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Negative Differential Resistance in Spin-Crossover Molecular Devices.

Dongzhe Li1,2, Yongfeng Tong3, Kaushik Bairagi3

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We observed negative differential resistance (NDR) in spin-crossover (SCO) molecular devices. This electronic behavior is intrinsic to the SCO molecule

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Area of Science:

  • Molecular electronics
  • Quantum phenomena
  • Surface science

Background:

  • Spin-crossover (SCO) molecules exhibit tunable electronic properties.
  • Negative differential resistance (NDR) is a key characteristic for molecular electronic devices.
  • Understanding molecular electronic behavior requires advanced experimental and theoretical approaches.

Purpose of the Study:

  • To investigate the origin of negative differential resistance (NDR) in spin-crossover (SCO) molecular devices.
  • To determine if NDR is an intrinsic property of the SCO molecule or influenced by experimental conditions.
  • To elucidate the electronic structure responsible for NDR in SCO systems.

Main Methods:

  • Low-temperature scanning tunneling microscopy (STM) and spectroscopy were employed.
  • Density functional theory (DFT) combined with nonequilibrium Green's function (NEGF) calculations were performed.
  • A generic theoretical model was developed to interpret experimental findings.

Main Results:

  • A pronounced NDR was observed in Fe(II) SCO molecules on surfaces.
  • The NDR was found to be robust across different substrates, temperatures, and SCO layer numbers.
  • DFT+NEGF calculations suggested NDR could be tip-dependent, but experimental evidence points to molecular origin.

Conclusions:

  • The observed NDR is intrinsically linked to the electronic structure of the SCO molecule.
  • A Coulomb blockade model involving three distinct molecular orbitals explains the NDR phenomenon.
  • This work provides fundamental insights into SCO molecular devices and their electronic properties.