Faraday Discussions: Challenges and prospects in organic photonics and electronics

Transcript

1. Morphology, dynamic disorder, and charge transport in an indoloindole-based hole-transporting material from a multi-level theoretical approach Manuel Pérez-Escribano, Alberto Fernández-Alarcón, Enrique Ortí, Juan Aragó, Jesús Cerdá,* Joaquín Calbo*
2. N N N N Introduction orthogonal → morphological stability methoxy groups → solution processability Hole transporting materials (HTMs) Organic HTMs • biodegradable • processability • low cost p-type semiconductor PCE > 21% µ ca. 10−3 cm2 V−1 s−1 π-π stacking dynamic disorder mesoscale ordering µ, PCE, stability indolo-indole unit:
3. Dynamic disorder: NVT molecular dynamics along 500 ps at 298 K (1 ps resolution) Computational methodology multi-level theoretical approach charge transport properties IDIDF vs spiro-OMeTAD Marcus theory Non-covalent interactions: NCIPLOT (promolecular densities) ( ) λ π λ πλ   ∆ + = −        2 2 2 1 exp 4 4 B B E k V k T k T λ + + + + = − + − 0 0 0 0 ( ) ( ) g g g g E E E E Internal reorganization energy Electronic coupling Dimer Fock operator (DIPRO) 𝜇𝜇𝑖𝑖𝑖𝑖 = � 𝑑𝑑𝑖𝑖𝑖𝑖 𝑘𝑘𝑖𝑖𝑖𝑖 𝐸𝐸𝑒𝑒𝑒𝑒𝑒𝑒 kinetic Monte Carlo 5x5x5 supercell for IDIDF 3x3x3 supercell for spiro-OMeTAD ( � 𝐸𝐸 ± σ) Amorphous phase: PackMol → NPT molecular simulations of up to 200 ns (ns resolution) (� 𝑉𝑉 ± σ) Electronic crystal structure calculations (PBEsol/HSE06)
4. Static crystals spiro-OMeTAD IDIDF
5. Static crystals NCI surfaces spiro-OMeTAD IDIDF spiro-OMeTAD IDIDF
6. Dynamic disorder Energy Coupling
7. µ (IDIDF) µ (spiro-OMeTAD) Crystal (0 K) 7.448 0.325 Crystal (298 K) 2.418 4.2 × 10-2 Amorphousa 1.1 × 10-3 4.9 × 10-5 Experimentalb 1.7 × 10−3 (TF) 4 × 10−5 (TF) 1.3 × 10−3 (SC) a Mean mobility values are presented. b A mobility of 0.97 cm2 V−1 s−1 was reported for the analogous non- fluorinated 4H4TIDID in a vacuum-deposited polycrystalline field-effect device.30 Dynamic disorder & Amorphous phase IDIDF spiro-OMeTAD cm2 V−1 s−1
8. Manu Alberto Jesús Acknowledgements PID2020-119748GA-I00 funded by MCIN/AEI/10.13039/501100011033