化学物理
In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this…
A wide variety of reactions are reported to be dramatically accelerated in aqueous microdroplets, making them a promising platform for environmentally clean chemical synthesis. However to fully utilize the microdroplets for accelerating…
Spin is a fundamental property of any many-electron system. The ability of density functional theory to accurately predict the physical properties of a system, while varying its spin, is crucial for describing magnetic materials and…
A very robust and efficient hybrid analytic-numerical Fock build, aMECP+aCOSx, has been developed for accelerating HF/DFT calculations. The essential idea is to extract those portions of the Fock matrix that can readily be evaluated…
Accurate estimation of the contribution from dispersion interactions to the total energy is important for many molecular systems and low-dimensional solids. In this work we demonstrate how the recently developed linear-scaling many-body…
The Variational Quantum Eigensolver (VQE) is a promising hybrid algorithm, utilizing both quantum and classical computers to obtain the ground state energy of molecules. In this context, this study applies VQE to investigate the ground…
Microheterogeneity, as a fundamental natural property, is widely presented in a range of microscopic systems such as polymer systems, biomacromolecular systems, and nanosystems, however, the construction of molecular systems of this form…
The sustainable production of many bulk chemicals relies on heterogeneous catalysis. The rational design or improvement of the required catalysts critically depends on insights into the underlying mechanisms at the atomic scale. In recent…
Intermolecular charge-transfer (xCT) excited states important for various practical applications are challenging for many standard computational methods. It is highly desirable to have an affordable method that can treat xCT states…
The ground state of second-quantized quantum chemistry Hamiltonians provides access to an important set of chemical properties. Wavefunctions based on ML architectures have shown promise in approximating these ground states in a variety of…
Real-time propagation methods for chemistry and physics are invariably formulated using variational techniques. The time-dependent bivariational principle (TD-BIVP) is known to be the proper framework for coupled-cluster type methods, and…
Strong coupling between excitons and confined modes of light presents a promising pathway to tunable and enhanced energy transport in organic materials. By forming hybrid light-matter quasiparticles, exciton-polaritons, electronic…
Biofouling represents a critical challenge in marine transportation, healthcare, and food manufacturing, among other industries, as it promotes contamination and increases maintenance costs. Zwitterionic polymers, known for their…
In this work, we propose a decoupled support vector regression (SVR) approach for direct canonical polyadic decomposition (CPD) of a potential energy surface (PES) through a set of discrete training energy data. This approach, denoted by…
We present the theory and implementation of a highly efficient relativistic third-order algebraic diagrammatic construction [ADC(3)] method based on a four-component (4c) Dirac-Coulomb (DC) Hamiltonian for the calculation of ionization…
We've studied the B800 part of Rhodoblastus acidophilus light-harvesting complex (LH2) by several quantum chemical techniques based on the density functional theory (DFT) and determined the specific method and a minimal reliable model…
In the molecular quantum chemistry community, coupled-cluster (CC) methods are well-recognized for their systematic convergence and reliability. The extension of the theory to extended systems has been comparably recent, so that…
Friction is a phenomenon that manifests across all spatial and temporal scales, from the molecular to the macroscopic scale. It describes the dissipation of energy from the motion of particles or abstract reaction coordinates and arises in…
Hedin's $GW$ approximation to the electronic self-energy has been impressively successful to calculate quasiparticle energies, such as ionization potentials, electron affinities, or electronic band structures. The success of this fairly…
Efficient hybrid DFT simulations of solid state materials would be extremely beneficial for computational chemistry and materials science, but is presently bottlenecked by difficulties in computing Hartree-Fock (HF) exchange with plane wave…