Detailed understanding of solid-solid interface structure-function relations is critical for the improvement and wide deployment of all solid-state batteries. The interfaces between lithium phosphorous oxynitride ("LiPON") solid electrolyte material and lithium metal anode, between LiPON and Li(x)CoO(2) cathode surfaces, have been reported to generate solid electrolyte interphase ("SEI")-like products and/or disordered regions. Using electronic structure calculations and crystalline LiPON models with atomic-layer-deposition-like stoichiometry, we predict LiPON models with purely P-N-P backbones are kinetically inert towards lithium at room temperature. In contrast, transfer of oxygen atoms from low-energy Li(x)CoO(2) (104) surfaces to LiPON is much faster under ambient conditions. The mechanisms of the primary reaction steps, LiPON motifs that readily react with lithium metal, experimental results on amorphous LiPON to partially corroborate these predictions, and possible mitigation strategies to reduce degradations are discussed. LiPON interfaces are found to be useful case studies for highlighting the importance of kinetics-controlled processes during battery assembly at moderate processing temperatures.
Nucleation during solidification in multi-component alloys is a complex process that comprises the competition between different crystalline phases as well as chemical composition and ordering. Here, we combine transition interface sampling with an extensive committor analysis to investigate the atomistic mechanisms during the initial stages of nucleation in $\text{Ni}_3\text{Al}$. The formation and growth of crystalline clusters from the melt are strongly influenced by the interplay between three descriptors: the size, crystallinity, and chemical short-range order of the emerging nuclei. We d…
Using a fast and accurate neural network potential we are able to systematically explore the energy landscape of large unit cells of bulk magnesium oxide with the minima hopping method. The potential is trained with a focus on the near-stoichiometric compositions, in particular on suboxides, i.e., Mg$_x$O$_{1-x}$ with $0.50<x<0.60$. Our extensive exploration demonstrates that for bulk stoichiometric compounds, there are several new low-energy rocksalt-like structures in which Mg atoms are octahedrally six--coordinated and form trigonal prismatic motifs with different stacking sequences. Furthe…
Femtosecond laser excitation of solid-state systems creates non-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering we gain a detailed understanding of the complex non-equilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wavevector resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable …
Molecular dynamics simulations using an interatomic potential developed by artificial neural network deep machine learning are performed to study the local structural order in Al90Tb10 metallic glass. We show that more than 80% of the Tb-centered clusters in Al90Tb10 glass have short-range order (SRO) with their 17 first coordination shell atoms stacked in a '3661' or '15551' sequence. Medium-range order (MRO) in Bergman-type packing extended out to the second and third coordination shells is also clearly observed. Analysis of the network formed by the '3661' and '15551' clusters show that ~82…
Porous crystalline nitinol is widely applied in various fields of science and technology due to the unique combination of physical and mechanical properties as well as biocompatibility. Porous amorphous nitinol is characterized by improved mechanical properties compared to its crystalline analogues. Moreover, this material is more promising from the point of view of fundamental study and practical application. The production of porous amorphous nitinol is a difficult task requiring rapid cooling protocol and optimal conditions to form a stable porous structure. In the present work, based on th…
The size-dependent phase stability of gamma-Al2O3 was studied by large-scale molecular dynamics simulations over a wide temperature range from 300 to 900 K. For the gamma-Al2O3 crystal, a bulk transformation to alpha-Al2O3 by an FCC-to-HCP transition of the O sublattice is still kinetically hindered at 900 K. However, local distortions of the FCC O-sublattice by the formation of quasi-octahedral Al local coordination spheres become thermally activated, as driven by the partial covalency of the Al-O bond. On the contrary, spherical gamma-Al2O3 NPs (with sizes of 6 and 10 nm) undergo a crystalli…
Charge Transport in Thin-Film Transistors Based on Liquid-Crystalline Phthalocyanines
Universidade Federal de Santa Catarina（圣卡塔琳娜联邦大学）；Institut national de la recherche scientifique, Centre Énergie Matériaux Télécommunications（国家科学研究研究所，能源材料电信中心）；Centre de Recherche Paul Pascal, Université de Bordeaux & CNRS（保罗·帕斯卡研究中心，波尔多大学与法国国家科学研究中心）
Whereas knowledge of a crystalline material's unit cell is fundamental to understanding the material's properties and behavior, there are not obvious analogues to unit cells for disordered materials despite the frequent existence of considerable medium-range order. This article views a material's structure as a collection of local atomic environments that are sampled from some underlying probability distribution of such environments, with the advantage of offering a unified description of both ordered and disordered materials. Crystalline materials can then be regarded as special cases where t…
High-quality factor plasmonic devices are crucial components in the fields of nanophotonics, quantum computing and sensing. The majority of these devices are required to be fabricated on non-lattice matched or transparent amorphous substrates. Plasmonic devices quality factor is mainly defined by ohmic losses, scattering losses at grain boundaries, and in-plane plasmonic scattering losses of a metal - substrate system. Here, we demonstrate the deposition technique to e-beam evaporate ultralow-loss silver thin films on transparent lattice-mismatched substrates. The process is based on evolution…
Energy storage technologies that can meet the unprecedented demands of a sustainable energy system based on intermittent energy sources require new battery materials. We investigate high ionic conductors, Li$_3$ClO glasses. In the present work we use a first principles method to model the amorphous structure of the glass. We characterize the structure by means of radial distribution functions, radial disctributions functions and coordination numbers. We compare to their crystalline counterparts. The electronic structure of the glass is compared to that of the crystalline material. The band gap…
The formation of the positive, fixed charge at c-Si(111)/a-Si$_3$N$_{3.5}$:H interfaces
现代电子设备是不可想象的，没有良好的控制形成界面的异质结构。这些通常涉及至少一种无定形材料。建模这样的接口提出了一个重大的挑战，因为一个有意义的结果只能通过使用巨大的模型或从许多统计独立的样本绘制。在这里，我们报告晶体硅（c-Si）和非晶氮化硅（a-Si $_3$ N $_{3.5}$：H），这是无处不在的商业太阳能电池之间的界面的高吞吐量计算的结果。这些发现只是部分地调和了我们所理解的关键特征。在界面处，存在三重配位的Si原子。这是由于非晶部分和结晶部分之间的结构不匹配造成的。未掺杂的c-Si的局域费米能级远低于a-SiN：H的费米能级。为了使器件中的费米能级对准，电荷从a-SiN：H部分转移到c-Si部分，从而在界面处产生大量带正电荷的三重配位Si原子。这就解释了在界面处存在排斥空穴的正的固定电荷。
