化学物理
In a recent contribution [Fishman, V.; Lesiuk, M.; Martin, J.M.L.; Boese, A.D., J. Chem. Theory Comput. 2025, 21, 2311-2324], we introduced another angle at benchmarking non-covalent interactions by not just benchmarking interaction…
Short-range correlations in electrolyte solutions lead to oscillatory profiles of water polarization and ionic concentration at electrode-electrolyte interfaces. The recently developed density-potential-polarization functional theory…
We derive analytical expressions for chemical potentials within the random phase approximation (RPA), equivalently the $GW$ energy functional evaluated using non interacting Green's functions ($G_s$). The chemical potential is obtained…
Accurate atomistic simulations of gas-surface scattering require potential energy surfaces that remain reliable over broad configurational and energetic ranges while retaining the efficiency needed for extensive trajectory sampling. Here,…
Norrish type I reactions selectively cleave carbon-carbon bonds directly adjacent to carbonyl groups. Despite their broad use in combination with aromatic carbonyls for additive manufacturing and dental UV curing applications, the nature of…
Condensed-phase spectral line shapes encode the strength and timescale of interactions between molecules and their environments, yet these ideas are often difficult to introduce at the undergraduate level due to their reliance on formal…
We model, simulate, and analyze the intramolecular modes of liquid H2O and D2O to elucidate how energy excitation, relaxation, and vibrational dephasing interplay through anharmonic mode-mode coupling. Our analysis employs two-dimensional…
We introduce sbml4md, a newly developed algorithm implemented as a software package to extract parameters of multimode anharmonic Brownian (MAB) models from molecular dynamics (MD) trajectories for simulating nonlinear vibrational spectra…
In computational chemistry of molecular materials, strong static correlation effects appear when electronic states, often involving the ground state, become quasi-degenerate, as occurs, for example, in bond-breaking processes. Such…
We have developed a non-isothermal analytical model for the impedance of the cathode catalyst layer (CCL) in a PEM fuel cell. In-phase harmonic perturbations to the current density and temperature reduce the impedance and the static…
Quantum Monte Carlo (QMC) methods deliver highly accurate electronic structure calculations but are computationally intensive. The quantum Monte Carlo kernel library (QMCkl) provides a modular, portable collection of high-performance…
The vastness of chemical space makes generalization a central challenge in the development of machine learning interatomic potentials (MLIPs). While MLIPs could enable large-scale atomistic simulations with near-quantum accuracy, their…
We derived and implemented the calculation of the one-body reduced density matrix for Aufbau suppressed coupled cluster theory, from which excited state natural orbitals and one-body properties, like atomic populations and dipole moments,…
We propose schemes to produce highly nuclear-spin polarized small molecules in an intense and cold molecular beam via microwave or infrared rotational excitation, followed by hyperfine-induced quantum beats. Repumping schemes can be used to…
TENSO is a versatile and powerful open-source software package for numerically exact simulations of the dynamics of quantum systems immersed in structured thermal environments. It is based on a tree tensor network decomposition of the…
Quantum-matter theory (QMT), based on the Schr\"odinger or Dirac equations, is firmly established for both intra- and intermolecular interactions. However, there are two key issues with QMT. First, its applicability to large molecular…
We present a computational study of the laser-driven quantum dynamics of positronium (Ps), PsH, and PsCl at the time-dependent Hartree-Fock level of theory. To eliminate finite-basis effects and to properly capture continuum dynamics, we…
Proton transfer is central to many processes of chemical interest. The simulation of proton transfer dynamics requires the inclusion of nuclear quantum effects, such as zero-point energy, nuclear delocalization, and tunneling. Herein, we…
In J. Chem. Phys. 152, 144105 (2020) Lehtola et al introduced the efficient Gaussian-basis representation of Superposition of Atomic Potentials (SAP) which "can be easily implemented in any Gaussian-basis quantum chemistry code in terms of…
Rare nonadiabatic reactions are a key component of many important molecular processes but are challenging to capture with direct dynamical simulations. In this paper, we combine our recently developed mapping approach to surface hopping…