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Related Experiment Video

Updated: Jul 26, 2025

All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics
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Single-molecule photoelectron tunnelling spectroscopy.

Haojie Liu1, Lijue Chen1, Hao Zhang1

  • 1State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering & Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen University, Xiamen, China.

Nature Materials
|June 22, 2023
PubMed
Summary
This summary is machine-generated.

We developed a novel single-molecule photoelectron tunnelling spectroscopy technique to map charge transport beyond the highest occupied molecular orbital-lowest unoccupied molecular orbital gap. This method reveals resonant transport channels and their electric field modulation in molecular junctions.

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Area of Science:

  • Molecular electronics
  • Charge transport phenomena
  • Spectroscopic techniques

Background:

  • Understanding charge transport in molecular junctions is crucial for developing advanced molecular devices.
  • Existing methods often struggle to map transmission beyond the highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap.
  • Characterizing energy-dependent transport properties requires advanced experimental approaches.

Purpose of the Study:

  • To develop and demonstrate a single-molecule photoelectron tunnelling spectroscopy (SM-PETS) approach for mapping transmission beyond the HOMO-LUMO gap.
  • To investigate charge transport through a single diketopyrrolopyrrole molecule junction at room temperature.
  • To quantitatively assess the influence of electric fields on frontier molecular orbitals.

Main Methods:

  • Utilized an ultrafast-laser combined scanning tunnelling microscope-based break junction setup.
  • Employed single-molecule photoelectron tunnelling spectroscopy to probe transmission pathways.
  • Performed density functional theory (DFT) calculations to determine transmission spectra.

Main Results:

  • Identified two resonant transport channels in ultrafast photocurrent, ranging from 1.31 eV to 1.77 eV.
  • These channels correspond to the LUMO+1 and LUMO+2 energy levels, aligning with DFT predictions.
  • Demonstrated the modulation of resonant peaks by varying bias voltages, enabling quantitative electric field effect characterization.

Conclusions:

  • The developed SM-PETS technique successfully maps transmission beyond the HOMO-LUMO gap in single-molecule junctions.
  • This method provides insights into energy-dependent charge transport and the impact of electric fields on molecular orbitals.
  • SM-PETS offers a powerful new avenue for exploring charge transport mechanisms in molecular systems.