4.8 Article

Vibrational Frequency Used as Internal Clock Reference to Access Molecule-Metal Charge-Transfer Times

Journal

PHYSICAL REVIEW LETTERS
Volume 126, Issue 11, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.126.116801

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Funding

  1. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [223848855-SFB 1083]

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The dynamical charge transfer processes at molecule-metal interfaces, occurring on a few femtosecond timescale, can be accessed through vibrational excitations, with the characteristic timescale derived using the vibrational oscillation period as an internal clock reference.
Dynamical charge transfer processes at molecule-metal interfaces proceed in the few fs timescale that renders them highly relevant to electronic excitations in optoelectronic devices. Yet, knowledge thereof is limited when electronic ground state situations are considered that implicate charge transfer directly at the fermi energy. Here we show that such processes can be accessed by means of vibrational excitations, with nonadiabatic electron-vibron coupling leading to distinct asymmetric line shapes. Thereby the characteristic timescale of this interfacial dynamical charge transfer can be derived by using the vibrational oscillation period as an internal clock reference.

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