Electron-Phonon Coupling in Current-Driven Single-Molecule Junctions.
J Am Chem Soc
; 142(7): 3384-3391, 2020 Feb 19.
Article
en En
| MEDLINE
| ID: mdl-32070107
ABSTRACT
Vibrational excitations provoked by coupling effects during charge transport through single molecules are intrinsic energy dissipation phenomena, in close analogy to electron-phonon coupling in solids. One fundamental challenge in molecular electronics is the quantitative determination of charge-vibrational (electron-phonon) coupling for single-molecule junctions. The ability to record electron-phonon coupling phenomena at the single-molecule level is a key prerequisite to fully rationalize and optimize charge-transport efficiencies for specific molecular configurations and currents. Here we exemplarily determine the pertaining coupling characteristics for a current-carrying chemically well-defined molecule by synchronous vibrational and current-voltage spectroscopy. These metal-molecule-metal junction insights are complemented by time-resolved infrared spectroscopy to assess the intramolecular vibrational relaxation dynamics. By measuring and analyzing the steady-state vibrational distribution during transient charge transport in a bis-phenylethynyl-anthracene derivative using anti-Stokes Raman scattering, we find â¼0.5 vibrational excitations per elementary charge passing through the metal-molecule-metal junction, by means of a rate model ansatz and quantum-chemical calculations.
Texto completo:
1
Bases de datos:
MEDLINE
Tipo de estudio:
Prognostic_studies
Idioma:
En
Revista:
J Am Chem Soc
Año:
2020
Tipo del documento:
Article
País de afiliación:
Alemania