| 1. |
- Guan, Tianfu, et al.
(författare)
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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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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 17:22, s. 23010-23019
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Tidskriftsartikel (refereegranskat)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.
(författare)
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Colloidal PbS quantum dot stacking kinetics during deposition via printing
- 2020
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Ingår i: Nanoscale Horizons. - : Royal Society of Chemistry (RSC). - 2055-6764 .- 2055-6756. ; 5:5, s. 880-885
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Tidskriftsartikel (refereegranskat)abstract
- Colloidal PbS quantum dots (QDs) are attractive for solution-processed thin-film optoelectronic applications. In particular, directly achieving QD thin-films by printing is a very promising method for low-cost and large-scale fabrication. The kinetics of QD particles during the deposition process play an important role in the QD film quality and their respective optoelectronic performance. In this work, the particle self-organization behavior of small-sized QDs with an average diameter of 2.88 +/- 0.36 nm is investigated for the first time in situ during printing by grazing-incidence small-angle X-ray scattering (GISAXS). The time-dependent changes in peak intensities suggest that the structure formation and phase transition of QD films happen within 30 seconds. The stacking of QDs is initialized by a templating effect, and a face-centered cubic (FCC) film forms in which a superlattice distortion is also found. A body-centered cubic nested FCC stacking is the final QD assembly layout. The small size of the inorganic QDs and the ligand collapse during the solvent evaporation can well explain this stacking behavior. These results provide important fundamental understanding of structure formation of small-sized QD based films prepared via large-scale deposition with printing with a slot die coater.
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| 3. |
- Chen, Wei, et al.
(författare)
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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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Ingår i: ACS Applied Materials and Interfaces. - : NLM (Medline). - 1944-8244 .- 1944-8252. ; 12:41, s. 46942-46952
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Tidskriftsartikel (refereegranskat)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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| 4. |
- Jiang, Xinyu, et al.
(författare)
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Internal nanoscale architecture and charge carrier dynamics of wide bandgap non-fullerene bulk heterojunction active layers in organic solar cells
- 2020
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 8:44, s. 23628-23636
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Tidskriftsartikel (refereegranskat)abstract
- Bulk heterojunction (BHJ) organic solar cells have gained increasing attention in the past few years. In this work, active layers of a wide-bandgap polymer donor with benzodithiophene units PBDB-T-2F and a non-fullerene small molecule acceptor IT-M are assembled into photovoltaic devices with different amounts of solvent additive 1,8-diiodooctane (DIO). The influence of DIO on the nanoscale film morphology and crystalline structure as well as the charge carrier dynamics of the active layers are investigated by combining grazing-incidence small-angle X-ray scattering (GISAXS), grazing-incidence wide-angle X-ray scattering (GIWAXS), X-ray reflectivity (XRR), UV-visible (UV-vis) absorption spectroscopy, X-ray photoelectron spectroscopy (XPS), time-resolved photoluminescence (TRPL) and space charge limited current measurements, which are correlated with the corresponding performance of the solar cells. At 0.5 vol% DIO addition, the wide-bandgap non-fullerene organic solar cells show the best performance due to high open-circuit voltage and short-circuit current resulting from an improved charge carrier management due to the optimal inner nanoscale morphology of the active layers in terms of surface enrichment, crystallinity and crystalline orientation.
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| 5. |
- Kottwitz, Matthew, et al.
(författare)
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Single Atom Catalysts: A Review of Characterization Methods
- 2021
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Ingår i: Chemistry-Methods. - : John Wiley and Sons Inc. - 2628-9725. ; 1:6, s. 278-294
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Forskningsöversikt (refereegranskat)abstract
- Single atom catalysts (SACs) harbor a potential to exceed nanoparticle catalysts in terms of activity, stability and selectivity in a growing number of chemical reactions. Although their investigation is attracting significant attention, important fundamental questions focusing on key physicochemical properties of SACs (e. g., structure – property relationships, structural dynamics, reaction-driven restructuring) remain unanswered. A main challenge for research in the field is how to reliably characterize the environments of single atoms in the presence of complicating factors such as low weight loadings, strong metal-support interactions, and atomic and multiscale heterogeneity of bonding in the single atom sites. This review addresses this challenge – identifying catalytically relevant features of physicochemical properties of single atoms (charge state, electronic structure, atomic configuration, bonding interactions with a support) and surveying advanced tools/methods for characterizing them. The review places a strong emphasis on multimodal methods exploiting X-ray absorption, emission and photoelectron spectroscopies, and provides several examples from the authors’ research that demonstrate their use as powerful tools for SAC characterization.
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| 6. |
- Li, Yuanyuan, et al.
(författare)
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Active sites of atomically dispersed Pt supported on Gd-doped ceria with improved low temperature performance for CO oxidation
- 2023
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 14:44, s. 12582-12588
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Tidskriftsartikel (refereegranskat)abstract
- “Single-atom” catalysts (SACs) have been the focus of intense research, due to debates about their reactivity and challenges toward determining and designing “single-atom” (SA) sites. To address the challenge, in this work, we designed Pt SACs supported on Gd-doped ceria (Pt/CGO), which showed improved activity for CO oxidation compared to its counterpart, Pt/ceria. The enhanced activity of Pt/CGO was associated with a new Pt SA site which appeared only in the Pt/CGO catalyst under CO pretreatment at elevated temperatures. Combined X-ray and optical spectroscopies revealed that, at this site, Pt was found to be d-electron rich and bridged with Gd-induced defects via an oxygen vacancy. As explained by density functional theory calculations, this site opened a new path via a dicarbonyl intermediate for CO oxidation with a greatly reduced energy barrier. These results provide guidance for rationally improving the catalytic properties of SA sites for oxidation reactions.
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| 7. |
- Pan, Haodong, et al.
(författare)
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COVID‐19 and cognitive impairment : From evidence to SARS‐CoV‐2 mechanism
- 2024
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Ingår i: Brain‐X. - 2835-3153. ; 2:2
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Tidskriftsartikel (refereegranskat)abstract
- Caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), coronavirus disease 2019 (COVID-19) primarily manifests as respiratory dysfunction. However, emerging evidence suggests SARS-CoV-2 can invade the brain, leading to cognitive impairment (CI). It may spread to other brain regions through transsynaptic neurons, including the olfactory, optic, and vagus nerves. Moreover, it may invade the central nervous system through blood transmission or the lymphatic system. This review summarizes the neuroimaging evidence from clinical and imaging studies of COVID-19-associated CIs, including magnetic resonance imaging and 18F-fluorodeoxyglucose positron emission tomography-computed tomography. The mechanisms underlying COVID-19-associated CIs are currently being actively investigated. They include nonimmune effects, such as viral proteins, tissue hypoxia, hypercoagulability, and pathological changes in neuronal cells, and immune effects, such as microglia and astrocyte activation, peripheral immune cell infiltration, blood-brain barrier impairment, cytokine network dysregulation, and intestinal microbiota. Inflammation is the central feature. Both central and systemic inflammation may cause acute and persistent neurological changes, and existing evidence indicates that inflammation underlies the elevated risk of Alzheimer's disease. Finally, potential therapeutic options for COVID-19-associated CIs are discussed. In-depth research into the pathological mechanisms is still needed to help develop new therapies.
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| 8. |
- Wang, Haodong, et al.
(författare)
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Aliovalent Doping of CeO2 Improves the Stability of Atomically Dispersed Pt
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:44, s. 52736-52742
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Tidskriftsartikel (refereegranskat)abstract
- Atomically dispersed supported catalysts hold considerable promise as catalytic materials. The ability to employ and stabilize them against aggregation in complex process environments remains a key challenge to the elusive goal of 100% atom utilization in catalysis. Herein, using a Gd-doped ceria support for atomically dispersed surface Pt atoms, we establish how the combined effects of aliovalent doping and oxygen vacancy generation provide dynamic mechanisms that serve to enhance the stability of supported single-atom configurations. Using correlated, in situ X-ray absorption, photoelectron, and vibrational spectroscopy methods for the analysis of samples on the two types of support (with and without Gd doping), we establish that the Pt atoms are located proximal to Gd dopants, forming a speciation that serves to enhance the thermal stability of Pt atoms against aggregation.
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| 9. |
- Zhang, Erliang, et al.
(författare)
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Dietary Rhythmicity and Mental Health Among Airline Personnel
- 2024
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Ingår i: JAMA Network Open. - : American Medical Association (AMA). - 2574-3805. ; 7:7
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Tidskriftsartikel (refereegranskat)abstract
- IMPORTANCE: Misaligned dietary rhythmicity has been associated with metabolic diseases; however, its association with mental health remains largely unexplored.OBJECTIVE: To examine the association between dietary rhythms and the mental health condition of shift workers, specifically airline crew members.DESIGN, SETTING, AND PARTICIPANTS: This cross-sectional study analyzed data collected from the Civil Aviation Health Cohort of China, an ongoing large-scale health survey of pilots, flight attendants, and air security officers employed by major airline companies in China. Participants aged 18 to 60 years were invited through text messages to complete a web-based survey. The data collection period was December 2022 to March 2023. Statistical analysis was performed from July 24, 2023, to April 12, 2024.EXPOSURE: Data on timing of breakfast and dinner on workdays and rest days, daily time windows for food intake, and meal and eating jet lags were collected and calculated.MAIN OUTCOMES AND MEASURES: Anxiety and depressive symptoms were measured using the 7-item Generalized Anxiety Disorder Assessment and the 9-item Patient Health Questionnaire. Multivariate logistic regressions were performed to evaluate the associations of anxiety and depression with meal timing, eating window time, meal jet lag (ie, delayed meals), and eating jet lag (ie, delayed eating). All models were adjusted for individual socioeconomic, demographic, and lifestyle characteristics.RESULTS: Of the 22 617 participants (median [IQR] age, 29.1 [26.3-33.7] years; 13 712 males [60.6%]), 1755 (7.8%) had anxiety and 2768 (12.2%) had depression. After controlling for confounding factors, having dinner after 8 pm on morning-shift days was associated with increased odds of anxiety (adjusted odds ratio [AOR], 1.78; 95% CI, 1.53-2.05) and depression (AOR, 2.01; 95% CI, 1.78-2.27), compared with consuming dinner before 8 pm. Similar results were observed on night-shift days and rest days. An eating window of less than 12 hours was associated with reduced odds of anxiety (AOR, 0.84; 95% CI, 0.75-0.93) and depression (AOR, 0.81; 95% CI, 0.75-0.89) on morning-shift days; the results remained significant on rest days. Delayed dinner on morning-shift days was associated with increased odds of anxiety (AOR, 1.32; 95% CI, 1.13-1.54) and depression (AOR, 1.39; 95% CI, 1.22-1.58). On night-shift days, delayed dinner was associated with higher odds of anxiety (AOR, 1.22; 95% CI, 1.06-1.39) and depression (AOR, 1.21; 95% CI, 1.08-1.36). On morning-shift days, delayed eating rhythms were associated with higher odds of depression (AOR, 1.35; 95% CI, 1.13-1.61), whereas advanced eating rhythms were associated with lower odds of anxiety (AOR, 0.78; 95% CI, 0.70-0.87).CONCLUSIONS AND RELEVANCE: This cross-sectional study found that meal timing, long eating window, and meal jet lags were associated with increased odds of depression and anxiety. These findings underscore the need for interventions and supportive policies that help mitigate the adverse implications of shift work and irregular working hours for the mental health of shift workers.
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