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Molecular and Interfacial Calculations of Iron(II) Light Harvesters
Author(s) -
Fredin Lisa A.,
Wärnmark Kenneth,
Sundström Villy,
Persson Petter
Publication year - 2016
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201600062
Subject(s) - excited state , density functional theory , electron , adsorption , materials science , chemical physics , carbene , coupling (piping) , conduction band , photochemistry , chemistry , computational chemistry , catalysis , atomic physics , physics , organic chemistry , quantum mechanics , metallurgy
Iron–carbene complexes show considerable promise as earth‐abundant light‐harvesters, and adsorption onto nanostructured TiO 2 is a crucial step for developing solar energy applications. Intrinsic electron injection capabilities of such promising Fe II N ‐heterocyclic complexes (Fe‐NHC) to TiO 2 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 TiO 2 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 TiO 2 conduction band on ∼100 fs time scales.