化学物理
Classical molecular dynamics simulation is performed mostly using the established velocity Verlet integrator or other symplectic propagation schemes. In this work, an alternative formulation of numerical propagators for classical molecular…
We introduce an atomistic classifier based on a combination of spectral graph theory and a Voronoi tessellation method. This classifier allows for the discrimination between structures from different minima of a potential energy surface,…
Short-range corrections to long-range selected configuration interaction calculations are derived from perturbation theory considerations and applied to harmonium (with two to six electrons for some low-lying states). No fitting to…
Electron transfer reactions play an essential role in many chemical and biological processes. Fermi's Golden rule, which assumes that the coupling between electronic states is small, has formed the foundation of electron transfer rate…
We investigate whether making the friction spatially dependent on the reaction coordinate introduces quantum effects into the thermal reaction rates for dissipative reactions. Quantum rates are calculated using the numerically exact…
Photosynthetic organisms rely on a network of light-harvesting protein-pigment complexes to efficiently absorb sunlight and transfer excitation energy to reaction center proteins for charge separation. In photosynthetic purple bacteria,…
A long-standing challenge in mixed quantum-classical trajectory simulations is the treatment of entanglement between the classical and quantal degrees of freedom. We present a novel approach which describes the emergence of entangled states…
Quantum-chemical subsystem and embedding methods require complex workflows that may involve multiple quantum-chemical program packages. Moreover, such workflows require the exchange of voluminous data that goes beyond simple quantities such…
Quantum-chemical fragmentation methods offer an efficient approach for the treatment of large proteins, in particular if local target quantities such as protein--ligand interaction energies, enzymatic reaction energies, or spectroscopic…
Exploring nonequilibrium hot carriers from plasmonic metal nanostructures is a dynamic field in optoelectronics, driving photochemical reactions such as solar fuel generation. The hot carrier injection mechanism and the reaction rate are…
Dynamic nuclear polarization (DNP) involves a polarization transfer from unpaired electrons to hyperfine coupled nuclei and can increase the sensitivity of nuclear magnetic resonance (NMR) signals by several orders of magnitude. The…
A chemical reaction mechanism (CRM) is a sequence of molecular-level events involving bond-breaking/forming processes, generating transient intermediates along the reaction pathway as reactants transform into products. Understanding such…
Optimization has found numerous applications in engineering, particularly since 1960s. Many optimization applications in engineering have more than one objective (or performance criterion). Such applications require multi-objective (or…
Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…
Ionic liquids (ILs) are an exciting class of electrolytes finding applications in many areas from energy storage to solvents, where they have been touted as ``designer solvents'' as they can be mixed to precisely tailor the physiochemical…
Computational simulation of chemical and biological systems using ab initio molecular dynamics has been a challenge over decades. Researchers have attempted to address the problem with machine learning and fragmentation-based methods.…
In the realm of photochemistry, the significance of double excitations (also known as doubly-excited states), where two electrons are concurrently elevated to higher energy levels, lies in their involvement in key electronic transitions…
The magnitude of the rate of chemical reactions also depends on the position in the gravitational field, where a chemical reaction is being carried out. At weaker gravitational field rate of reaction is greater than the rate of reaction at…
Electronic structure methods built around double-electron excitations have a rich history in quantum chemistry. However, it seems to be the case that such methods are only suitable in particular situations and are not naturally equipped to…
A system of one electron in a Coulomb potential in an optical cavity is solved using a tensor-product light-matter basis. The problem was treated at the level of the Pauli-Fierz Hamiltonian describing both light and matter quantum…