化学物理
Understanding how gas mixtures diffuse and distribute within porous frameworks is central to designing advanced separation and storage materials. Here, we investigate the transport and spatial distribution of binary gas mixtures in a porous…
Graphene supported on a substrate in contact with water underpins a wide range of processes and technologies, yet its wettability remains controversial. Understanding how substrate charges and graphene's properties influence water…
With the rapidly growing availability of machine-learned interatomic potential (MLIP) models for chemistry, much current research focuses on the development of generally applicable and ``foundational'' MLIPs. An important question in this…
Machine learning interatomic potentials (MLIPs) are changing atomistic simulations in the field of chemistry and materials science. However, constructing a single universal MLIP that can accurately model molecular and crystalline systems…
This dissertation is founded on the central notion that structural correlations in dense fluids, such as dense gases, liquids, and glasses, are directly related to fundamental interatomic forces. This relationship was identified early in…
Aluminium monofluoride (AlF) is a promising candidate for laser cooling and the production of dense ultracold molecular gases, thanks to its relatively high chemical stability and diagonal Frank-Condon factors. In this study, we examine the…
Molecular dynamics is a valuable tool to probe biological processes at the atomistic level - a resolution often elusive to experiments. However, the credibility of molecular models is limited by the accuracy of the underlying force field,…
This work demonstrates that fine-tuning transforms foundational machine-learned interatomic potentials (MLIPs) to achieve consistent, near-ab initio accuracy across diverse architectures. Benchmarking five leading MLIP frameworks (MACE,…
This review presents the covalent chemistry of carbon within the spin-radical concept of electron interaction. Using the language of valence bond trimodality, the regions of classical spinless covalence and its spin counterpart are defined.…
Predicting quantum wavefunction probability distributions is crucial for computational chemistry and materials science, yet machine learning (ML) models often face a trade-off between accuracy and interpretability. This study compares…
Electronic resonances are metastable states with finite lifetimes, encountered in processes such as photodetachment, electron transmission, and Auger decay. Resonances appear in Hermitian quantum mechanics as increased density of states in…
Hyperpolarization approaches in magnetic resonance overcome the sensitivity limitations imposed by thermal magnetization and play an important role in a very wide range of modern applications. One of the newer strategies, variants of what…
The effect of increased electron-density (from adsorbed Li atoms) in polyacenes and in nano-ribbons with zig-zag edge is discussed in terms of resonance theoretical considerations and in terms edge-localized frontier molecular orbitals. The…
A recent report by Barik et al. [Nature Chemistry 14, 1098, 2022] on ambient-light-induced intermolecular Coulombic decay (ICD) in unbound pyridine monomers proposes the formation of a pyridine cation via intermolecular Coulombic decay…
Molecular spin qubits are promising candidates for quantum technologies, but their performance is limited by decoherence arising from diverse mechanisms. The complexity of the environment makes it challenging to identify the main source of…
Diffusion models promise to accelerate material design by directly generating novel structures with desired properties, but existing approaches typically require expensive and substantial labeled data ($>$10,000) and lack adaptability. Here…
The eT program is an open-source electronic structure program with emphasis on performance and modularity. As its name suggests, the program features extensive coupled cluster capabilities, performing well compared to other electronic…
We present GSCDB137, a rigorously curated benchmark library of 137 data sets (8377 entries) covering main-group and transition-metal reaction energies and barrier heights, (intramolecular) non-covalent interactions, dipole moments,…
Elucidating reaction mechanisms hinges on efficiently generating transition states (TSs), products, and complete reaction networks. Recent generative models, such as diffusion models for TS sampling and sequence-based architectures for…
Studying the anharmonicity in the infrared (IR) spectra of polycyclic aromatic hydrocarbons (PAHs) at elevated temperatures is important to understand vibrational features and chemical properties of interstellar dust, especially in the…