化学物理

Accurate vibrational spectra are essential for understanding how molecules behave, yet their computation remains challenging and benchmark data to reliably compare different methods are sparse. Here, we present high-accuracy eigenstate…

The application of the standard quasi-steady-state approximation to the Michaelis--Menten reaction mechanism is a textbook example of biochemical model reduction, derived using singular perturbation theory. However, determining the specific…

Material surface - analyte interactions play important roles in numerous processes including gas sensing. However, the effects of topological polar surface area (TPSA) of analytes on surface interactions during gas sensing have been so far…

Open-shell non-rigid molecular systems exhibiting an internal rotation are likely candidates for a coupling between the spin angular momentum of the unpaired electron and the torsional motion. This electron spin-torsion coupling lacked both…

Incorporating nuclear quantum effects into nonadiabatic dynamics remains a significant challenge. Herein we introduce new nonadiabatic dynamics approaches based on the recently developed constrained nuclear-electronic orbital (CNEO) theory.…

Corrosion in concrete prevents in-situ observation, necessitating models to provide insight into the local reaction currents. We present a computational method for predicting corrosion rates of reinforcements within concrete under natural…

We propose an end-to-end integrated strategy to produce highly accurate quantum chemistry (QC) synthetic datasets (energies and forces) aimed at deriving Foundation Machine Learning models for molecular simulation. Starting from Density…

We investigated the ultrafast structural dynamics of cyclobutanone following photoexcitation at $\lambda=200$ nm using gas-phase megaelectronvolt ultrafast electron diffraction. Our investigation complements the simulation studies of the…

The Ziegler-Rauk-Baerends multiplet sum method (MSM) assumes that density-functional theory (DFT) provides a good description of states dominated by a single determinant. It then uses symmetry to add static correlation to DFT. In our…

Building on our recent study [https://doi.org/10.1021/acs.jpclett.3c02052, J. Phys. Chem. Lett. 14, 8780 (2023)], we explore the generalization of the ground-state Kohn-Sham (KS) formalism of density-functional theory (DFT) to the (singlet)…

The Bethe-Salpeter equation has been extensively employed to compute the two-body electron-hole propagator and its poles which correspond to the neutral excitation energies of the system. Through a different time-ordering, the two-body…

Reduced density matrix functional theory (RDMFT) and coupled cluster theory restricted to paired double excitations (pCCD) are emerging as efficient methodologies for accounting for the so-called non-dynamic electronic correlation effects.…

To expand the QUEST database of highly-accurate vertical transition energies, we consider a series of large organic chromogens ubiquitous in dye chemistry, such as anthraquinone, azobenzene, BODIPY, and naphthalimide. We compute, at the CC3…

Electronic resonances are metastable states that can decay by electron loss. They are ubiquitous across various fields of science, such as chemistry, physics, and biology. However, current theoretical and computational models for resonances…

Hedin's equations provide an elegant route to compute the exact one-body Green's function (or propagator) via the self-consistent iteration of a set of non-linear equations. Its first-order approximation, known as $GW$, corresponds to a…

Life is homochiral and homochirality is a fundamental feature of living systems on Earth. While the exact mechanism that led to homochirality is still not fully understood, any realistic scenario on the origins of life needs to address the…

Life as we know it is homochiral, but the origins of biological homochirality on early Earth remain elusive. Shallow closed-basin lakes are a plausible prebiotic environment on early Earth, and most are expected to have significant…

Previous studies have primarily focused on the nonequilibrium thermodynamics of chemical reaction networks (CRNs) occurring in closed systems. In contrast, CRNs in open systems exhibit much richer nonequilibrium phenomena due to sustained…

Sensing and discriminating between enantiomers of chiral molecules remains a significant challenge in the design of sensor platforms. In the case of chemoresistive sensors, where detection relies on changes in electrical response upon…

Reliable trajectory-based nonadiabatic quantum dynamics methods at the atomic level are critical for understanding many important processes in real systems. The paper reports latest progress of nonadiabatic field (NaF), a conceptually novel…