Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion
We discuss the problem of electron transfer (ET) in mixed valence (MV) molecules that is at the core of molecular Quantum Cellular Automata (QCA) functioning. Theoretical modelling of tetrameric bi-electronic MV molecular square (prototype of basic QCA cell) is reported. The model involves interelec...
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| Format: | Article |
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MDPI AG
2022-08-01
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| Series: | Magnetochemistry |
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| Online Access: | https://www.mdpi.com/2312-7481/8/8/92 |
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| author | Andrew Palii Sergey Aldoshin Boris Tsukerblat |
| author_facet | Andrew Palii Sergey Aldoshin Boris Tsukerblat |
| author_sort | Andrew Palii |
| collection | DOAJ |
| description | We discuss the problem of electron transfer (ET) in mixed valence (MV) molecules that is at the core of molecular Quantum Cellular Automata (QCA) functioning. Theoretical modelling of tetrameric bi-electronic MV molecular square (prototype of basic QCA cell) is reported. The model involves interelectronic Coulomb repulsion, vibronic coupling and ET between the neighboring redox sites. Unlike the majority of previous studies in which molecular QCA have been analyzed only for particular case when the Coulomb repulsion energy significantly exceeds the ET energy, here we do not imply assumptions on the relative strength of these two interactions. Moreover, in the present work we go beyond the adiabatic semiclassical approximation often used in theoretical analysis of such systems in spite of the fact that this approximation ignores such an important phenomenon as quantum tunneling. By analyzing the electronic density distributions in the cells and the ell-cell response functions obtained from a quantum-mechanical solution of a complex multimode vibronic problem we have concluded that such key features of QCA cell as bistability and switchability can be achieved even under failure of the condition of strong Coulomb repulsion provided that the vibronic coupling is strong enough. We also show that the semiclassical description of the cell-cell response functions loses its accuracy in the region of strong non-linearity, while the quantum-mechanical approach provides correct results for this critically important region. |
| first_indexed | 2024-03-09T13:04:19Z |
| format | Article |
| id | doaj.art-fc4597eff5da429aa18a072257653aa3 |
| institution | Directory Open Access Journal |
| issn | 2312-7481 |
| language | English |
| last_indexed | 2024-03-09T13:04:19Z |
| publishDate | 2022-08-01 |
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| record_format | Article |
| series | Magnetochemistry |
| spelling | doaj.art-fc4597eff5da429aa18a072257653aa32023-11-30T21:51:30ZengMDPI AGMagnetochemistry2312-74812022-08-01889210.3390/magnetochemistry8080092Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb RepulsionAndrew Palii0Sergey Aldoshin1Boris Tsukerblat2Institute of Problems of Chemical Physics of Russian Academy of Sciences, 142432 Chernogolovka, RussiaInstitute of Problems of Chemical Physics of Russian Academy of Sciences, 142432 Chernogolovka, RussiaDepartment of Chemistry, Ben-Gurion University of the Negev, Beer-Sheva 84105, IsraelWe discuss the problem of electron transfer (ET) in mixed valence (MV) molecules that is at the core of molecular Quantum Cellular Automata (QCA) functioning. Theoretical modelling of tetrameric bi-electronic MV molecular square (prototype of basic QCA cell) is reported. The model involves interelectronic Coulomb repulsion, vibronic coupling and ET between the neighboring redox sites. Unlike the majority of previous studies in which molecular QCA have been analyzed only for particular case when the Coulomb repulsion energy significantly exceeds the ET energy, here we do not imply assumptions on the relative strength of these two interactions. Moreover, in the present work we go beyond the adiabatic semiclassical approximation often used in theoretical analysis of such systems in spite of the fact that this approximation ignores such an important phenomenon as quantum tunneling. By analyzing the electronic density distributions in the cells and the ell-cell response functions obtained from a quantum-mechanical solution of a complex multimode vibronic problem we have concluded that such key features of QCA cell as bistability and switchability can be achieved even under failure of the condition of strong Coulomb repulsion provided that the vibronic coupling is strong enough. We also show that the semiclassical description of the cell-cell response functions loses its accuracy in the region of strong non-linearity, while the quantum-mechanical approach provides correct results for this critically important region.https://www.mdpi.com/2312-7481/8/8/92quantum cellular automatacell-cell response functionmolecular cellmixed valence clusterselectron transferCoulomb repulsion |
| spellingShingle | Andrew Palii Sergey Aldoshin Boris Tsukerblat Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion Magnetochemistry quantum cellular automata cell-cell response function molecular cell mixed valence clusters electron transfer Coulomb repulsion |
| title | Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion |
| title_full | Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion |
| title_fullStr | Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion |
| title_full_unstemmed | Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion |
| title_short | Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion |
| title_sort | functional properties of tetrameric molecular cells for quantum cellular automata a quantum mechanical treatment extended to the range of arbitrary coulomb repulsion |
| topic | quantum cellular automata cell-cell response function molecular cell mixed valence clusters electron transfer Coulomb repulsion |
| url | https://www.mdpi.com/2312-7481/8/8/92 |
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