| 1. |
- Erbing, Axel, 1991-, et al.
(författare)
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Spatial microheterogeneity in the valence band of mixed halide hybrid perovskite materials
- 2022
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 13:32, s. 9285-9294
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Tidskriftsartikel (refereegranskat)abstract
- The valence band of lead halide hybrid perovskites with a mixed I/Br composition is investigated using electronic structure calculations and complementarily probed with hard X-ray photoelectron spectroscopy. In the latter, we used high photon energies giving element sensitivity to the heavy lead and halide ions and we observe distinct trends in the valence band as a function of the I : Br ratio. Through electronic structure calculations, we show that the spectral trends with overall composition can be understood in terms of variations in the local environment of neighboring halide ions. From the computational model supported by the experimental evidence, a picture of the microheterogeneity in the valence band maximum emerges. The microheterogeneity in the valence band suggests that additional charge transport mechanisms might be active in lead mixed halide hybrid perovskites, which could be described in terms of percolation pathways.
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| 2. |
- Vijayan, Anuja, et al.
(författare)
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Simple Method for Efficient Slot-Die Coating of MAPbI(3) Perovskite Thin Films in Ambient Air Conditions
- 2020
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 3:5, s. 4331-4337
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Tidskriftsartikel (refereegranskat)abstract
- Scalable methods for deposition of lead halide perovskite thin films are required to enable commercialization of the highly promising perovskite photovoltaics. Here, we have developed a slot-die coating process under ambient conditions for methylammonium lead iodide (MAPbI(3)) perovskite on heated substrates (about 90 degrees C on the substrate surface). Dense, highly crystalline perovskite films with large grains (100-200 mu m) were obtained by careful adjustment of the deposition parameters, using solutions that are similar but more dilute than those used in typical spin-coating procedures. Without any further after treatments, such as antisolvent treatment or vapor annealing, we achieved power conversion efficiencies up of 14.5% for devices with the following structure: conducting tin oxide glass (FTO)/TiO2/MAPbI(3)/spiro-MeOTAD/Au. The performance was limited by the significant roughness of the deposited films, resulting from the hot-casting method, and the relatively high deposition temperature, which led to a defect-rich surface due to loss of MAI.
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| 3. |
- Zhang, Xiaoliang, et al.
(författare)
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Inorganic CsPbI3 Perovskite Coating on PbS Quantum Dot for Highly Efficient and Stable Infrared Light Converting Solar Cells
- 2018
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Ingår i: Advanced Energy Materials. - : Wiley-VCH Verlagsgesellschaft. - 1614-6832 .- 1614-6840. ; 8:6
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Tidskriftsartikel (refereegranskat)abstract
- Solution-processed colloidal quantum dot (CQD) solar cells harvesting the infrared part of the solar spectrum are especially interesting for future use in semitransparent windows or multilayer solar cells. To improve the device power conversion efficiency (PCE) and stability of the solar cells, surface passivation of the quantum dots is vital in the research of CQD solar cells. Herein, inorganic CsPbI3 perovskite (CsPbI3-P) coating on PbS CQDs with a low-temperature, solution-processed approach is reported. The PbS CQD solar cell with CsPbI3-P coating gives a high PCE of 10.5% and exhibits remarkable stability both under long-term constant illumination and storage under ambient conditions. Detailed characterization and analysis reveal improved passivation of the PbS CQDs with the CsPbI3-P coating, and the results suggest that the lattice coherence between CsPbI3-P and PbS results in epitaxial induced growth of the CsPbI3-P coating. The improved passivation significantly diminishes the sub-bandgap trap-state assisted recombination, leading to improved charge collection and therefore higher photovoltaic performance. This work therefore provides important insight to improve the CQD passivation by coating with an inorganic perovskite ligand for photovoltaics or other optoelectronic applications.
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| 4. |
- Ali, Azmat, et al.
(författare)
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The Electronic Impact of Light-Induced Degradation in CsPbBr3 Perovskite Nanocrystals at Gold Interfaces
- 2024
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Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 15:14, s. 3721-3727
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Tidskriftsartikel (refereegranskat)abstract
- The understanding of the interfacial properties in perovskite devices under irradiation is crucial for their engineering. In this study we show how the electronic structure of the interface between CsPbBr3 perovskite nanocrystals (PNCs) and Au is affected by irradiation of X-rays, near-infrared (NIR), and ultraviolet (UV) light. The effects of X-ray and light exposure could be differentiated by employing low-dose X-ray photoelectron spectroscopy (XPS). Apart from the common degradation product of metallic lead (Pb0), a new intermediate component (Pbint) was identified in the Pb 4f XPS spectra after exposure to high intensity X-rays or UV light. The Pbint component is determined to be monolayer metallic Pb on-top of the Au substrate from underpotential deposition (UPD) of Pb induced from the breaking of the perovskite structure allowing for migration of Pb2+.
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| 5. |
- Andaji-Garmaroudi, Z., et al.
(författare)
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Elucidating and Mitigating Degradation Processes in Perovskite Light-Emitting Diodes
- 2020
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Ingår i: Advanced Energy Materials. - : Wiley-VCH Verlag. - 1614-6832 .- 1614-6840. ; 10:48
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Tidskriftsartikel (refereegranskat)abstract
- Halide perovskites have attracted substantial interest for their potential as disruptive display and lighting technologies. However, perovskite light-emitting diodes (PeLEDs) are still hindered by poor operational stability. A fundamental understanding of the degradation processes is lacking but will be key to mitigating these pathways. Here, a combination of in operando and ex situ measurements to monitor the performance degradation of (Cs0.06FA0.79MA0.15)Pb(I0.85Br0.15)3 PeLEDs over time is used. Through device, nanoscale cross-sectional chemical mapping, and optical spectroscopy measurements, it is revealed that the degraded performance arises from an irreversible accumulation of bromide content at one interface, which leads to barriers to injection of charge carriers and thus increased nonradiative recombination. This ionic segregation is impeded by passivating the perovskite films with potassium halides, which immobilizes the excess halide species. The passivated PeLEDs show enhanced external quantum efficiency (EQE) from 0.5% to 4.5% and, importantly, show significantly enhanced stability, with minimal performance roll-off even at high current densities (>200 mA cm−2). The decay half-life for the devices under continuous operation at peak EQE increases from <1 to ≈15 h through passivation, and ≈200 h under pulsed operation. The results provide generalized insight into degradation pathways in PeLEDs and highlight routes to overcome these challenges.
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| 6. |
- Berggren, Elin, et al.
(författare)
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Charge Transfer in the P(g42T-T) : BBL Organic Polymer Heterojunction Measured with Core-Hole Clock Spectroscopy
- 2023
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 127:49, s. 23733-23742
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Tidskriftsartikel (refereegranskat)abstract
- The conductivity of organic polymer heterojunction devices relies on the electron dynamics occurring along interfaces between the acceptor and donor moieties. To investigate these dynamics with chemical specificity, spectroscopic techniques are employed to obtain localized snapshots of the electron behavior at selected interfaces. In this study, charge transfer in blends (by weight 10, 50, 90, and 100%) of p-type polymer P(g(4)2T-T) (bithiophene-thiophene) and n-type polymer BBL (poly(benzimidazo-benzo-phenanthroline)) was measured by resonant Auger spectroscopy. Electron spectra emanating from the decay of core-excited states created upon X-ray absorption in the donor polymer P(g(4)2T-T) were measured in the sulfur KL2,3L2,3 Auger kinetic energy region as a function of the excitation energy. By tuning the photon energy across the sulfur K-absorption edge, it is possible to differentiate between decay paths in which the core-excited electron remained on the atom with the core-hole and those where it tunneled away. Analyzing the competing decay modes of these localized and delocalized (charge-transfer) processes facilitated the computation of charge-transfer times as a function of excitation energy using the core-hole clock method. The electron delocalization times derived from the measurements were found to be in the as/fs regime for all polymer blends, with the fastest charge transfer occurring in the sample with an equal amount of donor and acceptor polymer. These findings highlight the significance of core-hole clock spectroscopy as a chemically specific tool for examining the local charge tunneling propensity, which is fundamental to understanding macroscopic conductivity. Additionally, the X-ray absorption spectra near the sulfur K-edge in the P(g(4)2T-T) polymer for different polymer blends were analyzed to compare molecular structure, orientation, and ordering in the polymer heterojunctions. The 50% donor sample exhibited the most pronounced angular dependence of absorption, indicating a higher level of ordering compared to the other weight blends. Our studies on the electron dynamics of this type of all-polymer donor-acceptor systems, in which spontaneous ground-state electron transfer occurs, provide us with critical insights to further advance the next generation of organic conductors with mixed electron-hole conduction characteristics suitable for highly stable electrodes of relevance for electronic, electrochemical, and optoelectronic applications.
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| 7. |
- Cappel, Ute B., et al.
(författare)
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A broadly absorbing perylene dye for solid-state dye-sensitized solar cells.
- 2009
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 113:33, s. 14595-14597
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Tidskriftsartikel (refereegranskat)abstract
- We present a new perylene sensitizer, ID 176, for dye-sensitized solar cells (DSCs). The dye has the capability for very high photocurrents due to strong absorption from 400 to over 700 rim. Photocurrents Of LIP to 9 mA cm(-2) were achieved in solid-state DSCs employing the hole conductor 2,2'7,7'-tetrakis-(NN-di-p-methoxyphenylamine)-9,9'-spirobifluorene (spiro-MeOTAD), with a conversion efficiency of 3.2%. In contrast, the sensitizer did not perform well in conjunction with liquid iodide/tri-iodide electrolytes, suggesting a difference in the injection and regeneration mechanisms in these two types of dye-sensitized solar cells.
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| 8. |
- Cappel, Ute B., et al.
(författare)
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Characterization of the Interface Properties and Processes in Solid State Dye-Sensitized Solar Cells Employing a Perylene Sensitizer
- 2011
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 115:10, s. 4345-4358
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Tidskriftsartikel (refereegranskat)abstract
- We recently reported on a perylene sensitizer, ID176, which performs much better in solid state dye-sensitized solar cells than in those using liquid electrolytes with iodide/tri-iodide as the redox couple (J. Phys. Chem. C2009, 113, 14595-14597). Here, we present a characterization of the sensitizer and of the TiO2/dye interface by UV-visible absorption and fluorescence spectroscopy, spectroelectrochemistry, photoelectron spectroscopy, electroabsorption spectroscopy, photoinduced absorption spectroscopy, and femtosecond transient absorption measurements. We report that the absorption spectrum of the sensitizer is red-shifted by addition of lithium ions to the surface due to a downward shift of the excited state level of the sensitizer, which is of the same order of magnitude as the downward shift of the titanium dioxide conduction band edge. Results from photoelectron spectroscopy and electrochemistry suggest that the excited state is largely located below the conduction band edge of TiO2 but that there are states in the band gap of TiO2 which might be available for photoinduced electron injection. The sensitizer was able to efficiently inject into TiO2, when a lithium salt was present on the surface, while injection was much less effective in the absence of lithium ions or in the presence of solvent. In the presence of the hole conductor 2,2-,7,7-tetrakis-(N,N-di-p-methoxyphenyl-amine)-9,9-spirobifluorene (spiro-MeOTAD) and LiTFSI, charge separation was monitored by the emergence of a Stark shift of the dye in transient absorption spectra, and both injection and regeneration appear to be completed within 1 ps. Regeneration by spiro-MeOTAD is therefore several orders of magnitude faster than regeneration by iodide, and ID176 can even be photoreduced by spiro-MeOTAD.
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| 9. |
- Cappel, Ute B, et al.
(författare)
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Charge Generation Dynamics in CdS : P3HT Blends for Hybrid Solar Cells.
- 2013
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185 .- 1948-7185. ; 4:24, s. 4253-7
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Tidskriftsartikel (refereegranskat)abstract
- Development of design rules for hybrid inorganic-organic solar cells through understanding charge generation and recombination dynamics is an important pathway for the improvement of solar cell conversion efficiencies. In this Letter, we study the dynamics of charge generation in CdS:polymer blends by transient absorption spectroscopy. We show that charge generation following excitation of the inorganic component is highly efficient and can occur up to a few nanoseconds after excitation, allowing for diffusion of charges within the inorganic component to an interface. In contrast, charge generation following excitation of the organic component occurs on subpicosecond time scales but suffers from two loss processes, incomplete exciton dissociation and geminate recombination.
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| 10. |
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