Chemical Physics
Heavy atom compounds represent a challenge for computational chemistry, due to the need for simultaneous treatment of relativistic and correlation effects. Often such systems exhibit also strong correlation which hampers the application of…
The DMRG method, despite its favorable scaling, it is in practice not suitable for computations of dynamic correlation. Several approaches to include that in post-DMRG methods exist; in our group we focused on the tailored-CC (TCC)…
Recent developments in fully numerical methods promise interesting opportunities for new, compact atomic orbital (AO) basis sets that maximize the overlap to fully numerical reference wave functions, following the pioneering work of…
The concept of molecular similarity appears in many machine-learning algorithms based on the assumption that molecules with similar representations will also share similar properties. In this work, we propose a new way to study similarity…
Strong magnetic fields such as those found on white dwarfs have significant effects on the electronic structure of atoms and molecules. However, the vast majority of molecular studies in the literature in such fields are carried out with…
In a recent study [J. Chem. Theory Comput. 2021, 17, 1457-1468], some of us examined the accuracy of magnetizabilities calculated with density functionals representing the local density approximation (LDA), generalized gradient…
We introduce affordable computational strategies for calculating orbital and pair-orbital energies in atomic and molecular systems. Our methods are based on the pair Coupled Cluster Doubles (pCCD) ansatz and its orbital-optimized variant.…
Theoretical simulations of electron detachment processes are vital for understanding chemical redox reactions, semiconductor and electrochemical properties, and high-energy radiation damage. However, accurate calculations of ionized…
Metal phthalocyanines, a highly versatile class of aromatic, planar, macrocyclic molecules with a chelated central metal ion, are topical objects of ongoing research and particularly interesting due to their magnetic properties. However,…
This article reviews the concepts and methods of variational path sampling. These methods allow computational studies of rare events in systems driven arbitrarily far from equilibrium. Based upon a statistical mechanics of trajectory space…
This work presents a novel approach to distribute orbitals into subspaces within electron-pairing-based natural orbital functionals (NOFs). This approach modifies the coupling between weakly and strongly occupied orbitals by applying an…
The ability to prepare molecular ions in selected quantum states enables studies in areas such as chemistry, metrology, spectroscopy, quantum information, and precision measurements. Here, we demonstrate $(2+1)$ resonance-enhanced…
Combining Deep-UV second harmonic generation spectroscopy with molecular simulations, we confirm and quantify the specific adsorption of guanidinium cations to the air-water interface. Using a Langmuir analysis and measurements at multiple…
Water's ability to autoionize into hydroxide and hydronium ions profoundly influences surface properties, rendering interfaces either basic or acidic. While it is well-established that protons show an affinity to the air-water interface, a…
Ultrafast optical spectroscopy is a powerful technique for studying the dynamic processes of molecular systems in condensed phases. However, in molecular systems containing many dye molecules, the spectra can become crowded and difficult to…
Capture of anthropogenic CO2 is critical for mitigating climate change, and reducing the energy cost is essential for wide-scale deployment. Solubility of inorganic carbon in aqueous solutions depends on the pH, and electrochemical…
Machine learning (ML) offers considerable promise for the design of new molecules and materials. In real-world applications, the design problem is often domain-specific, and suffers from insufficient data, particularly labeled data, for ML…
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…