Exploring the write-in process in molecular quantum cellular automata: A combined modelingand first-principle approach
Research output: Contribution to journal › Research article › Contributed › peer-review
Contributors
Abstract
The molecular quantum cellular automata paradigm (m-QCA) offers a promising alternative framework to current CMOS implementations. A crucial aspect for implementing this technology concerns the construction of a device which effectively controls intramolecular charge-transfer processes. Tentative experimental implementations have been developed in which a voltage drop is created generating the forces that drive a molecule into a logic state. However, important factors such as the electric field profile, its possible time-dependency and the influence of temperature in the overall success of charge-transfer are relevant issues to be considered in the design of a reliable device. In this work, we theoretically study the role played by these processes in the overall intramolecular charge-transfer process. We have used a Landau-Zener (LZ) model, where different time-dependent electric field profiles have been simulated. The results have been further corroborated employing density functional tight-binding method. The role played by the nuclear motions in the electron-transfer process has been investigated beyond the Born-Oppenheimer approximation by computing the effect of the external electric field in the behavior of the potential energy surface. Hence, we demonstrate that the intramolecular charge-transfer process is a direct consequence of the coherent LZ nonadiabatic tunneling and the hybridization of the diabatic vibronic states which effectively reduces the trapping of the itinerant electron at the donor group.
Details
| Original language | English |
|---|---|
| Article number | 405502 |
| Journal | Journal of Physics Condensed Matter |
| Volume | 31 |
| Issue number | 40 |
| Publication status | Published - Jun 2019 |
| Peer-reviewed | Yes |
External IDs
| PubMed | 31195387 |
|---|---|
| ORCID | /0000-0001-8121-8041/work/142240855 |
| ORCID | /0000-0002-7673-3142/work/181861224 |
| ORCID | /0000-0002-6574-7848/work/211720285 |
Keywords
ASJC Scopus subject areas
Keywords
- charge transfer, density functional tight binding (DFTB), non-adiabatic coupling, quantum cellular automata