化学物理
Electron density prediction stands as a cornerstone challenge in molecular systems, pivotal for various applications such as understanding molecular interactions and conducting precise quantum mechanical calculations. However, the scaling…
The balancing of chemical equations is a basic problem in chemistry. A commonly employed method is to convert the task to a linear algebra problem, and then solve the null space of the constructed formula matrix. However, in this method,…
The bond distance is the simplest and most obvious indicator of the nature of a given chemical bond. However, for rare chemistry, it may happen that it is not yet firmly established. In this communication, we will show that the…
The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…
Electron density is a fundamental quantity, which can in principle determine all ground state electronic properties of a given system. Although machine learning (ML) models for electron density based on either an atom-centered basis or a…
This work outlines the foundations for being able to do a first-principle study of the adsorption process using the steepest-entropy-ascent quantum thermodynamic (SEAQT) framework, a framework able to predict the unique non-equilibrium path…
Milestoning is an accurate and efficient method for rare event kinetics calculations by constructing a continuous-time kinetic network connecting the reactant and product states. However, even with adequate sampling, its accuracy can also…
Recent breakthroughs in machine learning and artificial intelligence, fueled by scientific data, are revolutionizing the discovery of new materials. Despite the wealth of existing scientific literature, the availability of both structured…
We analyze the possibility of symmetry-lowering induced by pseudo-Jahn--Teller interactions in six previously studied azaphenalenes that are known to have their first excited singlet state (S$_1$) lower in energy than the triplet state…
We present a reduction of Milestoning (ReM) algorithm to analyze the high-dimensional Milestoning kinetic network. The algorithm reduces the Milestoning network to low dimensions but preserves essential kinetic information, such as local…
As an optimal one-dimensional reaction coordinate, the committor function not only describes the probability of a trajectory initiated at a phase space point first reaching the product state before reaching the reactant state, but also…
Milestoning is an efficient method for rare event kinetics calculation using short trajectory parallelization. Mean first passage time (MFPT) is the key kinetic output of Milestoning, whose accuracy crucially depends the initial…
Aromatic structures are fundamental for key biological molecules such as RNA and metabolites and the abundances of aromatic molecules on young planets are therefore of high interest. Recent detections of benzonitrile and other aromatic…
Machine learning potentials (MLPs) represent atomic interactions with quantum mechanical accuracy offering an efficient tool for atomistic simulations in many fields of science. However, most MLPs rely on local atomic energies without…
Two machine learning-aided thermodynamic integration schemes to compute the chemical potentials of atoms and molecules have been developed and compared. One is the particle insertion method, and the other combines particle insertion with…
In this paper, we analyze the properties of the recently proposed real-time equation-of-motion coupled-cluster (RT-EOM-CC) cumulant Green's function approach [J. Chem. Phys. 2020, 152, 174113]. We specifically focus on identifying the…
Excess molar enthalpies, $H_{\text{m}}^{\text{E}}$, have been measured using a Tian-Calvet microcalorimeter for the systems CH$_3$(CH$_2$)$_{u-1}$OH ($u$ = 1,2,3,4,7,10) + cyclohexylamine at 298.15 K and 0.1 MPa. The…
On-demand control of molecular actions is essential for realizing single-molecule functional devices. Such a control can be achieved by manipulating interactions between individual molecules and their nanoscale environment. In this study,…
Solid-state electrolytes, by enabling lithium metal anodes, may significantly increase the energy density of current lithium-ion batteries. However, similar to their liquid counterparts, these hard and stiff electrolytes can still be…
Wavefunction forms based on products of electron pairs are usually constructed as closed-shell singlets, which is insufficient when the molecular state has a nonzero spin or when the chemistry is determined by $d$- or $f-$electrons. A set…