Deep Learning for Optoelectronic Properties of Organic Semiconductors

Abstract: Atomistic modeling of energetic disorder in organic semiconductors (OSCs) and its effects on the optoelectronic properties of OSCs requires a large number of excited-state electronic-structure calculations, a computationally daunting task for many OSC applications. In this work, we advocate the use of deep learning to address this challenge and demonstrate that state-of-the-art deep neural networks (DNNs) are capable of predicting the electronic properties of OSCs at an accuracy comparable with the quantum chemistry methods used for generating training data. We extensively investigate the performances of four recent DNNs (deep tensor neural network, SchNet, message passing neural network, and multilevel graph convolutional neural network) in predicting various electronic properties of an important class of OSCs, i.e., oligothiophenes (OTs), including their HOMO and LUMO energies, excited-state energies and associated transition dipole moments. We find that SchNet shows the best performance for OTs of different sizes (from bithiophene to sexithiophene), achieving average prediction errors in the range of 20-80meV compared to the results from (time-dependent) density functional theory. We show that SchNet also consistently outperforms shallow feed-forward neural networks, especially in difficult cases with large molecules or limited training data. We further show that SchNet could predict the transition dipole moment accurately, a task previously known to be difficult for feed-forward neural networks, and we ascribe the relatively large errors in transition dipole prediction seen for some OT configurations to the charge-transfer character of their excited states. Finally, we demonstrate the effectiveness of SchNet by modeling the UV-Vis absorption spectra of OTs in dichloromethane and a good agreement is observed between the calculated and experimental spectra.