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Exciplex Stabilization in Asymmetric Acene Dimers.

Rachel A Krueger, Guillaume Blanquart

The Journal of Physical Chemistry. A

|February 12, 2019

Summary

Researchers calculated binding energies for mixed exciplexes of small acenes. Benzene-naphthalene and naphthalene-anthracene exciplexes showed moderate stabilization due to charge transfer and exciton delocalization.

Area of Science:

Photochemistry
Computational Chemistry
Spectroscopy

Background:

Excimers are crucial in photochemical processes like singlet fission and DNA damage.
Exciplex formation in mixed chromophore systems yields distinct spectral characteristics.
Understanding exciplexes informs about aggregate formation and chromophore orientation.

Purpose of the Study:

To predict aggregation effects in mixed small acene systems.
To calculate binding energies and minimum-energy geometries for mixed S1 exciplexes.
To evaluate the performance of time-dependent density functional theory (TDDFT) functionals for exciplex calculations.

Main Methods:

Utilized CASSCF/NEVPT2 multireference calculations for benchmark binding energies.
Employed TDDFT calculations with various exchange-correlation functionals.

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Investigated mixed exciplexes involving benzene, naphthalene, and anthracene.

Main Results:

Reported benchmark binding energies for benzene-naphthalene (18.2 kJ/mol), benzene-anthracene (27.7 kJ/mol), and naphthalene-anthracene (49.3 kJ/mol) exciplexes.
Observed inconsistent performance of TDDFT functionals, with errors dependent on monomer excitation character.
Found moderate exciplex stabilization in benzene-naphthalene and naphthalene-anthracene systems.

Conclusions:

Mixed exciplex stabilization arises from a combination of charge transfer and exciton delocalization.
TDDFT accuracy for exciplexes is sensitive to the chosen functional and monomer excitation.
Computational methods are valuable for predicting exciplex behavior in complex molecular systems.