| 1. |
- Abdi-Jalebi, Mojtaba, et al.
(författare)
-
Maximizing and stabilizing luminescence from halide perovskites with potassium passivation
- 2018
-
Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 555, s. 497-501
-
Tidskriftsartikel (refereegranskat)abstract
- Metal halide perovskites are of great interest for various high-performance optoelectronic applications. The ability to tune the perovskite bandgap continuously by modifying the chemical composition opens up applications for perovskites as coloured emitters, in building-integrated photovoltaics, and as components of tandem photovoltaics to increase the power conversion efficiency. Nevertheless, performance is limited by non-radiative losses, with luminescence yields in state-of-the-art perovskite solar cells still far from 100 per cent under standard solar illumination conditions. Furthermore, in mixed halide perovskite systems designed for continuous bandgap tunability2 (bandgaps of approximately 1.7 to 1.9 electronvolts), photoinduced ion segregation leads to bandgap instabilities. Here we demonstrate substantial mitigation of both non-radiative losses and photoinduced ion migration in perovskite films and interfaces by decorating the surfaces and grain boundaries with passivating potassium halide layers. We demonstrate external photoluminescence quantum yields of 66 per cent, which translate to internal yields that exceed 95 per cent. The high luminescence yields are achieved while maintaining high mobilities of more than 40 square centimetres per volt per second, providing the elusive combination of both high luminescence and excellent charge transport. When interfaced with electrodes in a solar cell device stack, the external luminescence yield—a quantity that must be maximized to obtain high efficiency—remains as high as 15 per cent, indicating very clean interfaces. We also demonstrate the inhibition of transient photoinduced ion-migration processes across a wide range of mixed halide perovskite bandgaps in materials that exhibit bandgap instabilities when unpassivated. We validate these results in fully operating solar cells. Our work represents an important advance in the construction of tunable metal halide perovskite films and interfaces that can approach the efficiency limits in tandem solar cells, coloured-light-emitting diodes and other optoelectronic applications.
|
|
| 2. |
- Caligiuri, Vincenzo, et al.
(författare)
-
Dry synthesis of bi-layer nanoporous metal films as plasmonic metamaterial
- 2024
-
Ingår i: Nanophotonics. - : Walter de Gruyter. - 2192-8606 .- 2192-8614. ; 13:7, s. 1159-1167
-
Tidskriftsartikel (refereegranskat)abstract
- Nanoporous metals are a class of nanostructured materials finding extensive applications in multiple fields thanks to their unique properties attributed to their high surface area and interconnected nanoscale ligaments. They can be prepared following different strategies, but the deposition of an arbitrary pure porous metal is still challenging. Recently, a dry synthesis of nanoporous films based on the plasma treatment of metal thin layers deposited by physical vapour deposition has been demonstrated, as a general route to form pure nanoporous films from a large set of metals. An interesting aspect related to this approach is the possibility to apply the same methodology to deposit the porous films as a multilayer. In this way, it is possible to explore the properties of different porous metals in close contact. As demonstrated in this paper, interesting plasmonic properties emerge in a nanoporous Au–Ag bi-layer. The versatility of the method coupled with the possibility to include many different metals, provides an opportunity to tailor their optical resonances and to exploit the chemical and mechanical properties of components, which is of great interest to applications ranging from sensing, to photochemistry and photocatalysis.
|
|
| 3. |
- Jalebi, Mojtaba Abdi, et al.
(författare)
-
Potassium- and Rubidium-Passivated Alloyed Perovskite Films : Optoelectronic Properties and Moisture Stability
- 2018
-
Ingår i: ACS Energy Letters. - : American Chemical Society (ACS). - 2380-8195. ; 3:11, s. 2671-2678
-
Tidskriftsartikel (refereegranskat)abstract
- Halide perovskites passivated with potassium or rubidium show superior photovoltaic device performance compared to unpassivated samples. However, it is unclear which passivation route is more effective for film stability. Here, we directly compare the optoelectronic properties and stability of thin films when passivating triple-cation perovskite films with potassium or rubidium species. The optoelectronic and chemical studies reveal that the alloyed perovskites are tolerant toward higher loadings of potassium than rubidium. Whereas potassium complexes with bromide from the perovskite precursor solution to form thin surface passivation layers, rubidium additives favor the formation of phase-segregated micron-sized rubidium halide crystals. This tolerance to higher loadings of potassium allows us to achieve superior passivation. We also find that exposure to a humid atmosphere drives phase luminescent properties with potassium segregation and grain coalescence for all compositions, with the rubidium-passivated sample showing the highest sensitivity to nonperovskite phase formation. Our work highlights the benefits but also the limitations of these passivation approaches in maximizing both optoelectronic properties and the stability of perovskite films.
|
|
| 4. |
- Orsborne, Sarah R.E., et al.
(författare)
-
Photogeneration of Spin Quintet Triplet-Triplet Excitations in DNA-Assembled Pentacene Stacks
- 2023
-
Ingår i: Journal of the American Chemical Society. - : American Chemical Society. - 0002-7863 .- 1520-5126. ; 145:9, s. 5431-5438
-
Tidskriftsartikel (refereegranskat)abstract
- Singlet fission (SF), an exciton-doubling process observed in certain molecular semiconductors where two triplet excitons are generated from one singlet exciton, requires correctly tuned intermolecular coupling to allow separation of the two triplets to different molecular units. We explore this using DNA-encoded assembly of SF-capable pentacenes into discrete π-stacked constructs of defined size and geometry. Precise structural control is achieved via a combination of the DNA duplex formation between complementary single-stranded DNA and the local molecular geometry that directs the SF chromophores into a stable and predictable slip-stacked configuration, as confirmed by molecular dynamics (MD) modeling. Transient electron spin resonance spectroscopy revealed that within these DNA-assembled pentacene stacks, SF evolves via a bound triplet pair quintet state, which subsequently converts into free triplets. SF evolution via a long-lived quintet state sets specific requirements on intermolecular coupling, rendering the quintet spectrum and its zero-field-splitting parameters highly sensitive to intermolecular geometry. We have found that the experimental spectra and zero-field-splitting parameters are consistent with a slight systematic strain relative to the MD-optimized geometry. Thus, the transient electron spin resonance analysis is a powerful tool to test and refine the MD-derived structure models. DNA-encoded assembly of coupled semiconductor molecules allows controlled construction of electronically functional structures, but brings with it significant dynamic and polar disorders. Our findings here of efficient SF through quintet states demonstrate that these conditions still allow efficient and controlled semiconductor operation and point toward future opportunities for constructing functional optoelectronic systems.
|
|
