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Naji, M. |
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Motta, Antonella |
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Aletan, Dirar |
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Mohamed, Tarek |
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Ertürk, Emre |
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Taccardi, Nicola |
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Kononenko, Denys |
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Petrov, R. H. | Madrid |
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Alshaaer, Mazen | Brussels |
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Bih, L. |
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Casati, R. |
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Muller, Hermance |
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Kočí, Jan | Prague |
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Šuljagić, Marija |
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Kalteremidou, Kalliopi-Artemi | Brussels |
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Azam, Siraj |
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Ospanova, Alyiya |
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Blanpain, Bart |
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Ali, M. A. |
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Popa, V. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Landes, Michael |
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Rignanese, Gian-Marco |
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Uhlig, Jens
Lund University
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (20/20 displayed)
- 2024Synthesis of well-ordered functionalized silicon microwires using displacement talbot lithography for photocatalysis
- 2022Iridium Catalyzed Dehydrogenation in a Continuous Flow Reactor as a Tool Towards Practical On-Board Hydrogen Generation From LOHCscitations
- 2022Photophysical Integrity of the Iron(III) Scorpionate Framework in Iron(III)-NHC Complexes with Long-Lived 2LMCT Excited Statescitations
- 2022Iridium‐Catalyzed Dehydrogenation in a Continuous Flow Reactor for Practical On‐Board Hydrogen Generation From Liquid Organic Hydrogen Carrierscitations
- 2021Dye-sensitized solar cells based on Fe N-heterocyclic carbene photosensitizers with improved rod-like push-pull functionalitycitations
- 2020Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering.citations
- 2020Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering.citations
- 2020Hot branching dynamics in a light‐harvesting iron carbene complex revealed by ultrafast x‐ray emission spectroscopycitations
- 2020Hot branching dynamics in a light‐harvesting iron carbene complex revealed by ultrafast x‐ray emission spectroscopycitations
- 2020Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scatteringcitations
- 2020Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scatteringcitations
- 2020Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scatteringcitations
- 2020More than protection : the function of TiO2 interlayers in hematite functionalized Si photoanodescitations
- 2020More than protection : The function of TiO2interlayers in hematite functionalized Si photoanodescitations
- 2020More than protection: the function of TiO2 interlayers in hematite functionalized Si photoanodescitations
- 2019Finding intersections between electronic excited state potential energy surfaces with simultaneous ultrafast X-ray scattering and spectroscopy.citations
- 2019Finding intersections between electronic excited state potential energy surfaces with simultaneous ultrafast X-ray scattering and spectroscopycitations
- 2019Hot Branching Dynamics in a Light-Harvesting Iron Carbene Complex Revealed by Ultrafast X-ray Emission Spectroscopy.citations
- 2017Ultrafast Electron Dynamics in Solar Energy Conversioncitations
- 2005Thin-film technology for HTSC Josephson devicescitations
Places of action
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article
Dye-sensitized solar cells based on Fe N-heterocyclic carbene photosensitizers with improved rod-like push-pull functionality
Abstract
A new generation of octahedral iron(ii)-N-heterocyclic carbene (NHC) complexes, employing different tridentate C^N^C ligands, has been designed and synthesized as earth-abundant photosensitizers for dye sensitized solar cells (DSSCs) and related solar energy conversion applications. This work introduces a linearly aligned push-pull design principle that reaches from the ligand having nitrogen-based electron donors, over the Fe(ii) centre, to the ligand having an electron withdrawing carboxylic acid anchor group. A combination of spectroscopy, electrochemistry, and quantum chemical calculations demonstrate the improved molecular excited state properties in terms of a broader absorption spectrum compared to the reference complex, as well as directional charge-transfer displacement of the lowest excited state towards the semiconductor substrate in accordance with the push-pull design. Prototype DSSCs based on one of the new Fe NHC photosensitizers demonstrate a power conversion efficiency exceeding 1% already for a basic DSSC set-up using only the I−/I3−redox mediator and standard operating conditions, outcompeting the corresponding DSSC based on the homoleptic reference complex. Transient photovoltage measurements confirmed that adding the co-sensitizer chenodeoxycholic acid helped in improving the efficiency by increasing the electron lifetime in TiO2. Time-resolved spectroscopy revealed spectral signatures for successful ultrafast (<100 fs) interfacial electron injection from the heteroleptic dyes to TiO2. However, an ultrafast recombination process results in undesirable fast charge recombination from TiO2back to the oxidized dye, leaving only 5-10% of the initially excited dyes available to contribute to a current in the DSSC. On slower timescales, time-resolved spectroscopy also found that the recombination dynamics (longer than 40 μs) were significantly slower than the regeneration of the oxidized dye by the redox mediator (6-8 μs). Therefore it is the ultrafast recombination down to fs-timescales, ...