Combined Experimental and DFT-TDDFT Computational Study of Photoelectrochemical Cell Ruthenium Sensitizers Export

@article{citeulike:4941324, abstract = {We report a combined experimental and computational study of several ruthenium(II) sensitizers originated from the [Ru(dcbpyH2)2(NCS)2], N3, and [Ru(dcbpyH2)(tdbpy)(NCS)2], N621, (dcbpyH2 = 4,4`-dicarboxy-2,2`-bipyridine, tdbpy = 4,4`-tridecyl-2,2`-bipyridine) complexes. A purification procedure was developed to obtain pure N-bonded isomers of both types of sensitizers. The photovoltaic data of the purified N3 and N621 sensitizers adsorbed on TiO2 films in their monoprotonated and diprotonated state, exhibited remarkable power conversion efficiency at 1 sun, 11.18 and 9.57\%, respectively. An extensive Density Functional Theory (DFT)Time Dependent DFT study of these sensitizers in solution was performed, investigating the effect of protonation of the terminal carboxylic groups and of the counterions on the electronic structure and optical properties of the dyes. The calculated absorption spectra are in good agreement with the experiment, thus allowing a detailed assignment of the UVvis spectral features of the two types of dyes. The computed alignments of the molecular orbitals of the different complexes with the band edges of a model TiO2 nanoparticle provide additional insights into the electronic factors governing the efficiency of dye-sensitized solar cell devices.}, author = {Nazeeruddin, Mohammad K. and De Angelis, Filippo and Fantacci, Simona and Selloni, Annabella and Viscardi, Guido and Liska, Paul and Ito, Seigo and Takeru, Bessho and Gratzel, Michael}, citeulike-article-id = {4941324}, citeulike-linkout-0 = {http://dx.doi.org/10.1021/ja052467l}, citeulike-linkout-1 = {http://pubs.acs.org/doi/abs/10.1021/ja052467l}, doi = {10.1021/ja052467l}, journal = {Journal of the American Chemical Society}, keywords = {solarcells}, month = {December}, number = {48}, pages = {16835--16847}, posted-at = {2009-06-24 09:44:05}, priority = {2}, title = {Combined Experimental and DFT-TDDFT Computational Study of Photoelectrochemical Cell Ruthenium Sensitizers}, url = {http://dx.doi.org/10.1021/ja052467l}, volume = {127}, year = {2005} }

TY - JOUR ID - citeulike:4941324 L3 - citeulike-article-id:4941324 N2 - We report a combined experimental and computational study of several ruthenium(II) sensitizers originated from the [Ru(dcbpyH2)2(NCS)2], N3, and [Ru(dcbpyH2)(tdbpy)(NCS)2], N621, (dcbpyH2 = 4,4`-dicarboxy-2,2`-bipyridine, tdbpy = 4,4`-tridecyl-2,2`-bipyridine) complexes. A purification procedure was developed to obtain pure N-bonded isomers of both types of sensitizers. The photovoltaic data of the purified N3 and N621 sensitizers adsorbed on TiO2 films in their monoprotonated and diprotonated state, exhibited remarkable power conversion efficiency at 1 sun, 11.18 and 9.57%, respectively. An extensive Density Functional Theory (DFT)Time Dependent DFT study of these sensitizers in solution was performed, investigating the effect of protonation of the terminal carboxylic groups and of the counterions on the electronic structure and optical properties of the dyes. The calculated absorption spectra are in good agreement with the experiment, thus allowing a detailed assignment of the UVvis spectral features of the two types of dyes. The computed alignments of the molecular orbitals of the different complexes with the band edges of a model TiO2 nanoparticle provide additional insights into the electronic factors governing the efficiency of dye-sensitized solar cell devices. IS - 48 JF - Journal of the American Chemical Society EP - 16847 TI - Combined Experimental and DFT-TDDFT Computational Study of Photoelectrochemical Cell Ruthenium Sensitizers VL - 127 SP - 16835 KW - solarcells AU - Nazeeruddin, Mohammad AU - De Angelis, Filippo AU - Fantacci, Simona AU - Selloni, Annabella AU - Viscardi, Guido AU - Liska, Paul AU - Ito, Seigo AU - Takeru, Bessho AU - Gratzel, Michael PY - 2005/12/01/ UR - http://dx.doi.org/10.1021/ja052467l ER -