| 1. |
- Boustedt, Jonas, 1965-, et al.
(author)
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It seemed like a good idea at the time
- 2011
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In: SIGCSE'11. - New York, NY, USA : ACM. - 9781450305006 ; , s. 163-164
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Conference paper (other academic/artistic)abstract
- We often learn of successful pedagogical experiments, but we seldom hear of the the ones that failed. For this special session we solicited submissions from the SIGCSE membership, selected the best from among these, and will have presentations at the session by the selected authors. Our contributions describe pedagogical approaches that seemed to be good ideas but turned out as failures. Contributors will describe their pedagogical experiment, the rationale for the experiment, evidence of failure, and lessons learned.
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| 2. |
- Campbell, Charles, et al.
(author)
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Bridging model and real catalysts: general discussion
- 2016
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In: Faraday Discussions. - 1359-6640 .- 1364-5498. ; 188, s. 565-589
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Journal article (other academic/artistic)abstract
- Charles Campbell opened the discussion of the paper by Hans-JoachimFreund: If you have a 3D gold particle and it spreads out to be a 2D particle whenyou adsorb CO2, it must gain energy stability. Did you estimate the energy changeof the overall process to do that?
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| 3. |
- Congrave, Daniel G., et al.
(author)
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Suppressing aggregation induced quenching in anthracene based conjugated polymers
- 2021
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In: Polymer Chemistry. - : Royal Society of Chemistry. - 1759-9954 .- 1759-9962. ; 12:12, s. 1830-1836
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Journal article (peer-reviewed)abstract
- Anthracene is a highly valuable building block for luminescent conjugated polymers, particularly when a large singlet-triplet energy gap (Delta E-ST) is desired. Unfortunately, the extended pi system of anthracene imparts a strong tendency for polymer aggregation, resulting in detrimental effects on its solid state photophysics. A large decrease in photoluminescence quantum yield (PLQY, phi(F)) on going from solution to the solid state is especially common, represented in terms of a low phi(R) (phi(R) = phi(F film)/phi(F sol.)). Significant and undesirable red-shifting of fluorescence in the solid state is also typical due to processes such as excimer formation. In this work a series of alkylene-encapsulated conjugated anthracene polymers is developed to overcome these challenging problems. We demonstrate a promising material which displays a good solid state PLQY that is effectively unchanged compared to solution measurements (phi(R) similar to 1, phi(F film) similar to 40%), alongside an identical PL 0-0 transition wavelength in solution and thin film. Such a direct transfer of luminescence properties from solution to the solid state is remarkable for a conjugated polymer and completely unprecedented for one based on anthracene.
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| 4. |
- Gray, Victor, Dr, 1988-, et al.
(author)
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Ligand-Directed Self-Assembly of Organic-Semiconductor/Quantum-Dot Blend Films Enables Efficient Triplet Exciton-Photon Conversion
- 2024
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 146:11, s. 7763-7770
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Journal article (peer-reviewed)abstract
- Blends comprising organic semiconductors and inorganic quantum dots (QDs) are relevant for many optoelectronic applications and devices. However, the individual components in organic-QD blends have a strong tendency to aggregate and phase-separate during film processing, compromising both their structural and electronic properties. Here, we demonstrate a QD surface engineering approach using electronically active, highly soluble semiconductor ligands that are matched to the organic semiconductor host material to achieve well-dispersed inorganic-organic blend films, as characterized by X-ray and neutron scattering, and electron microscopies. This approach preserves the electronic properties of the organic and QD phases and also creates an optimized interface between them. We exemplify this in two emerging applications, singlet-fission-based photon multiplication (SF-PM) and triplet-triplet annihilation-based photon upconversion (TTA-UC). Steady-state and time-resolved optical spectroscopy shows that triplet excitons can be transferred with near unity efficiently across the organic-inorganic interface, while the organic films maintain efficient SF (190% yield) in the organic phase. By changing the relative energy between organic and inorganic components, yellow upconverted emission is observed upon 790 nm NIR excitation. Overall, we provide a highly versatile approach to overcome longstanding challenges in the blending of organic semiconductors with QDs that have relevance for many optical and optoelectronic applications.
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| 5. |
- Toolan, Daniel T. W., et al.
(author)
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Insights into the Structure and Self-Assembly of Organic-Semiconductor/Quantum-Dot Blends
- 2022
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In: Advanced Functional Materials. - : John Wiley & Sons. - 1616-301X .- 1616-3028. ; 32:13
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Journal article (peer-reviewed)abstract
- Controlling the dispersibility of crystalline inorganic quantum dots (QD) within organic-QD nanocomposite films is critical for a wide range of optoelectronic devices. A promising way to control nanoscale structure in these nanocomposites is via the use of appropriate organic ligands on the QD, which help to compatibilize them with the organic host, both electronically and structurally. Here, using combined small-angle X-ray and neutron scattering, the authors demonstrate and quantify the incorporation of such a compatibilizing, electronically active, organic semiconductor ligand species into the native oleic acid ligand envelope of lead sulphide, QDs, and how this ligand loading may be easily controlled. Further more, in situ grazing incidence wide/small angle X-ray scattering demonstrate how QD ligand surface chemistry has a pronounced effect on the self-assembly of the nanocomposite film in terms of both small-molecule crystallization and QD dispersion versus ordering/aggregation. The approach demonstrated here shows the important role which the degree of incorporation of an active ligand, closely related in chemical structure to the host small-molecule organic matrix, plays in both the self-assembly of the QD and small-molecule components and in determining the final optoelectronic properties of the system.
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| 6. |
- Toolan, Daniel T. W., et al.
(author)
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Linking microscale morphologies to localised performance in singlet fission quantum dot photon multiplier thin films
- 2022
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In: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 10:31, s. 11192-11198
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Journal article (peer-reviewed)abstract
- Hybrid small-molecule/quantum dot films have the potential to reduce thermalization losses in single-junction photovoltaics as photon multiplication devices. Here grazing incidence X-ray scattering, optical microscopy and IR fluorescence microscopy (probing materials at two distinct wavelengths), provide new insight into highly complex morphologies across nm and mu m lengthscales to provide direct links between morphologies and photon multiplication performance. Results show that within the small molecule crystallites three different QD morphologies may be identified; (i) large quantum dot aggregates at the crystallite nucleus, (ii) relatively well-dispersed quantum dots and (iii) as aggregated quantum dots "swept" from the growing crystallite and that regions containing aggregate quantum dot features lead to relatively poor photon multiplication performance. These results establish how combinations of scattering and microscopy may be employed to reveal new insights into the structure and function of small molecule:quantum dot blends.
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| 7. |
- Weir, Michael P., et al.
(author)
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Ligand Shell Structure in Lead Sulfide–Oleic Acid Colloidal Quantum Dots Revealed by Small-Angle Scattering
- 2019
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In: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 10:16, s. 4713-4719
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Journal article (peer-reviewed)abstract
- Nanocrystal quantum dots are generally coated with an organic ligand layer. These layers are a necessary consequence of their chemical synthesis, and in addition they play a key role in controlling the optical and electronic properties of the system. Here we describe a method for quantitative measurement of the ligand layer in 3 nm diameter lead sulfide–oleic acid quantum dots. Complementary small-angle X-ray and neutron scattering (SAXS and SANS) studies give a complete and quantitative picture of the nanoparticle structure. We find greater-than-monolayer coverage of oleic acid and a significant proportion of ligand remaining in solution, and we demonstrate reversible thermal cycling of the oleic acid coverage. We outline the effectiveness of simple purification procedures with applications in preparing dots for efficient ligand exchange. Our method is transferrable to a wide range of colloidal nanocrystals and ligand chemistries, providing the quantitative means to enable the rational design of ligand-exchange procedures.
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| 8. |
- Westenhoff, Sebastian, et al.
(author)
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Exciton migration in a polythiophene: Probing the spatial and energy domain by line-dipole Forster-type energy transfer
- 2005
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In: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 122:9, s. 1-094903
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Journal article (peer-reviewed)abstract
- We study exciton migration in low molecular weight poly[3-(2,5-dioctylphenyl)thiophene] in dilute solution by means of ultrafast spectroscopy and Monte Carlo simulations of resonance energy transfer using the line-dipole Forster approach. The model includes the build-up of polymer chains, site-selective exciton generation, and diffusion through incoherent energy transfer. Time-resolved, ensemble-averaged experimental data are reproduced, namely photoluminescence spectral migration and stimulated emission anisotropy decays measured by streak camera and femtosecond transient absorption spectroscopy under site-selective excitation conditions. Importantly, the relatively simple line-dipole Forster-type approach beyond the point-dipole approximation reproduces both experiments quantitatively. Since explicit chain conformations are used in the model, the simulations yield a descriptive microscopic picture of exciton migration. The effective conjugation length (l(seg) = 2.9 nm, 7.4 monomer units) and the disorder of the chains (Omega = 0.8) are yielded as the only fitting parameters. We find an extra component that is not covered by our fits in anisotropy decays at early times for high excitation energies. This is interpreted within the context that the effective conjugation is limited by conformational disorder. (C) 2005 American Institute of Physics.
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| 9. |
- Wieduwilt, Matthew J., et al.
(author)
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Haploidentical vs sibling, unrelated, or cord blood hematopoietic cell transplantation for acute lymphoblastic leukemia
- 2022
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In: Blood Advances. - : American Society of Hematology. - 2473-9529 .- 2473-9537. ; 6:1, s. 339-357
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Journal article (peer-reviewed)abstract
- The role of haploidentical hematopoietic cell transplantation (HCT) using posttransplant cyclophosphamide (PTCy) for acute lymphoblastic leukemia (ALL) is being defined. We performed a retrospective, multivariable analysis comparing outcomes of HCT approaches by donor for adults with ALL in remission. The primary objective was to compare overall survival (OS) among haploidentical HCTs using PTCy and HLA-matched sibling donor (MSD), 8/8 HLAmatched unrelated donor (MUD), 7 /8 HLA-MUD, or umbilical cord blood (UCB) HCT. Comparing haploidentical HCT to MSD HCT, we found that OS, leukemia-free survival (LFS), nonrelapse mortality (NRM), relapse, and acute graft-versus-host disease (aGVHD) were not different but chronic GVHD (cGVHD) was higher in MSD HCT. Compared with MUD HCT, OS, LFS, and relapse were not different, but MUD HCT had increased NRM (hazard ratio [HR], 1.42; P = .02), grade 3 to 4 aGVHD (HR, 1.59; P = .005), and cGVHD. Compared with 7/8 UD HCT, LFS and relapse were not different, but 7/8 UD HCT had worse OS (HR, 1.38; P = .01) and increased NRM (HR, 2.13; P <_ .001), grade 3 to 4 aGVHD (HR, 1.86; P = .003), and cGVHD (HR, 1.72; P <_ .001). Compared with UCB HCT, late OS, late LFS, relapse, and cGVHD were not different but UCB HCT had worse early OS (<_18 months; HR, 1.93; P < .001), worse early LFS (HR, 1.40; P = .007) and increased incidences of NRM (HR, 2.08; P < .001) and grade 3 to 4 aGVHD (HR, 1.97; P < .001). Haploidentical HCT using PTCy showed no difference in survival but less GVHD compared with traditional MSD and MUD HCT and is the preferred alternative donor HCT option for adults with ALL in complete remission.
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| 10. |
- Zhang, Ming, et al.
(author)
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Identification of the target self-antigens in reperfusion injury.
- 2006
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In: Journal of Experimental Medicine. - : Rockefeller University Press. - 0022-1007 .- 1540-9538. ; 203:1, s. 141-52
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Journal article (peer-reviewed)abstract
- Reperfusion injury (RI), a potential life-threatening disorder, represents an acute inflammatory response after periods of ischemia resulting from myocardial infarction, stroke, surgery, or trauma. The recent identification of a monoclonal natural IgM that initiates RI led to the identification of nonmuscle myosin heavy chain type II A and C as the self-targets in two different tissues. These results identify a novel pathway in which the innate response to a highly conserved self-antigen expressed as a result of hypoxic stress results in tissue destruction.
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