PMC-IZ: A Simple Algorithm for the Electrostatics Calculation in Slab Geometric Molecular Dynamics Simulations.

Slab geometric systems are widely utilized in molecular simulations. However, an efficient, straightforward, and accurate method for calculating electrostatic interactions in these systems for molecular dynamics (MD) simulations is still needed. This review introduces a PME-like approach called PMC-IZ, specifically designed for slab geometric systems. Traditional approaches for long-range electrostatic interaction calculations in slab geometry typically involve Ewald summation, where the Gaussian charge density is summed within 3D unit cells and then integrated in the 2D periodic space. In the proposed approach here, the Poisson equation was solved for a single Gaussian charge density within 2Dl periodic space, followed by convolution within 3D unit cells using an effective potential as the convolution kernel for summation. The effective potential ensures that the solution within the region of interest adheres strictly to 2D periodic boundary conditions while inherently possessing 3D periodic boundary condition properties. The PMC-IZ method provides for such systems accurate treatment of electrostatic interactions, overcomes limitations associated with finite vacuum layers, and offers improved computational efficiency. We thus postulate that this method provides a valuable tool for studying electrostatic interactions in slab geometric system MD simulations. It has promising applications in various areas such as surface science, catalysis, and materials research, where accurate modeling of slab geometric electrostatic interactions is essential.

Nanoscale one-dimensional close packing of interfacial alkali ions driven by water-mediated attraction.

The permeability and selectivity of biological and artificial ion channels correlate with the specific hydration structure of single ions. However, fundamental understanding of the effect of ion-ion interaction remains elusive. Here, via non-contact atomic force microscopy measurements, we demonstrate that hydrated alkali metal cations (Na+ and K+) at charged surfaces could come into close contact with each other through partial dehydration and water rearrangement processes, forming one-dimensional chain structures. We prove that the interplay at the nanoscale between the water-ion and water-water interaction can lead to an effective ion-ion attraction overcoming the ionic Coulomb repulsion. The tendency for different ions to become closely packed follows the sequence K+ > Na+ > Li+, which is attributed to their different dehydration energies and charge densities. This work highlights the key role of water molecules in prompting close packing and concerted movement of ions at charged surfaces, which may provide new insights into the mechanism of ion transport under atomic confinement.

Artificial Intelligence Enhanced Molecular Simulations.

Molecular simulations, which simulate the motions of particles according to fundamental laws of physics, have been applied to a wide range of fields from physics and materials science to biochemistry and drug discovery. Developed for computationally intensive applications, most molecular simulation software involves significant use of hard-coded derivatives and code reuse across various programming languages. In this Review, we first align the relationship between molecular simulations and artificial intelligence (AI) and reveal the coherence between the two. We then discuss how the AI platform can create new possibilities and deliver new solutions to molecular simulations, from the perspective of algorithms, programming paradigms, and even hardware. Rather than focusing solely on increasingly complex neural network models, we introduce various concepts and techniques brought about by modern AI and explore how they can be transacted to molecular simulations. To this end, we summarized several representative applications of molecular simulations enhanced by AI, including from differentiable programming and high-throughput simulations. Finally, we look ahead to promising directions that may help address existing issues in the current framework of AI-enhanced molecular simulations.

Accelerating supramolecular aggregation by molecular sliding.

Diffusion-based translocation along DNA or RNA molecules is essential for genome regulatory proteins to execute their biological functions. The reduced dimensionality of the searching process makes the proteins bind specific target sites at a "faster-than-diffusion-controlled rate". We herein report a photoresponsive slider-track diffusion system capable of self-assembly rate acceleration, which consists of (-)-camphorsulfonic acid, 4-(4'-n-octoxylphenylazo)benzenesulfonic acid, and isotactic poly(2-vinylpyridine). The protonated pyridine rings act as the footholds for anionic azo sliders to diffusively bind and slide along polycationic tracks via electrostatic interactions. Ultraviolet light triggers the trans to cis isomerization and aggregation of azo sliders, which can be monitored by multiple spectroscopic methods without labeling. The presence of vinyl polymer track increases the aggregation rate of cis azobenzene up to ∼20 times, depending on the stereoregularity of the polymer chain, the acid/base ratio and the addition of salt. This system has a feature of simplicity, monitorability, controllability, and could find applications in designing molecular machines with desired functionalities.

Temperature-Dependent Photoluminescence of Manganese Halide with Tetrahedron Structure in Anti-Perovskites.

The temperature-dependent photoluminescence (PL) properties of an anti-perovskite [MnBr4]BrCs3 sample in the temperature range of 78-500 K are studied in the present work. This material exhibits unique performance which is different from a typical perovskite. Experiments showed that from room temperature to 78 K, the luminous intensity increased as the temperature decreased. From room temperature to 500 K, the photoluminescence intensity gradually decreased with increasing temperature. Experiments with varying temperatures repeatedly showed that the emission wavelength was very stable. Based on the above-mentioned phenomenon of the changing photoluminescence under different temperatures, the mechanism is deduced from the temperature-dependent characteristics of excitons, and the experimental results are explained on the basis of the types of excitons with different energy levels and different recombination rates involved in the steady-state PL process. The results show that in the measured temperature range of 78-500 K, the steady-state PL of [MnBr4]BrCs3 had three excitons with different energy levels and recombination rates participating. The involved excitons with the highest energy level not only had a high radiative recombination rate, but a high non-radiative recombination rate as well. The excitons at the second-highest energy level had a similar radiative recombination rate to the lowest energy level excitons and a had high non-radiative recombination rate. These excitons made the photoluminescence gradually decrease with increasing temperature. This may be the reason for this material's high photoluminescence efficiency and low electroluminescence efficiency.

Review on Tailoring PEDOT:PSS Layer for Improved Device Stability of Perovskite Solar Cells.

Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has high optical transparency in the visible light range and low-temperature processing condition, making it one of the most widely used polymer hole transport materials inverted perovskite solar cells (PSCs), because of its high optical transparency in the visible light range and low-temperature processing condition. However, the stability of PSCs based on pristine PEDOT:PSS is far from satisfactory, which is ascribed to the acidic and hygroscopic nature of PEDOT:PSS, and property differences between PEDOT:PSS and perovskite materials, such as conductivity, work function and surface morphology. This review summaries recent efficient strategies to improve the stability of PEDOT:PSS in PSCs and discusses the underlying mechanisms. This review is expected to provide helpful insights for further increasing the stability of PSCs based on commercial PEDOT:PSS.

Solution-Processed Highly Superparamagnetic and Conductive PEDOT:PSS/Fe3O4 Nanocomposite Films with High Transparency and High Mechanical Flexibility.

Multifunctional films can have important applications. Transparent and flexible films with high conductivity and magnetic properties can be used in many areas, such as electromagnetic interference (EMI) shielding, magnetic switching, microwave absorption, and also biotechnology. Herein, novel highly conductive and superparamagnetic thin films with excellent transparency and flexibility have been demonstrated. The films were formed from a poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS; Clevios PH1000) aqueous solution added with iron oxide (Fe3O4) nanoparticles that have a size of ∼20 nm by spin-coating. The PEDOT:PSS/Fe3O4 films have a high conductivity of 1080 S/cm through treatment with methylammonium iodide in an organic solvent. The high-conductivity PEDOT:PSS/Fe3O4 films can also have a saturation magnetization of 25.5 emu/g and an EMI shielding effectiveness of more than 40 dB in the 8-12.5 GHz (X band) frequency range. The PEDOT:PSS/Fe3O4 films have additional advantages, like excellent transparency, good mechanical flexibility, low cost, and light weight. In addition, we fabricate flexible PEDOT:PSS/Fe3O4 silk threads with a high magnetism and conductivity.

Significant Enhancement in the Thermoelectric Properties of PEDOT:PSS Films through a Treatment with Organic Solutions of Inorganic Salts.

Conducting polymers have promising thermoelectric application because they have many advantages including abundant elements, mechanical flexibility, and nontoxicity. The thermoelectric properties of conducting polymers strongly depend on their chemical structure and microstructure. Here, we report a novel and facile method to significantly enhance the thermoelectric properties of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) ( PEDOT: PSS) films through a treatment with organic solutions of inorganic salts. N,N-Dimethylformamide (DMF) and a common inorganic salt like zinc chloride (ZnCl2) are used as the solvent and solute of the solutions, respectively. The treatments can significantly increase both the Seebeck coefficient and electrical conductivity of the PEDOT: PSS films. The thermoelectric properties of the PEDOT: PSS films are sensitive to the experimental conditions, such as the salt concentration, treatment temperature, and the cation of the salts. After treatment at the optimal experimental conditions, the PEDOT: PSS films can exhibit a Seebeck coefficient of 26.1 µV/K and an electrical conductivity of over 1400 S/cm at room temperature. The corresponding power factor is 98.2 µW/(m·K(2)). The mechanism for the enhancement in the thermoelectric properties is attributed to the segregation of some PSSH chains from PEDOT: PSS and the conformation change of PEDOT chains as a result of the synergetic effects of inorganic salts and DMF.

PEDOT:PSS Films with Metallic Conductivity through a Treatment with Common Organic Solutions of Organic Salts and Their Application as a Transparent Electrode of Polymer Solar Cells.

UNLABELLED: A transparent electrode is an indispensable component of optoelectronic devices, and there as been a search for substitutes of indium tin oxide (ITO) as the transparent electrode. Poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) ( PEDOT: PSS) is a conducting polymer that is very promising as the next generation of materials for the transparent electrode if it can obtain conductivity as high as that of ITO. Here, we report the treatment of PEDOT: PSS with organic solutions to significantly enhance its conductivity. Common organic solvents like dimethylformamide and γ-butyrolactone and common organic salts like methylammonium iodide and methylammonium bromide are used for the organic solutions. The conductivity of pristine PEDOT: PSS films is only ∼0.2 S/cm, and it can be increased to higher than 2100 S/cm. The conductivity enhancement is much more significant than control treatments of PEDOT: PSS films with neat organic solvents or aqueous solutions of the organic salts. The mechanism for the conductivity enhancement is the synergetic effects of both the organic salts and organic solvents on the microstructure and composition of PEDOT: PSS. They induce the segregation of some PSSH chains from PEDOT: PSS. Highly conductive PEDOT: PSS films were studied as the transparent electrode of polymer solar cells. The photovoltaic efficiency is comparable to that with an ITO transparent electrode.

Transparent conductive oxide-free perovskite solar cells with PEDOT:PSS as transparent electrode.

Perovskite solar cells (PSCs) have been attracting considerable attention because of their low fabrication cost and impressive energy conversion efficiency. Most PSCs are built on transparent conductive oxides (TCOs) such as fluorine-doped tin oxide (FTO) or indium tin oxide (ITO), which are costly and rigid. Therefore, it is significant to explore alternative materials as the transparent electrode of PSCs. In this study, highly conductive and highly transparent poly(3,4-ethylenedioxythiophene):polystyrenesulfonate ( PEDOT: PSS) films were investigated as the transparent electrode of both rigid and flexible PSCs. The conductivity of PEDOT: PSS films on rigid glass or flexible poly(ethylene terephthalate) (PET) substrate is significantly enhanced through a treatment with methanesulfonic acid (MSA). The optimal power conversion efficiency (PCE) is close to 11% for the rigid PSCs with an MSA-treated PEDOT: PSS film as the transparent electrode on glass, and it is more than 8% for the flexible PSCs with a MSA-treated PEDOT: PSS film as the transparent electrode on PET. The flexible PSCs exhibit excellent mechanical flexibility in the bending test.

Significant different conductivities of the two grades of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate), Clevios P and Clevios PH1000, arising from different molecular weights.

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is promising to be the next-generation transparent electrode of optoelectronic devices. This paper reports the differences between two commercially available grades of PEDOT:PSS: Clevios P and Clevios PH1000. The as-prepared PEDOT:PSS films from Clevios P and Clevios PH1000 solutions have close conductivities of 0.2-0.35 S cm(-1). Their conductivities can be enhanced to 171 and 1164 S cm(-1), respectively, through a treatment with hydrofluoroacetone trihydrate (HFA). The differences between Clevios P and Clevios PH1000 were studied by various characterizations on PEDOT:PSS aqueous solutions and PEDOT:PSS films. The gel particles are larger in Clevios PH1000 solution than in Clevios P solution as revealed by dynamic light scattering and fluorescence spectroscopy of pyrene in these solutions. These results suggest that PEDOT of Clevios PH1000 has a higher average molecular weight than that of Clevios P. The difference in the molecular weight of PEDOT for the two grades of PEDOT:PSS is confirmed by the characterizations on their polymer films, including atomic force microscopy and temperature dependences of the resistances of as-prepared and HFA-treated PEDOT:PSS films. The different molecular weights of PEDOT also gives rise to significant differences in the electrochemical behaviors of the two grades of PEDOT:PSS, as revealed by the cyclic voltammetry, in situ UV-vis-NIR absorption spectroscopy and potentiostatic transient measurements.

Solution-processed metallic conducting polymer films as transparent electrode of optoelectronic devices.

The conductivity of PEDOT:PSS films was significantly enhanced from 0.3 S cm(-1) to 3065 S cm(-1) through a treatment with dilute sulfuric acids. PEDOT:PSS films with a sheet resistance of 39 Ω sq(-1) and transparency of around 80% at 550 nm are obtained. These PEDOT:PSS films with conductivity and transparency comparable to ITO can replace ITO as the transparent electrode of optoelectronic devices.

Significant conductivity enhancement of conductive poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) films through a treatment with organic carboxylic acids and inorganic acids.

Significant conductivity enhancement was observed on transparent and conductive poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) films after a treatment with organic and inorganic acids, including acetic acid, propionic acid, butyric acid, oxalic acid, sulfurous acid, and hydrochloric acid. The conductivity could be enhanced from 0.2 to over 200 S cm(-1), that is, by a factor of more than 1000. The conductivity enhancement was dependent on the structure of the acids and the experimental conditions during the treatment, such as the acid concentration and the temperature. The optimal temperature was in the range of 120 to 160 degrees C. The resistance dropped rapidly when a PEDOT:PSS film was treated with acid solution of high concentration, whereas it gradually increased and then decreased when it was treated with an acid solution of low concentration. The mechanism for this conductivity enhancement was studied by various chemical and physical characterizations. The temperature dependence of conductivity indicates that the energy barrier for charge hopping among the PEDOT chains become lower in the highly conductive PEDOT:PSS film after the acid treatment. The ultraviolet-visible-near-infrared (UV-vis-NIR) absorption spectroscopy, the X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) indicate the loss of polystyrene sulfonic acid (PSSH) chains from the PEDOT:PSS film after the acid treatment, and the atomic force microscopy (AFM) suggest conformational change of the polymer chains. Therefore, the conductivity enhancement is attributed to the loss of PSSH chains from the PEDOT:PSS film and the conformational change of the PEDOT chains, which are induced by the acids.