Systematic Computational Design and Optimization of Light Absorbing Dyes

The Journal of Physical Chemistry A, vol. 124, pp. 6380–6388

Abstract

We present a workflow to aid the discovery of new dyes for the role of a photosensitive unit in the dye-sensitized photo-electrochemical cells (DS-PECs). New structures are generated in a fully automated way using the Compound Attachment Tool (CAT) introduced in this work. These structures are characterized with efficient approximate density functional theory (DFT) methods, and molecules with favorable optical properties are suggested for possible further use in DS-PECs. As around 2500 structures are generated in this work, and as we aim for still larger volumes of compounds to screen in subsequent applications, we have assessed the reliability of low-cost screening methods and show that simplified time-dependent density functional theory (sTDDFT) provides a satisfying accuracy/cost ratio. From the dyes considered, we propose a set that can be suitable for panchromatic sensitization of the photoelectrode in DS-PECs to further increase DS-PEC efficiency.

Authors 5

1. Jelena Belić corresponding

   Vrije Universiteit Amsterdam

   Affiliation as printed

   Vrije Uversiteit Amsterdam , De Boelelaan 1083 , ,

   Vrije Uversiteit Amsterdam, De Boelelaan 1083, Amsterdam 1081 HV, The Netherlands

2. Bas van Beek

   Vrije Universiteit Amsterdam

   Affiliation as printed

   Vrije Uversiteit Amsterdam , De Boelelaan 1083 , ,

   Vrije Uversiteit Amsterdam, De Boelelaan 1083, Amsterdam 1081 HV, The Netherlands

3. Jan Paul Menzel Aachen

   Leiden University

   Affiliation as printed

   Leiden University , , Einsteinweg 55 , P.O. Box 9502 , ,

   Leiden Institute of Chemistry, Leiden University, Einsteinweg 55, P.O. Box 9502, Leiden 2300 RA, The Netherlands

4. Francesco Buda Aachen

   Leiden University

   Affiliation as printed

   Leiden University , , Einsteinweg 55 , P.O. Box 9502 , ,

   Leiden Institute of Chemistry, Leiden University, Einsteinweg 55, P.O. Box 9502, Leiden 2300 RA, The Netherlands

5. Lucas Visscher corresponding

   Vrije Universiteit Amsterdam

   Affiliation as printed

   Vrije Uversiteit Amsterdam , De Boelelaan 1083 , ,

   Vrije Uversiteit Amsterdam, De Boelelaan 1083, Amsterdam 1081 HV, The Netherlands