Academic Journal
Toward Accurate Post-Born–Oppenheimer Molecular Simulations on Quantum Computers: An Adaptive Variational Eigensolver with Nuclear-Electronic Frozen Natural Orbitals
| العنوان: | Toward Accurate Post-Born–Oppenheimer Molecular Simulations on Quantum Computers: An Adaptive Variational Eigensolver with Nuclear-Electronic Frozen Natural Orbitals |
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| المؤلفون: | Anton Nykänen, Aaron Miller, Walter Talarico, Stefan Knecht, Arseny Kovyrshin, Mårten Skogh, Lars Tornberg, Anders Broo, Stefano Mensa, Benjamin C. B. Symons, Emre Sahin, Jason Crain, Ivano Tavernelli, Fabijan Pavošević |
| سنة النشر: | 2023 |
| مصطلحات موضوعية: | Physiology, Biotechnology, Space Science, Biological Sciences not elsewhere classified, Mathematical Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Information Systems not elsewhere classified, toward accurate post, smallest systems described, hydrogen tunneling play, adaptive variational eigensolver, term quantum devices, current quantum devices, frozen natural orbital, sophisticated basis sets, minimal basis sets, quantum computers offer, cnot gate count, capture isotope effects, 2 , vqe method reduces, neo method , quantum computers, cnot count, vqe method, electronic orbital, classical computers, system size, several orders, resources required |
| الوصف: | Nuclear quantum effects such as zero-point energy and hydrogen tunneling play a central role in many biological and chemical processes. The nuclear-electronic orbital (NEO) approach captures these effects by treating selected nuclei quantum mechanically on the same footing as electrons. On classical computers, the resources required for an exact solution of NEO-based models grow exponentially with system size. By contrast, quantum computers offer a means of solving this problem with polynomial scaling. However, due to the limitations of current quantum devices, NEO simulations are confined to the smallest systems described by minimal basis sets, whereas realistic simulations beyond the Born–Oppenheimer approximation require more sophisticated basis sets. For this purpose, we herein extend a hardware-efficient ADAPT-VQE method to the NEO framework in the frozen natural orbital (FNO) basis. We demonstrate on H 2 and D 2 molecules that the NEO-FNO-ADAPT-VQE method reduces the CNOT count by several orders of magnitude relative to the NEO unitary coupled cluster method with singles and doubles while maintaining the desired accuracy. This extreme reduction in the CNOT gate count is sufficient to permit practical computations employing the NEO methodan important step toward accurate simulations involving nonclassical nuclei and non-Born–Oppenheimer effects on near-term quantum devices. We further show that the method can capture isotope effects, and we demonstrate that inclusion of correlation energy systematically improves the prediction of difference in the zero-point energy (ΔZPE) between isotopes. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | unknown |
| Relation: | https://figshare.com/articles/journal_contribution/Toward_Accurate_Post-Born_Oppenheimer_Molecular_Simulations_on_Quantum_Computers_An_Adaptive_Variational_Eigensolver_with_Nuclear-Electronic_Frozen_Natural_Orbitals/24791699 |
| DOI: | 10.1021/acs.jctc.3c01091.s001 |
| الاتاحة: | https://doi.org/10.1021/acs.jctc.3c01091.s001 https://figshare.com/articles/journal_contribution/Toward_Accurate_Post-Born_Oppenheimer_Molecular_Simulations_on_Quantum_Computers_An_Adaptive_Variational_Eigensolver_with_Nuclear-Electronic_Frozen_Natural_Orbitals/24791699 |
| Rights: | CC BY-NC 4.0 |
| رقم الانضمام: | edsbas.78B0CF07 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1021/acs.jctc.3c01091.s001 |
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