化学物理
Machine learning force field (MLFF) has emerged as a powerful data-driven tool for atomistic simulations, enabling large-scale and complex atomic systems to be simulated with accuracy comparable to \textit{ab initio} methods. However, MLFFs…
Aza-BODIPY dimers represent promising molecular systems for efficient triplet-state generation through either intramolecular-singlet fission (iSF) or spin-orbit charge transfer intersystem crossing (SOCT-ISC). In this work, we investigate…
Per- and polyfluoroalkyl substances are a class of synthetic chemical compounds widely used as coatings to lower surface energies. Yet the microscopic mechanisms of their weak interaction with water and organic compounds remain poorly…
Anisotropic two-dimensional diffraction signals encode additional structural information, including atom-pair angular distributions, beyond conventional isotropic scattering. However, experimental constraints such as beam stops result in…
The Weiner's theory (WT) is developed on the basis of the exactly solvable Schr\"odinger equation with trigonometric double-well potential (TDWP). The symmetric case of TDWP is considered. This modified version of WT (mWT) enables one to…
Accuracy, variationality, and convergence underpin the reliability of modern electronic structure methods, yet definitive benchmarks in the relativistic regime remain elusive due to the absence of numerically exact full configuration…
Auxiliary Field Quantum Monte Carlo (AFQMC) has emerged as a powerful framework for treating strongly correlated electronic systems, offering a favorable balance between computational cost and accuracy. In this paper, we present a novel…
In this work, we develop a new framework for computing atom-resolved contributions to optical properties based on atoms-in-molecules (AIM) schemes. The formalism is independent of the specific AIM method and is made rigorous by partitioning…
We present TUNA, an open-source quantum chemistry program specifically designed for atoms and diatomic molecules. Within this narrow molecular domain, a broad and consistent set of electronic structure methods and calculation types is…
Predicting the perceived intensity of odorants remains a fundamental challenge in sensory science due to the complex, non-linear behavior of their response, as well as the difficulty in correlating molecular structure with human perception.…
Computational chemistry has become an indispensable tool for generating data and insights, pervading all branches of experimental chemistry. Its most central concept is the potential energy hypersurface, key to all chemistry and materials…
Large thermal fluctuations of the liquid phase obscure the weak macroscopic electric field that drives electrochemical reactions, rendering the extraction of reliable interfacial charge distributions from ab initio molecular dynamics…
This study systematically investigates two multi-fidelity strategies used to train machine-learned force fields (MLFFs) -- pre-training/fine-tuning and multi-headed training -- and elucidates the mechanisms underpinning their success. For…
Machine-learned interatomic potentials (MLIPs) have rapidly progressed in accuracy, speed, and data efficiency in recent years. However, training robust MLIPs in multicomponent systems still remains a challenge. In this work, we train a…
Entropy scaling is a powerful technique that has been used for predicting transport properties of pure components over a wide range of states. However, modeling mixture diffusion coefficients by entropy scaling is an unresolved task. We…
Accurate prediction of acid dissociation constants (p$K_{\rm a}$) and the determination of dominant protonation states is critical in drug discovery, influencing molecular properties such as solubility, permeability, and protein-ligand…
Ultrafast light-driven chemical dynamics at surfaces are governed by energy transfer from excited electrons to vibrational degrees of freedom. When this nonadiabatic energy transfer is anisotropic, it can lead to dynamical steering effects…
We introduce stochastic GW with the orthogonalized projector augmented-wave method (OPAW-sGW). This implementation enables accurate quasiparticle band gaps on significantly coarser real-space grids than norm-conserving pseudopotential sGW…
Transition-state searches are central to understanding reaction mechanisms, but the high computational cost of density-functional theory (DFT) limits their application in high-throughput catalyst and materials discovery. Machine-learned…
Quantitative spectroscopic detection of dibromomethane, CH$_2$Br$_2$, for environmental monitoring, workplace safety, and exoplanetary studies is limited by the lack of accurate absorption cross-section data and rigorous spectroscopic…