Beyond Marcus theory and the Landauer–Büttiker approach in molecular junctions. II. A self-consistent Born approach
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- Jakub K. Sowa
- Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA
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- Neill Lambert
- Theoretical Quantum Physics Laboratory, RIKEN Cluster for Pioneering Research 3 , Wako-shi, Saitama 351-0198, Japan
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- Tamar Seideman
- Department of Chemistry, Northwestern University 1 , Evanston, Illinois 60208, USA
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- Erik M. Gauger
- SUPA, Institute of Photonics and Quantum Sciences, Heriot-Watt University 4 , Edinburgh EH14 4AS, United Kingdom
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説明
<jats:p>Marcus and Landauer–Büttiker approaches to charge transport through molecular junctions describe two contrasting mechanisms of electronic conduction. In previous work, we have shown how these charge transport theories can be unified in the single-level case by incorporating lifetime broadening into the second-order quantum master equation. Here, we extend our previous treatment by incorporating lifetime broadening in the spirit of the self-consistent Born approximation. By comparing both theories to numerically converged hierarchical-equations-of-motion results, we demonstrate that our novel self-consistent approach rectifies shortcomings of our earlier framework, which are present especially in the case of relatively strong electron–vibrational coupling. We also discuss circumstances under which the theory developed here simplifies to the generalized theory developed in our earlier work. Finally, by considering the high-temperature limit of our new self-consistent treatment, we show how lifetime broadening can also be self-consistently incorporated into Marcus theory. Overall, we demonstrate that the self-consistent approach constitutes a more accurate description of molecular conduction while retaining most of the conceptual simplicity of our earlier framework.</jats:p>
収録刊行物
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- The Journal of Chemical Physics
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The Journal of Chemical Physics 152 (6), 2020-02-10
AIP Publishing
