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Inverse molecular design from first principles: Tailoring organic chromophore spectra for optoelectronic applications

Green, James D; Fuemmeler, Eric G; Hele, Timothy JH; (2022) Inverse molecular design from first principles: Tailoring organic chromophore spectra for optoelectronic applications. The Journal of Chemical Physics , 156 (18) , Article 180901. 10.1063/5.0082311. Green open access

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Abstract

The discovery of molecules with tailored optoelectronic properties, such as specific frequency and intensity of absorption or emission, is a major challenge in creating next-generation organic light-emitting diodes (OLEDs) and photovoltaics. This raises the following question: How can we predict a potential chemical structure from these properties? Approaches that attempt to tackle this inverse design problem include virtual screening, active machine learning, and genetic algorithms. However, these approaches rely on a molecular database or many electronic structure calculations, and significant computational savings could be achieved if there was prior knowledge of (i) whether the optoelectronic properties of a parent molecule could easily be improved and (ii) what morphing operations on a parent molecule could improve these properties. In this Perspective, we address both of these challenges from first principles. We first adapt the Thomas-Reiche-Kuhn sum rule to organic chromophores and show how this indicates how easily the absorption and emission of a molecule can be improved. We then show how by combining electronic structure theory and intensity borrowing perturbation theory we can predict whether or not the proposed morphing operations will achieve the desired spectral alteration, and thereby derive widely applicable design rules. We go on to provide proof-of-concept illustrations of this approach to optimizing the visible absorption of acenes and the emission of radical OLEDs. We believe that this approach can be integrated into genetic algorithms by biasing morphing operations in favor of those that are likely to be successful, leading to faster molecular discovery and greener chemistry.

Type: Article
Title: Inverse molecular design from first principles: Tailoring organic chromophore spectra for optoelectronic applications
Location: United States
Open access status: An open access version is available from UCL Discovery
DOI: 10.1063/5.0082311
Publisher version: https://doi.org/10.1063/5.0082311
Language: English
Additional information: © 2022 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
UCL classification: UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
URI: https://discovery.ucl.ac.uk/id/eprint/10148852
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