Related papers: Accurate molecular dynamics and nuclear quantum ef…
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…
Over the past decades, atomistic simulations of chemical, biological and materials systems have become increasingly precise and predictive thanks to the development of accurate and efficient techniques that describe the quantum mechanical…
Conventional theoretical and computational approaches to fully coupled quantum molecular dynamics, i.e. when both the electrons and nuclei are treated as quantum-mechanical particles, are impractical for all but the smallest chemical…
Vibrational spectra of condensed and gas-phase systems containing light nuclei are influenced by their quantum-mechanical behaviour. The quantum dynamics of light nuclei can be approximated by the imaginary time path integral (PI)…
A new concept of the molecular structure optimization method based on quantum dynamics computations is presented. Nuclei are treated as quantum mechanical particles, as are electrons, and the many-body wave function of the system is…
A new method ( PI-DFT ) which combines path integrals and density functional theory is proposed as a pathway to many fields of physics. Within path integral theory it is possible to construct particle densities without explicitly…
The quantum nature of nuclei plays an important role in the accurate modelling of light atoms such as hydrogen, but it is often neglected in simulations due to the high computational overhead involved. It has recently been shown that…
To take into account nuclear quantum effects on the dynamics of atoms, the path integral molecular dynamics (PIMD) method used since 1980s is based on the formalism developed by R. P. Feynman. However, the huge computation time required for…
Understanding the reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…
Molecular dynamics simulations are an important tool for describing the evolution of a chemical system with time. However, these simulations are inherently held back either by the prohibitive cost of accurate electronic structure theory…
Evaluating multi-center molecular integrals with Cartesian Gaussian-type basis sets has been a long-standing bottleneck in electronic structure theory calculation for solids and molecules. We have developed a vector-coupling and…
Magnetic quadrupoles are essential components of particle accelerators like the Large Hadron Collider. In order to study numerically the stability of the particle beam crossing a quadrupole, a large number of particle revolutions in the…
We show how the path-integral formulation of quantum statistical mechanics can be used to construct practical {\em ab initio} techniques for computing the chemical potential of molecules adsorbed on surfaces, with full inclusion of quantum…
Quantum embedding schemes have the potential to significantly reduce the computational cost of first principles calculations, whilst maintaining accuracy, particularly for calculations of electronic excitations in complex systems. In this…
Real-time time-dependent density functional theory (RT-TDDFT) is known to be hindered by the very small time step (attosecond or smaller) needed in the numerical simulation due to the fast oscillation of electron wavefunctions, which…
Real-time computation of time-dependent quantum mechanical problems are presented for nuclear many-body problems. Quantum tunneling in nuclear fusion at low energy is described using a time-dependent wave packet. A real-time method of…
Quantum computing has the potential to reduce the computational cost required for quantum dynamics simulations. However, existing quantum algorithms for coupled electron-nuclear dynamics simulation either require fault-tolerant devices, or…
We present an accelerated ``on-the-fly'' coupled-cluster path-integral molecular dynamics (PIMD) method for finite-temperature simulations in which electron correlation and nuclear quantum effects are treated simultaneously. The approach is…
Here we describe an approach for simulating electronic structure on quantum computers with significantly lower asymptotic complexity than prior work. The approach uses a real-space first-quantised representation of the molecular Hamiltonian…
We introduce a novel approach for a fully quantum description of coupled electron-ion systems from first principles. It combines the variational quantum Monte Carlo (QMC) solution of the electronic part with the path integral (PI) formalism…