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Negative Differential Resistance in Spin-Crossover Molecular Devices

Abstract : We demonstrate, based on low-temperature scanning tunneling microscopy (STM) and spectroscopy, a pronounced negative differential resistance (NDR) in spin-crossover (SCO) molecular devices, where a Fe II SCO molecule is deposited on surfaces. The STM measurements reveal that the NDR is robust with respect to substrate materials, temperature, and the number of SCO layers. This indicates that the NDR is intrinsically related to the electronic structure of the SCO molecule. Experimental results are supported by density functional theory (DFT) with non-equilibrium Green's functions (NEGF) calculations and a generic theoretical model. While the DFT+NEGF calculations reproduce NDR for a special atomically-sharp STM tip, the effect is attributed to the energy-dependent tip density of states rather than the molecule itself. We, therefore, propose a Coulomb blockade model involving three molecular orbitals with very different spatial localization as suggested by the molecular electronic structure.
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https://hal.archives-ouvertes.fr/hal-03748764
Contributor : Dongzhe Li Connect in order to contact the contributor
Submitted on : Wednesday, August 10, 2022 - 6:08:45 AM
Last modification on : Friday, August 12, 2022 - 3:40:43 AM

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Dongzhe Li, Yongfeng Tong, Kaushik Bairagi, Massine Kelai, Yannick J Dappe, et al.. Negative Differential Resistance in Spin-Crossover Molecular Devices. Journal of Physical Chemistry Letters, American Chemical Society, 2022, 13, pp.7514-7520. ⟨10.1021/acs.jpclett.2c01934⟩. ⟨hal-03748764⟩

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