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Circularly polarized luminescence (CPL)‐active molecular materials have drawn increasing attention due to their promising applications for next‐generation display and optoelectronic technologies. Currently, it is challenging to obtain CPL materials with both large luminescence dissymmetry factor (glum) and high quantum yield (Φ). A pair of enantiomeric N N C‐type Pt(II) complexes (L/D)‐1 modified with chiral Leucine methyl ester are presented herein. Though the solutions of these complexes are CPL‐inactive, the spin‐coated thin films of (L/D)‐1 exhibit giantly‐amplified circularly polarized phosphorescences with |glum| of 0.53 at 560 nm and Φair of ~50 %, as well as appealing circular dichroism (CD) signals with the maximum absorption dissymmetry factor |gabs| of 0.37–0.43 at 480 nm. This superior CPL performance benefits from the hierarchical formation of crystalline fibrillar networks upon spin coating. Comparative studies of another pair of chiral Pt(II) complexes (L/D)‐2 with a symmetric N C N coordination mode suggest that the asymmetric N N C coordination of (L/D)‐1 are favorable for the efficient exciton delocalization to amplify the CPL performance. Optical applications of the thin films of (L/D)‐1 in CPL‐contrast imaging and inducing CP light generation from achiral emitters and common light‐emitting diode lamps have been successfully realized. [ABSTRACT FROM AUTHOR]

The development of a methodology for synthesizing value‐added urea (CO(NH2)2) via a renewable electricity‐driven C−N coupling reaction under mild conditions is highly anticipated. However, the complex catalytic active sites that act on the carbon and nitrogen species make the reaction mechanism unclear, resulting in a low efficiency of C−N coupling from the co‐reduction of carbon dioxide (CO2) and nitrate (NO3−). Herein, we propose a novel tandem catalyst of Mo‐PCN‐222(Co), in which the Mo sites serve to facilitate nitrate reduction to the *NH2 intermediate, while the Co sites enhance CO2 reduction to carbonic oxide (CO), thus synergistically promoting C−N coupling. The synthesized Mo‐PCN‐222(Co) catalyst exhibited a noteworthy urea yield rate of 844.11 mg h−1 g−1, alongside a corresponding Faradaic efficiency of 33.90 % at −0.4 V vs. reversible hydrogen electrode (RHE). By combining in situ spectroscopic techniques with density functional theory calculations, we demonstrate that efficient C−N coupling is attributed to a tandem system in which the *NH2 and *CO intermediates produced by the Mo and Co active sites of Mo‐PCN‐222(Co) stabilize the formation of the *CONH2 intermediate. This study provides an effective avenue for the design and synthesis of tandem catalysts for electrocatalytic urea synthesis. [ABSTRACT FROM AUTHOR]

Metal‐organic phosphorescent complexes containing Ir or Pt are work horse in organic light‐emitting diode (OLED) technology, which can harvest both singlet and triplet excitons in electroluminescence (EL) owing to strong heavy‐atom effect. Recently, organic room‐temperature phosphorescence (ORTP) have achieved high photoluminescence quantum yield (PLQY) in rigid crystalline state, which, however, is unsuitable for OLED fabrication, therefore leading to an EL efficiency far low behind those of metal‐organic phosphorescent complexes. Here, we reported a luminescence mechanism switch from thermally activated delayed fluorescence (TADF) in single crystal microwires to ORTP in amorphous thin‐films, based on a tert‐butylcarbazole difluoroboron β‐diketonate derivative of DtCzBF2. Tightly packed and well‐faceted single‐crystal microwires exhibit aggregation induced emission (AIE), enabling TADF microlasers at 473 nm with an optical gain coefficient as high as 852 cm−1. In contrast, loosely packed dimers of DtCzBF2 formed in guest‐host amorphous thin‐films decrease the oscillator strength of fluorescence transition but stabilize triplets for ORTP with a PLQY up to 61 %, leading to solution‐processed OLEDs with EQE approaching 20 %. This study opens possibilities of low‐cost ORTP emitters for high performance OLEDs and future low‐threshold electrically injected organic semiconductor lasers (OSLs). [ABSTRACT FROM AUTHOR]

Stimulated Raman scattering offers an alternative strategy to explore continuous‐wave (c.w.) organic lasers, which, however, still suffers from the limitation of inadequate Raman gain in organic material systems. Here we propose a metal‐linking approach to enhance the Raman gain of organic molecules. Self‐assembled microcrystals of the metal linked organic dimers exhibit large Raman gain, therefore allowing for c.w. Raman lasing. Furthermore, broadband tunable Raman lasing is achieved in the organic dimer microcrystals by adjusting excitation wavelengths. This work advances the understanding of Raman gain in organic molecules, paving a way for the design of c.w. organic lasers. [ABSTRACT FROM AUTHOR]

Macroscopic compass‐like magnetic alignment at low magnetic fields is natural for ferromagnetic materials but is seldomly observed in paramagnetic materials. Herein, we report a "paramagnetic compass" that magnetically aligns under ~mT fields based on the single‐crystalline framework constructed by lanthanide ions and organic ligands (Ln‐MOF). The magnetic alignment is attributed to the Ln‐MOF's strong macroscopic anisotropy, where the highly‐ordered structure allows the Ln‐ions' molecular anisotropy to be summed according to the crystal symmetry. In tetragonal Ln‐MOFs, the alignment is either parallel or perpendicular to the field depending on the easiest axis of the molecular anisotropy. Reversible switching between the two alignments is realized upon the removal and re‐adsorption of solvent molecules filled in the framework. When the crystal symmetry is lowered in monoclinic Ln‐MOFs, the alignments become even inclined (47°‐66°) to the field. These fascinating properties of Ln‐MOFs would encourage further explorations of framework materials containing paramagnetic centers. [ABSTRACT FROM AUTHOR]

The development of circularly polarized electroluminescence (CPEL) is currently hampered by the high difficulty and cost in the syntheses of suitable chiral materials and the notorious chirality diminishment issue in electrical devices. Herein, diastereomeric IrIII and RuII complexes with chiral (±)‐camphorsulfonate counteranions are readily synthesized and used as the active materials in circularly polarized light‐emitting electrochemical cells to generate promising CPELs. The addition of the chiral ionic liquid (±)‐1‐butyl‐3‐methylimidazole camphorsulfonate into the active layer significantly improves the device performance and the electroluminescence dissymmetry factors (≈10−3), in stark contrast to the very weak circularly polarized photoluminescence of the spin‐coated films of these diastereomeric complexes. Control experiments with enantiopure IrIII complexes suggest that the chiral anions play a dominant role in the electrically‐induced amplification of CPELs. [ABSTRACT FROM AUTHOR]

Abstract: Thermal‐responsive phosphorescent nanotubes have been fabricated from the co‐assembly of two neutral iridium complexes, which behave as the antenna chromophores and energy acceptors, respectively, in these highly ordered crystalline superstructures. By tuning the acceptor doping ratio in a range of 0 to 0.5 %, these tubes display color‐tunable phosphorescence from green to red at room temperature, and it is attributed to the highly efficient light‐harvesting and energy transfer within these materials. For the same reason, the acceptor emission in the nanotubes is amplified more than 800 times with respect to its pure non‐emissive solid sample. The doped tubes show reversible thermal‐responsiveness, in which the energy transfer was completely suppressed at 77 K and reactivated at room temperature. These processes were characterized by the in situ emission color (green, orange, and red) and spectral changes and lifetime measurements of isolated nanotubes. The temperature‐controlled exciton dynamics are responsible for the luminescent thermochromism in these crystalline materials. [ABSTRACT FROM AUTHOR]

Organic circularly polarized (CP) lasers have received increasing attention due to their future photoelectric applications. Here, we demonstrate a CP laser from a pure organic crystal‐filled microcavity without any chiral molecules or chiral structures. Benefited from the giant anisotropy and excellent laser gain of organic crystals, optical Rashba‐Dresselhaus spin‐orbit coupling effect can be induced and is conductive to the CP laser in such microcavities. The maximum dissymmetry factor of the CP lasing with opposite helicities reachs 1.2. Our strategy may provide a new idea for the design of CP lasers towards future 3D laser displays, information storage and other fields. [ABSTRACT FROM AUTHOR]

Nano‐ and micromaterials with anisotropic photoluminescence and photon transport have widespread application prospects in quantum optics, optoelectronics, and displays. But the nature of the polarization information of the out‐coupled light, with respect to that of the source luminescence, has never been explored in active optical‐waveguiding organic crystals. Herein, three different modes (selective, anisotropic, and consistent) of polarized‐photon out‐coupling are proposed and successfully implemented in a set of 2D organic microcrystals with highly linearly‐polarized luminescence. It is found that the polarization direction and degree of the luminescence out‐coupled through different waveguiding channels can either be essentially retained or distinctly changed with respect to those of the original luminescence, depending on the molecular arrangement and the orientation of transition dipole moments of the crystal. This work demonstrates the promising potential of 2D emissive microcrystals in multi‐channel polarized photon transport. [ABSTRACT FROM AUTHOR]

A diruthenium complex with a redox-active amine bridge has been designed, synthesized, and studied by single-crystal X-ray analysis and DFT and TDDFT calculations. It shows three well-separated redox processes with exclusive near-infrared (NIR) absorbance at each redox state. The electropolymerized film of a related vinyl-functionalized complex displays multistate NIR electrochromism with low operational potential, good contrast ratio, and long retention time. Flip-flop, flip-flap-flop, and ternary memories have been realized by using the obtained film (ca. 15-20 nm thick) with three electrochemical inputs and three NIR optical outputs that each displays three levels of signal intensity. [ABSTRACT FROM AUTHOR]

Conventional square‐planar platinum complexes typically form one‐dimensional assemblies as a result of unidirectional metallophilic and/or π⋅⋅⋅π intermolecular interactions. Organoplatinum(II) complexes with a cruciform shape are presented herein to construct two‐dimensional (2D) microcrystals with full‐color and white phosphorescence. These 2D crystals show unique monocomponent π⋅⋅⋅π stacking, from either the cyclometalating or noncyclometalating ligand, and the bicomponent alternate π⋅⋅⋅π stacking from both ligands along different facet directions. Anisotropic tri‐directional waveguiding is further implemented on a single hexagonal microcrystal. These results demonstrate the great capability of the organoplatinum(II) cruciform as a general platform to fabricate 2D phosphorescent micro‐/nanocrystals for advanced photonic applications. [ABSTRACT FROM AUTHOR]

A simple and general method is presented herein for the in situ preparations of circularly polarized luminescence (CPL)‐active microcrystals with a large luminescence dissymmetry factor glum, high fluorescence quantum efficiency (ΦFL), wide emission color tenability, and well‐ordered morphology. The reactions of pyridine‐containing achiral molecules 1–7 with chiral camphor sulfonic acid ((±)‐CSA) gave crystalline microplates formed by hydrogen bonding interactions between the protonated pyridinium units and the sulfonic anions. The chiral information of CSA are effectively transferred to the microcrystals by hydrogen bonding to afford full‐color CPL from deep‐blue to red with glum in the order of 10−2 and ΦFL up to 80 %. Moreover, organic microcrystals with high‐performance white CPL (ΦFL=46 %; |glum|=0.025) are achieved via the light‐harvesting energy transfer between blue and yellow emitters. [ABSTRACT FROM AUTHOR]

A dual‐site catalyst allows for a synergetic reaction in the close proximity to enhance catalysis. It is highly desirable to create dual‐site interfaces in single‐atom system to maximize the effect. Herein, we report a cation‐deficient electrostatic anchorage route to fabricate an atomically dispersed platinum–titania catalyst (Pt1O1/Ti1−xO2), which shows greatly enhanced hydrogen evolution activity, surpassing that of the commercial Pt/C catalyst in mass by a factor of 53.2. Operando techniques and density functional calculations reveal that Pt1O1/Ti1−xO2 experiences a Pt−O dual‐site catalytic pathway, where the inherent charge transfer within the dual sites encourages the jointly coupling protons and plays the key role during the Volmer–Tafel process. There is almost no decay in the activity of Pt1O1/Ti1−xO2 over 300 000 cycles, meaning 30 times of enhancement in stability compared to the commercial Pt/C catalysts (10 000 cycles). [ABSTRACT FROM AUTHOR]

Miniaturized lasers with high spectral purity and wide wavelength tunability are crucial for various photonic applications. Here we propose a strategy to realize broadband‐tunable single‐mode lasing based on a photoisomerization‐activated intramolecular charge‐transfer (ICT) process in coupled polymer microdisk cavities. The photoisomerizable molecules doped in the polymer microdisks can be quantitatively transformed into a kind of laser dye with strong ICT character by photoexcitation. The gain region was tailored over a wide range through the self‐modulation of the optically activated ICT isomers. Meanwhile, the resonant modes shifted with the photoisomerization because of a change in the effective refractive index of the polymer microdisk cavity. Based on the synergetic modulation of the optical gain and microcavity, we realized the broadband tuning of the single‐mode laser. These results offer a promising route to fabricate broadband‐tunable microlasers towards practical photonic integrations. [ABSTRACT FROM AUTHOR]

Single‐atom catalysts have attracted much attention. Reported herein is that regulating charge transfer of lattice oxygen atoms in serial single‐atom‐doped titania enables tunable hydrogen evolution reaction (HER) activity. First‐principles calculations disclose that the activity of lattice oxygen for the HER can be regularly promoted by substituting its nearest metal atom, and doping‐induced charge transfer plays an essential role. Besides, the realm of the charge transfer of the active site can be enlarged to the second nearest atom by creating oxygen vacancies, resulting in further optimization for the HER. Various single‐atom‐doped titania nanosheets were fabricated to validate the proposed model. Taking advantage of the localized charge transfer to the lattice atom is demonstrated to be feasible for realizing precise regulation of the electronic structures and thus catalytic activity of the nanosheets. [ABSTRACT FROM AUTHOR]

Organic solid‐state semiconductor lasers are attracting ever‐increasing interest for their potential application in future photonic circuits. Despite the great progress made in recent years, an organic laser from 3D chiral structures has not been achieved. Now, the first example of an organic nano‐laser from the micro‐helix structure of an achiral molecule is presented. Highly regular micro‐helixes with left/right‐handed helicity from a distyrylbenzene derivative (HM‐DSB) were fabricated and characterized under microscope spectrometers. These chiral micro‐helixes exhibit unique photonic properties, including helicity‐dependent circularly polarized luminescence (CPL), periodic optical waveguiding, and length‐dependent amplified spontaneous emission (ASE) behavior. The successful observation of laser behavior from the organic micro‐helix extends our understanding to morphology chirality of organic photonic materials and provides a new design strategy towards chiral photonic circuits. [ABSTRACT FROM AUTHOR]

Singlet fission (SF) holds the potential to boost the maximum power conversion efficiency of photovoltaic devices. Internal conversion (IC) has been considered as one of the major competitive deactivation pathways to transform excitation energy into heat. Now, using time‐resolved spectroscopy and theoretical calculation, it is demonstrated that, instead of a conventional IC pathway, an unexpected intramolecular singlet fission (iSF) process is responsible for excited state deactivation in isoindigo derivatives. The 1TT state could form at ultrafast rate and nearly quantitatively in solution. In solid films, the slipped stacked intermolecular packing of a thiophene‐functionalized derivative leads to efficient triplet pair separation, giving rise to an overall triplet yield of 181 %. This work not only enriches the pool of iSF‐capable materials, but also contributes to a better understanding of the iSF mechanism, which could be relevant for designing new SF sensitizers. [ABSTRACT FROM AUTHOR]

As a promising technique for CO2 fixation/utilization and energy conversion/storage, the metal–CO2 battery has been studied to improve its interconversion between CO2 and carbonates/oxalates. Herein, we propose and realize a reversible aqueous Zn–CO2 battery based on the reversible conversion between CO2 and liquid HCOOH on a bifunctional Pd cathode. The 3D porous Pd interconnected nanosheet with enriched edge and pore structure, has a highly electrochemical active surface to facilitate simultaneous selective CO2 reduction and HCOOH oxidation at low overpotentials. The resulting battery has a 1 V charge voltage, a cycling durability over 100 cycles, and a high energy efficiency of 81.2 %. The battery mechanism is proposed as Zn+CO2+2 H++2 OH−↔ ZnO+HCOOH+H2O, through which the reversible conversion between CO2 and liquid HCOOH was realized. [ABSTRACT FROM AUTHOR]

Abstract: A readily available small molecular hole‐transporting material (HTM), OMe‐TATPyr, was synthesized and tested in perovskite solar cells (PSCs). OMe‐TATPyr is a two‐dimensional π‐conjugated molecule with a pyrene core and four phenyl‐thiophene bridged triarylamine groups. It can be readily synthesized in gram scale with a low lab cost of around US$ 50 g−1. The incorporation of the phenyl‐thiophene units in OMe‐TATPyr are beneficial for not only carrier transportation through improved charge delocalization and intermolecular stacking, but also potential trap passivation via Pb–S interaction as supported by depth‐profiling XPS, photoluminescence, and electrochemical impedance analysis. As a result, an impressive best power conversion efficiency (PCE) of up to 20.6 % and an average PCE of 20.0 % with good stability has been achieved for mixed‐cation PSCs with OMe‐TATPyr with an area of 0.09 cm2. A device with an area of 1.08 cm2 based on OMe‐TATPyr demonstrates a PCE of 17.3 %. [ABSTRACT FROM AUTHOR]

Abstract: The electrochemical CO2 reduction (ECDRR), as a key reaction in artificial photosynthesis to implement renewable energy conversion/storage, has been inhibited by the low efficiency and high costs of the electrocatalysts. Herein, we synthesize a fluorine‐doped carbon (FC) catalyst by pyrolyzing commercial BP 2000 with a fluorine source, enabling a highly selective CO2‐to‐CO conversion with a maximum Faradaic efficiency of 90 % at a low overpotential of 510 mV and a small Tafel slope of 81 mV dec−1, outcompeting current metal‐free catalysts. Moreover, the higher partial current density of CO and lower partial current density of H2 on FC relative to pristine carbon suggest an enhanced inherent activity towards ECDRR as well as a suppressed hydrogen evolution by fluorine doping. Fluorine doping activates the neighbor carbon atoms and facilitates the stabilization of the key intermediate COOH* on the fluorine‐doped carbon material, which are also blocked for competing hydrogen evolution, resulting in superior CO2‐to‐CO conversion. [ABSTRACT FROM AUTHOR]

Abstract: Miniaturized nanowire nanolasers of 3D perovskites feature a high gain coefficient; however, room‐temperature optical gain and nanowire lasers from 2D layered perovskites have not been reported to date. A biomimetic approach is presented to construct an artificial ligh‐harvesting system in mixed multiple quantum wells (QWs) of 2D‐RPPs of (BA)2(FA)n−1PbnBr3n+1, achieving room‐temperature ASE and nanowire (NW) lasing. Owing to the improvement of flexible and deformable characteristics provided by organic BA cation layers, high‐density large‐area NW laser arrays were fabricated with high photostability. Well‐controlled dimensions and uniform geometries enabled 2D‐RPPs NWs functioning as high‐quality Fabry–Perot (FP) lasers with almost identical optical modes, high quality (Q) factor (ca. 1800), and similarly low lasing thresholds. [ABSTRACT FROM AUTHOR]

Singlet fission (SF), in which one singlet exciton (S1) splits into two triplets (T1) on adjacent molecules through a correlated triplet-pair 1(TT) state, requires precise but difficult tuning of exciton energetics and intermolecular electronic couplings in the solid state. Antiaromatic 4nπ dibenzopentalenes (DPs) are demonstrated as a new class of single-chromophore-based intramolecular SF materials that exhibit an optically allowed S2 state with E(S2)>2×E(T1) and an optically forbidden S1 state. Ultrafast population transfer from a high-lying S2 state to a 1(TT) state was observed in monomeric solution of styryl-substituted DP (SDP) on a sub-picosecond timescale. There is evidence of exciton diffusion (ED) of the 1(TT) state to yield two individual long-lived triplets in SDP thin film. The overall triplet yield via intramolecular SF and subsequent triplet-pair diffusion can be as high as 142±10 % in thin film. [ABSTRACT FROM AUTHOR]

The anisotropic refractive properties of two-dimensional organic single crystals lead to the Rashba-Dresselhaus effect inducing spin-splitting of cavity modes. Circularly Polarized Laser, Optical Microcavity, Organic Crystals, Spin-Orbit Coupling Keywords: Circularly Polarized Laser; Optical Microcavity; Organic Crystals; Spin-Orbit Coupling EN Circularly Polarized Laser Optical Microcavity Organic Crystals Spin-Orbit Coupling 1 1 1 02/21/23 20230220 NES 230220 B Circularly polarized lasing b with high dissymmetry factors has been realized in an organic crystal-filled cavity without any chiral materials or structures, as reported by Qing Liao, Hongbing Fu, and co-workers in their Research Article (e202213229). [Extracted from the article]

Development of nanowire photonics requires integration of different nanowire components into highly ordered functional heterostructures. Herein, we report a sequential self-assembly of binary molecular components into branched nanowire heterostructures (BNHs) via lattice-matched epitaxial growth, in which the microribbon backbone of 2,5-Bis(5-tert-butyl-2-benzoxazolyl)thiophene (BBOT) functions as blue-emitting microlaser source to pump the nanowire branches of BODIPY. By constructing Au electrodes on both branch sides and measuring the photocurrent in them, we successfully realize the integration of an organic laser and a power meter in a single device. This work provides a new insight into the integration of 1D organic nanostructures into BNHs for realizing organic multifunctional photonic devices. [ABSTRACT FROM AUTHOR]

A laser array on the nano- and microscale is a key component for integration in photonic devices, but remains a challenge when using semiconductor nanowire lasers. Here we report a low-threshold lateral-cavity microlaser, formed between two lateral-faces of a single-crystalline organic microbelt (OMB) of 1,4-dimethoxy-2,5-di[4′-(cyano)styryl]benzene (COPV). By cutting a single OMB into six pieces by a top-down two-photon processing technique, we successfully fabricated a compact and uniform 1×6 microlaser array along the length direction of the OMB. The microlasers had excellent reproducibility and addressable high precision, thus making them attractive candidates as miniaturized coherent light sources for future nanophotonics. [ABSTRACT FROM AUTHOR]

Coherent light signals generated at the nanoscale are crucial to the realization of photonic integrated circuits. Self-assembled nanowires from organic dyes can provide both a gain medium and an effective resonant cavity, which have been utilized for fulfilling miniaturized lasers. Excited-state intramolecular proton transfer (ESIPT), a classical molecular photoisomerization process, can be used to build a typical four-level system, which is more favorable for population inversion. Low-power driven lasing in proton-transfer molecular nanowires with an optimized ESIPT energy-level process has been achieved. With high gain and low loss from the ESIPT, the wires can be applied as effective FP-type resonators, which generated single-mode lasing with a very low threshold. The lasing wavelength can be reversibly switched based on a conformation conversion of the excited keto form in the ESIPT process. [ABSTRACT FROM AUTHOR]

Stapelkunde: Zwei verschiedene, aber verwandte Naphthalene bilden, gesteuert durch ihre H ‐ Brückenbindungen und π ‐ π ‐ Stapelung, unterschiedliche Nanostrukturen (siehe Bild). Diese Nanostrukturen wiesen einzigartige Merkmale hinsichtlich photonischer Begrenzung und Lichtweiterleitung auf, was einen Einsatz in nanophotonischen Schaltkreisen nahelegt. [ABSTRACT FROM AUTHOR]

Zink‐CO2‐Batterien. Eine reversible wässrige Zn‐CO2‐Batterie wird von Y. Wang et al. in der Zuschrift auf S. 17242 ff. vorgestellt. Dreidimensional verbundene poröse Pd‐Nanoblätter fungieren als Kathode und bewirken die elektrokatalytische CO2‐Reduktion und HCOOH‐Oxidation. [ABSTRACT FROM AUTHOR]