化学物理
The excessive application of pesticides, particularly the overreliance on insecticides for the protection of desirable crops from pests, has posed a significant threat to both ecological systems and human health due to environmental…
The field of molecular excitons and related supramolecular systems has largely focused on aggregates where nearest-neighbour couplings dominate. We propose that radically different states can be produced by moving beyond that paradigm. In…
We discuss a new strategy to compute partial Auger decay widths with equation-of-motion ionisation-potential coupled-cluster (EOMIP-CCSD) wave functions in the framework of non-Hermitian quantum mechanics, where the decaying character of…
We present an efficient and cost-effective implementation for the exact two-component atomic mean field (X2CAMF) based coupled cluster (CC) method, which integrates frozen natural spinors (FNS) and the Cholesky decomposition (CD) technique.…
The preference of water self-ions (hydronium and hydroxide) towards air/oil-water interfaces is one of the hottest topics in water research due to its importance for understanding properties, phenomena, and reactions of interfaces. In this…
Developing machine learning protocols for molecular simulations requires comprehensive and efficient datasets. Here we introduce the QMe14S dataset, comprising 186,102 small organic molecules featuring 14 elements (H, B, C, N, O, F, Al, Si,…
The work addresses the issue of precision measurement of the concentration of molecular gas components in the atmosphere and their isotopic composition. The primary focus is investigating the composition of gas mixtures and determining the…
The foundation model (FM) paradigm is transforming Machine Learning Force Fields (MLFFs), leveraging general-purpose representations and scalable training to perform a variety of computational chemistry tasks. Although MLFF FMs have begun…
The State--Specific Kohn--Sham Density Functional Theory [arXiv:physics/0506037] is used to derive the Kohn-Sham exchange-correlation potential $\vxc$ and exchange-correlation energy $\Eco$ as explicit functionals of $v_s$ and $\phi_1$,…
Spin engineering of advanced pulse sequences has had a transformative impact on the development of nuclear magnetic resonance (NMR) spectroscopy, to an extending degree also electron paramagnetic resonance (EPR), and the hybrid between the…
We introduce a method for computing quantum mechanical forces through surface integrals over the stress tensor within the framework of density functional theory. This approach avoids the inaccuracies of traditional force calculations using…
A gradient dependent formula is derived for the spinless one-particle density-matrix operator z from the differential virial theorem. A gradient dependent formula is also derived for a spinless one-particle density-matrix operator that can…
NMR acquisitions based on Ernst-angle excitations are widely used in analytical spectroscopy, as for over half a century they have been considered the optimal way for maximizing spectral sensitivity without compromising bandwidth or peak…
The theoretical investigation of gas adsorption, storage, separation, diffusion and related transport processes in porous materials relies on a detailed knowledge of the potential energy surface of molecules in a stationary environment. In…
We introduce a black-box auxiliary field quantum Monte Carlo (AFQMC) approach to perform highly accurate electronic structure calculations using configuration interaction singles and doubles (CISD) trial states. This method consistently…
In this work, the molecular enhancement factors of the $\mathcal{P,T}$-odd interactions involving the electron electric dipole moment ($W_\mathrm{d}$) and the scalar-pseudoscalar nucleon-electron couplings ($W_\mathrm{s}$) are computed for…
Excited-state nonadiabatic simulations with quantum mechanics/molecular mechanics (QM/MM) are essential to understand photoinduced processes in explicit environments. However, the high computational cost of the underlying quantum chemical…
Understanding the quantum dynamics of strongly coupled molecule-cavity systems remains a significant challenge in molecular polaritonics. This work develops a comprehensive self-consistent model simulating electromagnetic interactions of…
We study the applicability of the Hammett-inspired product (HIP) Ansatz to model relative substrate binding within homogenous organometallic catalysis, assigning $\sigma$ and $\rho$ to ligands and metals, respectively. Implementing an…
$^{1}$H spin-lattice nuclear magnetic resonance (NMR) relaxation experiments have been performed for water dispersions of functionalized silica nanoparticles of diameters of 25 and 45 nm. The experiments have been performed in a broad…