Related papers: Quantum Ring-Polymer Contraction Method: Including…
Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to…
We have applied path integral simulations, in combination with new ab initio based water potentials, to investigate nuclear quantum effects in liquid water. Because direct ab initio path integral simulations are computationally expensive, a…
The development and implementation of increasingly accurate methods for electronic structure calculations mean that, for many atomistic simulation problems, treating light nuclei as classical particles is now one of the most serious…
In this work, a path integral Car-Parrinello molecular dynamics simulation of liquid water is performed. It is found that the inclusion of nuclear quantum effects systematically improves the agreement of first principles simulations 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…
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…
Path integral-based simulation methodologies play a crucial role for the investigation of nuclear quantum effects by means of computer simulations. However, these techniques are significantly more demanding than corresponding classical…
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…
Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these…
It is now established that nuclear quantum motion plays an important role in determining water's hydrogen bonding, structure, and dynamics. Such effects are important to include in density functional theory (DFT) based molecular dynamics…
Light nuclei at room temperature and below exhibit a kinetic energy which significantly deviates from the predictions of classical statistical mechanics. This quantum kinetic energy is responsible for a wide variety of isotope effects of…
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)…
We report the implementation of a multi-CPU and multi-GPU massively parallel platform dedicated to the explicit inclusion of nuclear quantum effects (NQEs) in the Tinker-HP molecular dynamics (MD) package. The platform, denoted Quantum-HP,…
It is known that quantum computers, if available, would allow an exponential decrease in the computational cost of quantum simulations. We extend this result to show that the computation of molecular properties (energy derivatives) could…
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…
Although liquid water is ubiquitous in chemical reactions at roots of life and climate on the earth, the prediction of its properties by high-level ab initio molecular dynamics simulations still represents a formidable task for quantum…
We demonstrate the accuracy and efficiency of a recently introduced approach to account for nuclear quantum effects (NQE) in molecular simulations: the adaptive Quantum Thermal Bath (adQTB). In this method, zero point energy is introduced…
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…
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…
The computational cost of exact methods for quantum simulation using classical computers grows exponentially with system size. As a consequence, these techniques can only be applied to small systems. By contrast, we demonstrate that quantum…