H2020Индивидуална стипендия2020–2022

D3AiSF · Screening Database to Discover Donor-Acceptor copolymers for intramolecular Singlet Fission

„Хоризонт 2020“ — Действия „Мария Склодовска-Кюри“

Период: 2020-02-01 → 2022-05-03
Финансиране от ЕС: 191 149 €
Участници: 1
Схема: MSCA-IF

Линиите свързват координатора с партньорите.

Накратко на български

Специални полимери от донор-акцептор тип се анализират чрез компютърни симулации, за да се открият такива, които разделят един погълнат фотон на две частици. Това може да помогне за повишаване на ефективността на слънчевите панели.

Този кратък обзор е генериран от изкуствен интелект

Кратко обяснение, генерирано от езиков модел по текста на CORDIS. Оригиналът е по-долу.

Резултати накратко

Screening Database to Discover Donor-Acceptor copolymers for intramolecular Singlet Fission

Since 2006, singlet fission (SF) gained considerable interest due to its potential to increase solar cell efficiencies (J. Appl. Phys. 2006, 100, 074510). SF is a multiple exciton generation (MEG) process by which a singlet exciton (S1) splits into two triplet excitons (2T1), thereby generating two electron-hole pair carriers from each absorbed photon. Ultrafast singlet-triplet conversion takes place through a correlated triplet pair state (1(TT)) that has an overall singlet spin state. Thus, SF is often described as a two-step process involving two-chromophore centers. Initial research was mainly focused on intermolecular SF (xSF). However, the unpredictable molecular arrangement of the chromophores in the crystal prevents the rational design of new materials with appropriate arrangements for efficient xSF. In contrast, intramolecular SF (iSF) offers a solution to this problem. In 2015 particular attention was placed on donor-acceptor (DA)-type copolymers owing to their promising characteristics in displaying efficient iSF (Nat. Mater. 2015, 14, 426). The clear advantage of the DA copolymer scheme is its modularity, which allows to select different D and A units to build fission-capable polymers. Certainly, progress on iSF polymeric systems can benefit from computational efforts. The objective of this proposal is to combine state-of-the-art computational tools with fundamental concepts of quantum chemistry to advance the iSF field by means of high-throughput (HT) screening of efficient DA-polymers and quantum dynamics simulations. The first step of this project is to design an automated workflow to screen a large number of SF-capable DA-copolymers based on appropriate descriptors. In a second stage, the SF-performance of the very best potential candidates is evaluated in terms of real time quantum dynamics of the singlet splitting nonadiabatic process to ultimately assess the iSF capabilities of the promising candidates. After the completion of this project, we have proposed novel routes to the design of iSF capable D-A copolymers, either using a high-throughput screening protocol applied to a diverse database of D-A units (Chem. Mater. 2020, 32, 6515; 2021, 33, 2567), or using a simple molecular approach consisting at heteroatom oxidation of the building blocks in already existing D-A copolymers (Chem. Commun. 2022, 58, 1338). On the other side, our results unravelled the S1-to-1TT excited state decay mechanism in prototypical D-A copolymers (J. Phys. Chem. Lett. 2020, 11, 9788; 2021, 12, 7270) and turned the attention to two fundamental features that need to be considered in the future development of iSF D-A copolymers, which are coplanarity and triplet-pair dissociation (10.1021/acs.chemmater.2c00367).

Текст от CORDIS, на английски · Данни: CORDIS, © Европейски съюз

Цел на проекта

Singlet fission is a multiple exciton generation process where a singlet exciton splits into two triplet excitons in adjacent chromophore centers, resulting in generation of two electron-hole pair carriers from each absorbed photon. Molecular systems displaying this phenomenon are very desired because they can, for instance, increase the efficiency of solar cells which must possesses both favorable energetics and appropriate electronic coupling. In this context, intramolecular bi-chromophores are particularly interesting in terms of their singlet fission capabilities. Specifically, these donor-acceptor copolymers have both proper electronic structure characteristics and modular molecular architecture. Nonetheless, no rational design principles exist for designing these systems, with the current state-of-the-art being based, primarily, on trial-and-error strategies. Thus, the field is ripe for the insight that can be brought by theoretical work, which has the potential to discover, in silico, new efficient singlet fission compounds.The objective of the D3AiSF project is to combine state-of-the art computational tools with fundamental concepts of quantum chemistry in order to advance the intramolecular singlet fission field through high-throughput screening of efficient donor-acceptor copolymers and quantum dynamics simulations. The project’s first step involves designing an automated workflow capably of screening large numbers of singlet-fission capable donor-acceptor copolymers based on energy and coupling descriptors. Afterwards, a second stage focuses on the singlet-fission performance of the very best potential candidates, which are evaluated in terms of real time quantum dynamics of the nonadiabatic process, which will ultimately validate their relevance. Overall, this project stimulates both data-based theoretical chemistry and the field of intramolecular singlet fission through the computational design and discovery of novel materials.

Оригинален текст от CORDIS (на английски).

Участници

ECOLE POLYTECHNIQUE FEDERALE DE LAUSANNE · LausanneКоординаторШвейцария