Document Detail


A spectroscopic and DFT study of thiophene-substituted metalloporphyrins as dye-sensitized solar cell dyes.
MedLine Citation:
PMID:  19842477     Owner:  NLM     Status:  PubMed-not-MEDLINE    
Abstract/OtherAbstract:
A combination of density functional theory calculations, electronic absorption and resonance Raman spectroscopy has been applied to a series of beta-substituted zinc porphyrins to elucidate how the substituent affects the electronic structure of the metalloporphyrin and assign the nature of electronic transitions in the visible region. The use of conjugated beta substituents invokes a large perturbation to both the nature and energy of the frontier molecular orbitals and results in the generation of additional molecular orbitals from the parent metalloporphyrin species. A complicated electronic absorption spectra is observed which can be rationalised by an extension of Goutermans' four-orbital model. The excitations involved in the visible transitions have been determined using resonance Raman spectroscopy. This has revealed that the B band retains much of its original nature and is centred largely on the porphyrin core. Additional electronic transitions invoke population of orbitals localised on the substituent chain. The nature of the electronic transitions depends heavily on the type of beta substituent. The results of this investigation question some previously held beliefs for the rational design of metalloporphyrins for dye-sensitized solar cell applications.
Authors:
Samuel J Lind; Keith C Gordon; Sanjeev Gambhir; David L Officer
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Publication Detail:
Type:  Journal Article    
Journal Detail:
Title:  Physical chemistry chemical physics : PCCP     Volume:  11     ISSN:  1463-9076     ISO Abbreviation:  Phys Chem Chem Phys     Publication Date:  2009 Jul 
Date Detail:
Created Date:  2009-10-21     Completed Date:  2009-12-17     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  100888160     Medline TA:  Phys Chem Chem Phys     Country:  England    
Other Details:
Languages:  eng     Pagination:  5598-607     Citation Subset:  -    
Affiliation:
MacDiarmid Institute for Advanced Materials and Nanotechnology, Department of Chemistry, University of Otago, Dunedin, New Zealand.
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