| 1. |
- Liu, Yong-feng, et al.
(författare)
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Highly Soluble CsPbBr3 Perovskite Quantum Dots for Solution-Processed Light-Emission Devices
- 2021
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Ingår i: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; , s. 1162-1174
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Tidskriftsartikel (refereegranskat)abstract
- We report on the synthesis of CsPbBr3 perovskite quantum dots (PeQDs) with a high solubility of 75 g/L in toluene and a good film-forming property, as enabled by a dense layer of didodecyldimethylammonium bromide and octanoic acid surface ligands. The crystalline and monodisperse PeQDs feature a cubic-like shape, with an edge length of 10.1 nm, and a high photoluminescence quantum yield of greater than 90% in toluene solution and 36% as a thin film. We find that the PeQDs are n-type doped following the synthesis but also that they can be p-type and additionally n-type doped by in situ electrochemistry. These combined properties render the PeQDs interesting for the emitter in solution-processed light-emitting electrochemical cells (LECs), and we report a PeQD-LEC with air-stabile electrodes that emits with a narrow emission spectrum (λpeak = 514 nm, full width at half-maximum = 24 nm) and a luminance of 250 cd/m2 at 4 V and a luminance of 1090 cd/m2 at 6.8 V. To reach this performance, it was critical to include a thin solution-processed layer comprising p-type poly(vinyl carbazole) and a tetrahexylammonium tetrafluoroborate ionic liquid between the PeQD emission layer and the anode in order to compensate for the as-synthesized n-type doping of the PeQDs.
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| 2. |
- Xu, Weidong, 1988-, et al.
(författare)
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Rational molecular passivation for high-performance perovskite light-emitting diodes
- 2019
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Ingår i: Nature Photonics. - : Springer Nature Publishing AG. - 1749-4885 .- 1749-4893. ; 13:6, s. 418-424
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Tidskriftsartikel (refereegranskat)abstract
- A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecules has been identified as an attractive approach to tackle this issue. However, implementation of this approach has been hindered by a lack of deep understanding of how the molecular structures influence the effectiveness of passivation. We show that the so far largely ignored hydrogen bonds play a critical role in affecting the passivation. By weakening the hydrogen bonding between the passivating functional moieties and the organic cation featuring in the perovskite, we significantly enhance the interaction with defect sites and minimize non-radiative recombination losses. Consequently, we achieve exceptionally high-performance near-infrared perovskite light-emitting diodes with a record external quantum efficiency of 21.6%. In addition, our passivated perovskite light-emitting diodes maintain a high external quantum efficiency of 20.1% and a wall-plug efficiency of 11.0% at a high current density of 200 mA cm−2, making them more attractive than the most efficient organic and quantum-dot light-emitting diodes at high excitations.
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| 3. |
- Chen, Zhan, et al.
(författare)
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Photoluminescence Enhancement for Efficient Mixed-Halide Blue Perovskite Light-Emitting Diodes
- 2023
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Ingår i: Advanced Optical Materials. - : WILEY-V C H VERLAG GMBH. - 2162-7568 .- 2195-1071. ; 11:6
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Tidskriftsartikel (refereegranskat)abstract
- The development of highly efficient blue perovskite light-emitting diodes (PeLEDs) remains a big challenge, requiring more fundamental investigations. In this work, significant photoluminescence enhancement in mixed halide blue perovskite films is demonstrated by using a molecule, benzylphosphonic acid, which eventually doubles the external quantum efficiency to 6.3% in sky-blue PeLEDs. The photoluminescence enhancement is achieved by forming an oxide-bonded perovskite surface at grain boundaries and suppressing electron-phonon interaction, which enhances the radiative recombination rate and reduces the nonradiative recombination rate, respectively. Moreover, severe thermal quenching is observed in the blue perovskite films, which can be explained by a two-step mechanism involving exciton dissociation and electron-phonon interaction. The results suggest that enhancing the radiative recombination rate and reducing the electron-phonon interaction-induced nonradiative recombination rate are crucial for achieving blue perovskite films with strong emission at or above room temperature.
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| 4. |
- Qin, Leiqiang, 1987-, et al.
(författare)
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Flexible Solid-State Asymmetric Supercapacitors with Enhanced Performance Enabled by Free-Standing MXene-Biopolymer Nanocomposites and Hierarchical Graphene-RuOx Paper Electrodes
- 2020
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Ingår i: Batteries & Supercaps. - : WILEY-V C H VERLAG GMBH. - 2566-6223. ; 3:7, s. 604-610
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional (2D) transition metal carbides and carbonitrides, called MXenes, with metallic conductivity and hydrophilic surfaces, show great promise as electrode materials for supercapacitors. A major drawback of 2D nanomaterials is the re-stacking of the nanosheets, which prevents full utilization of surface area and blocks the access of the electrolyte. In this study, a free-standing nanocomposite paper electrode is realized by combining Mo1.33C MXene and positively charged biopolymer lignin (the second most abundant biopolymer in nature, L-DEA). The self-assembled layered architecture with alternating polymer and MXene flakes increases the interlayer space to promote ion transport, and with combining charge storage capability of the lignin derivative and MXene in an interpenetrating MXene/L-DEA nanocomposite, which offers an impressive capacitance of 503.7 F g(-1). Moreover, we demonstrate flexible solid-state asymmetric supercapacitors (ASCs) using Mo1.33C@L-DEA as the negative electrode and electrochemically exfoliated graphene with ruthenium oxide (EG@RuOx) as the positive electrode. This asymmetric device operates at a voltage window of 1.35 V, which is about two times wider than that of a symmetric Mo1.33C@L-DEA based supercapacitor. Finally, the ASCs can deliver an energy density of 51.9 Wh kg(-1) at a power density of 338.5 W kg(-1), with 86 % capacitance retention after 10000 charge-discharge cycles.
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| 5. |
- Adam, Rania Elhadi, 1978-, et al.
(författare)
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Graphene-based plasmonic nanocomposites for highly enhanced solar-driven photocatalytic activities
- 2019
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Ingår i: RSC Advances. - Cambridge : Royal Meteorological Society. - 2046-2069. ; 9:52, s. 30585-30598
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Tidskriftsartikel (refereegranskat)abstract
- High-efficiency photocatalysts are crucial for the removal of organic pollutants and environmental sustainability. In the present work, we report on a new low-temperature hydrothermal chemical method, assisted by ultrasonication, to synthesize disruptive plasmonic ZnO/graphene/Ag/AgI nanocomposites for solar-driven photocatalysis. The plasmonic nanocomposites were investigated by a wide range of characterization techniques, confirming successful formation of photocatalysts with excellent degradation efficiency. Using Congo red as a model dye molecule, our experimental results demonstrated a photocatalytic reactivity exceeding 90% efficiency after one hour simulated solar irradiation. The significantly enhanced degradation efficiency is attributed to improved electronic properties of the nanocomposites by hybridization of the graphene and to the addition of Ag/AgI which generates a strong surface plasmon resonance effect in the metallic silver further improving the photocatalytic activity and stability under solar irradiation. Scavenger experiments suggest that superoxide and hydroxyl radicals are responsible for the photodegradation of Congo red. Our findings are important for the fundamental understanding of the photocatalytic mechanism of ZnO/graphene/Ag/AgI nanocomposites and can lead to further development of novel efficient photocatalyst materials.
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| 6. |
- Adam, Rania Elhadi, 1978-, et al.
(författare)
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Synthesis of Mg-doped ZnO NPs via a chemical low-temperature method and investigation of the efficient photocatalytic activity for the degradation of dyes under solar light
- 2020
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Ingår i: Solid State Sciences. - : Elsevier. - 1293-2558 .- 1873-3085. ; 99
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Tidskriftsartikel (refereegranskat)abstract
- Doped semiconductors nanostructures (NSs) have shown great interest as a potential for green and efficient photocatalysis activities. Magnesium (Mg)-doped zinc oxide (ZnO) nanoparticles (NPs) has been synthesized by a one-step chemical low temperature (60 °C) co-precipitation method without further calcination and their photocatalytic performance for photodegradation of Methylene blue (MB) dye under the illumination of solar light is investigated. The crystal structure of the synthesized NPs is examined by X-ray diffraction (XRD). XRD data indicates a slight shift towards higher 2θ angle in Mg-doped samples as compared to the pure ZnO NPs which suggest the incorporation of Mg2+ into ZnO crystal lattice. X-ray photoelectron spectroscopy (XPS), UV–Vis spectrophotometer and cathodoluminescence (CL) spectroscopy, were used to study electronics, and optical properties, respectively. The XPS analysis confirms the substitution of the Zn2+ by the Mg2+ into the ZnO crystal lattice in agreement with the XRD data. The photocatalytic activities showed a significant enhancement of the Mg-doped ZnO NPs in comparison with pure ZnO NPs. Hole/radical scavengers were used to reveal the mechanism of the photodegradation. It was found that the addition of the Mg to the ZnO lattices increases the absorption of the hydroxyl ions at the surface of the NPs and hence acts as a trap site leading to decrease the electron-hole pair and consequently enhancing the photodegradation.
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| 7. |
- Chen, Jing-De, et al.
(författare)
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Hot-electron emission-driven energy recycling in transparent plasmonic electrode for organic solar cells
- 2022
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Ingår i: InfoMat. - : Wiley. - 2567-3165. ; 4:3
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Tidskriftsartikel (refereegranskat)abstract
- Plasmonic metal electrodes with subwavelength nanostructures are promising for enhancing light harvesting in photovoltaics. However, the nonradiative damping of surface plasmon polaritons (SPPs) during coupling with sunlight results in the conversion of the excited hot-electrons to heat, which limits the absorption of light and generation of photocurrent. Herein, an energy recycling strategy driven by hot-electron emission for recycling the SPP energy trapped in the plasmonic electrodes is proposed. A transparent silver-based plasmonic metal electrode (A-PME) with a periodic hexagonal nanopore array is constructed, which is combined with a luminescent organic emitter for radiative recombination of the injected hot-electrons. Owing to the suppressed SPP energy loss via broadband hot-electron emission, the A-PME achieves an optimized optical transmission with an average transmittance of over 80% from 380 to 1200 nm. Moreover, the indium-tin-oxide-free organic solar cells yield an enhanced light harvesting with a power conversion efficiency of 16.1%.
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| 8. |
- Chen, Shangzhi, et al.
(författare)
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Unraveling vertical inhomogeneity in vapour phase polymerized PEDOT:Tos films
- 2020
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 8, s. 18726-18734
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Tidskriftsartikel (refereegranskat)abstract
- The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) forms a promising alternative to conventional inorganic conductors, where deposition of thin films via vapour phase polymerization (VPP) has gained particular interest owing to high electrical conductivity within the plane of the film. The conductivity perpendicular to the film is typically much lower, which may be related not only to preferential alignment of PEDOT crystallites but also to vertical stratification across the film. In this study, we reveal non-linear vertical microstructural variations across VPP PEDOT:Tos thin films, as well as significant differences in doping level between the top and bottom surfaces. The results are consistent with a VPP mechanism based on diffusion-limited transport of polymerization precursors. Conducting polymer films with vertical inhomogeneity may find applications in gradient-index optics, functionally graded thermoelectrics, and optoelectronic devices requiring gradient doping.
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| 9. |
- Chen, Yongzhen, 1990-
(författare)
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Image dipoles and polarons in organic semiconductors
- 2021
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The rapid development of organic electronics depends on the synthesis of new π-conjugated molecules/polymers and the exploration of fundamental physics. However, most of the efforts have been concentrated on the former, leading to a lack of thorough understanding of many important concepts, which will become the ultimate limiting factor for overall performance and applications. Thereinto, the interface energetics in multilayer stacked optoelectronic devices and the electronic structure of doped organic semiconductors are two of the most complicated and yet inevitable topics in this field. A better understanding of them can provide needed additional insights into the operation of devices and give valuable guidance for device and molecule design. Hence, the aim of this thesis is to investigate these two fundamental issues using various spectroscopic characterizations and supported by computational modeling.The cathode/organic interface plays a critical role in achieving balanced charge transport and improved stability in organic electronic devices. Employing stable cathode materials, however, typically results in large electron injection barriers and sub-optimal devices. Using small-molecule electron transport materials (ETMs) as interlayers is an effective approach to reduce the electron injection barriers, but the working mechanism is still under debate. By studying the energy level alignment behavior of ETMs on different types of substrates, we find the work function of the substrate is reduced by an extra “image” dipole formed at the interface and within the first layer of the ETM film. The use of non-reactive substrates and the results from X-ray photoelectron spectroscopy core level analysis exclude the orbital hybridization theory, which states that an ETM-metal complex may form at the interface. The characterization results on molecular orientation disqualify an explanation using intrinsic molecular dipole moments. Instead, experiments demonstrate that the interface dipole depends on the areal density and direction of lone electron pairs on the heteroatoms in ETMs, which is similar to previous observations in tertiary aliphatic amines. This behavior is well described by the so-called “double dipole step” model, where one dipole formed by the nitrogen nuclei and the lone pairs in the organic side points from the substrate surface to the organic film and the other one formed by their image charges in the electrode side shows the same direction.The polaron charge carrier is another important concept involved in multiple (opto)electronic processes during device operation, such as charge transport, exciton recombination/dissociation. Although numerous experimental and theoretical efforts have been made, there is still a lack of comprehensive studies on the electronic structure of negative polarons due to their high air sensitivity, including correlation between the valence band structure measured by ultraviolet photoelectron spectroscopy (UPS) and the optical band gap derived from the UV−vis−NIR absorption. In the present work, we are able to integrate the optical and electrical measurements with photoelectron spectroscopy to collect all information without breaking an ultra-high vacuum. Negative polarons formed in alkali metal-doped polymers are detected with new polaronic states below the Fermi level and lower energy absorption bands arising from the excitation from polaronic states to unoccupied states. In addition, the Fermi level shifts toward the conduction band with increasing the doping ratio, and the doubly-occupied polaronic state shows slightly lower energy than the topmost valance band peak of the neutral polymer. These observations are supported by the density functional theory (DFT) simulations, from which we also demonstrate that polaron pairs rather than bipolarons are preferentially formed at high doping ratios. By comparison of different polymer and dopant systems, we find the polymer-dopant interaction and the polaron delocalization are dependent on the distortion of the polymer backbone and the size of the dopant, properties that in turn affect the conductivity and air stability of the n-doped materials.I hope that the findings presented in the thesis can greatly promote the understanding of the energetics of the ETMs/cathode interface and the electronic structures of negative polarons in alkali metal-doped polymers, contributing to further providing new guidelines for the molecular design and improve the device performance.
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| 10. |
- Chen, Yongzhen, 1990-, et al.
(författare)
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Understanding Interface Dipoles at an Electron Transport Material/Electrode Modifier for Organic Electronics
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:39, s. 47218-47225
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Tidskriftsartikel (refereegranskat)abstract
- Interface dipoles formed at an electrolyte/electrode interface have been widely studied and interpreted using the "double dipole step" model, where the dipole vector is determined by the size and/or range of motion of the charged ions. Some electron transport materials (ETMs) with lone pairs of electrons on heteroatoms exhibit a similar interfacial behavior. However, the origin of the dipoles in such materials has not yet been explored in great depth. Herein, we systematically investigate the influence of the lone pair of electrons on the interface dipole through three pyridine derivatives B2-B4PyMPM. Experiments show that different positions of nitrogen atoms in the three materials give rise to different hydrogen bonds and molecular orientations, thereby affecting the areal density and direction of the lone pair of electrons. The interface dipoles of the three materials predicted by the "double dipole step" model are in good agreement with the ultraviolet photoelectron spectroscopy results both in spin-coated and vacuum-deposited films. These findings help to better understand the ETMs/electrode interfacial behaviors and provide new guidelines for the molecular design of the interlayer.
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