化学物理
Attosecond technologies provide unique opportunities to study electron dynamics and electron correlation on their intrinsic timescales. From a theoretical perspective, this places strong constraints as an accurate treatment of electron…
Recent discoveries of electron-induced coherence in both resonant and non-resonant interactions have introduced new perspectives in the field. In non-resonant processes, coherence has been observed in dipolar dissociation, where…
Molecular simulations of complex chemical systems, such as catalysis, electrochemistry, and energy storage, often need to capture the interplay of effects such as electronic structure, finite-temperature fluctuations, and electric-field…
Intramolecular electron transport in biological systems is typically described as a diffusive hopping process, according to the semi-classical rate theories of Marcus and Hopfield combined with classical Pauli-type master equations.…
Multireference behavior in molecules often arises when a small gap between frontier orbitals results in mixing of closed and open-shell configurations. Standard multireference diagnostics of this regime usually rely on correlated…
The Obara-Saika (OS) method is one of the most widely used techniques in quantum chemistry for evaluating electron repulsion integrals (ERIs) via a set of recurrence relations that build higher angular momentum integrals from lower-order…
Experiments have shown that, by tuning a microcavity to resonance with a vibrational mode of the molecules contained within it, one can modify chemical properties, such as reaction rates. This gives rise to the exciting prospect of steering…
Molecular spintronics seeks to control spin states in single molecules for ultrafast switching and efficient information processing. Transition metal complexes are promising candidates for such applications due to their modular ligand…
The highly variable physico-chemical properties of thin molecular films play an essential role in numerous research fields ranging from biophysics to the fabrication of functional devices such as molecular sensors. The properties of…
Machine learning interatomic potentials are trained to predict energies and forces but built to be sampled: their purpose is to drive molecular simulations whose observables average over the equilibrium distribution the potential defines.…
We introduce an additive reference correction for the transcorrelated (TC) method and its three-body mean-field approximation (xTC), to improve energy differences computed in small orbital basis sets. The correction is motivated by the…
Atmospheric entry processes are characterized by high-enthalpy gas flows in strong thermo-chemical non-equilibrium. Accurate simulations of such conditions remain challenging due to the extreme conditions and the complex influence of…
Non-collinear density functional theories were developed to extend the use of established collinear exchange-correlation functionals to systems with unpaired electrons in the presence of significant spin-orbit coupling. A comparison of…
Hydrogen bonds are the fundamental backbone for deoxyribo-nucleic acid (DNA) stability. In this letter we propose a new strategy based on plasmonic cavities to perform a local manipulation of hydrogen bonds in DNA. The analysis is performed…
We introduce a radical-fragment many-body expansion at the two-body level (MBE2) for quantum chemistry of linear alkanes. Instead of heterolytic bond cleavage with hydrogen capping atoms and electrostatic embedding like in Fragment…
Advances in deep learning architectures and representations have enabled ML-driven chemical property prediction, but state-of-the-art (SOTA) models have remained largely confined to independent codebases and lack support for diverse…
The COSMO-SAC-Phi model developed by Soares et al. extends the COSMO-SAC activity-coefficient framework into a full equation of state by explicitly accounting for pressure effects. In this approach, pure substances and mixtures are…
The size-dependent strong-field ionization and dissociation dynamics of (H$_2$O)$_n$ (n=1-4) are investigated using real-time time-dependent density functional theory (RT-TDDFT) coupled to Ehrenfest molecular dynamics under a common…
Hydrogen-based direct reduction of metal oxides is a ubiquitous solid-gas redox process central to geophysics, sustainable metallurgy, redox energy cycles and catalysis. During this process, hydrogen removes lattice oxygen to form water,…
Predicting electronic fundamental gaps at finite temperature has remained conceptually and practically challenging. We address this in three connected steps. First, we extend generalized Kohn--Sham hybrid density functional theory to…