We formulate and implement the Variational Quantum Eigensolver Self Consistent Field (VQE-SCF) algorithm in combination with polarizable embedding (PE), thereby extending PE to the regime of quantum computing. We test the resulting algorithm, PE-VQE-SCF, on quantum simulators and demonstrate that the computational stress on the quantum device is only slightly increased in terms of gate counts compared to regular VQE-SCF. On the other hand, no increase in shot noise was observed. We illustrate how PE-VQE-SCF may lead to the modeling of real chemical systems using a simulation of the reaction barrier of the Diels-Alder reaction between furan and ethene as an example.
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http://dx.doi.org/10.1063/5.0190594 | DOI Listing |
J Phys Chem Lett
January 2025
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Criegee intermediates (CIs) are potentially significant oxidants and a major source of OH radicals in the troposphere. The -CHCHOO intermediate has been confirmed as a crucial component of CIs in the atmospheric environment. Although previous studies have provided some experimental and theoretical rate constants, inconsistencies among these data remain, and the experimental data do not cover the full range of temperatures present in the troposphere.
View Article and Find Full Text PDFNPJ Comput Mater
December 2024
Department of Chemistry, University of Zurich, Winterthurerstrasse 190, Zurich, 8057 Switzerland.
We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by presenting a specific implementation of periodic range-separated DFT coupled to a quantum circuit ansatz, whereby the variational quantum eigensolver and the quantum equation-of-motion algorithm are used to obtain the low-lying spectrum of the embedded fragment Hamiltonian. The application of this scheme to study localized electronic states in materials is showcased through the accurate prediction of the optical properties of the neutral oxygen vacancy in magnesium oxide (MgO).
View Article and Find Full Text PDFACS Photonics
December 2024
SUPA, School of Physics and Astronomy, University of St Andrews, St Andrews KY16 9SS, U.K.
We derive the transition rates, dephasing rates, and Lamb shifts for a system consisting of many molecules collectively coupled to a resonant cavity mode. Using a variational polaron master equation, we show that strong vibrational interactions inherent to molecules give rise to multi-phonon processes and suppress the light-matter coupling. In the strong light-matter coupling limit, multiphonon contributions to the transition and dephasing rates strongly dominate over single-phonon contributions for typical molecular parameters.
View Article and Find Full Text PDFChem Sci
January 2025
Faculty of Chemistry, Institute of Theoretical Chemistry, Universität Wien A-1090 Vienna Austria
Recent developments in quantum computing are highly promising, particularly in the realm of quantum chemistry. Due to the noisy nature of currently available quantum hardware, hybrid quantum-classical algorithms have emerged as a reliable option for near-term simulations. Mixed quantum-classical dynamics methods effectively capture nonadiabatic effects by integrating classical nuclear dynamics with quantum chemical computations of the electronic properties.
View Article and Find Full Text PDFSci Adv
December 2024
Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY 14853, USA.
De novo peptide design exhibits great potential in materials engineering, particularly for the use of plastic-binding peptides to help remediate microplastic pollution. There are no known peptide binders for many plastics-a gap that can be filled with de novo design. Current computational methods for peptide design exhibit limitations in sampling and scaling that could be addressed with quantum computing.
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