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Summary

Femtosecond charge transfer dynamics were studied in molecular frameworks. The charge transfer rate depends on the mediating molecular orbital, showing control is possible via resonant charge injection.

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Area of Science:

Molecular dynamics
Physical chemistry
Materials science

Background:

Understanding charge transfer (CT) is crucial for molecular electronics and energy applications.
Self-assembled monolayers (SAMs) offer tunable molecular architectures for studying charge transport.
Femtosecond spectroscopy provides insights into ultrafast charge dynamics.

Purpose of the Study:

To investigate the femtosecond charge transfer dynamics in SAMs with varying backbones.
To determine the influence of molecular orbital character on CT efficiency and rate.
To explore the potential for controlling CT through resonant charge injection.

Main Methods:

Utilized resonant Auger spectroscopy.
Employed the core hole clock method for time-resolved measurements.
Studied a series of SAMs with oligo(phenylenethynylene) and oligo(phenyl) backbones.

Main Results:

Characteristic charge transfer times were measured with femtosecond resolution.
CT times showed a strong dependence on the mediating molecular orbital's character.
Demonstrated a correlation between MO character and CT efficiency.

Conclusions:

The mediating molecular orbital significantly dictates charge transfer rates in molecular frameworks.
Resonant injection of charge carriers into specific molecular orbitals offers a pathway for controlling CT.
Findings have implications for designing efficient molecular electronic and energy transfer systems.