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A Fast Transient Absorption Study of Co(AcAc)₃.

Luisa Ferrari¹, Mauro Satta², Amedeo Palma³

¹CNR-ISM, Division of Ultrafast Processes in Materials (FLASHit), Area della Ricerca di Roma Tor Vergata, Rome, Italy.

Frontiers in Chemistry

|June 6, 2019

Summary

Femtosecond transient absorption spectroscopy reveals ultrafast dynamics in Cobalt tris(acetylacetonate) (Co(AcAc)3) excited states. Intersystem crossing and internal conversion dominate de-excitation, with non-radiative decay limiting long-lived states for technological applications.

Keywords:

TDDFT (time-dependent density functional theory) calculations charge - transfer fast transient absorption femtosecand laser pulses metal complexes

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Area of Science:

Quantum Chemistry
Photochemistry
Materials Science

Background:

Transition metal coordination complexes are crucial for understanding quantum chemistry, including ligand field theory.
Studying excited-state dynamics of these complexes is vital for tailoring electronic properties for technological applications.

Purpose of the Study:

To investigate the excited-state dynamics of Cobalt tris(acetylacetonate) (Co(AcAc)3) in solution using femtosecond transient absorption spectroscopy.
To elucidate the de-excitation pathways and electronic properties of Co(AcAc)3 for potential technological uses.

Main Methods:

Femtosecond transient absorption spectroscopy was employed to probe ultrafast excited-state dynamics.
Density functional theory (DFT) combined with the polarizable continuum model (PCM) was used for geometric and electronic state characterization.
Time-dependent density functional theory (TD-DFT) calculations were performed to analyze excited states and spin-orbit coupling.

Main Results:

Ligand to metal charge transfer excitation showed biphasic dynamics with an ultrafast rise (0.07 ± 0.04 ps) and decay (1.5 ± 0.3 ps).
Ligand field excitation dynamics exhibited similar rise (0.07 ± 0.04 ps) and decay (1.8 ± 0.3 ps) times.
Calculations suggest ultrafast rise is due to intersystem crossing, and picosecond decay is attributed to internal conversion within the triplet state manifold.

Conclusions:

The observed ultrafast dynamics in Co(AcAc)3 are significantly influenced by intersystem crossing and internal conversion processes.
Non-radiative decay pathways are dominant, preventing the formation of long-lived excited states (>5 ps).
Understanding these dynamics is key for designing cobalt coordination complexes with tailored electronic properties for advanced applications.