This study investigated the ultrafast excited-state dynamics in two ruthenium polypyridyl complexes, namely (bpy)2Ru(MQ)24+ and (bpy)2Ru(MQ')24+ (Ru-MQ and Ru-MQ'), where bpy = 2,2'-bipyridine, MQ = N-methyl-4,4'-bipyridine and MQ' = N-methyl-3,3'-dimethyl-4,4'-bipyridine. Broadband near-UV-visible transient absorption (TA) spectroscopy on Ru-MQ provides unequivocal evidence for bpy → MQ ligand-to-ligand electron transfer that occurs within 10 ps following 100 fs excitation of the Ru → bpy metal-to-ligand charge transfer (MLCT) state. Experimental results and density functional theory (DFT) calculations support the hypothesis that bpy → MQ electron transfer is gated by "flattening" of the MQ ligand mediated by torsion around the inter-ring C-C bond. Spin density plots obtained from the DFT calculations point toward the dihedral angle in MQ ligand being critical for the transition between the Ru → bpy and Ru → MQ3 MLCT states. The excited state model is further supported by parallel studies on Ru-MQ' in which the conformational change within MQ' is limited by steric constraints. Excitation wavelength-dependent TA studies on Ru-MQ indicate that the relative populations of the Ru → bpy and Ru → MQ3 MLCT states initially generated upon photoexcitation depend on the excitation wavelength. This behavior arises from the broad distribution of MQ conformers present in the ground state, which selectively absorb at different wavelengths.

The development of aqueous iron-metal batteries (AIBs) is critically hindered by the severe parasitic hydrogen evolution reaction (HER) at the anodes and the resulting structural degradation of the cathode. Moving beyond conventional additive-based approaches, this work presents a kinetically targeted strategy to suppress HER and enhance overall cell stability through an isotope-engineered deuterated water (D2O)-based electrolyte. Leveraging the intrinsic differences in zero-point energy between deuterium and hydrogen, D2O features a substantially higher activation energy barrier for water dissociation, effectively taming the reactivity of the problematic Fe anode. Concurrently, control experiments in Fe metal-free configurations reveal that this isotope effect extends a vital secondary stabilization to the cathode host, establishing a cooperative, dual-side protection mechanism. Consequently, the D2O-based electrolyte enables a highly reversible iron anode with an average Coulombic efficiency of 99.6% and grants Fe||MoS2 full cells a stable lifespan of 2000 cycles with an 87.6% capacity retention at 0.5 A g-1. This work highlights the potential of isotopic modulation as a targeted, high-efficacy strategy for stabilizing high-performance aqueous batteries.

The synergistic effect of elongated exciton transport and strong exciton-CT state coupling facilitates the generation of long-lived reactive charges in NIR organic photocatalysts.

This study reports the synthesis, photophysical characterization, and near-infrared (near-IR) optical limiting (OL) response of a two-photon absorbing chromophore, 1, and two metal-organic chromophores, Ru-1 and Ir-1. Chromophore 1 was designed by connecting triphenylamine units to the 5,5 '-positions of a 2,2 '-bipyridine core through alkyne linkages, forming a centrosymmetric, quadripolar donor-acceptor-donor (D-A-D) architecture known to promote strong two-photon absorption (2PA). The metal-organic chromophores Ru-1 and Ir-1 were designed to exploit the high spin-orbit coupling of Ru(II) and Ir(III), enabling efficient population of long-lived triplet states that can undergo triplet excited-state absorption (ESA). The excited states of all target molecules were investigated by using femtosecond and nanosecond transient absorption spectroscopy. The optical limiting performance of the chromophores in solution toward 5 ns pulses was evaluated by using an open aperture, nonlinear transmission set up. Ru-1 and Ir-1 display strong OL responses to 5 ns pulses at 1064 nm, arising from two distinct nonlinear pathways: 2PA and ESA. These findings provide valuable insight into the molecular design strategies required to achieve dual-mechanism optical limiting materials suitable for practical applications.

Quantum shells (QSs) with efficient multiexciton emission can generate multiple excitons per particle under high-energy excitation, thereby improving exciton utilization under intense X-ray exposure and offering strong potential for X-ray-based scintillation applications. However, these QSs are typically composed of low-atomic-number (Z) elements, which substantially limits their X-ray absorption efficiency and leads to poor X-ray sensitivity. Here, we overcome this fundamental limitation by introducing a high-Z antenna-sensitization strategy that couples QSs to heavy-element molecular absorbers, which act as X-ray harvesting centers and funnel energy into the QSs via efficient interfacial transfer. By combining enhanced X-ray absorption with efficient interfacial energy transfer and improved exciton utilization, we achieve more than an order-of-magnitude increase in multiexciton-driven QS radioluminescence (RL) relative to pristine shells. Additionally, a high X-ray imaging resolution of 25.2 lp mm-1 was achieved, exceeding the performance of most previously reported X-ray imaging scintillators. These findings offer a promising design strategy for advancing QS-based materials toward high-performance X-ray imaging applications.

Organic-metal halide hybrids have advantageous luminous qualities and can be processed at low temperatures. These materials present a sustainable, cost-efficient, and effective solution for X-ray scintillators compared to all-inorganic scintillators. However, challenges, such as surface photon scattering and difficult uniformity control of the scintillator surface, continue to impede resolution improvement. In this study, we present a melt-quenching process to incorporate a zero-dimensional hybrid halide (MTP)2MnBr4 (methyltriphenylphosphonium bromide = MTPBr) into a microporous silicon substrate (3 x 3 cm). The (MTP)2MnBr4 glass embedded microporous silicon substrate scintillator screen achieves exceptional X-ray performance metrics by exploiting its outstanding luminescence properties, high optical transparency, and effective photon wave guidance via microporous arrays on screen surfaces. It delivers a high X-ray light yield of 16,840 photons/MeV, with a low detection limit of 135 nGy/s, and achieves an exceptional X-ray imaging spatial resolution of 25 lp/mm. Furthermore, the (MTP)2MnBr4 single crystal grown via low-temperature evaporation shows remarkable retention of radioluminescence intensity and an exceptional light yield of 60,790 photons/MeV. This approach combines low toxicity, ease of processing, scalability, low detection limit, significant light yield, and high spatial resolution, making it suitable for widespread adoption in various X-ray applications.

The development of high-voltage Li metal batteries is crucial to meeting increasing demand for high specific energy. However, their high-temperature operation remains a huge challenge due to reduced electrolyte oxidation stability and aggravated interfacial side reactions. Herein, a multimodal 19F nuclear magnetic resonance technique is developed to reveal temperature-mediated evolution of electrolyte anion solvation chemistry, thus identifying its vital roles in stabilizing high-voltage positive electrodes. A universal solvent screening strategy is proposed to customize an anion-anchored compact solvation structure electrolyte with large-size and anion-compressed solvation structure. This strategy simultaneously elevates anti-oxidation ability, stabilizes electrode-electrolyte interphase, and maintains structural integrity of the positive electrodes. Consequently, a 317 Wh kg-1 Li metal pouch cell based on the total cell mass achieves high thermal safety and cycling stability at 55 °C. Our work elucidates the reaction mechanisms of solvation structure and interfacial chemistry in high-temperature and high-voltage Li metal batteries, which offers insightful guidance for designing wide-temperature battery electrolytes.

The increasing demand for high-speed X-ray imaging requires scintillators with high light yield and fast response. Perovskite nanocrystals are promising candidates due to their distinctive optical properties and solution processability. However, the fabrication of thick X-ray films, which are several orders of magnitude thicker than conventional optoelectronic devices, leads to severe material waste and reduced light yield caused by strong spectral overlap and self-absorption. In addition, conventional synthesis methods often suffer from low reaction yields and uncontrolled exciton pathways. Here, we develop a low-temperature polar-solvent synthesis method that achieves a reaction yield of 162 mg mL-1 and optimizes exciton routing for improved energy transfer. This approach increases the Stokes shift and reduces the radioluminescence decay to 7.19 ns. Consequently, high-speed X-ray imaging at 7,680 frames per second with a spatial resolution of 27.6 line-pairs per millimeter is achieved, supporting sustainable commercialization of perovskite nanocrystal scintillators for dynamic X-ray imaging.

Lead-free perovskite-related materials are gaining significant attention as X-ray scintillators due to their low toxicity and high X-ray absorption cross section, which leads to a high light yield. The zero-dimensional copper halide Cs3Cu2I5 (CCI) exhibits a very high photoluminescence quantum yield and blue emission, making it compatible with photomultipliers with a higher photon detection efficiency in this wavelength range. However, the oxidation of copper, along with the phase transition to a less emissive one-dimensional copper halide, presents significant stability challenges for these powerful scintillation materials, ultimately limiting their potential for future commercialization. In this work, we propose heavy atom doping with bismuth, which not only enhances the oxidation resistance of copper but also inhibits the phase transformation. By addition of trivalent bismuth during the antisolvent synthesis, we achieved nearly 60% increase in radioluminescence and a spatial resolution of 19 lp/mm while maintaining the original blue emission. We also compared the scintillation properties of our CCI:Bi with those of commercial LYSO:Ce, both of which emit at a peak wavelength of 450 nm. By irradiating the materials at varying dose rates, we evaluated their sensitivity to changes in irradiation. LYSO:Ce generates 33,000 photons/MeV, while our CCI:Bi produces over 66,000 photons/MeV, based on radioluminescence area comparisons. Furthermore, the calculated detection limits are 46 nGy/s for CCI:Bi-over 100 times lower than the standard dose for medical examinations-and 95 nGy/s for LYSO:Ce. These findings underscore the significant potential of CCI:Bi as a highly sensitive and stable X-ray scintillator.

High-voltage additives play a crucial role in stabilizing high-energy alkali metal batteries. However, the prevailing additives, typically strongly solvating solvents (e.g., esters, sulfones, and nitriles), face challenges in simultaneously stabilizing highly reactive metal anodes and high-voltage cathodes. Here, we introduce a new concept in additive design by proposing non-solvating additives (NSAs), which selectively solvate anions while barely coordinating to cations. This “anti-solvation” effect brings notable improvement in antioxidation and kinetic enrichment of NSAs at the cathode during charging while preserving high-quality metal deposition. A model electrolyte demonstrates exceptional resilience against high-voltage Na3V2(PO4)2F3 (NVPF3) cathode and Na anode, as evidenced by the decent shelf-storage Coulombic efficiency for Na||Cu after 100 days and capacity retention for Na||NVPF3 after aging for 60 days. This paradigm shift from strongly solvating additives to NSAs suggests that, by prioritizing kinetic anion-additive distribution over traditional cationic solvation-centric approaches/anion aggregates, interfacial stability of opposing electrodes can be simultaneously obtained.

InAs colloidal quantum dots (CQDs) are promising for shortwave infrared (SWIR) optoelectronics, due to their size-tunable optical properties, compatibility with CMOS technology, and compliance with the RoHS directive. However, increasing CQD size to achieve extended SWIR (eSWIR) bandgaps and improving charge transport often compromises colloidal stability. Ultralong InAs colloidal quantum nanorods (CQNRs) were synthesized through chemical control using lithium bis(trimethylsilyl)amide (LiN(Si(CH3)3)2), which promotes their elongation, enabling the synthesis of nanorods up to ∼200 nm in length. Transitioning from spherical QDs to nanorods allows size extension without inducing aggregation or precipitation. The resulting CQNRs exhibit excellent colloidal stability and absorption up to 2000 nm in the eSWIR region. Photodiodes fabricated from these CQNRs exhibit very low dark current (6 μA cm-2) and high external quantum efficiency (10.6%), attributed to enhanced percolation pathways with reduced hopping resistance, consistent with four-dimensional scanning transmission electron microscopy and lateral transport measurements. Ultralong, colloidally stable InAs CQNRs combine extended eSWIR absorption with efficient charge transport, making them suitable for environmentally compliant large CQDs in next-generation high-performance eSWIR optoelectronic devices.

Ligand-modified metal nanoclusters (NCs) have emerged as candidate materials for catalysis owing to their well-defined yet tunable structure and their metal centers' high nuclearity. We posited that NC-based catalytic behavior will depend on ligand properties, the accessibility of active sites, and their atomic configuration. We synthesized a series of Cu NC-based catalysts, tuned local hydrophobicity through ligand adjustment, balanced the ligand coverage and active site exposure, and found that we were, in this way, able to engender efficient electrosynthesis of acetate via CO electroreduction. Computation and operando spectroscopy show that asymmetric Cu-Cu sites, which determine the CO binding strength, impact the bifurcation step after C-C coupling. The best of these catalysts, Cu13Nap, achieved an acetate Faradaic efficiency (FE) of 86% and an energy efficiency of 29% in a 5 bar system, exceeding the single C2+ FE of <50% previously achieved by NC-based catalysts.

Efficient color converters are essential for achieving high -3-dB bandwidths and net data rates in optical wireless communications (OWCs). Here, we emphasize the significance of lanthanide-based metal-organic frameworks (MOFs) combined with an effective energy transfer strategy for developing high-performance color converters in OWC systems. In this approach, we successfully reduced the photoluminescence (PL) lifetime from 1.3 ms of the MOF to 4.6 ns of the MOF-chromophore composite, achieved through an efficient energy transfer process in the cavity and surface of the MOFs. This significant reduction in PL lifetime led to a dramatic increase in the -3-dB bandwidth, rising from less than 0.1 to 65.7 MHz. Most importantly, a net data rate of 1.076 GB/s was achieved, marking the first successful demonstration of lanthanide-based MOFs as color converters that facilitate data transmission rates exceeding 1 GB/s. Notably, both the -3-dB bandwidth and net data rate surpass those of most reported organic and inorganic materials, underscoring the exceptional potential of lanthanide-based MOFs when combined with an efficient energy transfer strategy. We believe this combination paves the way for further innovations in high-speed OWC technologies.

Organic-inorganic metal halide glasses (OIMHGs) are promising materials for high-resolution X-ray imaging due to their transparency and tunable properties. However, their practical applications are severely limited by a transition from the glassy state to a polycrystalline phase under ambient conditions, leading to significant optical and performance degradation. Herein, the underlying mechanism of the rapid glass-to-crystal transition in methyltriphenylphosphonium-based hybrid materials (MTP)2MnBr4 is systematically investigated through X-ray absorption fine structure (XAFS) measurements, X-ray scattering analysis, and ab initio molecular dynamics simulations. For the first time, it is demonstrated that this transition is driven by the water molecules, which significantly influence the spatial arrangement of the organic (MTP+) and inorganic ([MnBr4]2-) components within the materials framework. To address the severe instability of this X-ray imaging glass in air, a novel composite encapsulation strategy is developed that integrates quartz glass layers with a waterproof parylene polymer coating. Consequently, the glass-to-crystal transition is substantially suppressed, enhancing the stability of the synthesized glass by over 100 times. This improvement enabled the material to maintain a spatial resolution of 26.3 lp mm-1 for more than twelve months. These findings underscore the critical role of environmental stability strategies in enhancing OIMHG-based scintillators for next-generation X-ray imaging applications.

The invention of non-fullerene acceptors has made it possible for organic solar cells to quickly improve their power conversion efficiencies to over 19

Copper(I) halide-based emitters have recently garnered significant attention for their potential in X-ray imaging applications owing to their efficient emission, facile synthesis, and low toxicity. While several strategies have been proposed to improve scintillation efficiency in these systems, the critical role of Cu-I cores─particularly during ultrafast energy conversion and transport─has received limited attention. In this work, we introduce a unified ligand strategy to construct a series of zero-dimensional copper(I) iodide clusters, including a Cu1I1 monomer, Cu2I2 rhomboid dimer, and Cu4I4 cubane tetramer, all exhibiting near-unity photoluminescence quantum yield (ϕPL). This approach enables a systematic investigation of how the core architecture governs radioluminescence (RL) behavior and efficiency beyond ϕPL. Our results demonstrate that the core geometry has a strong influence on both thermal stability and exciton relaxation pathways. Notably, low-temperature PL-RL differences uncover a previously unrecognized exciton relaxation channel intrinsic to the cubane cluster, allowing a fraction of excitons to directly populate the 3CC state. This process confines exciton generation, transport, and radiative recombination within the Cu-I cubane, thereby potentially increasing the exciton transfer efficiency and enhancing scintillation efficiency. These findings provide critical insights into the fundamental scintillation mechanisms and structure-property relationships of Cu-I clusters, establishing core geometry as a key design principle for the development of next-generation, high-performance scintillators.

Advanced X-ray imaging scintillators hold great potential for medical diagnostics, security screening, and aerospace applications. However, organic materials encounter significant challenges in achieving high X-ray absorption and efficient exciton utilization due to their low atomic number and weak intersystem crossing (ISC), resulting in limited triplet emission when exposed to light excitation. Here, organometallic materials incorporating heavy-atom metal centers and organic linkers are developed as highly efficient X-ray imaging scintillators, exhibiting near-unity ISC and remarkable phosphorescence efficiency. Their optimized triplet-state properties and enhanced exciton utilization enable superior performance in X-ray imaging, offering improved sensitivity and spatial resolution. Notably, these materials achieve an ultralow X-ray detection limit of 84 nGy s-1, an impressive imaging resolution of 26.9 lp mm-1, and an outstanding light yield of 70.5 k photons MeV-1, substantially outperforming conventional organic and inorganic scintillators available in the X-ray imaging market. Moreover, these organometallic scintillators demonstrate nearly a threefold improvement in X-ray sensitivity at low temperatures, highlighting their significant potential for low-temperature X-ray imaging.

Solution‐based methods have emerged as a promising approach for large‐scale and low‐cost electronics fabrication. However, solution processing has rarely realized high‐performance p ‐type transistors, impeding the advancement of solution‐processed electronics. Among the various solution‐processable material families, van der Waals (vdW) systems stand out due to several attractive features, one of which is the atomically defined interfaces that facilitate carrier charge transport, enabling enhanced device performance. Here, the preparation of transistors based on single tellurium (Te) nanowires (NW) is demonstrated, achieving high mobilities averaging ≈370 cm 2 V −1 s −1 . Notably, subsequent studies reveal that devices based on Te‐Te NW junctions exhibit mobilities comparable to those of the individual NWs forming the junction. This indicates that the vdW contact between the Te NWs causes negligible degradation in the mobility, which aligns with the theoretical calculations. Based on this finding, a large‐area 1D Te NWs vdW film is further prepared, consisting of a large number of 1D Te NWs interconnected by vdW junctions. The resulting transistors can still maintain remarkable operating characteristics, including an average field‐effect hole mobility of ≈94.9 cm 2 V −1 s −1 , a subthreshold swing of ≈248.6 mVdec −1 , a current on/off ratio of ≈10 4 , and a low operating voltage of 1 V.

Lead-free, all-inorganic halide nanocrystals hold promise for advanced devices, with chloride-based variants offering stability, tunable band gaps, and easy processing. However, these nanocrystals face synthesis challenges due to the low solubility and complex coordination of heavy metal chloride salts. The conventional ligand-assisted reprecipitation (LARP) method is incompatible with chloride-based crystals, while the hot-injection technique is slow and complex, hindering efficient synthesis and scalability. We present a modified LARP method using an acid-mediated strategy to synthesize undoped and Sb3+-doped Rb3InCl6 nanocrystals. These nanocrystals maintain colloidal stability for up to 6 months and exhibit a large Stokes shift (230 nm), a high photoluminescence quantum yield (PLAY) of 68.01%, low self-absorption, and a high light yield of 15,500 photons/MeV. The flexible nanocrystal composite film with polysulfone achieves an X-ray imaging resolution of 18.5 line pairs per millimeter (lp mm--1-1). The colloidal solution and film of Rb3InCl6:Sb nanocrystals exhibit strong radioluminescence and linear responses under X-ray irradiation, highlighting their potential for medical radiography.

Cu(I) halide-based scintillators are emerging as eco-friendly alternatives to traditional X-ray imaging scintillators because of their high luminescence efficiency and solution processability. Although much progress has been made in zero-dimensional (0D) Cu-I cluster scintillators, there has been limited focus on one-dimensional (1D) Cu-I coordination polymers because of their lower luminescence efficiencies. This study presents a ligand halogen engineering strategy for significantly enhancing the photoluminescence efficiency of 1D Cu-I coordination polymers by utilizing halogen-based chemical modifications. The chlorine-modified ligands increase structural rigidity, reducing electronic repulsion between copper and iodine atoms and minimizing photon loss through non-radiative recombination pathways, resulting in an impressive photoluminescence quantum yield of nearly 100%. The designed scintillators demonstrate improved radioluminescence intensity, low detection limits, and exceptional spatial resolution (16 lp/mm). This research offers an approach for creating highly emissive 1D Cu-I coordination polymers and highlights their potential in X-ray imaging applications in medical diagnosis and security checks.