Ab initio molecular dynamics on quantum computers

Fedorov, Dmitry A.; Otten, Matthew J.; Gray, Stephen K.; Alexeev, Yuri

doi:10.1063/5.0046930

Ab initio molecular dynamics on quantum computers

Journal Article · Fri Apr 23 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0046930· OSTI ID:1798042

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Oak Ridge Associated Univ., Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Ab initio molecular dynamics (AIMD) is a valuable technique for studying molecules and materials at finite temperatures where the nuclei evolve on potential energy surfaces obtained from accurate electronic structure calculations. In this work, we present an approach to running AIMD simulations on noisy intermediate-scale quantum (NISQ)-era quantum computers. The electronic energies are calculated on a quantum computer using the variational quantum eigensolver (VQE) method. Algorithms for computation of analytical gradients entirely on a quantum computer require quantum fault-tolerant hardware, which is beyond NISQ-era. Therefore, we compute the energy gradients numerically using finite differences, the Hellmann-Feynman theorem, and a correlated sampling technique. This method only requires additional classical calculations of electron integrals for each degree of freedom without any additional computations on a quantum computer beyond the initial VQE run. As a proof of concept, AIMD simulations are demonstrated for the H-2 molecule on IBM quantum devices. In addition, we demonstrate the validity of the method for larger molecules using full configuration interaction wave functions. As quantum hardware and noise mitigation techniques continue to improve, the method can be utilized for studying larger molecular systems.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Fusion Energy Sciences (FES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1798042

Alternate ID(s):: OSTI ID: 1780355

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 16 Vol. 154; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Ab-initio molecular dynamics
Active noise control
Computer simulation
Electronic structure methods
Full configuration interaction
Hellmann Feynman theorem
Potential energy surfaces
Quantum computing
Quantum measurement theory
Stochastic processes

Ab initio molecular dynamics on quantum computers

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