This research is designed to understand the processes of wetting film formation and stability during the vaporization of volatile liquid droplets on surfaces featuring micro-structured triangular posts arranged in a rectangular grid pattern. Depending on the posts' density and aspect ratio, we ascertain either spherical-cap-shaped drops characterized by a mobile three-phase contact line or circular/angular drops featuring a pinned three-phase contact line. Liquid films emerge from drops of the later class, gradually covering the initial footprint of the drop, supporting a diminishing cap-shaped drop. Drop evolution is dictated by the posts' density and aspect ratio, while the orientation of the triangular posts demonstrably has no impact on the contact line's movement. Our systematic numerical energy minimization experiments concur with prior findings, suggesting that the spontaneous retraction of a wicking liquid film is only subtly influenced by the micro-pattern's alignment with the film edge.
Within computational chemistry, tensor algebra operations, like contractions, consume a large portion of the computational time on large-scale computing platforms. Due to the pervasive use of tensor contractions involving substantial multi-dimensional tensors in electronic structure theory, the creation of various tensor algebra frameworks designed for heterogeneous computing has been motivated. A framework for productive and high-performance, portable development of scalable computational chemistry methods, Tensor Algebra for Many-body Methods (TAMM), is introduced in this paper. The computational description within TAMM is isolated from the high-performance execution process on available computing systems. By implementing this design, scientific application developers (domain experts) can dedicate themselves to the algorithmic aspects through the tensor algebra interface furnished by TAMM, while high-performance computing engineers can concentrate on enhancing various aspects of the underlying structure, including optimal data distribution, refined scheduling algorithms, and effective utilization of intra-node resources (like graphics processing units). TAMM's modular framework facilitates its support of different hardware architectures and the incorporation of novel algorithmic enhancements. Our approach to the sustainable development of scalable ground- and excited-state electronic structure methods, using the TAMM framework, is described here. Examining case studies reveals the simplicity of use, including the measurable performance and productivity gains when compared with alternative frameworks.
Intramolecular charge transfer is disregarded by charge transport models of molecular solids, which adhere to a single electronic state per molecule. This approximation is limited by the exclusion of materials exhibiting quasi-degenerate, spatially separated frontier orbitals, specifically non-fullerene acceptors (NFAs) and symmetric thermally activated delayed fluorescence emitters. Chloroquine cost Considering the electronic structure of room-temperature molecular conformers of the prototypical NFA ITIC-4F, we posit that the electron resides on one of the two acceptor blocks with a mean intramolecular transfer integral of 120 meV, which compares favorably with intermolecular coupling strengths. Therefore, a minimal basis of acceptor-donor-acceptor (A-D-A) molecules comprises two molecular orbitals localized specifically on the acceptor sections. This foundation's integrity remains, despite geometric distortions within an amorphous solid, unlike the basis of the two lowest unoccupied canonical molecular orbitals, that demonstrates stability only when encountering thermal fluctuations in a crystalline structure. The single-site approximation for A-D-A molecules in their common crystalline arrangements can lead to a charge carrier mobility estimate that is off by a factor of two.
Antiperovskite's capacity for solid-state battery applications is attributable to its low cost, high ion conductivity, and customizable composition. Ruddlesden-Popper (R-P) antiperovskite, an upgrade from the simple antiperovskite material, displays improved stability and significantly enhances conductivity when integrated within the simple structure. Nonetheless, the theoretical study of R-P antiperovskite remains limited, thus impeding its advancement. This study provides a computational assessment of the newly reported, readily synthesizable R-P antiperovskite LiBr(Li2OHBr)2, which is investigated here for the first time. Calculations were performed to compare the transport performance, thermodynamic characteristics, and mechanical properties of hydrogen-rich LiBr(Li2OHBr)2 versus the hydrogen-lacking LiBr(Li3OBr)2. The presence of protons in LiBr(Li2OHBr)2 is implicated in its propensity for defects, and the production of additional LiBr Schottky defects could potentially improve its lithium-ion conductivity. genetic heterogeneity The material LiBr(Li2OHBr)2, with its extremely low Young's modulus of 3061 GPa, presents itself as an effective sintering aid. Despite their calculated Pugh's ratio (B/G) values of 128 and 150 for LiBr(Li2OHBr)2 and LiBr(Li3OBr)2 respectively, R-P antiperovskites demonstrate a mechanical brittleness, making them unsuitable candidates for solid electrolyte applications. Our analysis using the quasi-harmonic approximation determined a linear thermal expansion coefficient of 207 × 10⁻⁵ K⁻¹ for LiBr(Li2OHBr)2, which exhibits more favorable electrode compatibility than LiBr(Li3OBr)2 and even the simple antiperovskites. Our research comprehensively explores the practical application of R-P antiperovskite within the design and function of solid-state batteries.
Selenophenol's equilibrium structure has been examined through the application of rotational spectroscopy and high-level quantum mechanical calculations, offering fresh perspectives on the electronic and structural characteristics of this selenium compound, which are relatively unknown. Using fast-passage techniques employing chirped pulses, the broadband microwave spectrum in the jet-cooled 2-8 GHz cm-wave region was determined. Measurements utilizing narrow-band impulse excitation extended the frequency spectrum to 18 GHz. Spectral signatures were acquired for various monosubstituted 13C species, as well as for six selenium isotopes (80Se, 78Se, 76Se, 82Se, 77Se, and 74Se). The unsplit rotational transitions, linked to the non-inverting a-dipole selection rules, could be partially reproduced using a semirigid rotor model. Given the internal rotation barrier of the selenol group, the vibrational ground state is split into two subtorsional levels, which in turn doubles the dipole-inverting b transitions. Modeling double-minimum internal rotation produced a very low barrier height (42 cm⁻¹, B3PW91), considerably less than that of thiophenol's (277 cm⁻¹). Consequently, the monodimensional Hamiltonian indicates a significant vibrational gap of 722 GHz, accounting for the lack of observed b transitions in our frequency spectrum. MP2 and density functional theory calculations were scrutinized alongside the experimentally derived rotational parameters. The equilibrium structure was finalized based on the results of several advanced ab initio calculations. Finally, a Born-Oppenheimer (reBO) structure was achieved at the coupled-cluster CCSD(T) ae/cc-wCVTZ level, incorporating corrections for the wCVTZ wCVQZ basis set enhancement, derived from MP2 calculations. deep-sea biology Employing a mass-dependent methodology incorporating predicates, an alternative rm(2) structure was generated. The contrasting results from the two methods underline the exceptional accuracy of the reBO structure, while concurrently providing data about other molecules containing chalcogens.
Employing an expanded equation of motion for dissipation, this paper investigates the dynamics of electronic impurity systems. The Hamiltonian, deviating from the original theoretical formalism, introduces quadratic couplings to characterize the interaction of the impurity with its surrounding environment. By leveraging the quadratic fermionic dissipaton algebra, the proposed augmented dissipaton equation of motion provides a potent instrument for investigating the dynamic characteristics of electronic impurity systems, especially in scenarios where nonequilibrium and strong correlation effects are prominent. Numerical explorations of the Kondo impurity model aim to reveal the temperature-dependent nature of the Kondo resonance.
A thermodynamically consistent approach, the General Equation for Non-Equilibrium Reversible Irreversible Coupling (generic) framework, elucidates the progression of coarse-grained variables. The framework postulates a universal structure for Markovian dynamic equations governing coarse-grained variable evolution, guaranteeing both energy conservation (first law) and entropy increase (second law). Yet, the imposition of time-variant external forces can infringe upon the energy conservation law, demanding structural alterations within the framework. For dealing with this concern, we initiate with a strict and exact transport equation pertaining to the average of a collection of coarse-grained variables, originating from a projection operator methodology, and encompassing external forces. The statistical mechanics of the generic framework, under external forcing, are elucidated by this approach utilizing the Markovian approximation. Accounting for external forcing's impact on the system's evolution, while maintaining thermodynamic consistency, is achieved through this process.
In applications like electrochemistry and self-cleaning surfaces, amorphous titanium dioxide (a-TiO2) coatings are frequently employed, its water interface being a key element. Nevertheless, the fine-scale structures of the a-TiO2 surface and its interaction with water remain poorly characterized. This work employs a cut-melt-and-quench procedure, utilizing molecular dynamics simulations and deep neural network potentials (DPs) trained on density functional theory data, to model the a-TiO2 surface.