化学物理
The computation of magnetizability tensors using gauge-including atomic orbitals is discussed in the context of Cholesky decomposition for the two-electron repulsion integrals with a focus on the involved doubly differentiated integrals.…
Vacuum polarisation (VP) and electron self energy (SE) are implemented and evaluated as quantum electrodynamic (QED) corrections in a (quasi-relativistic) two-component zeroth order regular approximation (ZORA) framework. For VP, the…
Increasing the enzyme concentration generally speeds up enzymatic reactions. However, in this Letter, we show that increasing the enzyme concentration can also slow down the enzymatic reaction. We consider a simple allosteric protein with…
The anisotropic potential energy surface of the (H$_2$)$_2$ dimer represents a challenging problem for many-body methods. Here, we determine the potential energy curves of five different dimer configurations (T, Z, X, H, L) using the…
Instanton theory relates the rate constant for tunneling through a barrier to the periodic classical trajectory on the upturned potential energy surface whose period is $\tau=\hbar/(k_{\rm B}T)$. Unfortunately, the standard theory is only…
Water isotope separation, specifically separating heavy from light water, is a socially significant issue due to the usage of heavy water in applications such as nuclear magnetic resonance, nuclear power, and spectroscopy. Separation of…
The Density Matrix Renormalization Group (DMRG) method has become a prominent tool for simulating strongly correlated electronic systems characterized by dominant static correlation effects. However, capturing the full scope of electronic…
In this work we explore theoretically whether a parity-violating/chiral light-matter interaction is required to capture all relevant aspects of chiral polaritonics or if a parity-conserving/achiral theory is sufficient (e.g.…
We describe the implementation details of periodic local coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)] using local natural orbitals (LNOs) and $k$-point symmetry. We discuss…
Electronic coherences are key to understanding and controlling photo-induced molecular transformations. We identify a crucial quantum-mechanical feature of electron-nuclear correlation, the projected nuclear quantum momenta, essential to…
We develop a static quantum embedding scheme that utilizes different levels of approximations to coupled cluster (CC) theory for an active fragment region and its environment. To reduce the computational cost, we solve the local fragment…
We propose a general technique to produce cold spin-polarized molecules, in which rotationally excited states are first populated by coherent microwave excitation, and then allowed to spin-flip and relax via collisional quenching, which…
We investigate the dependence of the yield of positive secondary ions created upon impact of primary He, B and Ne ions on geometry and electronic and nuclear energy deposition by the projectiles. We employ pulsed beams in the medium energy…
We present a novel approach to address the challenges of variable occupation numbers in direct optimization of density functional theory (DFT). By parameterizing both the eigenfunctions and the occupation matrix, our method minimizes the…
The accurate prediction of solvation free energy is of significant importance as it governs the behavior of solutes in solution. In this work, we apply a variety of machine learning techniques to predict and analyze the alchemical free…
We report on the application of the recently developed Fano-ADC(2,2) method to compute total and partial Auger decay widths of molecular core-hole states, including explicit evaluation of double Auger decay branching ratios. The method…
New metal-organic frameworks (MOFs) are periodically synthesized all over the world due to the wide range of societally and environmentally relevant applications they possess. However, the mechanisms and thermodynamics associated to MOF…
Charge transfer (CT) processes that are electronically non-adiabatic are ubiquitous in chemistry, biology, and materials science, but their theoretical description requires diabatic states or adiabatic excited states. For complex systems,…
A coherent vibrational wavepacket is launched and manipulated in the symmetric stretch (a$_1$) mode of CBr$_4$, by impulsive stimulated Raman scattering from non-resonant 400 nm laser pump pulses with various peak intensities on the order…
The increasing availability of GPUs for scientific computing has prompted interest in accelerating quantum chemical calculations through their use. The complexity of integral kernels for high angular momentum basis functions however often…