiation monitoring and high-precision medical imaging applications.
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SYNTHETIC METALS
·
2025
·
IF 4.6
Maolin He,Zijie Wang,Yong Chen,Yuheng Li,Junjie Wu,Peng Gao
Perovskite solar cells (PSCs) have achieved remarkable power conversion efficiencies (PCEs) exceeding 27 %, yet their long-term operational stability remains a significant barrier to commercialization. The state-of-the-art hole transport layer (HTL) based on Spiro-OMeTAD relies on hygroscopic lithium salts and volatile co-additives to boost conductivity, which inevitably accelerates interfacial degradation. Here, we introduce a molecular co-doping strategy in which a brominated dithieno[3,2-b:2′,3′-d]pyrrole derivative (DTP-OMe-2Br) is incorporated into Spiro-OMeTAD to synergistically combine their advantages. Owing to its planar donor-rich framework and bromine functionalities, DTP-OMe-2Br preferentially localizes at the perovskite/HTL interface, enhancing hole mobility, passivating undercoordinated Pb²⁺ defects, and increasing hydrophobicity without disrupting Spiro’s film-forming properties. As a result, devices achieve a champion PCE of 24.41 %, surpassing the 23.06 % of the pristine Spiro-OMeTAD reference, and retain over 85 % of their initial efficiency after 2500 h in ambient air. This work demonstrates that rationally designed small-molecule additives can serve as multifunctional interfacial modifiers for hybrid HTLs, offering a generalizable route toward high-efficiency and durable PSCs.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Quanlin Chen,Yangbin Xu,Qingming Wu,Yanxing Feng,Zhiqiang Huang,Hai Jia,Shaoming Ying,Xiaohui Huang
Accurate and chip-integrated full-Stokes polarization detection is essential for advancing multifunctional optoelectronic systems. However, conventional approaches relying on optical filters often suffer from significant optical losses and poor sensitivity under weak-light conditions. Here, we report an efficient full-Stokes polarimeter based on a 1D chiral-polar perovskite, (R/S-NEA)PbI3. The intrinsic anisotropic and chiral structure of the (R/S-NEA)PbI3 single crystal enables both high linear and circular polarization sensitivity. Moreover, the polar structure induces a giant bulk photovoltaic effect (BPVE) of up to 8 V, enabling efficient carrier extraction under zero bias and significantly suppressing noise currents to the ∼fA level, resulting in an exceptional specific detectivity of 4.1 × 1013 Jones. These combined properties enable accurate, self-powered full-Stokes polarization detection, with the fabricated single-crystal-based polarimeter achieving an average Stokes parameter error (ΔS1–3) of less than 3%. Notably, the polarimeter demonstrates an ultra-low detection limit of 0.4 μW cm−2, representing the highest sensitivity among comparable polarimeters reported to date. With easy on-chip integration, the polarimeter showcases precise full-Stokes imaging capabilities.
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Materials Futures
·
2025
·Vol. 4
·期 4
·045103
·
IF 10.8
Rui Zhang,Bobo Ma,Yuqi Cui,Chengyu Tan,Bingbing Chen,Yiming Li,Jiangjian Shi,Huijue Wu,Yanhong Luo,Dongmei Li,Jianhui Chen,Qingbo Meng
CsPbI3 perovskites with suitable bandgaps ∼1.70 eV present distinct advantages for top-cell photovoltaic materials in tandem solar cells, however, relevant work has been rarely reported. This work designed a sandwich-like MoOX/Ag/MoOX (MAM) buffer layer as the front cell window layer to maximize incident light utilization efficiency for semi-transparent CsPbI3 solar cells and four terminal (4-T) stacked cells. Further investigation revealed that the MAM has to experience in-situ reaction between Ag metal and fresh MoOX, which can simultaneously ensure the transparency of the buffer layer and improve the carrier transportation and collection, except for protecting the underlying spiro-OMeTAD layer from the bombardment of magnetron sputtering. Thanks to this MAM buffer layer and a tunnel oxide passivating contact (TOPCon) bottom cell with edge passivation, semi-transparent CsPbI3 devices (aperture area: 0.50 cm2) demonstrated a power conversion efficiency (PCE) of 18.86% while corresponding 4-T CsPbI3/TOPCon tandem solar cells (PSTSCs) presented the PCE of 26.55%. Besides, we also fabricated semi-transparent CsPbI3 minimodules with 16.67% PCE and 4-T PSTSCs with 26.41% PCE (aperture area: 6.62 cm2). This work provided a new scalable strategy for transparent buffer layers by constructing in-situ generated sandwich structured buffer layer, which is suitable for perovskite tandem solar cells.
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Advanced Energy Materials
·
2022
·Vol. 12
·期 41
·2201463
·
IF 29.698
Yingjie Hu,Xiaobing Hu,Lu Zhang,Tao Zheng,Jiaxue You,Binxia Jia,Yabin Ma,Xinyi Du,Lei Zhang,Jincheng Wang,Bo Che,Tao Chen,Shengzhong (Frank) Liu
Understanding the key factor driving the efficiency and stability of semiconductor devices is vital. To date, the key factor influencing the long-term stability of perovskite solar cells (PSCs) remains unknown because of the many influencing factors. In this work, through machine learning, the influences of five factors, including grain size, defect density, bandgap, fluorescence lifetime, and surface roughness, on the efficiency and stability of PSCs have been revealed. It is found that the bandgap has the greatest influence on the efficiency, and the surface roughness and grain size are most influential to the long-term stability. A mathematical model is given to predict efficiency based on fluorescence lifetime and bandgap. Guided by the model, four groups of experiments are conducted to confirm the machine-learning predictions and a PSC with 23.4% efficiency and excellent long-term stability is obtained, as manifested by retention of 97.6% of the initial efficiency after 3288 h aging in the ambient environment, the best stability under these conditions. This work shows that machine learning is an effective means to enrich semiconductor physical models.
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ADVANCED MATERIALS
·
2022
·Vol. 34
·期 45
·2205028
·
IF 32.086
Yuqi Cui,Jiangjian Shi,Fanqi Meng,Bingcheng Yu,Shan Tan,Shan He,Chengyu Tan,Yiming Li,Huijue Wu,Yanhong Luo,Dongmei Li,Qingbo Meng
All-inorganic CsPbI 3 perovskite has emerged as an important photovoltaic material due to its high thermal stability and suitable bandgap for tandem devices. Currently, the cell performance of CsPbI 3 solar cells is mainly subject to a large open-circuit voltage ( V OC ) deficit. Herein, a multifunctional room-temperature molten salt, dimethylamine acetate (DMAAc) is demonstrated, which not only directly acts as a solvent for precursor solutions, but also regulates the phase conversion process of the CsPbI 3 film for high-efficiency photovoltaics. DMAAc can stabilize the DMAPbI 3 structure and eliminate the Cs 4 PbI 6 intermediate phase, which is easily spatially segregated. Meanwhile, a new homogeneous intermediate phase DMAPb(I,Ac) 3 is formed, which finally affords high-quality CsPbI 3 films. With this approach, the charge capture activity of defects in the CsPbI 3 film is significantly suppressed. Consequently, a V OC of 1.25 V and >21% power conversion efficiency are achieved, which is the record highest reported thus far. This intermediate phase-regulation strategy is believed to be applicable to other perovskite material systems.
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