| 1. |
- Guan, Tianfu, et al.
(author)
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Decoding the Self-Assembly Plasmonic Interface Structure in a PbS Colloidal Quantum Dot Solid for a Photodetector
- 2023
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In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 17:22, s. 23010-23019
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Journal article (peer-reviewed)abstract
- Hybrid plasmonic nanostructures have gained enormous attention in a variety of optoelectronic devices due to their surface plasmon resonance properties. Self-assembled hybrid metal/quantum dot (QD) architectures offer a means of coupling the properties of plasmonics and QDs to photodetectors, thereby modifying their functionality. The arrangement and localization of hybrid nanostructures have an impact on exciton trapping and light harvesting. Here, we present a hybrid structure consisting of self-assembled gold nanospheres (Au NSs) embedded in a solid matrix of PbS QDs for mapping the interface structures and the motion of charge carriers. Grazing-incidence small-angle X-ray scattering is utilized to analyze the localization and spacing of the Au NSs within the hybrid structure. Furthermore, by correlating the morphology of the Au NSs in the hybrid structure with the corresponding differences observed in the performance of photodetectors, we are able to determine the impact of interface charge carrier dynamics in the coupling structure. From the perspective of architecture, our study provides insights into the performance improvement of optoelectronic devices.
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| 2. |
- Chen, Wei, et al.
(author)
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In situ Grazing-Incidence Small-Angle X-ray Scattering Observation of Gold Sputter Deposition on a PbS Quantum Dot Solid
- 2020
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In: ACS Applied Materials and Interfaces. - : NLM (Medline). - 1944-8244 .- 1944-8252. ; 12:41, s. 46942-46952
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Journal article (peer-reviewed)abstract
- For PbS quantum dot (QD)-based optoelectronic devices, gold is the most frequently used electrode material. In most device architectures, gold is in direct contact with the QD solid. To better understand the formation of the interface between gold and a close-packed QD layer at an early stage, in situ grazing-incidence small-angle X-ray scattering is used to observe the gold sputter deposition on a 1,2-ethanedithiol (EDT)-treated PbS QD solid. In the kinetics of gold layer growth, the forming and merging of small gold clusters (radius less than 1.6 nm) are observed at the early stages. The thereby formed medium gold clusters (radius between 1.9-2.4 nm) are influenced by the QDs' templating effect. Furthermore, simulations suggest that the medium gold clusters grow preferably along the QDs' boundaries rather than as a top coating of the QDs. When the thickness of the sputtered gold layer reaches 6.25 nm, larger gold clusters with a radius of 5.3 nm form. Simultaneously, a percolation layer with a thickness of 2.5 nm is established underneath the gold clusters. This fundamental understanding of the QD-gold interface formation will help to control the implementation of sputtered gold electrodes on close-packed QD solids in device manufacturing processes.
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| 3. |
- Gensch, Marc, et al.
(author)
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Correlating Optical Reflectance with the Topology of Aluminum Nanocluster Layers Growing on Partially Conjugated Diblock Copolymer Templates
- 2021
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In: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:47, s. 56663-56673
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Journal article (peer-reviewed)abstract
- Large-scale fabrication of metal cluster layers for usage in sensor applications and photovoltaics is a huge challenge. Physical vapor deposition offers large-scale fabrication of metal cluster layers on templates and polymer surfaces. In the case of aluminum (Al), only little is known about the formation and interaction of Al clusters during sputter deposition. Complex polymer surface morphologies can tailor the deposited Al cluster layer. Here, a poly(methyl methacrylate)-block-poly(3-hexylthiophen-2,5-diyl) (PMMA-b-P3HT) diblock copolymer template is used to investigate the nanostructure formation of Al cluster layers on the different polymer domains and to compare it with the respective homopolymers PMMA and P3HT. The optical properties relevant for sensor applications are monitored with ultraviolet-visible (UV-vis) measurements during the sputter deposition. The formation of Al clusters is followed in situ with grazing-incidence small-angle X-ray scattering (GISAXS), and the chemical interaction is revealed by X-ray photoelectron spectroscopy (XPS). Furthermore, atomic force microscopy (AFM) and field emission scanning electron microscopy (FESEM) yield topographical information about selective wetting of Al on the P3HT domains and embedding in the PMMA domains in the early stages, followed by four distinct growth stages describing the Al nanostructure formation.
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| 4. |
- Gensch, Marc, et al.
(author)
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Selective Silver Nanocluster Metallization on Conjugated Diblock Copolymer Templates for Sensing and Photovoltaic Applications
- 2021
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 4:4, s. 4245-4255
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Journal article (peer-reviewed)abstract
- Polymer-metal composite films with nanostructured metal and/or polymer interfaces show a significant perspective for optoelectronic applications, for example, as sensors or in organic photovoltaics (OPVs). The polymer components used in these devices are mostly nanostructured conductive polymers with conjugated pi-electron systems. Enhanced OPV's power conversion efficiencies or sensor sensitivity can be achieved by selective metal deposition on or into polymer templates. In this study, we exploit time-resolved grazing-incidence X-ray scattering to observe the metal-polymer interface formation and the cluster crystallite size in situ during silver (Ag) sputter deposition on a poly(3-hexylthiophene-2,5-diyl)-b-poly(methyl methacrylate) (PMMA-b-P3HT) template. We compare the arising nanoscale morphologies with electronic properties, determine Ag growth regimes, and quantify the selective Ag growth for the diblock copolymer (DBC) template using the corresponding homopolymer thin films (P3HT and PMMA) as a reference. Hence, we are able to describe the influence of the respective polymer blocks and substrate effects on the Ag cluster percolation: the percolation threshold is correlated with the insulator-to-metal transition measured in situ with resistance measurements during the sputter deposition. The Ag cluster percolation on PMMA-b-P3HT starts already on the network of the hexagonal P3HT domain before a complete metal film covers the polymer surface, which is complemented by microscopic measurements. In general, this study demonstrates a possible method for the selective Ag growth as a scaffold for electrode preparation in nanoelectronics and for energy harvesting applications.
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| 5. |
- Guo, Renjun, et al.
(author)
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Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen
- 2021
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In: Nature Energy. - : Springer Nature. - 2058-7546. ; 6:10, s. 977-
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Journal article (peer-reviewed)abstract
- Extensive studies have focused on improving the operational stability of perovskite solar cells, but few have surveyed the fundamental degradation mechanisms. One aspect overlooked in earlier works is the effect of the atmosphere on device performance during operation. Here we investigate the degradation mechanisms of perovskite solar cells operated under vacuum and under a nitrogen atmosphere using synchrotron radiation-based operando grazing-incidence X-ray scattering methods. Unlike the observations described in previous reports, we find that light-induced phase segregation, lattice shrinkage and morphology deformation occur under vacuum. Under nitrogen, only lattice shrinkage appears during the operation of solar cells, resulting in better device stability. The different behaviour under nitrogen is attributed to a larger energy barrier for lattice distortion and phase segregation. Finally, we find that the migration of excessive PbI2 to the interface between the perovskite and the hole transport layer degrades the performance of devices under vacuum or under nitrogen. Understanding degradation mechanisms in perovskite solar cells is key to their development. Now, Guo et al. show a greater degradation of the perovskite structure and morphology for devices operated under vacuum than under nitrogen.
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| 6. |
- Liang, Suzhe, et al.
(author)
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Tailoring the Optical Properties of Sputter-Deposited Gold Nanostructures on Nanostructured Titanium Dioxide Templates Based on In Situ Grazing-Incidence Small-Angle X-ray Scattering Determined Growth Laws
- 2021
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In: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:12, s. 14283-14295
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Journal article (peer-reviewed)abstract
- Gold/titanium dioxide (Au/TiO2) nanohybrid materials have been widely applied in various fields because of their outstanding optical and photocatalytic performance. By state-of-the-art polymer templating, it is possible to make uniform nanostructured TiO2 layers with potentially large-scale processing methods. We use customized polymer templating to achieve TiO2 nanostructures with different morphologies. Au/TiO2 hybrid thin films are fabricated by sputter deposition. An indepth understanding of the Au morphology on the TiO2 templates is achieved with in situ grazing-incidence small-angle X-ray scattering (GISAXS) during the sputter deposition. The resulting Au nanostructure is largely influenced by the TiO2 template morphology. Based on the detailed understanding of the Au growth process, characteristic distances can be selected to achieve tailored Au nanostructures at different Au loadings. For selected sputter-deposited Au/TiO2 hybrid thin films, the optical response with a tailored localized surface plasmon resonance is demonstrated.
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| 7. |
- Liang, Suzhe, et al.
(author)
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Template-Induced Growth of Sputter-Deposited Gold Nanoparticles on Ordered Porous TiO2 Thin Films for Surface-Enhanced Raman Scattering Sensors
- 2022
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 5:5, s. 7492-7501
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Journal article (peer-reviewed)abstract
- Ordered porous gold/titanium dioxide (Au/TiO2) hybrid nanostructured films are specifically interesting in large-scale applications using localized surface plasmon resonances (LSPRs) and surface-enhanced Raman scattering (SERS). Deposition of Au nanoparticles via sputter deposition is one of the promising technologies to establish optically active sites at low cost in combination with nanostructured TiO2 films. In this work, we investigate the optical response of sputter-deposited Au/TiO2 nanohybrid thin films with a focus on the plasmonic response and application as molecular sensors. The LSPR peak red shifts with an increasing thickness of deposited Au. The Raman intensity of deposited molecules, probed with rhodamine 6G (R6G), depends on the deposited gold thickness. It has its maximum at an effective Au thickness of 3.4 nm. To elucidate the origin of this behavior, we apply in situ grazing-incidence small-angle X-ray scattering (GISAXS) to investigate the growth kinetics of Au on a TiO2 template during sputter deposition. On the basis of time-resolved GISAXS, the growth characteristics of sputter-deposited Au on a TiO2 template with a final effective Au layer thickness around the percolation threshold is described with the well-known four-stage model of nucleation and cluster formation, diffusion-mediated growth, adsorption-mediated growth, and grain growth. The maximum in SERS intensity is corroborated by the existence and optimal size of hot spots in the narrow space occurring between the sputter-deposited Au clusters, on staying below the percolation threshold. On the basis of the growth laws extracted, we give a guideline for tailoring the ordered porous Au/TiO2 nanohybrid thin films for SERS sensor applications.
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| 8. |
- Reck, Kristian A., et al.
(author)
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Early-stage silver growth during sputter deposition on SiO2 and polystyrene - Comparison of biased DC magnetron sputtering, high-power impulse magnetron sputtering (HiPIMS) and bipolar HiPIMS
- 2024
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In: Applied Surface Science. - : Elsevier BV. - 0169-4332 .- 1873-5584. ; 666
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Journal article (peer-reviewed)abstract
- The integration of silver thin films into optoelectronic devices has gained much interest due to their exceptional properties in terms of conductivity and compatibility with flexible substrates. For this type of application, ultrathin layers are desirable, because of their optical transparency. Standard direct current magnetron sputtering (DCMS) is known to lead to undesirable formation of islands at low effective film thicknesses on typical substrates like SiO2 or polystyrene (PS). Therefore, in this study, we explore high-power impulse magnetron sputtering (HiPIMS) with optional further acceleration of metal ions by biasing the substrate or an additional positive pulse (bipolar HiPIMS) for the fabrication of ultra-thin silver layers. The morphology and electrical properties of ultra-thin silver layers with selected effective thicknesses are characterized on SiO2 and PS substrates. The growth evolution of characteristic parameters is further investigated by in-situ grazing-incidence small-angle Xray scattering (GISAXS). The results show that HiPIMS deposition yields films with a higher density of clusters than DCMS leading to a percolation threshold at lower effective film thicknesses. This effect is amplified by further ion acceleration. Thus, we suggest HiPIMS as a promising technique for fabricating ultra-thin, conductive layers on organic and oxide substrates.
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| 9. |
- Xiao, Tianxiao, et al.
(author)
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Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell
- 2024
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In: Nano Energy. - : Elsevier BV. - 2211-2855 .- 2211-3282. ; 125
-
Journal article (peer-reviewed)abstract
- Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems.
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| 10. |
- Yin, Shanshan, et al.
(author)
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Tailored fabrication of quasi-isoporous and double layered alpha-Fe2O3 thin films and their application in photovoltaic devices
- 2023
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In: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947 .- 1873-3212. ; 455, s. 140135-
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Journal article (peer-reviewed)abstract
- A series of α-Fe2O3 thin films with distinct morphologies are prepared via a facile polystyrene-block-polyethylene oxide templated sol–gel method. By tailoring the poor solvent contents and FeCl3-to-polymer weight ratio in the sol–gel solutions, quasi-isoporous α-Fe2O3 thin films with different substructures and thicknesses are obtained. Via a thermal annealing post-treatment, double layered structures are induced by a synergistic dewetting and Oswald ripening effect. Special focus is set on the α-Fe2O3 thin films prepared with no annealing/annealing-medium FeCl3 concentration, as they possess uniform periodic structures, which is suitable to be used as hole blocking modification layer of perovskite solar cells (PSCs). An improved power conversion efficiency (PCE) is obtained when the double layered α-Fe2O3 thin film is applied as the hole blocking modification layer for PSCs. The improved PCE primarily originates from the increased VOC, which probably benefits from the synergistic effect of the suppressed charge carrier recombination at the interfaces, the enhanced light transmittance as well as the superior electron extraction capacity.
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| 11. |
- Zou, Yuqin, et al.
(author)
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The Influence of CsBr on Crystal Orientation and Optoelectronic Properties of MAPbI(3)-Based Solar Cells
- 2022
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In: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 14:2, s. 2958-2967
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Journal article (peer-reviewed)abstract
- Crystal orientations are closely related to the behavior of photogenerated charge carriers and are vital for controlling the optoelectronic properties of perovskite solar cells. Herein, we propose a facile approach to reveal the effect of lattice plane orientation distribution on the charge carrier kinetics via constructing CsBr-doped mixed cation perovskite phases. With grazing-incidence wide-angle X-ray scattering measurements, we investigate the crystallographic properties of mixed perovskite films at the microscopic scale and reveal the effect of the extrinsic CsBr doping on the stacking behavior of the lattice planes. Combined with transient photocurrent, transient photovoltage, and space-charge-limited current measurements, the transport dynamics and recombination of the photogenerated charge carriers are characterized. It is demonstrated that CsBr compositional engineering can significantly affect the perovskite crystal structure in terms of the orientation distribution of crystal planes and passivation of trap-state densities, as well as simultaneously facilitate the photogenerated charge carrier transport across the absorber and its interfaces. This strategy provides unique insight into the underlying relationship between the stacking pattern of crystal planes, photogenerated charge carrier transport, and optoelectronic properties of solar cells.
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