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We present a novel route to constructing cost-efficient semi-empirical approximations for the non-additive kinetic energy in subsystem density functional theory. The developed methodology is based on the use of Slater determinants composed…

Chemical Physics · Physics 2025-01-13 Larissa Sophie Eitelhuber , Denis G. Artiukhin

We present a simple and efficient method to optimize within energy minimization the determinantal component of the many-body wave functions commonly used in quantum Monte Carlo calculations. The approach obtains the optimal wave function as…

Other Condensed Matter · Physics 2009-11-11 Anthony Scemama , Claudia Filippi

We propose a method to optimize the multi-Slater determinants of the antisymmetrized molecular dynamics (AMD) in the linear combination form and apply it to the neutron-rich $^{10}$Be nucleus. The individual Slater determinants and their…

Nuclear Theory · Physics 2024-01-29 Takayuki Myo , Mengjiao Lyu , Qing Zhao , Masahiro Isaka , Niu Wan , Hiroki Takemoto , Hisashi Horiuchi

Classical optimization is a cornerstone of the success of variational quantum algorithms, which often require determining the derivatives of the cost function relative to variational parameters. The computation of the cost function and its…

Quantum Physics · Physics 2025-07-15 Muhammad Umer , Eleftherios Mastorakis , Dimitris G. Angelakis

In this work we propose a novel composite method for accurate calculation of the energies of many-electron atoms. The dominant contribution to the energy (pair energies) are calculated by using explicitly correlated factorisable coupled…

Atomic Physics · Physics 2018-12-12 Michal Przybytek , Michal Lesiuk

The performance of quantum algorithms for eigenvalue problems, such as computing Hamiltonian spectra, depends strongly on the overlap of the initial wavefunction and the target eigenvector. In a basis of Slater determinants, the…

Quantum Physics · Physics 2025-03-03 Daniel Marti-Dafcik , Hugh G. A. Burton , David P. Tew

In electronic structure theory, variational methods offer a valuable paradigm for approximating electronic ground states. However, for historical reasons, this principle is mostly restricted to model chemistries in pre-defined fixed basis…

Quantum Physics · Physics 2025-11-17 Fabian Langkabel , Stefan Knecht , Jakob S. Kottmann

Classical algorithms for predicting the equilibrium geometry of strongly correlated molecules require expensive wave function methods that become impractical already for few-atom systems. In this work, we introduce a variational quantum…

A one-electron Schroedinger equation based on special one-electron potentials for atoms is shown to exist that produces orbitals for an arbitrary molecule that are sufficiently accurate to be used without modification to construct single-…

Chemical Physics · Physics 2022-05-16 Jerry L. Whitten

Quantum computation is one of the most promising new paradigms for the simulation of physical systems composed of electrons and atomic nuclei, with applications in chemistry, solid-state physics, materials science, and molecular biology.…

Quantum Physics · Physics 2024-11-05 Jakob Günther , Alberto Baiardi , Markus Reiher , Matthias Christandl

We introduce an algorithm that can be used to perform stochastic perturbation theory (sPT) to correct any non-linearly parametrized wavefunction that can be optimized using orbital space Variational Monte Carlo (VMC). Although the…

Strongly Correlated Electrons · Physics 2018-03-13 Sandeep Sharma

Electronic structure simulation is an anticipated application for quantum computers. Due to high-dimensional quantum entanglement in strongly correlated systems, the quantum resources required to perform such simulations are far beyond the…

Quantum Physics · Physics 2022-01-25 Jie Liu , Zhenyu Li , Jinlong Yang

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…

Quantum Physics · Physics 2022-04-06 Utkarsh Azad , Harjinder Singh

Energy spectroscopy is a powerful tool with diverse applications across various disciplines. The advent of programmable digital quantum simulators opens new possibilities for conducting spectroscopy on various models using a single device.…

We present an improved formalism for quantum Monte Carlo calculations of energy derivatives and properties (e.g. the interatomic forces), with a multideterminant Jastrow-Slater function. As a function of the number $N_e$ of Slater…

Chemical Physics · Physics 2017-06-26 Roland Assaraf , Saverio Moroni , Claudia Filippi

Variational and perturbative relativistic energies are computed and compared for two-electron atoms and molecules with low nuclear charge numbers. In general, good agreement of the two approaches is observed. Remaining deviations can be…

Chemical Physics · Physics 2022-09-21 Dávid Ferenc , Péter Jeszenszki , Edit Mátyus

It has been well established that the Jastrow correlation factor can effectively capture the electron correlation effects, and thus, the efficient optimization of the many-body wave function including the Jastrow correlation factor is of…

Atomic Physics · Physics 2023-09-12 Masayuki Ochi

The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

We present a basis-set-free approach to the variational quantum eigensolver using an adaptive representation of the spatial part of molecular wavefunctions. Our approach directly determines system-specific representations of qubit…

Quantum Physics · Physics 2021-01-05 Jakob S. Kottmann , Philipp Schleich , Teresa Tamayo-Mendoza , Alán Aspuru-Guzik

The accurate computation of properties of large molecular systems is classically infeasible and is one of the applications in which it is hoped that quantum computers will demonstrate an advantage over classical devices. However, due to the…

Quantum Physics · Physics 2024-10-15 Michael A. Jones , Harish J. Vallury , Lloyd C. L. Hollenberg