化学物理

Diffusion-based samplers learn to sample complex, high-dimensional distributions using energies or log densities alone, without training data. Yet, they remain impractical for molecular sampling because they are often slower than molecular…

Identifying minimum-energy paths (MEPs) is crucial for understanding chemical reaction mechanisms but remains computationally demanding. We introduce MEPIN, a scalable machine-learning method for efficiently predicting MEPs from reactant…

Coarse-grained molecular dynamics often sacrifices accuracy and transferability for computational efficiency, but the use of machine learned potentials is helping coarse-grained models attain performance on par with atomistic molecular…

Determining the structure and following the structural evolution of molecules undergoing chemical reactions is one of the key goals of ultrafast molecular physics and chemistry. Recently, Coulomb explosion imaging has emerged as a promising…

Aromatic $\pi$-stacking interactions play an important role in both natural and artificial systems, influencing processes such as charge separation in photosynthesis and charge transport in organic semiconductors. Controlling the geometry…

Machine-learning potentials (MLPs) have become important tools for modern molecular simulations. However, developing models that simultaneously achieve high accuracy and high computational efficiency remains a significant challenge. In this…

Accurately simulating the non-Markovian dynamics of open quantum systems remains a significant challenge. While the recently proposed time-evolving matrix product operator (TEMPO) algorithm based on path integrals successfully circumvents…

Path integral molecular dynamics (PIMD), which maps a quantum particle onto a fictitious classical system of ring polymers and propagates the "beads" of this extended classical system using molecular dynamics, is widely used to capture…

Silicon-containing lithium-ion batteries can exhibit capacity gain early in life, which makes forecasting future cell behavior difficult. We have observed these anomalous trends even in conditions where known mechanisms, such as overhang…

$\mathtt{StochasticGW}$ is a code for computing accurate Quasi-Particle (QP) energies of molecules and material systems in the GW approximation. $\mathtt{StochasticGW}$ utilizes the stochastic Resolution of the Identity (sROI) technique to…

Protonated methane, CH5+, is a highly fluxional molecule with large spatial motions of the hydrogen atoms. The molecule's anharmonic effects and the delocalized wavefunction of the hydrogen atoms significantly affect the excitation spectrum…

Accurate thermochemical data with sub-chemical accuracy (within 1 kcal mol$^{-1}$ of the empirical ground truth) are essential for advancing computational chemistry methods. However, existing datasets that reach this level of accuracy…

A classical coulombic correlation functional in one-loop (1L) and local-density-approximation (LDA) is derived for electrolyte solutions, starting from a first-principles many-body partition function. The 1L-LDA functional captures…

Some rate of oxidation and reduction side-reactions will inevitably coexist in most rechargeable batteries, contributing to reversible and irreversible self-discharge. While parasitic reduction traps electrons, parasitic oxidation donates…

In this article, we present a method for computing accurate and scalable nuclear forces within the phaseless auxiliary-field quantum Monte Carlo (AFQMC) framework. Our approach leverages automatic differentiation of the energy functional to…

Transitions between distinct dynamical regimes are ubiquitous in nonequilibrium systems. As a prototypical example, deposition growth is often accompanied by irreversible morphological instabilities. Forecasting such transitions from…

Neural quantum states (NQS) provide a flexible and highly expressive parameterization of wave functions for strongly correlated problems in quantum chemistry. Despite rapid advances in network architectures, the evaluation of electronic…

Quantum-chemical calculations often make use of point-group theory to exploit molecular symmetry, resulting in a reduction of the computational cost and in insights into the electronic structure. This exploitation is often limited to…

We incorporate a solver for the fragment problem with accuracy beyond coupled cluster singles and doubles (CCSD) into the previously proposed static embedding framework, MPCC. To this end, we employ a CCSDT solver for the fragment…

Two-pulse correlation experiments performed using pulses of different intensities on Pd(111) with different CO coverages showed that the CO photodesorption probability depends on whether the strong or the weak pulse arrives first to the…