Manganese-based halides present promising applications in flexible devices in versatile scenarios due to their low toxicity, high quantum yield, facile synthesis, and compatibility with multiple excitation sources. Herein, two novel manganese-based halides are synthesized, namely (CTP)2MnCl4 and (BTP)2MnCl4 (CTP = (2-chlorobenzyl)triphenylphosphonium, BTP = benzyltriphenylphosphonium), utilizing a solvent evaporation method. High photoluminescence quantum yields are achieved, approximate to 98.5% and 88.4%, respectively. Upon mechanical stimulations, both materials exhibited intense green emission attributed to the recombination of electrons and holes. Effective force-induced luminescence can be realized using a flexible, force-responsive film derived from the two compounds. In addition, the (CTP)2MnCl4 and (BTP)2MnCl4 crystals exhibited remarkable X-ray scintillation properties. Based on commercial CsI, Tl scintillator standards, the calculated light yields for (CTP)2MnCl4 and (BTP)2MnCl4 single crystals are approximate to 89 000 and 49 000 photons/MeV, respectively. A flexible scintillation film is fabricated with (CTP)2MnCl4 and polydimethylsiloxane. Furthermore, a light-emitting fiber film with a large area of 20 cm x 25 cm is fabricated using (CTP)2MnCl4 and polymethyl methacrylate via an electrospinning method. The film is suitable for applications in emergency rescue, information recording, and emergency lighting. This research provides a new approach for synthesizing large-sized, high-performance luminescence materials with multiple excitation sources and their versatile applications.

Red emitting one-dimensional hybrid manganese chloride (TMA)MnCl 3 shows a near-unity PLQY, as well as the high anti-thermal quenching behavior due to the high structural rigidity.

The luminescence property of various compounds is developed in the photoelectric applications field, while the near‐infrared (NIR) dual‐band emission of compounds is extremely challenging. Herein, 0D Cu(I)‐based organic–inorganic module (ETA)3Cu6I9 is synthesized to achieve NIR and cyan dual‐band emission in metal halide systems. Density functional theory (DFT) calculations combined with comprehensive spectroscopic data reveal its emission mechanism. Under the excitation at 371 nm, (ETA)3Cu6I9 shows the broadband NIR emission peaking at 775 nm with a large wavelength, attributed to the triple‐cluster‐center (3CC) transition. Meanwhile, under 286 nm excitation, (ETA)3Cu6I9 shows a bright cyan emission peaking at 490 nm, attributed to the metal‐to‐ligand charge transfer (MLCT) or halide‐to‐ligand charge transfer (XLCT) transitions. Moreover, (ETA)3Cu6I9 presents relatively superior thermal and air stability. Benefiting from the good stability of (ETA)3Cu6I9, the as‐fabricated NIR‐LED device demonstrates great potential in biological imaging and night vision. This study opens up a new way for designing new non‐toxic NIR and cyan dual‐band emission materials, which guides to synthesize new materials in metal halide field.

Zero-dimensional (0D) hybrid metal halides, which consist of organic cations and isolated inorganic metal halide anions, have emerged as phosphors with efficient broadband emissions. However, these materials generally have too wide bandgaps and thus cannot be excited by blue light, which hinders their applications for efficient white light-emitting diodes (WLEDs). The key to achieving a blue-light-excitable 0D hybrid metal halide phosphor is to reduce the fundamental bandgap by rational chemical design. In this work, we report two designed hybrid copper(I) iodides, (Ph3MeP)(2)Cu4I6 and (Cy3MeP)(2)Cu4I6, as blue-light-excitable yellow phosphors with ultrabroadband emission. In these compounds, the [Cu4I6](2-) anion forms an I-6 octahedron centered on a cationic Cu-4 tetrahedron. The strong cation-cation bonding within the unique cationic Cu-4 tetrahedra enables significantly lowered conduction band minimums and thus narrowed bandgaps, as compared to other reported hybrid copper(I) iodides. The ultrabroadband emission is attributed to the coexistence of free and self-trapped excitons. The WLED using the [Cu4I6](2-) anion-based single phosphor shows warm white light emission, with a high luminous efficiency of 65 lm W-1 and a high color rendering index of 88. This work provides strategies to design narrow-bandgap 0D hybrid metal halides and presents two first examples of blue-light-excitable 0D hybrid metal halide phosphors for efficient WLEDs.

Scintillators with high light yield, low detection limit, large X-ray attenuation efficiency as well as stable and nontoxic compositions are of great importance for radiation detection applications. Here, 0D (C8H20N)(2)Cu2Br4 single crystals are obtained and show blue emission peaking at 468 nm with a near-unity photoluminescence quantum yield of 99.7%, a large Stokes shift of 148 nm (i.e., negligible self-absorption), and a good environmental stability along with strong X-ray absorption capability. Moreover, a high light yield of up to approximate to 91 300 photons/MeV and a low detection limit of 52.1 nGy(air) s(-1) are realized, which is more than one hundred times lower than the dose rate of 5.5 mu Gy(air) s(-1) required for X-ray medical diagnostics. (C8H20N)(2)Cu2Br4 ceramic wafer scintillation screen is fabricated by a cold pressing sintering process, and the clear contrast images of opaque metal box and electronic component with a spatial resolution of 9.54 lp mm(-1) are realized. This study not only designs a new lead-free metal halide scintillator, but also develops a universal strategy for the preparation of large-sized scintillator screen in nondestructive X-ray imaging.

Luminescent metal halide perovskites (MHPs) open new avenues for highly efficient radiation detection. To challenge the state‐of‐art technology, fundamental understanding of factors controlling radiation light yield of MHP scintillators is urgent. Herein, a design method is established by simultaneously considering charge‐transfer and recombination efficiencies via band alignment engineering in doped MHPs materials, and this strategy is corroborated experimentally and computationally by applying it to the luminescence of ns2 electron (Sb3+, Bi3+, and Te4+) doped vacancy‐ordered double perovskite Cs2ZrCl6. Alloying Te4+ into Cs2ZrCl6 is optimized and significantly improves the scintillation performance, including a twofold increase in light yield and a threefold increase in detection limit over pristine Cs2ZrCl6, and high‐resolution X‐ray imaging with 20 μm for 2D and 0.2 mm for 3D imaging. It is believed that doping engineering in MHPs enabling band alignment method holds great potential for the development of next‐generation MHP scintillators.

Laser-driven phosphor-converted white light sources are highly desirable for their unprecedented energy efficiency and lighting quality. However, important challenges remain due to a lack of efficient and stable red-emitting materials. Here Eu2+-activated oxide-based double perovskites are explored as red emitters with thermally stable photoluminescence. Sr3TaO5.5:Eu2+ ceramics exhibit a red emission band peaking at 620 nm upon blue laser pumping owing to the Eu2+ occupation at highly ordered substitutional lattice sites. A constructed laser-driven white light wheel under an incident power density of 19.2 W mm(-2) presents a record luminous flux of 1115 lm with an excellent color rendering index of 90. This study invigorates the development of Eu2+-activated oxide-based ceramics with thermally stable luminescence for laser-pumped lighting and display applications.

Cs2ZnBr4:Mn2+ and its composite film demonstrate good X-ray scintillation performances with a spatial resolution of 5.06 lp mm−1 in X-ray imaging.

Zero-dimensional (0D) hybrid metal halides are attractive owing to their distinctive structure as well as photoluminescence (PL) characteristics. To discover 0D hybrid metal halides with high photoluminescence quantum yield and good stability is of great significance for white light-emitting diodes (LEDs). Herein, a novel hybrid antimony chloride (CTP)2SbCl5 is synthesized, which shows a bright broad-band orange-red emission peaking at 620 nm under the low energy excitation (365 nm), achieving an excellent photoluminescence quantum yield of 96.8%. In addition, (CTP)2SbCl5 shows an additional emission peaking at 470 nm when excited at high energy (323 nm). PL spectra and density functional theory results demonstrate that the observed dual-band emission originates from the singlet and triplet self-trapped excitons confined in isolated [SbCl5]2- square pyramids. Moreover, (CTP)2SbCl5 presents relatively superior air stability, and the PL intensity still maintains 78% of the initial PL intensity when exposed to the air for above 2 weeks. Benefiting from high-efficiency PL emission and good stability of (CTP)2SbCl5, a stable warm white LED device with a 92.3% color rendering index was prepared by coating blue phosphor BaMgAl10O17:Eu2+, green (Sr,Ba)2SiO4:Eu2+, and orange-red (CTP)2SbCl5 on a 365 nm LED chip. This work provides an efficient luminescent material and also demonstrates the potential application of 0D hybrid antimony chloride in solid-state lighting.

铜(Ⅰ)基金属卤化物作为新一代环境友好的发光材料受到了研究者的广泛关注.本文采用溶剂辅助结晶法设计制备了一种新型零维金属卤化物发光材料(C12H24O6)NaCuBr2.在365 nm激发下,该化合物呈现出半峰宽为346 nm的超宽带橙红色发射,光致发光量子产率为42.6％.基于低温光谱、激发波长依赖的发射光谱和理论计算研究表明,峰值700 nm处的超宽带发射来自于Cu+离子3d轨道和Br-离子4p轨道间相互作用形成的简并能级.在低温下,(C12H24O6)NaCuBr2的晶格畸变导致能级的简并度降低,其荧光发射包含峰值为629 nm和735 nm的两个发射带.在高能激发下,电子跃迁到(C12H24O6)NaCuBr2的更高能级S3而带来的发射与77 K下观测到的480 nm处的发射峰相对应.采用(C12H24O6)NaCuBr2制备的白光发光二极管(LED)器件的显色指数高达90.6,表明其在全光谱照明领域具有潜在的应用前景.

Introduction:Recent advancements in reinforcement learning algorithms have accelerated the development of control models with high-dimensional inputs and outputs that can reproduce human movement. However, the produced motion tends to be less human-like if algorithms do not involve a biomechanical human model that accounts for skeletal and muscle-tendon properties and geometry. In this study, we have integrated a reinforcement learning algorithm and a musculoskeletal model including trunk, pelvis, and leg segments to develop control modes that drive the model to walk.Methods:We simulated human walking first without imposing target walking speed, in which the model was allowed to settle on a stable walking speed itself, which was 1.45 m/s. A range of other speeds were imposed for the simulation based on the previous self-developed walking speed. All simulations were generated by solving the Markov decision process problem with covariance matrix adaptation evolution strategy, without any reference motion data.Results:Simulated hip and knee kinematics agreed well with those in experimental observations, but ankle kinematics were less well-predicted.Discussion:We finally demonstrated that our reinforcement learning framework also has the potential to model and predict pathological gait that can result from muscle weakness.

铜（â ï¼‰åŸºé‡‘å±žå¤åŒ–ç‰©ä½œä¸ºæ–°ä¸€ä»£çŽ¯å¢ƒå‹å¥½çš„å‘å ‰ææ–™å—åˆ°äº†ç ”ç©¶è€ çš„å¹¿æ³›å ³æ³¨ã€‚æœ¬æ–‡é‡‡ç”¨æº¶å‰‚è¾ åŠ©ç»“æ™¶æ³•è®¾è®¡åˆ¶å¤‡äº†ä¸€ç§æ–°åž‹é›¶ç»´é‡‘å±žå¤åŒ–ç‰©å‘å ‰ææ–™ï¼ˆC12H24O6）NaCuBr2。在365 nm激发下，该化合物呈现出半峰宽为346 nmçš„è¶ å®½å¸¦æ©™çº¢è‰²å‘å°„ï¼Œå ‰è‡´å‘å ‰é‡å­äº§çŽ‡ä¸º42.6%ã€‚åŸºäºŽä½Žæ¸©å ‰è°±ã€æ¿€å‘æ³¢é•¿ä¾èµ–çš„å‘å°„å ‰è°±å’Œç†è®ºè®¡ç®—ç ”ç©¶è¡¨æ˜Žï¼Œå³°å€¼700 nmå¤„çš„è¶ å®½å¸¦å‘å°„æ¥è‡ªäºŽCu+离子3d轨道和Br-离子4p轨道间相互作用形成的简并能级。在低温下，（C12H24O6）NaCuBr2çš„æ™¶æ ¼ç•¸å˜å¯¼è‡´èƒ½çº§çš„ç®€å¹¶åº¦é™ä½Žï¼Œå ¶è§å ‰å‘å°„åŒ å«å³°å€¼ä¸º629 nm和735 nm的两个发射带。在高能激发下，电子跃迁到（C12H24O6）NaCuBr2的更高能级S3而带来的发射与77 K下观测到的480 nm处的发射峰相对应。采用（C12H24O6）NaCuBr2åˆ¶å¤‡çš„ç™½å ‰å‘å ‰äºŒæžç®¡ï¼ˆLED）器件的显色指数高达90.6ï¼Œè¡¨æ˜Žå ¶åœ¨å ¨å ‰è°±ç §æ˜Žé¢†åŸŸå ·æœ‰æ½œåœ¨çš„åº”ç”¨å‰æ™¯ã€‚

Hybrid metal halides, as a class of emerging luminescent materials, have received considerable attention for optoelectronic applications and beyond. The molecular dimensionality of hybrid metal halides is affected significantly by the organic ligands, leading to versatile energy-level structures and tunable photoluminescence (PL) behaviors. In this review, we summarize the structural characteristics of the different organic ligands in hybrid metal halides and especially focus on the establishment of structure–property relationships between organic ligand structures and luminescent properties in 0D hybrid metal halides. Finally, current research pursuits, challenges, and possible solutions are discussed for future studies.

The discovery of rare‐earth free luminescent materials with blue‐light‐excitable characteristic is of great importance for solid‐sate lighting applications. Herein, a Cu(I)‐based 0D luminescent hybrid ( 1,3‐dppH 2 ) 2 Cu 4 I 8 ∙H 2 O is synthesized by a facile solution method, and it shows the orange‐red emission peaking at 625 nm upon 460 nm excitation. The structure‐related luminescence mechanism has been elaborated by experimental and theoretical investigations. Moreover, the emission intensity remains unchanged even after continuous water treatment for 60 days due to the improved structural stability originating from intermolecular π–π interaction between organic cations. A warm white light‐emitting diode (LED) device with the color rendering index of 91.4% has been fabricated by combining the 440 nm LED chip, green‐emitting Lu 3 Al 5 O 12 :Ce 3+ , and ( 1,3‐dppH 2 ) 2 Cu 4 I 8 ∙H 2 O. This work provides a new design route towards 0D cuprous halide materials and will initiate more exploration of their intrinsic luminescence mechanism.

Metal clusters with color‐tunable radioluminescence have attracted growing attention as X‐ray detection materials. However, they are generally less scintillation‐efficient due to the coexistence of multiple exciton recombination centers. Herein, two new zero‐dimensional copper(I)‐based clusters (DIET)3Cu3X3 (DIET = 1,3‐Diethyl‐2‐thiourea, X = Cl, Br) are designed, which support the single channel photon emission (Cu cluster centered, CC) to enhance the scintillation performance. Those DIET ligands (L) anchoring with copper(I) ions not only generate direct CuL bonds, but also form a disorder [Cu3X3] cluster, which results in the intense X‐ray absorption. (DIET)3Cu3Br3 with low halogen electronegativity further weakens halogen‐to‐ligand charge transfer (XLCT) emission, enabling enhanced quantum efficiency (≈69%) and scintillation performance comparable to commercially available Lu3Al5O12:Ce. Moreover, the flexible thin film counterpart demonstrates legible X‐ray imaging with high spatial resolution of 11.71 lp mm−1. This study provides a feasible design principle to discover new metal cluster‐based scintillators and to further expand their radiation detection applications.

The dependence of photoluminescence quantum yield (PLQY) on the crystal structure of existing zero-dimensional ns(2) metal halides is analyzed with the help of principal component analysis and random forest methods. The primary role of the distance between metal ions in different compounds is revealed, and the influence of other structural features such as metal-halogen distance and the distortion of metal-halogen polyhedrons are quantified. Accordingly, the two previously unknown Sb3+-based zero-dimensional metal halides were synthesized to verify the obtained model. Experimental studies of the two compounds demonstrated good agreement with the predictions, and the PLQY of (C10H16N)(2)SbCl5 is found to be 96.5%. Via machine learning analysis, we demonstrate that concentration quenching is the main factor that determines PLQY for all s(2) ion metal halides, which will accelerate the discovery of new luminescence metal halides.

Zero-dimensional (0D) hybrid metal halides with unique compositional and structural tunability appear as an emerging class of luminescent materials, but near-infrared (NIR) emitters therein are largely unexplored to date. This study presents three novel 0D hybrid antimony chlorines with edge-sharing [Sb2Cl8](2-) dimers, showing unusual room-temperature broadband NIR emission with the maximum emission wavelength up to 1070 nm. Photoluminescence studies and density functional theory calculation demonstrate that the emissions originate from the highly localized excitons, and that the confined [Sb2Cl8](2-) dimers in these structures show low symmetry and a large degree of structural freedom. These hybrid antimony chlorines with [Sb2Cl8](2-) dimers expand the range of new NIR materials in 0D metal halides.

Doping impurity ions into semiconductor luminescent materials offers a unique pathway for inducing new emission centers and enabling photoluminescence (PL) tuning. Among various luminescence materials, doping Mn2+ into metal halide perovskites becomes a hot topic since Mn2+ ions demonstrate an energy transfer route from host to dopants, resulting in interesting photophysical properties. This review aims to discuss the PL properties of Mn2+ ions in halide perovskites nanocrystals or bulk crystals with different structural dimensions and local environments (MnX42– tetrahedron, MnX62– octahedron, or shortest Mn─Mn distance). In this regard, the effects of Mn2+ doping on the PL properties and their modifications are summarized. Variable ion exchange dynamics, increased emission intensity, and enhanced stability induced by Mn2+ doping are analyzed. These results also provide beneficial insights into applications of the doped luminescent halide perovskites. Finally, the present challenges in Mn2+‐doped luminescent halide perovskites are elaborated.

零维（0D）金属卤化物是一类新兴的发光材料体系,它们具有独特的"主-客"体结构,即独立的阴离子金属卤化物多面体客体规则有序地分布在有机阳离子或碱金属阳离子形成的主体框架中。这种具有相对较"软"晶格的0D金属卤化物材料的发光主要源于自陷激子（Self-trapped excitons, STEs）复合,其通常呈现出宽带发射,且具有大的斯托克斯位移。通过筛选不同的及多样化构型的金属卤化物多面体,将其与合适的有机阳离子或者Cs + 等组合,可形成多种新型结构的0D金属卤化物,并实现丰富的STEs发光特性,其可调节的荧光发射不仅可以覆盖整个可见光区,还可实现单相白光或近红外发光,成为光致发光材料研究领域的一个热点和重点。基于此,本文结合本课题组在该领域的研究工作基础,首先讨论了0D金属卤化物的光致发光机理;其次,介绍了具有不同多面体构型的0D金属卤化物材料的发光特性及应用;最后,总结了0D金属卤化物目前亟待解决的关键科学问题,并对0D金属卤化物的未来发展方向进行了展望。

Low-dimensional hybrid metal halides demonstrate broad-band emission and high photoluminescence quantum yield (PLQY) acting as excellent candidates for a new generation of luminescent materials in lighting fields. However, most luminescent metal halides can only be excited by ultraviolet radiation, and the discovery of high-efficient emitters with broad-band excitation characteristics, especially upon efficient blue light irradiation, is a challenge. Herein, a zero-dimensional (0D) Cu(I)-based organometallic halide (18-crown-6)(2)Na-2(H2O)(3)Cu4I6 (CNCI) was prepared with a green emission band centered at 536 nm and a near-unity PLQY (91.8%) upon excitation of 450 nm. Importantly, the ultrabroad excitation band covering a 300-500 nm range was observed in CNCI, and the luminescence mechanism has been discussed in detail. A white light-emitting diode (WLED) was fabricated with high luminous efficiency of 156 Im/W and a high color rendering index of 89.6. This work provides guidance for designing high-performance luminescent metal halides with suitable excitation characteristics and also promotes the application prospects of such materials in WLED fields.