化学物理
When time-propagating a wave packet representing a molecular system interacting with strong attosecond laser pulses, one needs to use an approach that is capable of describing intricate coupled electronic-nuclear events that require…
The simulation of excited states at low computational cost remains an open challenge for electronic structure (ES) methods. While much attention has been given to orthogonal ES methods, relatively little work has been done to develop…
The kinetic isotope effect (KIE) is essential in various chemical applications from reaction mechanism studies to tritium removal from water. Traditional KIE evaluation relies on experimental measurements or computational approaches like…
The widespread adoption of machine learning surrogate models has significantly improved the scale and complexity of systems and processes that can be explored accurately and efficiently using atomistic modeling. However, the inherently…
For noncovalent interactions (NCIs), the CCSD(T) coupled cluster method is widely regarded as the `gold standard'. With localized orbital approximations, benchmarks for ever larger NCI complexes are being published; yet tantalizing evidence…
Temperature gradients represent energy sources that can be harvested to generate steady reaction or transport fluxes. Technological developments could lead to the transfer of free energy from heat sources and sinks to chemical systems for…
An important question in polariton chemistry is whether reacting molecules are in thermal equilibrium with their surroundings. If not, can experimental changes observed in reaction rates of molecules in a cavity (even without optical…
The Kohn-Sham (KS) density matrix is one of the most essential properties in KS density functional theory (DFT), from which many other physical properties of interest can be derived. In this work, we present a parameterized representation…
Generative machine learning models like the Restricted Boltzmann Machine (RBM) provide a practical approach for ansatz construction within the quantum computing framework. This work introduces a method that efficiently leverages RBM and…
Accurate charge densities are essential for reliable electronic structure calculations because they significantly impact predictions of various chemical properties and in particular, according to the Hellmann-Feynman theorem, atomic forces.…
Incremental full configuration interaction (iFCI) is polynomial-cost approach to the FCI limit of electronic structure. This article introduces the many-body basis set amelioration (MBBSA) method, which is designed to allow iFCI to be…
Buckminsterfullerene, C$_{60}$, has not only a beautiful truncated icosahedral (soccerball) shape, but simple H\"uckel calculations predict a three-fold degenerate lowest unoccupied molecular orbital (LUMO) which can accomodate up to six…
Multi-configurational wave-function theory (MC-WFT) that combines complete active space self-consistent field (CASSCF) approach with subsequent state interaction (SI) treatment of spin-orbit coupling (SOC), abbreviated as CASSCF-SO, plays…
Protein aggregation into insoluble amyloid-like fibrils is implicated in a wide range of diseases and understanding its nucleation process is a key for mechanistic insights and advancing therapeutics. The electronic charge of the…
The complex absorbing potential (CAP) technique is one of the commonly used Non-Hermitian quantum mechanics approaches for characterizing electronic resonances. CAP combined with various electronic structure methods has shown promising…
Polyacetylene, a simple yet fascinating polymer, has been of great interest for its unique electronic properties. However, the role of electronic correlation effects in polyacetylene still has not been explored fully on an ab initio basis.…
A low-cost approach for stochastically sampling static exchange during TDHF-type propagation is presented. This enables the use of an excellent hybrid DFT starting point for stochastic GW quasiparticle energy calculations. Generalized…
We extend our recently developed sparse-stochastic fragmented exchange formalism for ground-state hybrid DFT (ngH-DFT) to calculate absorption spectra within linear-response time-dependent Generalized Kohn-Sham DFT (LR-GKS-TDDFT), for…
The generation of unidirectional motion has been a long-standing challenge in engineering of molecular motors and, more generally, machines. A molecular motor is characterized by a set of low energy states that differ in their…
Density Functional Theory has long struggled to obtain the exact exchange-correlational (XC) functional. Numerous approximations have been designed with the hope of achieving chemical accuracy. However, designing a functional involves…