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Suppressing depolarization by tail substitution in an organic supramolecular ferroelectric
摘要： Despite being very well established in the field of electro-optics, ferroelectric liquid crystals so far lacked interest from a ferroelectric device perspective due to a typically high operating temperature, a modest remnant polarization and/or poor polarization retention. Here, we experimentally demonstrate how simple structural modification of a prototypical ferroelectric liquid-crystal benzene-1,3,5-trisamide (BTA) – introduction of branched-tail substituents – results in materials with a wide operating temperature range and a data retention time of more than 10 years in thin-film solution-processed capacitor devices at room temperature. The observed differences between linear- and branched-tail compounds are analyzed using density functional theory (DFT) and molecular dynamics (MD) simulations. We conclude that morphological factors like improved packing quality and reduced disorder, rather than electrostatic interactions or intra/inter-columnar steric hindrance, underlay the superior properties of the branched-tailed BTAs. Synergistic effects upon blending of compounds with branched and linear side-chains can be used to further improve the materials’ characteristics.
关键词： liquid crystal,BTA,DFT,molecular dynamics,supramolecular,ferroelectric,polarization retention
更新于2025-09-19 17:15:36
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Phonon-Mediated and Weakly Size-Dependent Electron and Hole Cooling in CsPbBr <sub/>3</sub> Nanocrystals Revealed by Atomistic Simulations and Ultrafast Spectroscopy
摘要： We combine state-of-the-art ultrafast photoluminescence and absorption spectroscopy and nonadiabatic molecular dynamics simulations to investigate charge-carrier cooling in CsPbBr3 nanocrystals over a very broad size regime, from 0.8 nm to 12 nm. Contrary to the prevailing notion that polaron formation slows down charge-carrier cooling in lead-halide perovskites, no suppression of carrier cooling is observed in CsPbBr3 nanocrystals except for a slow cooling (over ~ 10 ps) of ‘warm’ electrons in the vicinity (within ~ 0.1 eV) of the conduction band edge. At higher excess energies, electrons and holes cool with similar rates, on the order of 1 eV ps-1 carrier-1 and increasing weakly with size. Our ab initio simulations suggest that cooling proceeds via fast phonon-mediated intra-band transitions driven by strong and size-dependent electron-phonon coupling. The presented experimental and computational methods yield the spectrum of involved phonons and may guide the development of devices utilizing hot charge carriers.
关键词： electron-phonon coupling,hot carriers,nonadiabatic molecular dynamics,Charge-carrier cooling,lead-halide perovskite nanocrystal,excited-states dynamics
更新于2025-09-19 17:13:59
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The effect of pulse duration on nanoparticle generation in pulsed laser ablation in liquids: Insights from large-scale atomistic simulations
摘要： The generation of colloidal solutions of chemically clean nanoparticles through pulsed laser ablation in liquids (PLAL) has evolved into a thriving research field that impacts industrial applications. The complexity and multiscale nature of PLAL make it difficult to untangle the various processes involved in the generation of nanoparticles and establish the dependence of nanoparticle yield and size distribution on the irradiation parameters. Large-scale atomistic simulations have yielded important insights into the fundamental mechanisms of ultrashort (femtoseconds to tens of picoseconds) PLAL and provided a plausible explanation of the origin of the experimentally observed bimodal nanoparticle size distributions. In this paper, we extend the atomistic simulations to short (hundreds of picoseconds to nanoseconds) laser pulses and focus our attention on the effect of the pulse duration on the mechanisms responsible for the generation of nanoparticles at the initial dynamic stage of laser ablation. Three distinct nanoparticle generation mechanisms operating at different stages of the ablation process and in different parts of the emerging cavitation bubble are identified in the simulations. These mechanisms are (1) the formation of a thin transient metal layer at the interface between the ablation plume and water environment followed by its decomposition into large molten nanoparticles, (2) nucleation, growth, and rapid cooling/solidification of small nanoparticles at the very front of the emerging cavitation bubble, above the transient interfacial metal layer, and (3) spinodal decomposition of a part of the ablation plume located below the transient interfacial layer, leading to the formation of a large population of nanoparticles growing in a high-temperature environment through inter-particle collisions and coalescence. The coexistence of the three distinct mechanisms of the nanoparticle formation at the initial stage of the ablation process can be related to the broad nanoparticle size distributions commonly observed in nanosecond PLAL experiments. The strong dependence of the nanoparticle cooling and solidification rates on the location within the low-density metal-water mixing region has important implications for the long-term evolution of the nanoparticle size distribution, as well as for the ability to quench the nanoparticle growth or dope them by adding surface-active agents or doping elements to the liquid environment.
关键词： phase explosion,pulsed laser ablation in liquids,molecular dynamics simulations,hydrodynamic instability,atomistic simulations,nanoparticles,nucleation and growth
更新于2025-09-19 17:13:59
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Effect of liquid environment on single-pulse generation of laser induced periodic surface structures and nanoparticles
摘要： The effect of a liquid environment on the fundamental mechanisms of surface nanostructuring and generation of nanoparticles by single pulse laser ablation is investigated in a closely integrated computational and experimental study. A large-scale molecular dynamics simulation of spatially-modulated ablation of Cr in water reveals a complex picture of dynamic interaction between the ablation plume and water, which involves rapid deceleration of the ablation plume by water environment, formation and prompt disintegration of a hot metal layer at the interface between the ablation plume and water, lateral redistribution and redeposition of a major fraction of the ablation plume, and eventual formation of smooth frozen surface features. A good agreement between the shapes of the surface features predicted in the simulation and the ones generated in single pulse laser ablation experiments performed for Cr in water supports the mechanistic insights revealed in the simulations. The results of this study suggest that the presence of liquid environment can eliminate the sharp features of surface morphology, reduce the amount of material removed from the target by more than an order of magnitude, and narrow down the nanoparticle size distribution as compared to laser ablation in vacuum. Moreover, the computational predictions of the effective incorporation of molecules constituting the liquid environment into the surface region of the irradiated target and the generation of high vacancy concentrations exceeding the equilibrium levels by more than an order of magnitude suggest a potential for hyperdoping of laser-generated surfaces by solutes present in the liquid environment.
关键词： Laser-Induced Periodic Surface Structures (LIPSS),Generation of Nanoparticles,Crystal Defects,Surface Morphology,Hyperdoping,Molecular Dynamics Simulations,Pulsed Laser Ablation in Liquids
更新于2025-09-19 17:13:59
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Multiscale coupled Maxwella??s equations and polarizable molecular dynamics simulation based on charge response kernel model
摘要： A computational scheme of coupled Maxwell’s equations and polarizable molecular dynamics simulation has been developed based on a multi-scale model to describe the coupled dynamics of light electromagnetic waves and molecules in crystalline solids, where the charge response kernel model is employed to incorporate electronic polarization of the molecules. The method is applicable to electronically non-resonant light–matter interaction systems that involve atomic motions in spectroscopy and photonics. Since the scheme simultaneously traces the light propagation in a medium on a macroscopic scale and the microscopic molecular motion under the light electric field, this enables us to treat the experimental setup and mimic its measurement process. As the first applications, we demonstrate three numerical examples of basic spectroscopies of an ice crystalline solid: simulations of reflection and transmission of visible light, infrared absorption measurement, and stimulated Raman scattering measurement. These examples show the detailed behaviors of the interacting light fields and molecules in the spectroscopic processes.
关键词： light–matter interaction,charge response kernel model,spectroscopy,photonics,Maxwell’s equations,polarizable molecular dynamics
更新于2025-09-19 17:13:59
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Inert gas cluster formation in sputter-deposited thin film CdTe solar cells
摘要： Magnetron sputtering is widely used for thin film deposition because it is a relatively low temperature process which also produces films with excellent uniformity. Unfortunately, in its use for the deposition of thin film CdTe devices, the inert working gas from the magnetron can incorporate into the film during the growth process and aggregate into large subsurface clusters during postprocessing. The gas clusters often occur at the CdS/CdTe interface causing delamination and blisters up to about 30 μm in diameter are readily observable on the film’s surface. The surface blisters are observed after postprocessing with CdCl2 at an elevated temperature but smaller inert gas clusters of several nanometres in diameter can be observed using high resolution transmission electron microscopy before the CdCl2 treatment. In this paper, these effects are investigated both experimentally and using molecular dynamics modelling. Some suggestions are also made as to how the effect might be minimised and higher efficiency solar devices fabricated.
关键词： Solar Cells,Cadmium Telluride,Argon bubbles,Molecular Dynamics,High Resolution Electron Microscopy,Magnetron Sputtering
更新于2025-09-19 17:13:59
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[IEEE 2019 IEEE 46th Photovoltaic Specialists Conference (PVSC) - Chicago, IL, USA (2019.6.16-2019.6.21)] 2019 IEEE 46th Photovoltaic Specialists Conference (PVSC) - Growth Evolution of Polycrystalline CdTe/CdS with Atomic Scale Resolution via Molecular Dynamics
摘要： A new method to study polycrystalline growth of CdTe layers has been developed using Molecular Dynamics (MD). The results show the creation of polycrystalline CdTe/CdS structures that closely recreate the morphology of experimental polycrystalline growth. The growth shows the nucleation and coalescence of grains at early stages for CdS on amorphous CdS and CdTe on polycrystalline CdS.
关键词： grain boundaries,grain growth evolution,polycrystalline structures,molecular dynamics
更新于2025-09-19 17:13:59
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Control of Charge Carrier Dynamics in Plasmonic Au Films by TiO <sub/><i>x</i> </sub> Substrate Stoichiometry
摘要： Plasmonic excitations in noble metals have many fascinating properties and give rise to a broad range of applications. We demonstrate, using non-adiabatic molecular dynamics combined with time-domain density functional theory, that chemical composition and stoichiometry of substrates can have a strong influence on charge dynamics. By changing oxygen content in TiO2, including stoichiometric, oxygen rich and oxygen poor phases, and Ti metal, one can alter lifetimes of charge carriers in Au by a factor of 5, and control the ratio of electron-to-hole relaxation rates by a factor of 10. Remarkably, a thin TiOx substrate alters so much charge carrier properties in much thicker Au films. Such large variations stem from the fact that the Ti and O atoms are much lighter than Au, and their vibrations are much faster at dissipating the energy. The control over a particular charge carrier and an energy range depends on the Au and TiOx level alignment, and the interfacial interaction strength. These factors are easily influenced by the TiOx stoichiometry. In particular, oxygen rich and poor TiO2 can be used to control holes and electrons, respectively, while metallic Ti affects both charge carriers. The detailed atomistic analysis of the interfacial and electron-vibrational interactions generates the fundamental understanding of the properties of plasmonic materials needed to design photovoltaic, photocatalytic, optoelectronic, sensing, nanomedical and other devices.
关键词： non-adiabatic molecular dynamics,substrate layers,time-domain density functional theory,metallic films,electron-phonon energy relaxation,surface plasmons
更新于2025-09-19 17:13:59
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Study of Structure and Electronic Properties of Heterointerfaces for Photovoltaic Applications
摘要： The linkage between the atomic structure and the electronic property is complex for heterointerfaces involving multicomponent organic?inorganic systems because of large configurations and chemical possibilities. Understanding the structure?property relationship at the interface becomes further complicated with an asymmetric structure of organic molecules compared to the interface between planer solids. Here, we report on ab inito molecular dynamics (AIMD) simulations of the perovskite/PCBM ([6,6]-phenyl-C61-butyric acid methyl ester) interface, where PCBM is an asymmetric molecule. Our AIMD calculations help us to navigate the vast number of possible atomic configurations of the interface. We have found that PCBM prefers to bind with the perovskite surface via an ester moiety over its fullerene moiety. The bonding at the interface and its stability are sensitive to the chemical composition at the perovskite surface, the PbI2-terminated surface making a stronger binding ≈1 eV with PCBM, compared to the MAI-terminated surface. Later, we systematically studied the role of atomic defects on the perovskite surface and interface and linked it to interface stability and electronic properties.
关键词： electronic properties,organic?inorganic systems,heterointerfaces,perovskite/PCBM interface,ab inito molecular dynamics
更新于2025-09-19 17:13:59
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Effects of LED Light Color and Intensity on Feather Pecking and Fear Responses of Layer Breeders in Natural Mating Colony Cages
摘要： The friction properties play an important role in diamond polishing, which significantly affect the interfacial contact and material removal. In this paper, the friction force and coefficient of friction (COF) during diamond polishing process were monitored under different loads and rotating speeds. The results show that the friction force and COF both increase with the load, and decrease with the rotating speed. The bearing capacity of liquid film is enhanced at large rotating speed, which leads to the decrease of friction force. According to the binomial law of friction, the increase of actual contact area caused by high load contributes to the increase of COF. Besides, it is found that the addition of H2O2 reduces the friction coefficient through surface adsorption. In order to further reveal the mechanism of friction variation at the atomic level, the friction behavior at a local area of interface between the diamond substrate and the abrasive particle in diamond polishing process was investigated by molecular dynamics (MD) method. The simulation results indicate that the interfacial bridge bonds formed between the substrate and particle under the action of load lead to the increase of friction force.
关键词： molecular dynamics,coefficient of friction,diamond,friction,polishing
更新于2025-09-19 17:13:59