相关论文: Quantum Mechanical Treatment of Variable Molecular…
We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires…
Accurate calculation of free energies and their derivatives is central to assessing the thermodynamic stability of molecular and particulate systems across length scales. Yet such quantities can be difficult to compute reliably in strongly…
We assess the predictive accuracy of perturbation theory based estimates of changes in covalent bonding due to linear alchemical interpolations among molecules. We have investigated $\sigma$ bonding to hydrogen, as well as $\sigma$ and…
We introduce a novel computational approach for the investigation of complex correlated electron materials which makes it possible to evaluate interatomic forces and thereby determine atomic displacements and structural transformations…
When two phases of water are at equilibrium, the ratio of hydrogen isotopes in each is slightly altered due to their different phase affinities. This isotopic fractionation process can be utilized to analyze water's movement in the world's…
The precise description of quantum nuclear fluctuations in atomistic modelling is possible by employing path integral techniques, which involve a considerable computational overhead due to the need of simulating multiple replicas of the…
The energy difference between two iso-electronic systems can be accurately approximated by the alchemical first order Hellmann-Feynmann derivative for the averaged Hamiltonian. This approximation is exact up to third order because…
We present a family of alchemical perturbation potentials that enable the calculation of hydration free energies of small to medium-sized molecules in a concerted single alchemical coupling step instead of the commonly used sequence of two…
We introduce a pseudo-mass parameterized Schr\"odinger-like alchemical equation which contains nuclear charges as variables, treating nuclear charges, nuclear coordinates and electronic coordinates on the equal footing. The eigenfunctions…
Alchemical transformations showed that perturbation theory can be applied also to changes in the atomic nuclear charges of a molecule. The alchemical path that connects two different chemical species involves the conceptualization of a…
We introduce a representation of any atom in any chemical environment for the generation of efficient quantum machine learning (QML) models of common electronic ground-state properties. The representation is based on scaled distribution…
Doping compounds can be considered a perturbation to the nuclear charges in a molecular Hamiltonian. Expansions of this perturbation in a Taylor series, i.e. quantum alchemy, has been used in literature to assess millions of derivative…
Quantum chemical calculations have attracted much attention as a practical application of quantum computing. Quantum computers can prepare superpositions of electronic states with various numbers of electrons on qubits. This special feature…
A parameterization strategy for molecular models on the basis of force fields is proposed, which allows a rapid development of models for small molecules by using results from quantum mechanical (QM) ab initio calculations and thermodynamic…
Quantum chemistry calculations such as the prediction of molecular properties and modeling of chemical reactions are a few of the critical areas where near-term quantum computers can showcase quantum advantage. We present a method to…
The exact and phaseless variants of Auxiliary-Field Quantum Monte Carlo (AFQMC) have been shown to be capable of producing accurate ground-state energies for a wide variety of systems including those which exhibit substantial electron…
We formulate a local picture of strongly correlated systems as a Feynman sum over atomic configurations. The hopping amplitudes between these atomic configurations are identified as the renormalization group charges, which describe the…
We study the magnetic field dependences of the conductivity in heavily doped, strongly disordered 2D quantum well structures within wide conductivity and temperature ranges. We show that the exact analytical expression derived in our…
Chemically accurate and comprehensive studies of the virtual space of all possible molecules are severely limited by the computational cost of quantum chemistry. We introduce a composite strategy that adds machine learning corrections to…
Quantum phase transitions have been the subject of intense investigations in the last two decades [1]. Among other problems, these phase transitions are relevant in the study of heavy fermion systems, high temperature superconductors and…