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  • 1.
    Eriksson K., Susanna
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Josefsson, Ida
    Ellis, Hanna
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Amat, Anna
    Pastore, Mariachiara
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Lindblad, Rebecka
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Eriksson, Anna I. K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Johansson, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Boschloo, Gerrit
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hagfeldt, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Fantacci, Simona
    Odelius, Michael
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Geometrical and energetical structural changes in organic dyes for dye-sensitized solar cells probed with photoelectron spectroscopy and DFT2016In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 1, p. 252-260Article in journal (Other academic)
    Abstract [en]

    The effects of alkoxy chain length in triarylamine based donor acceptor organic dyes are investigated with respect to the electronic and molecular surface structures on the performance of solar cells and the electron lifetime. The dyes were investigated when adsorbed on TiO2 in a configuration that can be used for dye sensitized solar cells (DSCs). Specifically, the two dyes D35 and D45 were compared using photoelectron spectroscopy (PES) and density functional theory (DFT) calculations. The differences in solar cell characteristics when longer alkoxy chains are introduced in the dye donor unit are attributed to geometrical changes in dye packing while only minor differences were observed in the electronic structure. A higher dye load was observed for D45 on TiO2. However, D35 based solar cells result in higher photocurrent although the dye load is lower. This is explained by different geometrical structures of the dyes on the surface.

  • 2. Gabrielsson, Erik
    et al.
    Tian, Haining
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Eriksson, Susanna K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Gao, Jiajia
    Chen, Hong
    Li, Fusheng
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Sun, Junliang
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Kloo, Lars
    Hagfeldt, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sun, Licheng
    Dipicolinic acid: a strong anchoring group with tunable redox and spectral behavior for stable dye-sensitized solar cells2015In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 51, no 18, p. 3858-3861Article in journal (Refereed)
    Abstract [en]

    Dipicolinic acidwas investigated as a new anchoring group for DSSCs. A pilot dye (PD2) bearing this new anchoring group was found to adsorb significantly stronger to TiO2 than its cyanoacrylic acid analogue. The electrolyte composition was found to have a strong effect on the photoelectrochemical properties of the adsorbed dye in the device, allowing the dye LUMO energy to be tuned by 0.5 eV. Using a pyridine-free electrolyte, panchromatic absorption of the dye on TiO2 extending to 900 nm has been achieved. Solar cells using PD2 and a Co(bpy)(3) based electrolyte showed unique stability under simulated sunlight and elevated temperatures.

  • 3.
    Lindblad, Rebecka
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Bi, Dongqin
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Park, Byung-wook
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Gorgoi, Mihaela
    Siegbahn, Hans
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Odelius, Michael
    Johansson, Erik M. J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Electronic Structure of TiO2/CH3NH3PbI3 Perovskite Solar Cell Interfaces2014In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 5, no 4, p. 648-653Article in journal (Refereed)
    Abstract [en]

    The electronic structure and chemical composition of efficient CH3NH3PbI3 perovskite solar cell materials deposited onto mesoporous TiO2 were studied using photoelectron spectroscopy with hard X-rays. With this technique, it is possible to directly measure the occupied energy levels of the perovskite as well as the TiO2 buried beneath and thereby determine the energy level matching of the interface. The measurements of the valence levels were in good agreement with simulated density of states, and the investigation gives information on the character of the valence levels. We also show that two different deposition techniques give results indicating similar electronic structures.

  • 4.
    Lindblad, Rebecka
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Jena, Naresh K
    Philippe, Bertrand
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Bi, Dongqin
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Lindblad, Andreas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Mandal, Suman
    Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore, India.
    Pal, Banabir
    Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore, India.
    Sarma, Dipankar Das
    Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore, India.
    Karis, Olof
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Siegbahn, Hans
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Johansson, Erik M.J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Odelius, Michael
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Electronic Structure of CH3NH3PbX3 Perovskites: Dependence on the Halide Moiety2015In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 119, no 4, p. 1818-1825Article in journal (Refereed)
    Abstract [en]

    A combination of measurements using photoelectron spectroscopy and calculations using density functional theory (DFT) was applied to compare the detailed electronic structure of the organolead halide perovskites CH3NH3PbI3 and CH3NH3PbBr3. These perovskite materials are used to absorb light in mesoscopic and planar heterojunction solar cells. The Pb 4f core level is investigated to get insight into the chemistry of the two materials. Valence level measurments are also included showing a shift of the valence band edges where there is a higher binding energy of the edge for the CH3NH3PbBr3 perovskite. These changes are supported by the theoretical calculations which indicate that the differences in electronic structure are mainly caused by the nature of the halide ion rather than structural differences. The combination of photoelectron spectroscopy measurements and electronic structure calculations is essential to disentangle how the valence band edge in organolead halide perovskites is governed by the intrinsic difference in energy levels of the halide ions from the influence of chemical bonding.

  • 5.
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.
    Towards Mixed Molecular Layers for Dye-Sensitized Solar Cells: A Photoelectron Spectroscopy Study2016Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The increasing demand for renewable energy has led to substantial research on different solar cell technologies. The dye-sensitized solar cell (DSC) is a technology utilizing dye molecules for light absorption. Dye molecules are adsorbed to a mesoporous semiconductor surface and after light absorption in the dye, charge separation occurs at this interface. Traditionally, DSCs have used layers of single dye species, but in recent efforts to enhance power conversion efficiency, more complex molecular layers have been designed to increase the light absorption. For example, the most efficient DSCs use a combination of two dye molecules, and such dye co-adsorption is studied in this thesis.

    A key to highly efficient DSCs is to understand the dye/semiconductor interface from a molecular perspective. One way of gaining this understanding is by using an element specific, surface sensitive technique, such as photoelectron spectroscopy (PES).

    In this thesis, PES is used to understand new complex dye/semiconductor interfaces. Dyes adsorbed to semiconductor surfaces are analyzed using PES in terms of geometric and electronic surface structure.  The investigations ultimately target the effects of co-adsorbing dyes with other dyes or co-adsorbents.

    PES shows that Ru dyes can adsorb in mixed configurations to TiO2. Co-adsorption with an organic dye affects the configuration of the Ru dyes. As a consequence, shifts in energy level alignment and increased dye coverage are observed. The dyes are affected at a molecular level in ways beneficial for solar cell performance. This is called collaborative sensitization and is also observed in todays most efficient DSC.

    Dye molecules are generally sensitive to high temperatures and the substantial decrease in power conversion efficiency after heat-treatment can be understood using PES. Furthermore, comparing two mesoscopic TiO2 morphologies used in DSCs show differences in trap state density in the band gap, explaining the photovoltage difference in DSCs comprising these morphologies. Using mixed molecular layers on NiO results in significant improvements of p-type DSC power conversion efficiency. PES shows that changed adsorption configuration contribute to this effect.

    This thesis shows that PES studies can be used to obtain insight into functional properties of complex DSC interfaces at a molecular level.

    List of papers
    1. Geometrical and energetical structural changes in organic dyes for dye-sensitized solar cells probed with photoelectron spectroscopy and DFT
    Open this publication in new window or tab >>Geometrical and energetical structural changes in organic dyes for dye-sensitized solar cells probed with photoelectron spectroscopy and DFT
    Show others...
    2016 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 1, p. 252-260Article in journal (Other academic) Published
    Abstract [en]

    The effects of alkoxy chain length in triarylamine based donor acceptor organic dyes are investigated with respect to the electronic and molecular surface structures on the performance of solar cells and the electron lifetime. The dyes were investigated when adsorbed on TiO2 in a configuration that can be used for dye sensitized solar cells (DSCs). Specifically, the two dyes D35 and D45 were compared using photoelectron spectroscopy (PES) and density functional theory (DFT) calculations. The differences in solar cell characteristics when longer alkoxy chains are introduced in the dye donor unit are attributed to geometrical changes in dye packing while only minor differences were observed in the electronic structure. A higher dye load was observed for D45 on TiO2. However, D35 based solar cells result in higher photocurrent although the dye load is lower. This is explained by different geometrical structures of the dyes on the surface.

    National Category
    Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-230853 (URN)10.1039/c5cp04589d (DOI)000368755500027 ()
    Funder
    Swedish Research CouncilCarl Tryggers foundation Swedish Energy AgencyStandUp
    Available from: 2014-08-31 Created: 2014-08-31 Last updated: 2017-12-05Bibliographically approved
    2. Molecular degradation of D35 and K77 sensitizers when exposed to temperatures exceeding 100 °C investigated by photoelectron spectroscopy
    Open this publication in new window or tab >>Molecular degradation of D35 and K77 sensitizers when exposed to temperatures exceeding 100 °C investigated by photoelectron spectroscopy
    Show others...
    2016 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 12, p. 8598-8607Article in journal (Refereed) Published
    Abstract [en]

    Degradation of the materials in dye-sensitized solar cells at elevated temperatures is critical for use in real applications. Both during fabrication of the solar cell and under real working conditions the solar cells will be exposed to heat. In this work, mesoporous TiO2 electrodes sensitized with the dyes D35 and K77 were subject to heat-treatment and the effects of this were thereafter investigated by photoelectron spectroscopy. For D35 it was found that heat-treatment changes the binding configuration inducing an increased interaction between the sulfur of the linker unit and the TiO2 surface. The interaction resulting from the change in binding configuration also affects the position of the HOMO level, where a shift of + 0.2 eV is observed when heated to 200 degrees C. For K77, parts of the thiocyanate units are detached and the nitrogen atom leaves the electrode whereas sulfur remains on the surface in various forms of sulfurous oxides. The total dye coverage of K77 gets reduced by heat-treatment. The HOMO level gets progressively less pronounced due to a loss of HOMO level electrons as a consequence of the lower dye coverage when heat-treated, which leads to a lower excitation rate and lower efficiency. The results are discussed in the context of performance for dye-sensitized solar cells.

    National Category
    Atom and Molecular Physics and Optics Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-283259 (URN)10.1039/C5CP07921G (DOI)000372249100031 ()26949128 (PubMedID)
    Funder
    Swedish Energy Agency, P221191-5Swedish Research Council FormasSwedish Research Council, 2014-6018, 2012-4721
    Available from: 2016-04-12 Created: 2016-04-12 Last updated: 2017-11-30Bibliographically approved
    3. Coadsorption of Dye Molecules at TiO2 Surfaces: A Photoelectron Spectroscopy Study
    Open this publication in new window or tab >>Coadsorption of Dye Molecules at TiO2 Surfaces: A Photoelectron Spectroscopy Study
    Show others...
    2016 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 120, no 23, p. 12484-12494Article in journal (Refereed) Published
    Abstract [en]

    The effects of coadsorbing the amphiphilic ruthenium-based dye Z907 (cis-bis(isothiocyanato)(2,20-bipyridy1-4,40-dicarboxylato)(4,40-dinony1-20-bipyridy1)-ruthenium(II)) with the coadsorbent DPA (n-decylphosphonic acid) and with the organic dye D35 ((E)-3-(5-(4-(bis(2',4'-dibutoxybiphenyl-4-yl)amino)phenyl)thiophen-2-yl)-2-cyanoacrylic acid) on mesoporous TiO2 were investigated using photoelectron spectroscopy (PES). Z907 is expected to adsorb to the TiO2 surface via the carboxylic acid groups. However, Z907 also shows signs of interacting with the TiO2 via the sulfur of the thiocyanate groups, and this interaction is affected by both the addition of DPA and D35. DPA, when added, exchanges with Z907 at the TiO2 surface, and each Z907 is replaced by six DPA molecules, but it does not affect the energy level alignment between Z907 and TiO2 substantially. Adding D35 to Z907 induces changes in the adsorption configuration of Z907 by the means of suppressing the interaction of the thiocyanate ligands and the TiO2 surface. The HOMO level of Z907 is shifted by the addition of D35. Coadsorbing Z907 with D35 thus gives changes at a molecular level, meaning that this is an example of collaborative sensitization.

    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:uu:diva-299720 (URN)10.1021/acs.jpcc.6b02521 (DOI)000378196200019 ()
    Funder
    Swedish Energy Agency, P221191-5Swedish Research Council FormasSwedish Research Council, 2014-6018 2012-4721
    Available from: 2016-07-26 Created: 2016-07-26 Last updated: 2017-11-28Bibliographically approved
    4. Interface Structure Effects upon Co-Adsorption of Black Dye and D35 on TiO2
    Open this publication in new window or tab >>Interface Structure Effects upon Co-Adsorption of Black Dye and D35 on TiO2
    Show others...
    (English)Manuscript (preprint) (Other academic)
    National Category
    Condensed Matter Physics Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-300851 (URN)
    Available from: 2016-08-18 Created: 2016-08-15 Last updated: 2016-08-25
    5. Mesoporous TiO2 microbead electrodes for solid state dye-sensitized solar cells
    Open this publication in new window or tab >>Mesoporous TiO2 microbead electrodes for solid state dye-sensitized solar cells
    Show others...
    2014 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 4, no 91, p. 50295-50300Article in journal (Refereed) Published
    Abstract [en]

    Mesoporous TiO2 microbead films have been investigated as working electrodes for solid state dye sensitized solar cells and 3.5% efficiency was achieved for 4 micrometer thick films under 1 sun illumination. Compared to conventional mesoporous solar cells, microbead films have higher porosity, increased open circuit voltage, lower fill factor and current density, faster transport time and lower electron lifetime. Cross sectional scanning electron microscopy results show that the pore filling of a solid hole conductor (spiro-OMeTAD) inside the entire mesoporous bead film is very good even for 4 micrometer thick films. The high porosity of the microbead film allows good penetration of spiro in thick films, while its high surface area ensures good dye coverage. X-ray photoelectron spectroscopy data reveals a lower density of intra-bandgap trap states for microbead films compared to conventional mesoporous TiO2 films, which could be in part responsible for faster transport of electrons and higher voltage in microbead films. Optimization of microbead films for solid state dye sensitized solar cells can be an interesting possibility for highly efficient and relatively thick film solid state solar cells.

    National Category
    Chemical Sciences
    Identifiers
    urn:nbn:se:uu:diva-238099 (URN)10.1039/c4ra10049b (DOI)000343715000100 ()
    Available from: 2014-12-15 Created: 2014-12-09 Last updated: 2017-12-05Bibliographically approved
    6. Enhancement of p-Type Dye-Sensitized Solar Cell Performance by Supramolecular Assembly of Electron Donor and Acceptor
    Open this publication in new window or tab >>Enhancement of p-Type Dye-Sensitized Solar Cell Performance by Supramolecular Assembly of Electron Donor and Acceptor
    Show others...
    2014 (English)In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 4, p. 4282-Article in journal (Refereed) Published
    Abstract [en]

    Supramolecular interactions based on porphyrin and fullerene derivatives were successfully adopted to improve the photovoltaic performance of p-type dye-sensitized solar cells (DSCs). Photoelectron spectroscopy (PES) measurements suggest a change in binding configuration of ZnTCPP after co-sensitization with C60PPy, which could be ascribed to supramolecular interaction between ZnTCPP and C60PPy. The performance of the ZnTCPP/C60PPy-based p-type DSC has been increased by a factor of 4 in comparison with the DSC with the ZnTCPP alone. At 560 nm, the IPCE value of DSCs based on ZnTCPP/C60PPy was a factor of 10 greater than that generated by ZnTCPP-based DSCs. The influence of different electrolytes on charge extraction and electron lifetime was investigated and showed that the enhanced V-oc from the Co2+/(3+)(dtbp)(3)-based device is due to the positive E-F shift of NiO.

    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:uu:diva-222728 (URN)10.1038/srep04282 (DOI)000332374500002 ()
    Available from: 2014-04-17 Created: 2014-04-14 Last updated: 2017-12-05
  • 6.
    Oscarsson, Johan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Eriksson K., Susanna
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Lindblad, Rebecka
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Johansson, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Eriksson, Anna I. K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Siegbahn, Hans
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Interface Structure Effects upon Co-Adsorption of Black Dye and D35 on TiO2Manuscript (preprint) (Other academic)
  • 7.
    Oscarsson, Johan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Fredin, Kristofer
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Ahmadi, Sareh
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Eriksson, Anna I. K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Johansson, Erik M. J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Molecular degradation of D35 and K77 sensitizers when exposed to temperatures exceeding 100 °C investigated by photoelectron spectroscopy2016In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 12, p. 8598-8607Article in journal (Refereed)
    Abstract [en]

    Degradation of the materials in dye-sensitized solar cells at elevated temperatures is critical for use in real applications. Both during fabrication of the solar cell and under real working conditions the solar cells will be exposed to heat. In this work, mesoporous TiO2 electrodes sensitized with the dyes D35 and K77 were subject to heat-treatment and the effects of this were thereafter investigated by photoelectron spectroscopy. For D35 it was found that heat-treatment changes the binding configuration inducing an increased interaction between the sulfur of the linker unit and the TiO2 surface. The interaction resulting from the change in binding configuration also affects the position of the HOMO level, where a shift of + 0.2 eV is observed when heated to 200 degrees C. For K77, parts of the thiocyanate units are detached and the nitrogen atom leaves the electrode whereas sulfur remains on the surface in various forms of sulfurous oxides. The total dye coverage of K77 gets reduced by heat-treatment. The HOMO level gets progressively less pronounced due to a loss of HOMO level electrons as a consequence of the lower dye coverage when heat-treated, which leads to a lower excitation rate and lower efficiency. The results are discussed in the context of performance for dye-sensitized solar cells.

  • 8.
    Oscarsson, Johan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Hahlin, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Johansson, Erik M. J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Eriksson, Susanna K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Lindblad, Rebecka
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Eriksson, Anna I. K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.
    Zia, Azhar
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Siegbahn, Hans
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Coadsorption of Dye Molecules at TiO2 Surfaces: A Photoelectron Spectroscopy Study2016In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 120, no 23, p. 12484-12494Article in journal (Refereed)
    Abstract [en]

    The effects of coadsorbing the amphiphilic ruthenium-based dye Z907 (cis-bis(isothiocyanato)(2,20-bipyridy1-4,40-dicarboxylato)(4,40-dinony1-20-bipyridy1)-ruthenium(II)) with the coadsorbent DPA (n-decylphosphonic acid) and with the organic dye D35 ((E)-3-(5-(4-(bis(2',4'-dibutoxybiphenyl-4-yl)amino)phenyl)thiophen-2-yl)-2-cyanoacrylic acid) on mesoporous TiO2 were investigated using photoelectron spectroscopy (PES). Z907 is expected to adsorb to the TiO2 surface via the carboxylic acid groups. However, Z907 also shows signs of interacting with the TiO2 via the sulfur of the thiocyanate groups, and this interaction is affected by both the addition of DPA and D35. DPA, when added, exchanges with Z907 at the TiO2 surface, and each Z907 is replaced by six DPA molecules, but it does not affect the energy level alignment between Z907 and TiO2 substantially. Adding D35 to Z907 induces changes in the adsorption configuration of Z907 by the means of suppressing the interaction of the thiocyanate ligands and the TiO2 surface. The HOMO level of Z907 is shifted by the addition of D35. Coadsorbing Z907 with D35 thus gives changes at a molecular level, meaning that this is an example of collaborative sensitization.

  • 9.
    Pazoki, Meysam
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Yang, L.
    Park, Byung-Wook
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Johansson, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Hagfeldt, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Boschloo, Gerrit
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Mesoporous TiO2 microbead electrodes for solid state dye-sensitized solar cells2014In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 4, no 91, p. 50295-50300Article in journal (Refereed)
    Abstract [en]

    Mesoporous TiO2 microbead films have been investigated as working electrodes for solid state dye sensitized solar cells and 3.5% efficiency was achieved for 4 micrometer thick films under 1 sun illumination. Compared to conventional mesoporous solar cells, microbead films have higher porosity, increased open circuit voltage, lower fill factor and current density, faster transport time and lower electron lifetime. Cross sectional scanning electron microscopy results show that the pore filling of a solid hole conductor (spiro-OMeTAD) inside the entire mesoporous bead film is very good even for 4 micrometer thick films. The high porosity of the microbead film allows good penetration of spiro in thick films, while its high surface area ensures good dye coverage. X-ray photoelectron spectroscopy data reveals a lower density of intra-bandgap trap states for microbead films compared to conventional mesoporous TiO2 films, which could be in part responsible for faster transport of electrons and higher voltage in microbead films. Optimization of microbead films for solid state dye sensitized solar cells can be an interesting possibility for highly efficient and relatively thick film solid state solar cells.

  • 10.
    Philippe, Bertrand
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Park, Byung-Wook
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Lindblad, Rebecka
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Ahmadi, Sareh
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Johansson, Erik M. J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Chemical and Electronic Structure Characterization of Lead Halide Perovskites and Stability Behavior under Different Exposures-A Photoelectron Spectroscopy Investigation2015In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 27, no 5, p. 1720-1731Article in journal (Refereed)
    Abstract [en]

    The past few years, two perovskite materials have attracted much attention in the solar cell community: CH3NH3PbI3 and CH3NH3PbI3xClx. While these materials are usually characterized using their structure (via X-ray diffraction (XRD)) and performance within solar cell communities, not so much attention has been devoted to their surface chemical composition and, specifically, the surface composition. Photoelectron spectroscopy (PES) can easily fulfill this task, and, in addition to chemical information, PES provides an overall picture of the electronic structure of the perovskite and its relation to mesoporous TiO2 when studied with hard X-rays. In this work, CH3NH3PbI3 and CH3NH3PbI3xClx have been compared with each other and also to CH3NH3PbI3, and it appears that, despite very different morphologies and kinetics of formation, the two former materials present a very similar electronic structure and chemical composition (i.e., no chlorine is observed in the final CH3NH3PbI3xClx materials). Nevertheless, chlorine is very important during the preparation, because it affects the formation of crystalline CH3NH3PbI3. We have also exposed the classical CH3NH3PbI3 to various environments, such as water, temperature, and long-time storage in air and argon, and followed changes of the surface composition with PES. The main result of the different exposures is that the perovskite is decomposed into PbI2, but an important point is that this degradation seems to occur already at 100 degrees C and is not only related to large humidity. Indeed, even in an inert atmosphere such as argon, a slow degradation to PbI2 is observed. The results obtained are crucial for a better understanding of this material and will help to improve not only the post-conditioning of the cells but also their synthesis.

  • 11.
    Tian, Haining
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Oscarsson, Johan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Gabrielsson, Erik
    KTH, Stockholm.
    Eriksson, Susanna K.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Lindblad, Rebecka
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Xu, Bo
    Hao, Yan
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Boschloo, Gerrit
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Johansson, Erik M. J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Gardner, James M.
    Hagfeldt, Anders
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Rensmo, Håkan
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
    Sun, Licheng
    KTH, Stockholm.
    Enhancement of p-Type Dye-Sensitized Solar Cell Performance by Supramolecular Assembly of Electron Donor and Acceptor2014In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 4, p. 4282-Article in journal (Refereed)
    Abstract [en]

    Supramolecular interactions based on porphyrin and fullerene derivatives were successfully adopted to improve the photovoltaic performance of p-type dye-sensitized solar cells (DSCs). Photoelectron spectroscopy (PES) measurements suggest a change in binding configuration of ZnTCPP after co-sensitization with C60PPy, which could be ascribed to supramolecular interaction between ZnTCPP and C60PPy. The performance of the ZnTCPP/C60PPy-based p-type DSC has been increased by a factor of 4 in comparison with the DSC with the ZnTCPP alone. At 560 nm, the IPCE value of DSCs based on ZnTCPP/C60PPy was a factor of 10 greater than that generated by ZnTCPP-based DSCs. The influence of different electrolytes on charge extraction and electron lifetime was investigated and showed that the enhanced V-oc from the Co2+/(3+)(dtbp)(3)-based device is due to the positive E-F shift of NiO.

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