Interface states, negative differential resistance, and rectification in molecular junctions with transition-metal contacts
Bibliographic record
Abstract
We present a theory of nonlinear transport phenomena in molecular junctions where single thiolated organic molecules bridge transition metal nanocontacts whose densities of states have strong $d$ orbital components near the Fermi level. At moderate bias, we find electron transmission between the contacts to be mediated by interface states within the molecular highest-occupied-molecular-orbital--lowest-unoccupied-molecular-orbital gap that arise from hybridization between the thiol-terminated ends of the molecules and the $d$ orbitals of the transition metals. Because these interface states are localized mainly within the metal electrodes, we find their energies to accurately track the electrochemical potentials of the contacts when a variable bias is applied across the junction. We predict resonant enhancement and reduction of the interface state transmission as the applied bias is varied, resulting in negative differential resistance (NDR) in molecular junctions with Pd nanocontacts. We show that these nonlinear phenomena can be tailored by suitably choosing the nanocontact materials: If a Rh electrode is substituted for one Pd contact, we predict enhancement of these NDR effects. The same mechanism is also predicted to give rise to rectification in Pd/molecule/Au junctions. The dependences of the interface state resonances on the orientation of the metal interface, the adsorption site of the molecule, and the separation between the thiolated ends of the molecule and the metal contacts are also discussed.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".