Conductance Switching in an Organometallic Single-Electron Transistor Using Current-Constrained Reduced-Density Matrix Theory
| Autor: | David A. Mazziotti, Manas Sajjan, Shayan Hemmatiyan |
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| Rok vydání: | 2021 |
| Předmět: |
010304 chemical physics
Condensed matter physics Electronic correlation Chemistry Conductance Coulomb blockade Electronic structure 010402 general chemistry 01 natural sciences Resonance (particle physics) 0104 chemical sciences Excited state 0103 physical sciences Molecular conductance Molecular orbital Physical and Theoretical Chemistry |
| Zdroj: | The Journal of Physical Chemistry A. 125:5448-5455 |
| ISSN: | 1520-5215 1089-5639 |
| DOI: | 10.1021/acs.jpca.1c02267 |
| Popis: | We report switching of molecular conductance at finite bias in a binuclear organometallic complex and its cation which were previously experimentally analyzed at low voltages to see the signature of Kondo resonance. The variational reduced density matrix theory is applied to show that the system is strongly multireferenced especially in its charged form. We also study the molecular conductance of both forms using recently developed current-constrained two-electron reduced density matrix theory which is capable of handling strong electronic correlation. We compare the results against an uncorrelated 1-electron reduced density matrix version of conductance calculations using Hartree-Fock molecular orbitals. We observe that despite quantitative disagreements, the qualitative trend in the conductance is correctly predicted to be favorable for the cationic partner by both methods. We explain the results using the inherently high density of states for the low-lying excited states in the cationic partner which is also replicable from uncorrelated electronic structure methods. Our results not only indicate that the low-bias conductance trend is maintained even beyond the Kondo regime and produces quantitative agreement with that of the experiment but also identifies important physical markers that are responsible for the high conductance of the charged species. |
| Databáze: | OpenAIRE |
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