Reliable Prediction with Tuned Range-Separated Functionals of the Singlet-Triplet Gap in Organic Emitters for Thermally Activated Delayed Fluorescence (TADF)
KAUST DepartmentKAUST Solar Center (KSC)
Materials Science and Engineering Program
Physical Sciences and Engineering (PSE) Division
Permanent link to this recordhttp://hdl.handle.net/10754/559600
MetadataShow full item record
AbstractThe thermally activated delayed fluorescence (TADF) mechanism has recently attracted much interest in the field of organic light-emitting diodes (OLEDs). TADF relies on the presence of a very small energy gap between the lowest singlet and triplet excited states. Here, we demonstrate that time-dependent density functional theory (TD-DFT) in the Tamm-Dancoff Approximation can be very successful in the calculations of the lowest singlet and triplet excitation energies and the corresponding singlet-triplet gap when using nonempirically tuned range-separated functionals. Such functionals provide very good estimates in a series of 17 molecules used in TADF-based OLED devices, with mean absolute deviations of 0.15 eV for the vertical singlet excitation energies and 0.09 eV [0.07 eV] for the adiabatic [vertical] singlet-triplet energy gaps as well as low relative errors and high correlation coefficients compared to the corresponding experimental values. They significantly outperform conventional functionals, a feature which is rationalized on the basis of the amount of exact-exchange included and the delocalization error. The present work provides a reliable theoretical tool for the prediction and development of novel TADF-based materials with low singlet-triplet energetic splittings.
CitationReliable Prediction with Tuned Range-Separated Functionals of the Singlet-Triplet Gap in Organic Emitters for Thermally Activated Delayed Fluorescence (TADF) 2015:150709155133001 Journal of Chemical Theory and Computation
PublisherAmerican Chemical Society (ACS)
- Theoretical rationalization of the singlet-triplet gap in OLEDs materials: impact of charge-transfer character.
- Authors: Moral M, Muccioli L, Son WJ, Olivier Y, Sancho-García JC
- Issue date: 2015 Jan 13
- Dissecting the accountability of parameterized and parameter-free single-hybrid and double-hybrid functionals for photophysical properties of TADF-based OLEDs.
- Authors: Alipour M, Karimi N
- Issue date: 2017 Jun 21
- Impact of Dielectric Constant on the Singlet-Triplet Gap in Thermally Activated Delayed Fluorescence Materials.
- Authors: Sun H, Hu Z, Zhong C, Chen X, Sun Z, Brédas JL
- Issue date: 2017 Jun 1
- Kinetics of thermal-assisted delayed fluorescence in blue organic emitters with large singlet-triplet energy gap.
- Authors: Dias FB
- Issue date: 2015 Jun 28
- Triplet harvesting with 100% efficiency by way of thermally activated delayed fluorescence in charge transfer OLED emitters.
- Authors: Dias FB, Bourdakos KN, Jankus V, Moss KC, Kamtekar KT, Bhalla V, Santos J, Bryce MR, Monkman AP
- Issue date: 2013 Jul 19