Issue 28, 2014

Predicting phosphorescent lifetimes and zero-field splitting of organometallic complexes with time-dependent density functional theory including spin–orbit coupling

Abstract

The (photo)physical properties of organometallic complexes are crucially affected by relativistic effects. In a non- or scalar-relativistic picture, triplet states are threefold degenerate. Spin–orbit coupling lifts this degeneracy (zero-field splitting, ZFS) and enables phosphorescence from the three triplet-like states to the ground state. The fine structure and radiative lifetimes of phosphorescent organometallic complexes are important properties for designing efficient organic light-emitting diodes (OLEDs). Here we show that experimental ZFSs and phosphorescent lifetimes for a large variety of organometallic complexes are well reproduced by self-consistent spin–orbit coupling TDDFT (SOC-TDDFT) calculations with a continuum solvation model. By comparing with perturbative SOC-TDDFT and gas phase calculations, we find that both full spin–orbit and solvation effects are important for the predicted properties. SOC-TDDFT is thus shown to be a useful predictive tool for the rational design of phosphors in OLEDs and other optoelectronic devices.

Graphical abstract: Predicting phosphorescent lifetimes and zero-field splitting of organometallic complexes with time-dependent density functional theory including spin–orbit coupling

Supplementary files

Article information

Article type
Paper
Submitted
24 Dec 2013
Accepted
11 Mar 2014
First published
12 Mar 2014

Phys. Chem. Chem. Phys., 2014,16, 14523-14530

Author version available

Predicting phosphorescent lifetimes and zero-field splitting of organometallic complexes with time-dependent density functional theory including spin–orbit coupling

K. Mori, T. P. M. Goumans, E. van Lenthe and F. Wang, Phys. Chem. Chem. Phys., 2014, 16, 14523 DOI: 10.1039/C3CP55438D

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