FWO Proposal: Singlet Fission: Molecular Design through a Synergistic Computational and Conceptual Approach

Activity: OtherWritten proposal

Description

Solar cells constitute a crucial cornerstone in transitioning the global energy production from fossil fuels to a CO2 neutral future. To boost the performance of silicon solar cells beyond their thermodynamic efficiency, singlet fission (SF) has attracted tremendous interest as a multiple exciton generation process with quantum efficiencies up to 200%. A central bottleneck in this field is the limited number of chromophores fulfilling the strict energy matching conditions required for SF. Tetracene and pentacene remain the most investigated materials for SF despite their poor photostability. This proposal aims to develop a novel conceptual framework to identify operative SF chromophores with enhanced stability. A synergistic strategy combining the concept of ground- and excited-state aromaticity and conceptual DFT (CDFT) descriptors is proposed to fine-tune the excited-state energy levels and stability of organic compounds. A diverse compound library with wide
structural diversity will be generated and characterized with first-principle calculations for the relevant excitation energies and multiradical character. Structure-property relationships across different core structures are targeted by means of advanced electronic, energetic, and magnetic aromaticity descriptors. In a final step, we take up the challenge to extend CDFT towards excitedstate properties and establish the interplay between the response functions and photochemical
stability.
Period1 Feb 20251 Mar 2025
Degree of RecognitionNational