AI Article Synopsis
- Researchers examined how molecular conductance changes in a binuclear organometallic complex and its cation, previously studied at low voltages for Kondo resonance.
- They applied variational reduced density matrix theory to show strong multireference character, especially in the cation, and used two-electron reduced density matrix theory to analyze conductance in both forms.
- Results indicate that while there are some quantitative differences, both methods predict that the cation has favorable conductance due to its high density of states in low-lying excited states, consistent with experimental observations.
Article Abstract
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.
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| http://dx.doi.org/10.1021/acs.jpca.1c02267 | DOI Listing |
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