Computational hole mobilities in (pseudo-)amorphous organic semiconductors.

Area of Science:

• Materials Science
• Computational Chemistry
• Organic Electronics

Background:

• Accurate modeling of charge transport in organic semiconductors is crucial for device performance.
• Amorphous and pseudo-amorphous films in optoelectronic devices present modeling challenges.
• Understanding morphology's impact on charge transport is key for material design.

Purpose of the Study:

• To develop a multiscale computational protocol for predicting hole mobilities in non-crystalline organic semiconductors.
• To investigate the influence of different film morphologies on charge transport properties.
• To establish a framework for the rational design of next-generation organic semiconductors.

Main Methods:

• Integration of density functional theory (DFT), molecular dynamics (MD), docking, and kinetic Monte Carlo (KMC) simulations.
• Modeling of amorphous, pseudo-amorphous films, and docking aggregates.
• Prediction of hole mobilities for ten hole-transporting molecules.

Main Results:

• Achieved order-of-magnitude accuracy in predicting hole mobilities.
• Demonstrated that considering both amorphous disorder and molecular aggregates is essential for accurate predictions.
• Reproduced experimentally observed mobility trends, correlating them with molecular structure (planarity, π-conjugation).

Conclusions:

• The developed multiscale computational protocol provides a robust, morphology-aware framework.
• This approach enables the in silico design and optimization of organic semiconductors.
• Explicitly accounting for film morphology is critical for understanding and predicting charge transport in organic electronic materials.