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Li, Xiaoe,Nazeeruddin, Mohammad K.,Thelakkat, Mukundan,Barnes, Piers R. F.,Vilar, Ramó,n,Durrant, James R. The Royal Society of Chemistry 2011 Physical chemistry chemical physics Vol.13 No.4
<P>We report the application of spectroelectrochemical techniques to compare the hole percolation dynamics of molecular networks of two ruthenium bipyridyl complexes adsorbed onto mesoporous, nanocrystalline TiO<SUB>2</SUB> films. The percolation dynamics of the ruthenium complex <I>cis</I>-di(thiocyanato)(2,2′-bipyridyl-4,4′-dicarboxylic acid)-(2,2′-bipyridyl-4,4′-tridecyl) ruthenium(<SMALL>II</SMALL>), N621, is compared with those observed for an analogous dye with an additional tri-phenyl amine (TPA) donor moiety, <I>cis</I>-di(thiocyanato)(2,2′-bipyridyl-4,4′-dicarboxylic acid)-(2,2′-bipyridyl-4,4′-bis(vinyltriphenylamine)) ruthenium(<SMALL>II</SMALL>), HW456. The <I>in situ</I>oxidation of these ruthenium complexes adsorbed to the TiO<SUB>2</SUB> films is monitored by cyclic voltammetry and voltabsorptometry, whilst the dynamics of hole (cation) percolation between adsorbed ruthenium complexes is monitored by potentiometric spectroelectrochemistry and chronoabsorptometry. The hole diffusion coefficient, <I>D</I><SUB>eff</SUB>, is shown to be dependent on the dye loading on the nanocrystalline TiO<SUB>2</SUB> film, with a threshold observed at ∼60% monolayer surface coverage for both dyes. The hole diffusion coefficient of HW456 is estimated to be 2.6 × 10<SUP>−8</SUP> cm<SUP>2</SUP>/s, 20-fold higher than that obtained for the control N621, attributed to stronger electronic coupling between the TPA moieties of HW456 accelerating the hole percolation dynamics. The presence of mercuric ions, previously shown to bind to the thiocyanates of analogous ruthenium complexes, resulted in a quenching of the hole percolation for N621/TiO<SUB>2</SUB> films and an enhancement for HW456/TiO<SUB>2</SUB> films. These results strongly suggest that the hole percolation pathway is along the overlapped neighbouring -NCS groups for the N621 molecules, whereas in HW456 molecules cation percolation proceeds between intermolecular TPA ligands. These results are discussed in the context of their relevance to the process of dyeregeneration in dye sensitised solar cells, and to the molecular wiring of wide bandgap inorganic materials for battery and sensing applications.</P> <P>Graphic Abstract</P><P>We employ spectroelectrochemical techniques to compare the hole percolation dynamics of two ruthenium bipyridyl complexes adsorbed onto mesoporous TiO<SUB>2</SUB> films. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c0cp01013h'> </P>
Thermal Behavior of Methylammonium Lead-Trihalide Perovskite Photovoltaic Light Harvesters
Dualeh, Amalie,Gao, Peng,Seok, Sang Il,Nazeeruddin, Mohammad Khaja,Grä,tzel, Michael American Chemical Society 2014 Chemistry of materials Vol.26 No.21
<P>Recently organic–inorganic hybrid perovskites have attracted attention as light harvesting materials in mesoscopic cells. While a considerable number of deposition and formation methods have been reported for the perovskite crystalline material, most involve an annealing step. As such, the thermal behavior of this material and its individual components is of crucial interest. Here, we examine the thermal properties of the CH<SUB>3</SUB>NH<SUB>3</SUB>PbX<SUB>3</SUB> (X = I or Cl) perovskite using thermogravimetric analysis. The role of the precursors is exposed, and the effect of the formation of excess organic species is investigated. The sublimation behavior of the organic component is intensively scrutinized. Furthermore, differential scanning calorimetry is employed to probe the crystal phase structure, revealing subtle differences depending on the deposition method.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/cmatex/2014/cmatex.2014.26.issue-21/cm502468k/production/images/medium/cm-2014-02468k_0004.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/cm502468k'>ACS Electronic Supporting Info</A></P>
Delcamp, Jared H.,Yella, Aswani,Nazeeruddin, Mohammad K.,Grä,tzel, Michael The Royal Society of Chemistry 2012 Chemical communications Vol.48 No.17
<P>Acceptor motifs based on nitrogen containing heterocycles have been synthesized for use in dye-sensitized solar cells (DSCs). Through the selective addition of nitrogen atoms and increased conjugation of the nitrogen containing heterocycles the excited-state oxidation potential, <I>E</I><SUB>(S+/S*)</SUB>, may be conveniently tuned with minimal effect on the ground-state oxidation potential, <I>E</I><SUB>(S+/S)</SUB>, of the dye.</P> <P>Graphic Abstract</P><P>A series of nitrogen containing heterocyclic acceptors are shown to tune the excited-state oxidation potential of D-π-A dyes for DSCs. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c2cc17142b'> </P>
Shavaleev, N.M.,Scopelliti, R.,Gratzel, M.,Nazeeruddin, M.K. Elsevier Sequoia [etc.] 2012 Inorganica chimica acta Vol.388 No.-
Two new cationic iridium(III) complexes with cyclometalating 1-phenylindazole or 2-phenyl-1,2,3-triazole ligands, [(C@<SUP>N</SUP>)<SUB>2</SUB>Ir(4,4'-di-tert-butyl-2,2'-dipyridyl)](PF<SUB>6</SUB>), exhibit yellow or green phosphorescence with quantum yields and excited state lifetimes of up to 45% and 840ns in argon-saturated dichloromethane solution at room temperature.
Ameen, Sadia,Akhtar, M. Shaheer,Nazim, M.,Nazeeruddin, Mohammad Khaja,Shin, Hyung-Shik Elsevier 2018 Nano energy Vol.49 No.-
<P><B>Abstract</B></P> <P>This work explains the synthesis of an efficient organic hole transporting material based on 4,4′-(5,5′-(thiazolo[5,4-<I>d</I>]thiazole-2,5-diyl)bis(furan-5,2-diyl))bis(N,N-diphenylaniline) (TP-FTzF-TP) and the replacement of poly(3,4-ethylenedio-xythiophene): poly(styrenesulfonate) (PEDOT:PSS) layer by simple O<SUB>2</SUB> plasma treatment for perovskite solar cells (PSCs). The introduction of furan spacer groups significantly tuned the absorption and the electrochemical properties of the organic hole transporting material. The ITO(O<SUB>2</SUB> plasma)/TP-FTzF-TP/CH<SUB>3</SUB>NH<SUB>3</SUB>PbI<SUB>3</SUB>/PC<SUB>61</SUB>BM/Au configuration based PSC exhibited a high power conversion efficiency (PCE) of ~ 16.4% which showed a momentous improvement as compared to PCEs of ~ 11.6% and ~ 10.5% achieved by ITO/PEDOT:PSS/TP-FTzF-TP/CH<SUB>3</SUB>NH<SUB>3</SUB>PbI<SUB>3</SUB>/PC<SUB>61</SUB>BM/Au and ITO/TP-FTzF-TP/CH<SUB>3</SUB>NH<SUB>3</SUB>PbI<SUB>3</SUB>/PC<SUB>61</SUB>BM/Au devices, respectively. The superior performances of PSC were accredited to fast hole injection from the valence band of CH<SUB>3</SUB>NH<SUB>3</SUB>PbI<SUB>3</SUB> into the suitable HOMO and a high hole mobility of TP-FTzF-TP HTM.</P> <P><B>Highlights</B></P> <P> <UL> <LI> A furan-bridged based HTM is synthesized and characterized by spectroscopic techniques. </LI> <LI> HOMO of HTM is found to be in proper alignment with the energy levels of perovskite material. </LI> <LI> An inverted configuration consisting of ITO (O2 plasma)/TP-FTzF-TP/CH3NH3PbI3/PC61BM/Au, exhibits an excellent PCE of ~ 16.4%. </LI> <LI> The short-circuit current density of ~ 21.94 mA/cm2, V<SUB>OC</SUB> of ~ 1.04 V and FF of ~ 0.72 under 1 sun condition. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>A furan-bridged hole transporting material (HTM) is synthesized and characterized by spectroscopic techniques. The highest occupied molecular orbitals of the HTM are found to be in proper alignment with the energy levels of perovskite material. The HTM in combination with the hybrid methylammonium lead triiodide (MAPbI3) perovskite in an inverted configuration consisting of ITO (O2 plasma)/TP-FTzF-TP/CH3NH3PbI3/PC61BM/Au, exhibit an excellent power conversion efficiency of ~ 16.4%. The short-circuit current density of ~ 21.94 mA/cm2, VOC of ~ 1.04 V and FF of ~ 0.72 under 1 sun condition.</P> <P>[DISPLAY OMISSION]</P>
De Angelis, Filippo,Vitillaro, Giuseppe,Kavan, Ladislav,Nazeeruddin, Mohammad. K.,Grä,tzel, Michael American Chemical Society 2012 JOURNAL OF PHYSICAL CHEMISTRY C - Vol.116 No.34
<P>We present a first-principles computational investigation on the adsorption mode and electronic structure of the highly efficient heteroleptic ruthenium dye C101, [NaRu(4,4′-bis(5-hexylthiophene-2-yl)-2,2′-bipyridine)(4-carboxylic acid-4′-carboxylate-2,2′-bipyridine)(NCS)<SUB>2</SUB>], on anatase TiO<SUB>2</SUB> models exposing the (001) and (101) surfaces. The electronic structure of the TiO<SUB>2</SUB> models shows a conduction band energy upshift for the (001)-surface ranging between ∼50 and ∼110 meV compared with the (101) surface, in agreement with previous interfacial impedance and recent spectro-electrochemical data. TDDFT excited-state calculations provided the same optical band gap, within 0.01 eV, for the (001)- and (101) models. Two dominant adsorption modes for C101 dye adsorption on the (001) and (101) surfaces were found, which differ by the binding of the dye carboxylic groups to the TiO<SUB>2</SUB> surfaces (bridged bidentate vs monodentate), leading to sizably different tilting of the anchoring bipyridine plane with respect to the TiO<SUB>2</SUB> surface. The different adsorption mode leads to a smaller dye coverage on the (001) surface, as experimentally found, due to partial contact of the thiophene and alkyl bipyridine substituents with the TiO<SUB>2</SUB> surface. For the energetically favored adsorption modes, we calculate a larger average spatial separation, by 1.3 Å, between the dye-based HOMO and the semiconductor surface in (001) and (101) TiO<SUB>2</SUB> models. In terms of simple nonadiabatic electron-transfer considerations, our model predicts a retardation of the charge recombination kinetics, in agreement with the experimental observations.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpccck/2012/jpccck.2012.116.issue-34/jp306186y/production/images/medium/jp-2012-06186y_0008.gif'></P>
Charged cyclometalated iridium(III) complexes that have large electrochemical gap
Shavaleev, N.M.,Scopelliti, R.,Baranoff, E.,Gratzel, M.,Nazeeruddin, M.K. Elsevier Sequoia [etc.] 2012 Inorganica chimica acta Vol.383 No.-
Bis-cyclometalated cationic Ir(III) diimine complexes [Ir(C@<SUP>N</SUP>)<SUB>2</SUB>(N@<SUP>N</SUP>)](PF<SUB>6</SUB>) with 1-phenylpyrazoles (C@<SUP>N</SUP>) and 1-(4'-tert-butyl-2'-pyridyl)pyrazole (N@<SUP>N</SUP>) are white solids that have absorption onset below 425nm and electrochemical gap of up to 3.5V.