Molecular and Interfacial Calculations of Iron(II) Light Harvesters

Summary, in English

Iron-carbene complexes show considerable promise as earth-abundant light-harvesters, and adsorption onto nanostructured TiO₂ is a crucial step for developing solar energy applications. Intrinsic electron injection capabilities of such promising Fe^II N-heterocyclic complexes (Fe-NHC) to TiO₂ are calculated here, and found to correlate well with recent experimental findings of highly efficient interfacial injection. First, we examine the special bonding characteristics of Fe-NHC light harvesters. The excited-state surfaces are examined using density functional theory (DFT) and time-dependent DFT (TD-DFT) to explore relaxed excited-state properties. Finally, by relaxing an Fe-NHC adsorbed on a TiO₂ nanocluster, we show favorable injection properties in terms of interfacial energy level alignment and electronic coupling suitable for efficient electron injection of excited electrons from the Fe complex into the TiO₂ conduction band on ∼100 fs time scales.

• Författare: Lisa A. Fredin; Kenneth Wärnmark; Villy Sundström; Petter Persson
• Avdelning/ar: Kemisk fysik; Centrum för analys och syntes; Beräkningskemi; NanoLund: Centre for Nanoscience; eSSENCE: The e-Science Collaboration
• Publiceringsår: 2016-04-07
• Språk: Engelska
• Sidor: 667-675
• Publikation/Tidskrift/Serie: ChemSusChem
• Volym: 9
• Issue: 7
• Länkar: http://dx.doi.org/10.1002/cssc.201600062
• Dokumenttyp: Artikel i tidskrift
• Förlag: John Wiley & Sons Inc.
• Ämne: Theoretical Chemistry
• Nyckelord: density functional theory; photochemistry; potential energy surfaces; quantum chemistry; solar energy
• Status: Published
• ISBN/ISSN/Övrigt: ISSN: 1864-5631