Lithium-Ion Dynamic and Storage of Atomically Precise Halogenated Nanographene Assemblies via Bottom-Up Chemical Synthesis.

Graphene has received much scientific attention as an electrode material for lithium-ion batteries because of its extraordinary physical and electrical properties. However, the lack of structural control and restacking issues have hindered its application as carbon-based anode materials for next generation lithium-ion batteries. To improve its performance, several modification approaches such as edge-functionalization and electron-donating/withdrawing substitution have been considered as promising strategies.

Comparative Study of the Orientation and Order Effects on the Thermoelectric Performance of 2D and 3D Perovskites.

Calcium titanium oxide has emerged as a highly promising material for optoelectronic devices, with recent studies suggesting its potential for favorable thermoelectric properties. However, current experimental observations indicate a low thermoelectric performance, with a significant gap between these observations and theoretical predictions. Therefore, this study employs a combined approach of experiments and simulations to thoroughly investigate the impact of structural and directional differences on the thermoelectric properties of two-dimensional (2D) and three-dimensional (3D) metal halide perovskites.

Highly Efficient MAPbI-Based Quantum Dots Exhibiting Unusual Nonblinking Single Photon Emission at Room Temperature.

Highly emissive semiconductor nanocrystals, or so-called quantum dots (QDs) possess a variety of applications from displays and biology labeling, to quantum communication and modern security. Though ensembles of QDs have already shown very high photoluminescent quantum yields (PLQYs) and have been widely utilized in current optoelectronic products, QDs that exhibit high absorption cross-section, high emission intensity, and, most important, nonblinking behavior at single-dot level have long been desired and not yet realized at room temperature. In this work, infrared-emissive MAPbI-based halide perovskite QDs is demonstrated.

Hybrid Machine Learning-Enabled Potential Energy Model for Atomistic Simulation of Lithium Intercalation into Graphite from Plating to Overlithiation.

Graphite is one of the most widely used negative electrode materials for lithium ion batteries (LIBs). However, because of the rapid growth of demands pursuing higher energy density and charging rates, comprehensive insights into the lithium intercalation and plating processes are critical for further boosting the potential of graphite electrodes. Herein, by utilizing the dihedral-angle-corrected registry-dependent potential (DRIP) (Wen et al.

Remarkably Deep Moiré Potential for Intralayer Excitons in MoSe/MoS Twisted Heterobilayers.

A moiré superlattice formed in twisted van der Waals bilayers has emerged as a new tuning knob for creating new electronic states in two-dimensional materials. Excitonic properties can also be altered drastically due to the presence of moiré potential. However, quantifying the moiré potential for excitons is nontrivial.

Sweetening Lithium Metal Interface by High Surface and Adhesive Energy Coating of Crystalline α-d-Glucose Film to Inhibit Dendrite Growth.

The notorious growth of lithium (Li) dendrites and the instability of the solid electrolyte interface (SEI) during cycling make Li metal anodes unsuitable for use in commercial Li-ion batteries. Herein, the use of simple sugar coating (α-d-glucose) is demonstrated on top of Li metal to halt the growth of Li dendrites and stabilize the SEI. The α-d-glucose layer possesses high surface and adhesive energies toward Li, which promote the homogenous stripping and plating of Li ions on top of the Li metal.

Microstructure Maps of Complex Perovskite Materials from Extensive Monte Carlo Sampling Using Machine Learning Enabled Energy Model.

Revealing the process-structure-property (PSP) relationships of chemically complex mixed-ion perovskite requires comprehensive insights into correlations between microstructures and chemical compositions. However, experimentally determining the microstructural information about complex perovskites over the composition space is a challenging task. In this study, a machine learning enabled energy model was trained for MAFAPb(BrI) mixed-ion perovskite for fast and extensive sampling over the compositional/permutational spaces to map the ion-mixing energies, chemical ordering, and atomic strains.

Molecular Simulations of the Microstructure Evolution of Solid Electrolyte Interphase during Cyclic Charging/Discharging.

Lithium (Li) metal is regarded as one of the most promising anode materials for use in next-generation high-energy-density rechargeable batteries because of its high volumetric and gravimetric specific capacity, as well as low reduction potential. Unfortunately, uncontrolled dendritic Li growth during cyclic charging/discharging leads to low columbic efficiency and critical safety issues. Hence, comprehensive understanding of the formation mechanism for Li-dendrite growth, particularly at the onset of dendrite formation, is essential for developing Li-metal anode batteries.

Self-Assembly Behavior of Diacetylenic Acid Molecules upon Vapor Deposition: Odd-Even Effect on the Film Morphology.

A series of linear carboxylic acids containing diacetylenic units at different positions along the chain (C H (C≡C) (CH ) COOH, n=7-11) were vacuum-deposited on clean silica substrates. The morphologies of the initial films after UV irradiation were studied. A clear odd-even effect on the morphology of the initial film was observed in that, depending on the spacer length between the diacetylenic unit and carboxyl head group, rings or dendrites of acid dimer layers were obtained.

Modulating Performance and Stability of Inorganic Lead-Free Perovskite Solar Cells via Lewis-Pair Mediation.

Fully inorganic perovskites based on Bi and Sb are emerging as alternatives that overcome the toxicity and low stability of their Pb-based perovskite counterparts. Nevertheless, the thin film fabrication of Pb-free perovskites remains a struggle, with poor morphologies and incomplete conversions greatly inhibiting device performance. In this study, we modulated the crystallization of an all-inorganic dimer phase of a Sb perovskite (d-CsSbI) through gradual increase in the annealing temperature, accompanied by the use of Lewis bases for adduct formation.

Fast and Accurate Artificial Neural Network Potential Model for MAPbI Perovskite Materials.

Hybrid organic-inorganic perovskite materials are promising materials for photovoltaic and optoelectronic applications. Nevertheless, the construction of a computationally efficient potential model for atomistic simulations of perovskite with high fidelity to ab initio calculations is not a trivial task given the chemically complex nature of perovskite in terms of its chemical components and interatomic interactions. In the present study, we demonstrate that artificial neural network (ANN) models can be employed for efficient and accurate potential energy evaluation of MAPbI perovskite materials.

ZnO/Silicon-Rich Oxide Superlattices with High Thermoelectric Figure of Merit: A Comprehensive Study by Experiment and Molecular Dynamic Simulation.

ZnO is a direct band gap material that has numerous optoelectronic applications. Recently, the thermoelectric behavior of ZnO has drawn much attention because it is expected to enrich the multifunctional application of ZnO. However, the high thermal conductivity nature of ZnO (∼50 W/(m·K)) is a challenge to further increase its thermoelectrtic figure of merit ( ZT).

A lithium passivated MoO nanobelt decorated polypropylene separator for fast-charging long-life Li-S batteries.

Dissolution of lithium polysulfide (LiPS) into the electrolyte during discharging, causing shuttling of LiPS from the cathode to the lithium (Li) metal, is mainly responsible for the capacity decay and short battery life of lithium-sulfur batteries (LSBs). Herein, we designed a separator comprising polypropylene (PP) coated with MoO3 nanobelts (MNBs), prepared through facile grinding of commercial MoO3 powder. The formation of Li2Sn-MoO3 during discharging inhibited the polysulfide shuttling; during charging, Li passivated LixMoO3 facilitated ionic transfer during the redox reaction by decreasing the charge transfer resistance.

Mitigating Metal Dendrite Formation in Lithium-Sulfur Batteries via Morphology-Tunable Graphene Oxide Interfaces.

Despite issues related to dendrite formation, research on Li metal anodes has resurged because of their high energy density. In this study, graphene oxide (GO) layers are decorated onto Li metal anodes through a simple process of drop-casting and spray-coating. The self-assembly of GO is exploited to synthesize coatings having compact, mesoporous, and macroporous morphologies.

Single-Crystal Antimonene Films Prepared by Molecular Beam Epitaxy: Selective Growth and Contact Resistance Reduction of the 2D Material Heterostructure.

Single-crystal antimonene flakes are observed on sapphire substrates after the postgrowth annealing procedure of amorphous antimony (Sb) droplets prepared by using molecular beam epitaxy at room temperature. The large wetting angles of the antimonene flakes to the sapphire substrate suggest that an alternate substrate should be adopted to obtain a continuous antimonene film. By using a bilayer MoS/sapphire sample as the new substrate, a continuous and single-crystal antimonene film is obtained at a low growth temperature of 200 °C.

Folding Sheets with Ion Beams.

Focused ion beams (FIBs) are versatile tools with cross-disciplinary applications from the physical and life sciences to archeology. Nevertheless, the nanoscale patterning precision of FIBs is often accompanied by defect formation and sample deformation. In this study, the fundamental mechanisms governing the large-scale plastic deformation of nanostructures undergoing FIB processes are revealed by a series of molecular dynamic simulations.

Multiscale Molecular Simulation of Solution Processing of SMDPPEH: PCBM Small-Molecule Organic Solar Cells.

Solution-processed small-molecule organic solar cells are a promising renewable energy source because of their low production cost, mechanical flexibility, and light weight relative to their pure inorganic counterparts. In this work, we developed a coarse-grained (CG) Gay-Berne ellipsoid molecular simulation model based on atomistic trajectories from all-atom molecular dynamics simulations of smaller system sizes to systematically study the nanomorphology of the SMDPPEH/PCBM/solvent ternary blend during solution processing, including the blade-coating process by applying external shear to the solution. With the significantly reduced overall system degrees of freedom and computational acceleration from GPU, we were able to go well beyond the limitation of conventional all-atom molecular simulations with a system size on the order of hundreds of nanometers with mesoscale molecular detail.

PSII-LHCII supercomplex organizations in photosynthetic membrane by coarse-grained simulation.

Green plant photosystem II (PSII) and light-harvesting complex II (LHCII) in the stacked grana regions of thylakoid membranes can self-organize into various PSII-LHCII supercomplexes with crystalline or fluid-like supramolecular structures to adjust themselves with external stimuli such as high/low light and temperatures, rendering tunable solar light absorption spectrum and photosynthesis efficiencies. However, the mechanisms controlling the PSII-LHCII supercomplex organizations remain elusive. In this work, we constructed a coarse-grained (CG) model of the thylakoid membrane including lipid molecules and a PSII-LHCII supercomplex considering association/dissociation of moderately bound-LHCIIs.

Electrode materials, thermal annealing sequences, and lateral/vertical phase separation of polymer solar cells from multiscale molecular simulations.

The nanomorphologies of the bulk heterojunction (BHJ) layer of polymer solar cells are extremely sensitive to the electrode materials and thermal annealing conditions. In this work, the correlations of electrode materials, thermal annealing sequences, and resultant BHJ nanomorphological details of P3HT:PCBM BHJ polymer solar cell are studied by a series of large-scale, coarse-grained (CG) molecular simulations of system comprised of PEDOT:PSS/P3HT:PCBM/Al layers. Simulations are performed for various configurations of electrode materials as well as processing temperature.

Morphology, molecular stacking, dynamics and device performance correlations of vacuum-deposited small-molecule organic solar cells.

The "all carbon" organic solar cells (OSCs) based on the homocyclic molecule tetraphenyldibenzoperiflanthene (DBP) as a donor and C60 as an acceptor were comprehensively characterized. The optimized planar-mixed heterojunction device with a DBP:C60 mixture ratio of DBP : C60 (1 : 2) exhibited a power conversion efficiency of 4.47%.

2-Alkyl-5-thienyl-substituted benzo[1,2-b:4,5-b']dithiophene-based donor molecules for solution-processed organic solar cells.

In this study, we have strategically designed and convergently synthesized two novel, symmetrical, and linear A-D-A-type π-conjugated donor molecules (TBDTCNR, TBDTCN), each containing a planar electron-rich 2-octylthiene-5-yl-substituted benzodithiophene (TBDT) unit as the core, flanked by octylthiophene units and end-capped with electron-deficient cyanoacetate (CNR) or dicyanovinyl (CN) units. We thoroughly characterized both of these materials and investigated the effects of the end groups (CNR, CN) on their optical, electrochemical, morphological, and photovoltaic properties. We then fabricated solution-processed bulk heterojunction organic solar cells incorporating TBDTCNR and TBDTCN.

Ab initio calculations of the reaction pathways for methane decomposition over the Cu (111) surface.

Growth of large-area, few-layer graphene has been reported recently through the catalytic decomposition of methane (CH(4)) over a Cu surface at high temperature. In this study, we used ab initio calculations to investigate the minimum energy pathways of successive dehydrogenation reactions of CH(4) over the Cu (111) surface. The geometries and energies of all the reaction intermediates and transition states were identified using the climbing image nudged elastic band method.

Thin film compressive stresses due to adatom insertion into grain boundaries.

Atomic simulations of the growth of polycrystalline Ni demonstrate that deposited atoms incorporate into the film at boundaries, resulting in compressive stress generation. Incorporated atoms can also leave the boundaries and thus relieve compressive stress. This leads to a complex interplay between growth stress, adatom incorporation, and surface structure.

Dislocation injection, reconstruction, and atomic transport on {001} Au terraces.

High-resolution electron microscopy investigations of Au films show that adatoms on (100) surfaces insert into the underlying terrace to form surface dislocations. This injection readily occurs when the number of adatoms on a terrace is approximately 20 atoms or less. The surface dislocation glides along the terrace, but is repelled from the edges.