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Vibronic recovering of functionality of quantum cellular automata based on bi-dimeric square cells with violated condition of strong Coulomb repulsionстатья
Статья опубликована в высокорейтинговом журнале
Статья опубликована в журнале из списка Web of Science и/или Scopus- Авторы: Tsukerblat Boris, Palii Andrew, Zilberg Shmuel, Korchagin Denis, Aldoshin Sergey, Clemente-Juan Juan Modesto
- Журнал: Journal of Chemical Physics
- Том: 157
- Номер: 7
- Год издания: 2022
- Издательство: AIP Publishing
- Местоположение издательства: United States
- Первая страница: 074308
- DOI: 10.1063/5.0096182
- Аннотация: Strong Coulomb repulsion between the two charges in a square planar mixed-valence cell in quantum cellular automata (QCA) allows us toencode the binary information in the two energetically beneficial diagonal distributions of the electronic density. In this article, we pose aquestion: to what extent is this condition obligatory for the design of the molecular cell? To answer this question, we examine the ability touse a square-planar cell composed of one-electron mixed valence dimers to function in QCA in a general case when the intracell Coulombinteraction U is not supposed to be extremely strong, which means that it is comparable with the characteristic electron transfer energy (violatedstrong U limit). Using the two-mode vibronic model treated within the semiclassical (adiabatic) and quantum-mechanical approaches,we demonstrate that strong vibronic coupling is able to create a considerable barrier between the two diagonal-type charge configurations,thus ensuring bistability and polarizability of the cells even if the Coulomb barrier is not sufficient. The cases of weak and moderate Coulombrepulsion and strong vibronic coupling are exemplified by consideration of the cation radicals of the two polycyclic derivatives of norbornadiene[C12H12]+and [C17H16]+ with the terminal C=C chromophores playing the role of redox sites. By using the detailed ab initio data,we reveal the main characteristics of the bi-dimeric cells composed of these molecules and illustrate the pronounced effect of the vibronicrecovery clearly manifesting itself in the shape of the cell–cell response function. Revealing such “vibronic recovery” of strong localizationwhen the strong U limit is violated suggests a way to a significant expansion of the class of molecular systems suitable as QCA cells.
- Добавил в систему: Алдошин Сергей Михайлович