Massive Theoretical Screen of Hole Conducting Organic Materials in the Heteroacene Family by Using a Cloud-Computing Environment

Abstract

Materials exhibiting higher mobilities than conventional organic semiconducting materials such as fullerenes and fused thiophenes are in high demand for applications in printed electronics. To discover new molecules in the heteroacene family that might show improved charge mobility, a massive theoretical screen of hole conducting properties of molecules was performed by using a cloud-computing environment. Over 7 000 000 structures of fused furans, thiophenes and selenophenes were generated and 250 000 structures were randomly selected to perform density functional theory (DFT) calculations of hole reorganization energies. The lowest hole reorganization energy calculated was 0.0548 eV for a fused thioacene having 8 aromatics rings. Hole mobilities of compounds with the lowest 130 reorganization energy were further processed by applying combined DFT and molecular dynamics (MD) methods. The highest mobility calculated was 1.02 and 9.65 cm2/(V s) based on percolation and disorder theory, respectively, for compounds containing selenium atoms with 8 aromatic rings. These values are about 20 times higher than those for dinaphthothienothiophene (DNTT).

De Novo Design of Molecules with Low Hole Reorganization Energy Based on a Quarter-Million Molecule DFT Screen

“…Another illustrative work is reported by Hachmann et al, where HOMOs and LUMOs of more than 2 million compounds were calculated to screen compounds for organic solar cells . A massive theoretical screen of hole-conducting heteroacene molecules has also recently been reported by our group, where hole reorganization energies of quarter million heteroacenes were calculated using a cloud computing environment and various promising structures were identified …”

Design of Organic Electronic Materials With a Goal-Directed Generative Model Powered by Deep Neural Networks and High-Throughput Molecular Simulations

“…These simulations are now possible because of recent improvements in predictive accuracy and that one can cost-effectively access such predictions at a large scale. A recent example of organic semiconductor design ( Matsuzawa et al, 2020b ) demonstrates how the state-of-the-art physics-based simulation technology powered by a large-scale computing environment accessible to the scientific community can be utilized to produce a large number of reliable materials databases for the development of new materials. The automated large-scale quantum chemical and machine learning predictive schemes used in work are designed to utilize a similar strategy in developing new organic electronic materials.…”

“…Atomic-scale simulation has been an essential tool for navigating the enormous chemical space of novel OLED materials ( Halls et al, 2015 ; Halls et al, 2016 ). With increasing high-throughput computational capabilities, massive theoretical screening of millions of compounds has become a reality ( Matsuzawa et al, 2020a ). The ready availability of high-quality computational data generated from simulations is proving to be a gold mine for data-driven prediction of material properties, thereby realizing a significant speed-up in assessing key control variables for designing novel materials.…”

High-throughput virtual screening for organic electronics: a comparative study of alternative strategies

“… 331 , N. N. Matsuzawa et al constructed a very large set of rigid acenes with two to eight fused rings and substituted with carbon, oxygen, sulphur and selenium. 270 Since random permutation methods can quickly generate an unfeasible number of molecules, in this case over 7 M structures, a selection of a smaller subset is often necessary for the screening. The selection can be random, guided by some loose logic or by synthetic score.…”

“…Hopping transport theory, despite being not fully applicable to molecular semiconductors, due to its simplicity and low computational cost, remains a frequent method of choice in the majority of HTVS studies, including those using large databases, [269][270][271] as well as those evaluating smaller libraries of structures. [272][273][274][275] Applying this theory to screen the CSD, as the world's largest repository of small organic/metal-organic molecules whose crystalline structures are experimentally known, 186 C. Schober et al made an important contribution demonstrating, for the first time, that large scale screening of materials for transport applications is possible.…”