化学物理
Density functional theory is one of the most efficient and widely used computational methods of quantum mechanics, especially in fields such as solid state physics and quantum chemistry. From the theoretical perspecive, its central object…
The spin-orbital entanglement in $5d^1$ transition metal ions embedded in double perovskites, where anomalous effective magnetic dipole moments are frequently observed, is quantified by the spin-orbital von Neumann entropy $\Delta S_{\rm…
This study address the computational determination of catalytic reaction rates by moving beyond traditional Transition State Theory (TST), addressing its limitations in complex systems. The Hill relation framework, integrated with Adaptive…
Ab initio quantum chemical methods for accurately computing interactions between molecules have a wide range of applications but are often computationally expensive. Hence, selecting an appropriate method based on accuracy and computational…
The supercritical state of matter is usually described as a continuous phase without sharp boundaries between liquid and gas regions. However, under non-equilibrium conditions, this view breaks down. Here we report an experimental…
In this communication, we examine new formalisms for the construction of the external space when correlating reference wavefunctions built from nonorthogonal determinant expansions. Defining the external space in nonorthogonal approaches is…
The disconnect between AI-generated molecules with desirable properties and their synthetic feasibility remains a critical bottleneck in computational discovery of drugs and materials. While generative AI has accelerated the proposal of…
The hydrogen entry behavior of a partially Zn-coated steel sheet in NaCl solutions was investigated employing a polyaniline-based hydrogenochromic sensor, electrochemical hydrogen permeation tests, and potential measurements using a…
L-edge X-ray absorption spectra for first-row transition metal complexes are obtained from relativistic equation-of-motion singles and doubles coupled-cluster (EOM-CCSD) calculations that make use of the core-valence separation (CVS)…
Aqueous solutions are crucial in chemistry, biology, environmental science, and technology. The chemistry of solutes is influenced by the surrounding solvation shell of water molecules, which have different chemical properties than bulk…
This article solves two major tasks that frequently arise in the theory of electron collisions with a target molecular cation. First, it extends the energy-dependent frame transformation treatment(EDFT), which is needed to map fixed-nuclei…
This work presents our theoretical study of the dissociative recombination (DR) of the closed-shell diatomic system CF$^+$ based on an approach recently applied to the CH$^+$ molecule. Our extended treatment uses the UK R-matrix theory and…
This article presents a method of computing bound state potential curves and autoionizing curves using fixed-nuclei R-matrix data extracted from the Quantemol-N software suite. It is a method based on two related approaches of multichannel…
We present a fragment-based framework for analyzing exciton couplings within the $GW$-Bethe-Salpeter Equation formalism using localized molecular orbitals, and assess how excitonic states in molecular dimers can be decomposed into local and…
For glymes of general formula CH3O(CH2CH2O)uCH3, with u = 1, 2, 3, 4, the densities of the (2-propanol + glyme) systems at temperatures ranging from (293.15 to 303.15) K and at pressure 0.1 MPa were determined using a DSA 5000 densimeter…
Recently, the coherent modified Redfield theory (CMRT) has been widely used to simulate the excitation-energy-transfer (EET) processes in photosynthetic systems. However, the numerical simulation of the CMRT is computationally expensive…
A major challenge in using spin-flip time-dependent density functional theory (SF-TD-DFT) for spin-flip-down excitations is the presence of spin contamination. While several improved methods have been developed in the past, a simple and…
The illumination of catalytic surfaces with a continuous or pulsed stream of photons dynamically modulates surface chemistry for faster rates, higher conversion, or product selectivity control. To establish fundamental principles of dynamic…
Chemical systems are traditionally described by lists of species, reactions, and externally imposed kinetic laws, a framework that lacks an intrinsic algebraic structure governing how transformations compose. We propose an axiomatic…
In this work, we extend selected configuration interaction (SCI) methods beyond energies and expectation values by introducing a linear response (LR) framework for molecular response properties. Existing SCI approaches are capable of…