Related papers: A Machine-Learning Accelerated Grand Canonical Sam…
Proton-coupled electron transfers (PCET) are elementary steps in electrocatalysis. However, accurate calculations of PCET rates remain challenging, especially considering nuclear quantum effects (NQEs) under a constant potential condition.…
Nuclear quantum effects (NQEs) on the structures and transport properties of dense liquid hydrogen at densities of 10-100 g/cm3 and temperatures of 0.1-1 eV are fully assessed using \textit{ab initio} path-integral molecular dynamics…
The contribution of nuclear quantum effects (NQEs) to the properties of various hydrogen-bound systems, including biomolecules, is increasingly recognized. Despite the development of many acceleration techniques, the computational overhead…
Proton-coupled electron transfer (PCET) is foundational to catalysis, bioenergetics, and energy conversion, yet capturing and disentangling the coupled motions of electrons, protons, and solvent has remained a major experimental challenge.…
A theoretical scheme for the treatment of an open molecular system with electrons and nuclei is proposed. The idea is based on the Grand Canonical description of a quantum region embedded in a classical reservoir of molecules. Electronic…
We introduce a simple method for characterizing reactive pathways in quantum systems. Flux auto- correlation and cross-correlation functions are employed to develop a quantitative measure of dynamical coupling in quantum transition events,…
Quantum embedding is a fundamental prerequisite for applying quantum machine learning techniques to classical data, and has substantial impacts on performance outcomes. In this study, we present Neural Quantum Embedding (NQE), a method that…
Atomistic simulations based on the first-principles of quantum mechanics are reaching unprecedented length scales. This progress is due to the growth in computational power allied with the development of new methodologies that allow the…
Supercooled water is expected to exhibit a liquid--liquid phase transition between low- and high-density liquid states, possibly terminating in a liquid--liquid critical point in the experimentally difficult no man's land. Because the…
Using first-principles molecular dynamics, we study the influence of nuclear quantum effects (NQEs) and nonlocal exchange--correlation density functionals (DFs) near molecular dissociation in liquid hydrogen. NQEs strongly influence…
Hydrogen atom transfer (HAT) reactions are essential in many biological processes, such as radical migration in damaged proteins, but their mechanistic pathways remain incompletely understood. Simulating HAT is challenging due to the need…
Quantum computing (QC) provides a promising avenue toward enabling quantum chemistry calculations, which are classically impossible due to a computational complexity that increases exponentially with system size. As fully fault-tolerant…
A quantum statistical model of nuclear multifragmentation is proposed. The recurrence equation method used within the canonical ensemble makes the model solvable and transparent to physical assumptions and allows to get results without…
Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…
Interatomic potentials learned using machine learning methods have been successfully applied to atomistic simulations. However, accurate models require large training datasets, while generating reference calculations is computationally…
Nuclear quantum effects such as zero-point energy and hydrogen tunnelling play a central role in many biological and chemical processes. The nuclear-electronic orbital (NEO) approach captures these effects by treating selected nuclei…
The quantum computation of electronic energies can break the curse of dimensionality that plagues many-particle quantum mechanics. It is for this reason that a universal quantum computer has the potential to fundamentally change…
Here we report an observation of cation-dependent nonadiabaticity in a proton-coupled electron transfer electrode process (PCET) during hydrogen evolution at electrified interfaces of Au(111) single-crystal electrode and electrolytes by…
The ability to perform ab initio molecular dynamics simulations using potential energies calculated on quantum computers would allow virtually exact dynamics for chemical and biochemical systems, with substantial impacts on the fields of…
Accurate calculation of strongly correlated electronic systems requires proper treatment of both static and dynamic correlations, which remains challenging for conventional methods. To address this, we present VQE-PDFT,aquantum-classical…