rISC - the game of strategic molecular design for high efficiency OLEDs
Lead Research Organisation:
Newcastle University
Department Name: Sch of Natural & Environmental Sciences
Abstract
Abstracts are not currently available in GtR for all funded research. This is normally because the abstract was not required at the time of proposal submission, but may be because it included sensitive information such as personal details.
Organisations
People |
ORCID iD |
| Thomas Penfold (Principal Investigator) |
Publications
Ahmad S
(2022)
Rapid predictions of the colour purity of luminescent organic molecules
in Journal of Materials Chemistry C
El-Zubir O
(2022)
Circularly polarised luminescence in an RNA-based homochiral, self-repairing, coordination polymer hydrogel.
in Journal of materials chemistry. C
Giret Y
(2021)
A quantum dynamics study of the hyperfluorescence mechanism
in Journal of Materials Chemistry C
Gu Q
(2022)
Excited-State Lifetime Modulation by Twisted and Tilted Molecular Design in Carbene-Metal-Amide Photoemitters.
in Chemistry of materials : a publication of the American Chemical Society
L. Dos Santos P
(2022)
Fine-Tuning the Photophysics of Donor-Acceptor (D-A 3 ) Thermally Activated Delayed Fluorescence Emitters Using Isomerisation
in ChemPhotoChem
Laidlaw B
(2021)
On the factors influencing the chiroptical response of conjugated polymer thin films.
in Chemical communications (Cambridge, England)
Pander P
(2021)
Exceptionally fast radiative decay of a dinuclear platinum complex through thermally activated delayed fluorescence.
in Chemical science
Penfold T
(2022)
Tailoring Donor-Acceptor Emitters to Minimise Localisation Induced Quenching of Thermally Activated Delayed Fluorescence
in ChemPhotoChem
Penfold TJ
(2023)
Mind the GAP: quantifying the breakdown of the linear vibronic coupling Hamiltonian.
in Physical chemistry chemical physics : PCCP
Pope T
(2023)
Modelling the effect of dipole ordering on charge-carrier mobility in organic semiconductors
in Organic Electronics
| Description | Through a new conceptual design of Thermally Activated Delayed Fluorescence (TADF) molecules, we have shown that it is possible to achieve both a reverse intersystem crossing (rISC) rate > 1x10^7 s-1 and a unity photoluminescence quantum yield (PLQY), a combination previously considered untenable. The difference in this new material is the high density of coupled excited states which enhances rISC through a spin-vibronic coupling mechanism. However, despite the rapid rISC this emitter is far from optimal and we have recently identified excited state conformational dynamics responsible for slower secondary channels, giving poor roll-off performance and degradation of the emitter. Our results to date have demonstrated the key molecular factors which control the conformational dynamics responsible for slower secondary channels. This has been published [https://doi.org/10.1002/cptc.202200243] and current work in this area is focusing on developing new materials which minimise these factors and increase the performance of the TADF molecules while ensuring emission occurs in the important blue region of the spectrum. In terms of controlling the conformational dynamics, we have also shown that non-covalent interactions can manipulate the excited state dynamics controlling the TADF properties. We are presently refining these simulations and seeking to synthesise the molecules to demonstrate experimentally. Finally, in OLEDS, the outcome of excited state processes depends heavily on the nature of the state generated during excitation. The selection rules for light-matter interactions are well established and therefore how to define the excited states accessible is understood. However, this is not the case for excited states formed by electrical excitation, a process critical for the efficiency of OLEDs. As part of this project we developed and used kinetic monte-carlo simulations to demonstrate the substantial probability of forming hot excitons during the charge recombination process with state as much as 0.5 eV higher than the lowest excited state. While these results reveal that the "hot exciton" path to potentially achieve high efficiency, the excess energy is likely to have significant implications for blue emitters in OLEDs. The publication of this work is currently in progress. |
| Exploitation Route | High performing molecules will be protected with IP and the outcome of our simulations on hot exciton formation will be taken to companies to encourage their use in designing molecules. |
| Sectors | Electronics,Energy |
| Title | A Quantum Dynamics Study on the Hyperfluorescence Mechanism |
| Description | Calculation outputs related to the papers;
A Quantum Dynamics Study on the Hyperfluorescence Mechanism README:: This dataset contains the following calculation outputs. -----------------------------Calculation on TBPe:----------------------------- Electronic Structure (#State refers to the electronic state of TBPe)-----------------------------Geometry optimisation outputs of TBPE:............OPTIMISATION_#State.outOptimised geometries of TBPe:.....................GEOMETRY_#State.xyzGround state frequencies output of TBPe:..........FREQUENCIES_S0.outElectronic structure calculation of TBPe:.........ELECTRONIC_STRUCTURE_#State.outGradient calculation output of TBPe:..............GRADIENT_#State.out Coupling calculations: (#Distance corresponds to the intermolecular distance/sqrt(3) )-----------------------------Electronic structure + FED couplings along the intermolecular distance:At the Au-Cz Co-planar geometry for Singlets:.....COUPLING-COPLANAR-R#Distance-SINGLETS.outAt the Au-Cz Co-planar geometry for Triplets:.....COUPLING-COPLANAR-R#Distance-TRIPLETS.outAt the Au-Cz Perpendicular geometry for Singlets:.COUPLING-PERPENDICULAR-R#Distance-SINGLETS.outAt the Au-Cz Perpendicular geometry for Triplets:.COUPLING-PERPENDICULAR-R#Distance-TRIPLETS.out Electronic structure + FED couplings along the Au-Cz Torsion \varphi: (#Angle refers to the values of \varphi)At a distance of 14 for Singlets:.................COUPLING-PHI#Angle-SINGLETS.outAt a distance of 14 for Triplets:.................COUPLING-PHI#Angle-TRIPLETS.out Electronic structure + FED couplings along \theta_i: (#Angle refers to the values of the theta angles)At a distance of 14 and the co-planar geometry:...COUPLING-THETAx-#Angle.outAt a distance of 14 and the co-planar geometry:...COUPLING-THETAy-#Angle.outAt a distance of 14 and the co-planar geometry:...COUPLING-THETAz-#Angle.out Dynamics:----------------------------- With the T1 TBPe state for different \varepsilon' values: (#Epsilon' refers to the value of epsilon')Operator files:...................................DYNAMICS_T1_#Epsilon'.opInput files:......................................DYNAMICS_T1_#Epsilon'.inp Without the T1 TBPe state for different energies of S1E: (#Epsilon refers to the value of epsilon)Operator files:...................................DYNAMICS_noT1_#Epsilon.opInput files:......................................DYNAMICS_noT1_#Epsilon.inp -----------------------------Calculation on TBRb:----------------------------- Electronic Structure (#State refers to the electronic state of TBRb)-----------------------------Geometry optimisation outputs of TBRb:............TBRb_OPTIMISATION_#State.outOptimised geometries of TBRb:.....................TBRb_GEOMETRY_#State.xyzGround state frequencies output of TBRb:..........TBRb_FREQUENCIES_S0.outElectronic structure calculation of TBRb:.........TBRb_ELECTRONIC_STRUCTURE_#State.outGradient calculation output of TBRb:..............TBRb_GRADIENT_#State.out Coupling calculations: (#Distance corresponds to the intermolecular distance/sqrt(3) )-----------------------------Electronic structure + FED couplings along the intermolecular distance:At the Au-Cz Co-planar geometry for Singlets:.....TBRb_COUPLING-COPLANAR-R#Distance-SINGLETS.outAt the Au-Cz Co-planar geometry for Triplets:.....TBRb_COUPLING-COPLANAR-R#Distance-TRIPLETS.outAt the Au-Cz Perpendicular geometry for Singlets:.TBRb_COUPLING-PERPENDICULAR-R#Distance-SINGLETS.outAt the Au-Cz Perpendicular geometry for Triplets:.TBRb_COUPLING-PERPENDICULAR-R#Distance-TRIPLETS.out Electronic structure + FED couplings along the Au-Cz Torsion \varphi: (#Angle refers to the values of \varphi)At a distance of 14 for Singlets:.................TBRb_COUPLING_PHI#Angle-SINGLETS.out |
| Type Of Material | Database/Collection of data |
| Year Produced | 2020 |
| Provided To Others? | Yes |
| URL | https://data.ncl.ac.uk/articles/dataset/A_Quantum_Dynamics_Study_on_the_Hyperfluorescence_Mechanism/... |
| Title | Fine tuning isomerization crucial to enhance TADF spin vibronic coupling |
| Description | Calculation outputs related to the paper: Fine tuning isomerization crucial to enhance TADF spin vibronic coupling Paloma L. dos Santos, Daniel de Sa Pereira, Andrew P. Monkman, Thomas J. Penfold, Julien Eng, Jonathan S. Ward and Martin R. Bryce README FILE Ground state optimisation:........................OPTIMISATION-GS.out Frequency calculation at GS:......................FREQUENCY-GS.out S1 optimisation:..................................OPTIMISATION-S1.out T1 optimisation:..................................OPTIMISATION-T1.out Electronic structure at GS in Toluene:............ELECTRONIC_STRUCTURE-GS-TOLUENE.out Electronic structure at S1 in Toluene:............ELECTRONIC_STRUCTURE-S1-TOLUENE.out Electronic structure at T1 in Toluene:............ELECTRONIC_STRUCTURE-T1-TOLUENE.out Electronic structure at GS in CH2Cl2:.............ELECTRONIC_STRUCTURE-GS-TOLUENE.out Electronic structure at S1 in CH2Cl2:.............ELECTRONIC_STRUCTURE-S1-TOLUENE.out Electronic structure at T1 in CH2Cl2:.............ELECTRONIC_STRUCTURE-T1-TOLUENE.out AIMD snapshots for Absorption in Toluene:.........ABSORPTION-MD-TOLUENE-###.out AIMD snapshots for Absorption in CH2Cl2:..........ABSORPTION-MD-CH2Cl2-###.out AIMD snapshots for Emission in Toluene:.........EMISSION-MD-TOLUENE-###.out AIMD snapshots for Emission in CH2Cl2:..........EMISSION-MD-CH2Cl2-###.out |
| Type Of Material | Database/Collection of data |
| Year Produced | 2022 |
| Provided To Others? | Yes |
| URL | https://data.ncl.ac.uk/articles/dataset/Fine_tuning_isomerization_crucial_to_enhance_TADF_spin_vibro... |
| Title | Fine tuning isomerization crucial to enhance TADF spin vibronic coupling |
| Description | Calculation outputs related to the paper: Fine tuning isomerization crucial to enhance TADF spin vibronic coupling Paloma L. dos Santos, Daniel de Sa Pereira, Andrew P. Monkman, Thomas J. Penfold, Julien Eng, Jonathan S. Ward and Martin R. Bryce README FILE Ground state optimisation:........................OPTIMISATION-GS.out Frequency calculation at GS:......................FREQUENCY-GS.out S1 optimisation:..................................OPTIMISATION-S1.out T1 optimisation:..................................OPTIMISATION-T1.out Electronic structure at GS in Toluene:............ELECTRONIC_STRUCTURE-GS-TOLUENE.out Electronic structure at S1 in Toluene:............ELECTRONIC_STRUCTURE-S1-TOLUENE.out Electronic structure at T1 in Toluene:............ELECTRONIC_STRUCTURE-T1-TOLUENE.out Electronic structure at GS in CH2Cl2:.............ELECTRONIC_STRUCTURE-GS-TOLUENE.out Electronic structure at S1 in CH2Cl2:.............ELECTRONIC_STRUCTURE-S1-TOLUENE.out Electronic structure at T1 in CH2Cl2:.............ELECTRONIC_STRUCTURE-T1-TOLUENE.out AIMD snapshots for Absorption in Toluene:.........ABSORPTION-MD-TOLUENE-###.out AIMD snapshots for Absorption in CH2Cl2:..........ABSORPTION-MD-CH2Cl2-###.out AIMD snapshots for Emission in Toluene:.........EMISSION-MD-TOLUENE-###.out AIMD snapshots for Emission in CH2Cl2:..........EMISSION-MD-CH2Cl2-###.out |
| Type Of Material | Database/Collection of data |
| Year Produced | 2022 |
| Provided To Others? | Yes |
| URL | https://data.ncl.ac.uk/articles/dataset/Fine_tuning_isomerization_crucial_to_enhance_TADF_spin_vibro... |
| Title | Tailoring Donor-Acceptor Emitters to Minimise Localisation Induced Quenching of Thermally Activated Delayed Fluorescence |
| Description | Calculation outputs related to the paper: Tailoring Donor-Acceptor Emitters to Minimise Localisation Induced Quenching of Thermally Activated Delayed Fluorescence Thomas James Penfold, Julien Eng README #MOL refers to the molecule and can be: D1-A1 D2-A1 D2-A2 D2-A3 D2-A4 D2-A5 D2-A6 D2-A7 D2-A8 D3-A1 D4-A1 Ground state optimisation:........................OPTIMISATION_GS_#MOL.out S1 optimisation:..................................OPTIMISATION_S1_#MOL.out S1 Symmetry optimisation:.........................OPTIMISATION_S1SYM_#MOL.out Electronic structure at the GS geo:...............ELECTRONIC_STRUCTURE_GS_#MOL.out Electronic structure at the S1 geo:...............ELECTRONIC_STRUCTURE_S1_#MOL.out Electronic structure at the S1 Sym. geo:..........ELECTRONIC_STRUCTURE_S1SYM_#MOL.out ab initio molecular dynamics in the GS............AIMD_GS_#MOL.out ab initio molecular dynamics in S1................AIMD_S1_#MOL.out |
| Type Of Material | Database/Collection of data |
| Year Produced | 2022 |
| Provided To Others? | Yes |
| URL | https://data.ncl.ac.uk/articles/dataset/Tailoring_Donor-Acceptor_Emitters_to_Minimise_Localisation_I... |
| Title | Tailoring Donor-Acceptor Emitters to Minimise Localisation Induced Quenching of Thermally Activated Delayed Fluorescence |
| Description | Calculation outputs related to the paper: Tailoring Donor-Acceptor Emitters to Minimise Localisation Induced Quenching of Thermally Activated Delayed Fluorescence Thomas James Penfold, Julien Eng README #MOL refers to the molecule and can be: D1-A1 D2-A1 D2-A2 D2-A3 D2-A4 D2-A5 D2-A6 D2-A7 D2-A8 D3-A1 D4-A1 Ground state optimisation:........................OPTIMISATION_GS_#MOL.out S1 optimisation:..................................OPTIMISATION_S1_#MOL.out S1 Symmetry optimisation:.........................OPTIMISATION_S1SYM_#MOL.out Electronic structure at the GS geo:...............ELECTRONIC_STRUCTURE_GS_#MOL.out Electronic structure at the S1 geo:...............ELECTRONIC_STRUCTURE_S1_#MOL.out Electronic structure at the S1 Sym. geo:..........ELECTRONIC_STRUCTURE_S1SYM_#MOL.out ab initio molecular dynamics in the GS............AIMD_GS_#MOL.out ab initio molecular dynamics in S1................AIMD_S1_#MOL.out |
| Type Of Material | Database/Collection of data |
| Year Produced | 2022 |
| Provided To Others? | Yes |
| URL | https://data.ncl.ac.uk/articles/dataset/Tailoring_Donor-Acceptor_Emitters_to_Minimise_Localisation_I... |