化学物理
We study the ring-opening decomposition of ethylene carbonate in the presence of a single lithium atom and on the surface of lithium metal. Combining accurate electronic structure theory, enhanced sampling, and machine learning, we…
Experiments [1] have shown that auto-kirigami structures can grow on the surface of graphene because the graphene-graphene adhesion energy is greater than the graphene-substrate interaction. In this work molecular dynamics (MD) simulations…
The electric double layer (EDL) governs electrocatalysis, energy conversion, and storage, yet its atomic structure, capacitance, and reactivity remain elusive. Here we introduce a machine learning interatomic potential framework that…
The term pristine interface was introduced by Beattie and Djerdjev 20 years ago for emulsions that consist of only water and oil with no surfactant. They are different from Pickering emulsions, which are also surfactant-free but stabilized…
We use selected configuration interaction to calculate the zero-temperature mid-infrared (2800-3800 cm$^{-1}$) vibrational spectra of a water monomer, dimer, trimer, and hexamer in its cage and prism geometries. We use the recently…
Ab initio thermodynamics is a widespread, computationally efficient approach to predict the stable configuration of a surface in contact with a surrounding (gas or liquid) environment. In a prevalent realization of this approach, this…
Dimensional analysis is fundamental to the formulation and validation of physical laws, ensuring that equations are dimensionally homogeneous and scientifically meaningful. In this work, we use Lean 4 to formalize the mathematics of…
Molecular dynamics computer simulations have been conducted on neat liquid methanol, using three different united atom (three site) interatomic potentials: TraPPE [J. Phys. Chem. B 105, 3093 (2001)], UAM-I [J. Mol. Liq. 323, 114576 (2021)]…
Recent advancements have led to the development of bright and heavy metal-free blue-emitting quantum dot light-emitting diodes (QLEDs). However, consensus understanding of their distinct photophysical and electroluminescent dynamics remains…
The components of the radial correlation energy density are calculated and analyzed for the atoms from He to Ar. The components include the nucleus-electron potential correlation energy density, the kinetic correlation energy density and…
The vibrational averaging module of the Dalton Project was extended to work also with the Amsterdam Density Functional (ADF) program, making it possible to calculate vibrational corrections to properties and at the same time include a…
Monitoring $^{90}$Sr contamination in milk following a nuclear accident is critical due to its radiotoxicity and calcium-mimicking behaviour, leading to accumulation in bones and teeth. This study presents a high-efficiency protocol for…
We present an efficient implementation of four-component linear response coupled cluster singles and doubles (4c-LRCCSD) theory that enables accurate and computationally efficient calculation of polarizabilities for systems containing heavy…
Chemical reaction optimisation is essential for synthetic chemistry and pharmaceutical development, demanding the extensive exploration of many reaction parameters to achieve efficient and sustainable processes. We report $\alpha$-PSO, a…
Energy functions for pure and heterogenous systems are one of the backbones for molecular simulation of condensed phase systems. With the advent of machine learned potential energy surfaces (ML-PESs) a new era has started. Statistical…
We systematically investigate the calculation of excited states in quantum chemistry using auxiliary field quantum Monte Carlo (AFQMC). Symmetry allows targeting of the lowest triplet excited states in AFQMC based on restricted open-shell…
The prevailing view that solid-state diffusion is negligible at low temperatures is challenged by rapid sulfur and barium isotope exchange between natural barite crystals and aqueous solutions in laboratory experiments. This assumption…
The fermion sign problem constitutes a fundamental computational bottleneck across a plethora of research fields in physics, quantum chemistry and related disciplines. Recently, it has been suggested to alleviate the sign problem in…
Accurately modeling chemical reactions at the atomistic level requires high-level electronic structure theory due to the presence of unpaired electrons and the need to properly describe bond breaking and making energetics. Commonly used…
Ring-polymer molecular dynamics (RPMD) has become a popular method for describing chemical reactions due to its ability to simultaneously capture tunneling, zero-point energy, anharmonicity and recrossing. Here we highlight that despite its…