No abstract

Solution-processed metal halide perovskites have been recognized as one of the most promising semiconductors, with applications in light-emitting diodes (LEDs), solar cells and lasers. Various additives have been widely used in perovskite precursor solutions, aiming to improve the formed perovskite film quality through passivating defects and controlling the crystallinity. The additive’s role of defect passivation has been intensively investigated, while a deep understanding of how additives influence the crystallization process of perovskites is lacking. Here, we reveal a general additive-assisted crystal formation pathway for FAPbI3 perovskite with vertical orientation, by tracking the chemical interaction in the precursor solution and crystallographic evolution during the film formation process. The resulting understanding motivates us to use a new additive with multi-functional groups, 2-(2-(2-Aminoethoxy)ethoxy)acetic acid, which can facilitate the orientated growth of perovskite and passivate defects, leading to perovskite layer with high crystallinity and low defect density and thereby record-high performance NIR perovskite LEDs (~800 nm emission peak, a peak external quantum efficiency of 22.2% with enhanced stability).

A single-layer polymer stabilized liquid crystal (PSLC) film reflecting both right- and left-circularly polarized light has been developed by a wash-out/refill method. The PSLC film was achieved by prefabricating the polymer network with a left-handed helical structure and then refilling a cholesteric liquid crystal with a right-handed helical structure into the network. The reflection intensity of the PSLC film is close to 100% when the pitch lengths of the two opposite helical structures are the same. It was demonstrated that the memory effect of the polymer network is an important mechanism for the resulting film properties.

Effective and safe hemodialysis is essential for patients with acute kidney injury and chronic renal failures. However, the development of effective anticoagulant agents with safe antidotes for use during hemodialysis has proven challenging. Here, we describe DNA origami-based assemblies that enable the inhibition of thrombin activity and thrombus formation. Two different thrombin-binding aptamers decorated DNA origami initiates protein recognition and inhibition, exhibiting enhanced anticoagulation in human plasma, fresh whole blood and a murine model. In a dialyzer-containing extracorporeal circuit that mimicked clinical hemodialysis, the origami-based aptamer nanoarray effectively prevented thrombosis formation. Oligonucleotides containing sequences complementary to the thrombin-binding aptamers can efficiently neutralize the anticoagulant effects. The nanoarray is safe and immunologically inert in healthy mice, eliciting no detectable changes in liver and kidney functions or serum cytokine concentration. This DNA origami-based nanoagent represents a promising anticoagulant platform for the hemodialysis treatment of renal diseases.

Chiral Pb(Sn)‐I hybrid organic–inorganic perovskites exhibit outstanding chiral‐induced spin selectivity (CISS) performance, but the nontoxic lead‐free hybrid materials with high stability are still greatly desired for spin filtering in spintronic applications. We synthesize chiral hybrid copper halides (R/S‐MBA)2CuX4 (MBA=methylbenzylammonium; X=Cl, Br) with characteristic 0D CuX4 tetrahedral structural motifs, combining the low toxicity of Cu2+ and air stability of halide ions (Cl− and Br−). Despite similar structural and electronic features, (R/S‐MBA)2CuBr4 shows much smaller chiroptical activity than the chloride counterpart. Magnetically conductive atomic force microscopy measurements display a typical spin‐polarized charge‐transport property with high efficiency up to 90 % for both copper halides. Our work expands the CISS effect into eco‐friendly and stable metal–organic halides, which is promising for applications in spintronics based on transition‐metal hybrid systems.

PCMSOLVER is an open-source library for continuum electrostatic solvation. It can be combined with any quantum chemistry code and requires a minimal interface with the host program, greatly reducing programming effort. As input, PCMSOLVER needs only the molecular geometry to generate the cavity and the expectation value of the molecular electrostatic potential on the cavity surface. It then returns the solvent polarization back to the host program. The design is powerful and versatile: minimal loss of performance is expected, and a standard single point self-consistent field implementation requires no more than 2 days of work. We provide a brief theoretical overview, followed by two tutorials: one aimed at quantum chemistry program developers wanting to interface their code with PCMSOLVER, the other aimed at contributors to the library. We finally illustrate past and ongoing work, showing the library's features, combined with several quantum chemistry programs.The past 10 years have seen theoretical and computational methods become an invaluable complement to experiment in the practice of chemistry. Understanding experimental observations of chemical phenomena, ranging from reaction barriers to spectroscopies, requires proper in silico simulations to achieve insight into the fundamental processes at work. Quantum chemistry program packages have evolved to tackle this everincreasing range of possible applications, with a particular focus on computational performance and scalability. These latter concerns have driven a large body of recent developments, but it has become apparent that similar efforts have to be devoted into the software development infrastructure and practices. Code bases in quantum chemistry have grown over a number of years, in most cases without an overarching vision on the architecture and design of the code. As more features continue to be added, the friction with legacy code bases makes itself felt: either the code undergoes a time-consuming rewrite or it becomes the domain of few experts. Both approaches are wasteful of resources and can seriously hinder the reproducibility of computational results. It is essential to find more effective ways of organizing scientific code and programming efforts in quantum chemistry. To be able to manage the growing complexity of quantum chemical program packages, the keywords efficiency and scalability

Abstract:In recent years, there has been extensive research and continuous development on second-order nonlinear optical (NLO) crystal materials due to their potential applications in telecommunications, THz imaging and spectroscopy, optical information processing, and optical data storage. Recent progress in second-order NLO ionic organic crystal materials is reviewed in this article. Research has shown that the second-order nonlinear optical properties of organic crystal materials are closely related to their molecular structures. The basic structures of ionic organic conjugated molecules with excellent nonlinear optical properties are summarized. The effects of molecular structure, for example, conjugated π electron systems, electronic properties of donor-acceptor groups, and different counter-anion effects on second order NLO properties and crystal packing are studied.

Poly(3‐hexylthiophene) (P3HT)‐based organic solar cells (OSCs) have attracted much attention due to their advantages of low‐cost production and matured roll‐to‐roll manufacture. However, the efficiency of P3HT‐based OSCs lag much behind the non‐P3HT ones due to their negligible absorption of long wavelengths of light over 650 nm, high‐lying highest occupied molecular orbitals (HOMO), and difficulty of controlling morphology. In this study, the alkyl chains of the nonfullerene acceptors are replaced with alkoxy chains to achieve synergistic enhancement of all three parameters ( short circuit current density (JSC), open circuit voltage (VOC), and fill factor (FF)) and thus significant increase of power conversion efficiency for P3HT‐based OSCs. As a result, the OSCs exhibit a maxima efficiency of 6.6%. The P3HT‐based systems are systematically studied with optical spectroscopy, photoluminescence, cyclic voltametry, space charge limit current, grazing incident wide‐angle X‐ray scattering, transient absorption spectroscopy, transmission electron microscope, and atomic force microscopy to probe the mechanism, which reveal that introducing alkoxy chains simultaneously increases the energy levels of the HOMO and the lowest unoccupied molecular orbitals, enhances the light absorption, improves the rigidity of the backbone and charge transport mobility, and tunes the molecular orientation and film morphology, thus improving the photovoltaic performance. This contribution provides an important guidance in the design of novel nonfullerene acceptors for high‐performance P3HT‐based OSCs.