Systematic Computational Design and Optimization of Light Absorbing Dyes.

Area of Science:

• Materials Science
• Computational Chemistry
• Renewable Energy

Background:

• Dye-sensitized photo-electrochemical cells (DS-PECs) are crucial for renewable energy applications.
• Developing novel photosensitive dyes is key to enhancing DS-PEC efficiency.
• Current dye discovery methods can be time-consuming and resource-intensive.

Purpose of the Study:

• To establish an automated workflow for the discovery of new dyes for DS-PECs.
• To assess the reliability and cost-effectiveness of computational screening methods for dye discovery.
• To identify promising dye candidates for panchromatic sensitization in DS-PECs.

Main Methods:

• Development of the Compound Attachment Tool (CAT) for automated generation of new molecular structures.
• Characterization of generated structures using efficient approximate density functional theory (DFT) methods.
• Evaluation of simplified time-dependent density functional theory (sTDDFT) for cost-effective screening of optical properties.

Main Results:

• A workflow was established, generating approximately 2500 new molecular structures.
• Simplified time-dependent density functional theory (sTDDFT) demonstrated a favorable accuracy/cost ratio for screening.
• A set of dyes suitable for panchromatic sensitization of DS-PEC photoelectrodes was identified.

Conclusions:

• The automated workflow accelerates the discovery of novel DS-PEC dyes.
• sTDDFT is a reliable and efficient method for large-scale computational screening of dyes.
• The identified dyes hold potential for significantly improving DS-PEC performance.