This work demonstrates the feasibility of regulating exciton diffusion and hole transfer to promote efficient charge generation, and achieving high-performance OPV devices by increasing short-circuit current density. Fast and efficient charge generation requires an increased exciton diffusion length and faster hole transfer. In addition, the reduced trap state in the ternary system is also beneficial for reducing recombination of charges. This work reveals the co-mechanism of charge generation and trap state on J _SC.

Comprehensive Summary

Charge generation, a critical process in the operation of organic solar cell (OSC), requires thorough investigation in an ultrafast perspective. This work demonstrates that the utilization of alloy model for the non-fullerene acceptor (NFA) component can regulate the crystallization properties of active layer films, which in turn affects exciton diffusion and hole transfer (HT), ultimately influencing the charge generation process. By incorporating BTP-eC7 as a third component, without expanding absorption range or changing molecular energy levels but regulating the ultrafast exciton diffusion and HT processes, the power conversion efficiency (PCE) of the optimized PM6:BTP-eC9:BTP-eC7 based ternary OSC is improved from 17.30% to 17.83%, primarily due to the enhancement of short-circuit current density (J _SC). Additionally, the introduction of BTP-eC7 also reduces the trap state density in the photoactive layer which helps to reduce the loss of J _SC. This study introduces a novel approach for employing ternary alloy models by incorporating dual acceptors with similar structures, and elucidates the underlying mechanism of charge generation and J _SC in ternary OSCs.

Seventeen new lindenane sesquiterpenoid dimers (LSDs), chlorajaponins A—Q (1—17), including two rearranged skeleton meroterpenoids (1—2), and 13 reported analogs (18—30) were isolated from the Chloranthus japonicus Sieb. Compounds 1, 2, and 18 demonstrated significant inhibitory effects on lipid accumulation, dose-dependently reduced TG and TC levels, and significantly downregulated expression of FASN and SERBP1 validated by western blot assay. Moreover, compounds 19—22 and 25 exhibited the most potent anti-inflammatory effects with IC₅₀ values of 7.89, 6.25, 2.98, 10.77, and 3.60 μmol/L, respectively.

Comprehensive Summary

Seventeen undescribed lindenane-related sesquiterpenoid dimers, chlorajaponins A—Q (1—17), and 13 reported analogs (18—30) were isolated from Chloranthus japonicus Sieb. Compound 1 possesses an unprecedented 3/5/7/5/5/6/5/3 fused octacyclic scaffold, featuring a 6(5→4)-abeo-lindenane monomer, while 2 exhibits a 3/5/6/6/5/6/5/3 fused octacyclic scaffold. Their structures were determined through a combination of spectroscopic analyses and X-ray crystallography. Compounds 1, 2, and 18 demonstrated significant inhibitory effects on lipid accumulation and effectively reduced the levels of triglycerides and total cholesterol, as well as the levels of aspartate aminotransferase and alanine aminotransferase in a HepG2 cell model. In addition, compounds 1, 2, and 18 significantly suppressed the protein expression of the fatty acid synthase (FASN) and the sterol regulatory element-binding protein 1 (SREBP1). Moreover, the anti-inflammatory assay showed that compounds 19—22 and 25 inhibited the NO production induced by lipopolysaccharide in RAW 264.7 macrophages with IC₅₀ values of 7.89 ± 0.44, 6.25 ± 0.46, 2.98 ± 0.29, 10.77 ± 0.60, and 3.60 ± 0.28 μmol/L.

A series of cross-linked and phosphine-doped cathode interlayers (CILs), namely c-NDI:P₀, c-NDI:P₁, c-NDI:P₂, and c-NDI:P₃, are developed for inverted organic solar cells. We elucidate the relationship between the depletion region width at the heterojunction interface and the electron extraction ability of CILs. By incorporating c-NDI:P₀, a low depletion width of 0.8 nm along with a high power conversion efficiency (PCE) of 17.7% can be obtained in the inverted OSC based on PBDB-TF:BTP-eC9.

Comprehensive Summary

Cathode interlayers (CILs) play an essential role in achieving efficient organic solar cells (OSCs). However, the electronic structure at the electrode/CIL/active layer interfaces and the underlying mechanisms for electron collection remain unclear, which becomes a major obstacle to develop high-performance CILs. Herein, we investigate the relationship of the electron collection abilities of four cross-linked and n-doped CILs (c-NDI:P₀, c-NDI:P₁, c-NDI:P₂, c-NDI:P₃) with their electronic structure of space charge region at heterojunction interface. By accurately calculating the depletion region width according to the barrier height, doping density and permittivity, we put forward that the optimal thickness of CIL should be consistent with the depletion region width to realize the minimum energy loss. As a result, the depletion region width is largely reduced from 13 nm to 0.8 nm at the indium tin oxide (ITO)/c-NDI:P₀ interface, resulting in a decent PCE of 17.7% for the corresponding inverted OSCs.

An asymmetric synthesis of dihydrospirotryprostatin B was achieved through silica gel-mediated cyclization of tryptamine-ynamide based on a chiral pool strategy.

Comprehensive Summary

An asymmetric synthesis of dihydrospirotryprostatin B was achieved in 15 steps (8 purifications) from L-tryptophan. The main feature of our synthetic strategy is the efficient construction of spirocyclic oxindole intermediate containing a chiral quaternary carbon center, involving the silica gel-mediated cyclization of tryptamine-ynamide and oxidation under neat conditions.

The immobilization of triphenylamine into MOF with photoredox inert Sr nodes can successfully control the photo-generated electrons transfer from the excited triphenylamine to O₂ and realize the heterogeneous catalytic oxidation of thiols to disulfides.

Comprehensive Summary

The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the disulfides. Triphenylamine and its derivatives (TPAs) are promising for the above reaction, but suffer from the easy polymerization and difficult separation. To overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates, herein, we constructed one TPA-based metal-organic framework (MOF), (Me₂NH₂)[Sr(TCBPA)]·DMA·3H₂O (1), by direct self-assembly of tris(4′-carboxybiphenyl)amine (H₃TCBPA) and photoredox inert strontium ion (Sr²⁺). DFT calculations revealed that the valence band maximum (VBM) and the conduction band minimum (CBM) are mainly located on TCBPA^3–, successfully inhibiting the undesirable electron migration to metal nodes. Experimental results indicated that 1 displays superior performance than homogeneous H₃TCBPA, which may result from the abundant π···π and C—H···π interactions between the well-arranged TCBPA^3– and the build-in electric field between the anionic framework and the Me₂NH₂ ⁺. This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

The divergent synthesis of versatile 3,3’-disubstituted oxetane amino acids by utilizing visible-light-induced photocatalytic decarboxylative Giese-type reaction has been demonstrated.

Comprehensive Summary

The divergent synthesis of versatile 3,3′-disubstituted oxetane amino acids by utilizing visible-light-induced photocatalytic decarboxylative Giese-type reaction has been demonstrated. 3-Methyleneoxetane-derived substrates are readily available in a single-step and highly reactive as radical acceptors, allowing the production of versatile oxetane γ- and α-amino acids in high yields. A distinct ring strain release-driven radical addition mechanism was preliminarily revealed. The preparative power was further highlighted by the application in the synthesis of oxetane-containing dipeptides and azetidine amino acids, as well as the transformation of the product into novel oxetane-containing spiro-heterocycle pharmacophore.

Chiral induction agent can control the formation of the absolute configuration of racemate ligands. Two pairs of homochiral metal-organic frameworks (MOFs) were synthesized with the presence of enantiopure camphoric acid (D/L-cam). Importantly, DCF-17 and LCF-17 exhibit the efficient circularly polarized luminescent (CPL) activity with a luminescence dissymmetry factor (g _lum) value of –1.0 × 10^–2 and +9.2 ×10^–3, respectively.

Comprehensive Summary

The crystallization of chiral molecules is of great significance to understand the origin and evolution of hierarchical chirality and reveal the relationships between structural chirality and circularly polarized luminescence (CPL) activity. Here, we report two pairs of chiral metal–organic frameworks (MOFs) (DCF-17/LCF-17, DCF-18/LCF-18) by utilizing tetradentate ligands tetra(3-imidazoylphenyl)ethylene (TIPE) and 4,4'-[4',5'-bis[4-(4-pyridinyl)phenyl][1,1':2',1”-terphenyl]-4,4”-diyl]bis[pyridine] (TPPP) as linkers. It can be observed that the spontaneous resolution of the achiral ligands is converted into the induced resolution, and the ligands form the absolute configuration by using enantiopure camphoric acid (cam) as chiral induced reagent (CIR). As a result, the racemate MOFs can be driven to generate absolute homochiral crystallization. Another two achiral MOFs [Cd(D-cam)(TPPP)_0.5] (AF-1, AF = achiral framework) and [Cd(L-cam)(TPPP)_0.5] (AF-2) were prepared. The position disorder of D/L-cam skeleton causes the generation of nonchiralization, further leading to disappearance of symmetry breaking of TPPP. For the perspective of structure, this is the first report which reveals the chiral transfer and nonchiralization between chiral induced agents and tetradentate ligands. Besides, DCF-17 and LCF-17 show CPL with luminescence dissymmetry factor (g _lum) of –1.0 × 10^-2 and +9.2 × 10^–3, respectively. This work provides the useful evidences to reveal the induced chiral crystallization and the construction of CPL-active crystalline materials.

Comprehensive Summary

Stability against oxygen is an important factor affecting the performance of organic semiconductor devices. Improving photooxidation stability can prolong the service life of the device and maintain the mechanical and photoelectric properties of the device. Generally, various encapsulation methods from molecular structure to macroscopic device level are used to improve photooxidation stability. Here, we adopted a crystallization strategy to allow 14H-spiro[dibenzo[c,h]acridine-7,9′-uorene] (SFDBA) to pack tightly to resist fluorescence decay caused by oxidation. In this case, the inert group of SFDBA acts as a “steric armor”, protecting the photosensitive group from being attacked by oxygen. Therefore, compared with the fluorescence quenching of SFDBA powder under 2 h of sunlight, SFDBA crystal can maintain its fluorescence emission for more than 8 h under the same conditions. Furthermore, the photoluminescence quantum yields (PLQYs) of the crystalline film is 327% higher than that of the amorphous film. It shows that the crystallization strategy is an effective method to resist oxidation.

Destructive quantum interference of the m-OPE molecules was consistently regulated by substituents with progressively heightened electron effect.

Comprehensive Summary

Investigating the quantum interference effect in single molecules is essential to comprehensively understand the underlying mechanism of single-molecule charge transport. In this study, we employed the mother molecule m-OPE and introduced a series of side groups with various electronic effects at the 2-position of the central phenyl ring, creating four daughter m-OPE derivatives. The single molecular conductivities of these molecule wires were measured using the scanning tunneling microscope breaking junction technique. Our findings demonstrate that the substitutions regularly modulate the destructive quantum interference occurring within the m-OPE molecules. By combining optical and electrochemical investigations, along with density functional theory computations, we discover that the conductivity of the molecules corresponds to the electron-donating/withdrawing ability of the substituents. Specifically, by adjusting the electron structures of the molecular backbone, we can systematically tailor the destructive quantum interference in the m-OPE molecules.

The incorporation of valine residues into the polypeptide coatings significantly reduced the macrophage uptake of the nanoparticles, which was not observed for the nanoparticles modified with other amino acid residues like leucine, phenylalanine, isoleucine, and norvaline.

Comprehensive Summary

The structural and surface properties of nanomedicines play an important role in determining their biological fate. Surface chemistry of nanomedicines is one of the key parameters, where researchers used various strategies such as PEGylation to avoid the undesired clearance of nanoparticles (NPs) for enhanced targeting effect. Nevertheless, the fine-tuning of surface chemistry through polymer functionalization remains largely unexplored. In this concise report, we find that the incorporation of only 10 mol% valine residues into the surface-anchored poly(_L-glutamic acid) significantly lowered the macrophage uptake of NPs. The introduction of other hydrophobic amino acid residues, however, increased the NPs internalization instead. The chirality and the side-chain structure of valine played an important role in the unexpected uptake behavior. We believe this work highlights the impact of slight changes of the surface-anchored polymer structure on the behavior of NPs, drawing people's attention to the careful design of surface chemistry to optimize the nanomedicine design.