化学物理
Molecular dynamics simulations are indispensable for exploring the behavior of atoms and molecules. Grounded in quantum mechanical principles, quantum molecular dynamics provides high predictive power but its computational cost is dominated…
The development of chemical engineering technology is a multi-stage process that encompasses laboratory research, scaling up, and industrial deployment. This process demands interdisciplinary col laboration and typically incurs significant…
Spiropyran is a prototype photoswitch that undergoes photoinduced ring-opening via C-O bond fission. The quantum yield for this photochemical reaction is low, with photophysical relaxation being the dominant process. Previous theoretical…
Neural operators are capable of capturing nonlinear mappings between infinite-dimensional functional spaces, offering a data-driven approach to modeling complex functional relationships in classical density functional theory (cDFT). In this…
We model Auger spectra using second-order M\o ller-Plesset perturbation (MP2) theory combined with complex-scaled basis functions. For this purpose, we decompose the complex MP2 energy of the core-hole state into contributions from specific…
New routes for transforming nitrogen into ammonia at ambient conditions would be a milestone toward an energy efficient and economically attractive production route in comparison to the traditional Haber-Bosch process. Recently, the…
The quantum-classical hybrid variational quantum eigensolver (VQE) algorithm is arguably the most popular noisy intermediate-scale quantum (NISQ) era approach to quantum chemistry. We consider the underexplored quantum annealing eigensolver…
The ability to control chemical reactions by coupling organic molecules to confined light in a cavity has recently attracted much attention. While most previous studies have focused on single-mode photonic or plasmonic cavities, here we…
We present a configuration interaction (CI) framework which serves quantitative and conceptual purposes for charge delocalization and electron transfer processes in molecular systems. The electronic Hamiltonian is expressed in a basis of…
Excited-state gradients and derivative couplings are critical for simulating excited-state dynamics. However, their calculations are very expensive within the coupled-cluster framework due to the steep scaling. In this work, we present two…
Spectroscopic techniques based on core-level excitations provide powerful tools for probing molecular and electronic structures with high spatial resolution. However, accurately calculating spectral features at the L or M edges is…
In a recent paper, J. Chem. Phys. 162, 214101 (2025), a novel approach for the rigidification of a molecular cluster was proposed, in which starting with an all-atom (AA) potential, a coarse-grained (CG) potential for the associated cluster…
In this work, we introduce a correction to the unitary coupled cluster method with single and double excitations (UCCSD) that incorporates the effects of missing triple excitations through a treatment that is correct through fifth-order in…
Temperature-accelerated sliced sampling (TASS) is a well-established enhanced sampling method that facilitates exhaustive exploration of high-dimensional collective variable (CV) space through directed sampling employing a combination of…
Being a numerically exact method for the simulation of dynamics in open quantum systems, the hierarchical equations of motion (HEOM) still suffers from the curse of dimensionality. In this study, we propose a novel MCE-HEOM method, which…
We report a study of the electronic and nuclear relaxation dynamics of the photoexcited RNA base uracil in the gas phase, using time-resolved core level photoelectron spectroscopy together with high level calculations. The dynamics was…
Machine learning interatomic potentials (MLIPs) provide a computationally efficient alternative to quantum mechanical simulations for predicting material properties. Message-passing graph neural networks, commonly used in these MLIPs, rely…
We present a framework for atomistic simulations of surface catalysis under electrochemical bias. The framework makes use of extended Lagrangian Born-Oppenheimer quantum-based molecular dynamics (XL-BOMD) simulations, which provide the…
Atomistic simulations of matter, especially those that leverage first-principles (ab initio) electronic structure theory, provide a microscopic view of the world, underpinning much of our understanding of chemistry and materials science.…
Molecular visualization software has long supported research and education in chemical and structural sciences, but consumer devices constrained to 2D inputs and outputs pose two major challenges: they poorly convey 3D nature, and 3D…