化学物理
We present Einstein coefficient spectra and a detailed-balance derivation of generalized Einstein relations between them that is based on the connection between spontaneous and stimulated emission. If two broadened levels or bands overlap…
Accurately predicting infrared (IR) spectra in computational chemistry using ab initio methods remains a challenge. Current approaches often rely on an empirical approach or on tedious anharmonic calculations, mainly adapted to semi-rigid…
The multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method and the density matrix renormalization group (DMRG) are powerful workhorses applied mostly in different scientific fields. Although both methods are based on tensor…
The injection of hydrogen into the natural-gas grid is an alternative during the process of a gradual decarbonization of the heat and power supply. When dealing with hydrogen-enriched natural gas mixtures, the performance of the reference…
Supercritical oxidation processes in jet-stirred reactors (JSR) have been modeled based on ideal gas assumption. This can lead to significant errors in or complete misinterpretation of modeling results. Therefore, this study newly developed…
This paper derives and demonstrates a new, purely density-based ab initio approach for calculation of the energies and properties of many-electron systems. It is based upon the discovery of relationships that govern the "mechanics" of the…
A comprehensive theoretical understanding of electron-photon correlation is essential for describing the reshaping of molecular orbitals in quantum electrodynamics (QED) environments. The strong coupling QED Hartree-Fock (SC-QED-HF) theory…
Reduced density matrix functional theory (RDMFT) calculations are usually implemented in a decoupled manner, where the orbital and occupation optimizations are repeated alternately. Typically, orbital updates are performed using the unitary…
We employ state-of-the-art quantum chemistry methods to study the structure-to-property relationship in polyanilines (PANIs) of different lengths and oxidation states. Specifically, we focus on leucoemeraldine, emeraldine, and…
The transfer of population between two intersecting quantum states is the most fundamental dynamical event that governs a broad variety of processes in physics, chemistry, biology and material science. Whereas any two-state description…
An adequate understanding of NOx interacting chemistry is a prerequisite for a smoother transition to carbon lean and carbon free fuels such as ammonia and hydrogen. In this regard, this study presents a comprehensive study on the H atom…
We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires…
Surfaces of colloidal nanocrystals are frequently passivated with carboxylate ligands which exert significant effects on their optoelectronic properties and chemical stability. Experimentally, binding geometries of such ligands are…
A common, yet unmodelled experimental phenomenon is explained first through the experimental data and then through modelling efforts. The phenomenon is a large, temporary loss in voltage during constant current discharge. This effect can be…
Battery safety is important, yet safety limits are normally static and do not evolve as batteries degrade. Consequently, many battery systems are overengineered to meet increasingly stringent safety demands. In this work we show that…
The numerical cost of variational methods suggests using perturbative approaches to determine the electronic structure of molecular systems. In this work, a sequential construction of effective Hamiltonians drives the definition of…
Densities, $\rho$, speeds of sound, $c$, and refractive indices, $n_{\text{D}}$, have been measured for the systems N,N-dimethylformamide (DMF) + propanone, + 2-butanone, or + 2-pentanone in the temperature ($T$) range from 293.15 to 303.15…
The development of X-ray free-electron lasers (XFELs) has enabled ultrafast X-ray diffraction (XRD) experiments, which are capable of resolving electronic/vibrational transitions and structural changes in molecules, or capturing molecular…
This study aims to reveal the important role and the respective rate rules of H atom abstractions by NO2 for better understanding NOX hydrocarbon interactions. To this end, H atom abstractions from C2 to C5 alkanes and alkenes 15 species by…
A nonlinear phase-field model is developed to simulate corrosion damage. The motion of the electrode$-$ electrolyte interface follows the usual kinetic rate theory for chemical reactions based on the Butler-Volmer equation. The model links…