Chemical Physics
We employ large-scale density matrix renormalization group calculations to study the quantum phases of dipolar molecules confined in bent (zigzag) endofullerene chains, as a function of the chain angle $\gamma$. For LiF, ferroelectric order…
A new family of ionic basis sets, denoted i{\sigma}XZ1, is presented for molecular calculations on systems containing monovalent ions. The basis sets extend the SIGMA family by explicitly accounting for the different electronic structure of…
Interfacial charge-transfer processes play a critical role in plasmon-enhanced spectroscopy, yet the energetic conditions governing charge-transfer resonance within molecule-metal nanocavities remain poorly understood. Here, plasmonic…
Density matrix embedding theory (DMET) provides an elegant framework in quantum chemistry to describe local properties of chemical systems that allows a high-level method being used to solve an embedded subsystem constructed based on a…
Strong-field photoionization of molecules and molecular clusters gives rise to a rich variety of fragmentation pathways governed by charge localization and redistribution on ultrafast timescales. Here, we report a velocity-map imaging study…
Capturing the ultrafast structural dynamics that occur at the solid-liquid interface is key to understanding adsorption, desorption, diffusion, and aggregation processes in catalysis and interfacial chemical reactions. Hard-X-ray scattering…
Catalysts are essential for sustainable chemical manufacturing, yet discovering novel architectures remains a bottleneck dominated by trial-and-error experimentation and computationally intensive screening. In complex reactions such as…
Cryptochromes are blue-light-sensitive flavoproteins that play central roles in biological function. In European robin (Erithacus rubecula) ErCry4a proteins, optical excitation of their flavin chromophore forms a long-lived radical pair…
Computational modeling plays a central role in advancing our understanding of electro-chemical reactions and may thus guide the rational development of sustainable energy technologies. Despite significant methodological progress, achieving…
Modeling the quantum dynamics of plasmonic excitations -- collective oscillations of free electrons interacting with light -- remains a significant theoretical challenge, particularly due to the need to accurately describe their quantum…
Zn-metalloproteins play vital roles in numerous metabolic processes, making them high-value targets for structure-based drug design. To advance these efforts, it is useful to unravel the individual components of the intermolecular…
Highly successful drugs, such as transition-state inhibitors, were designed by mimicking the precise geometry of enzymatic transition states, a strategy that requires quantum chemistry accurate enough to specify molecular structure at…
The low-frequency dielectric response of liquid water is commonly described by a dominant Debye relaxation together with additional faster contributions whose microscopic origin remains debated. Here we show that the dielectric function of…
Roaming reactions are organized not by potential-energy saddles but by transition states that are unstable invariant objects in phase space, periodic orbits in the two degrees of freedom studied here. To ask what controls roaming, we modify…
The Hessian of the ring polymer spring potential in the standard Trotter path integral is a $P\times P$ symmetric circulant matrix with a centroid eigenvalue of zero. All such matrices commute and are diagonalised by the same bead to normal…
Characterization of the decomposition products of energized Criegee intermediates is essential for assessing their impact on the chemical evolution of the atmosphere. Here, a generic and microscopically resolved approach is used to…
We present a multiconfigurational binary-encounter (MC-BE) framework for direct analytical evaluation of electron-impact electronic-excitation cross sections for dipole-allowed transitions from ab initio excited-state data. The method…
We present a unified, memory-bounded GPU realization of equation-of-motion coupled-cluster (EOM-CC) excited-state gradients and interstate nonadiabatic couplings (NACMEs) on a single 8\,GB consumer GPU. Both are built from one contraction…
Strong light-matter coupling in optical cavities provides a versatile platform for modulating chemical structure, reactivity, and spectroscopy, and hence motivates the development of ab initio cavity quantum electrodynamics (cQED) methods…
Understanding the physics of many-body complex dynamical systems is typically non-trivial. High-dimensional analysis approaches are often deemed necessary to prevent losing important information. Typically, these use order parameters or…