10 research outputs found

    From Chalcogen Bonding to S–π Interactions in Hybrid Perovskite Photovoltaics

    Get PDF
    The stability of hybrid organic–inorganic halide perovskite semiconductors remains a significant obstacle to their application in photovoltaics. To this end, the use of low‐dimensional (LD) perovskites, which incorporate hydrophobic organic moieties, provides an effective strategy to improve their stability, yet often at the expense of their performance. To address this limitation, supramolecular engineering of noncovalent interactions between organic and inorganic components has shown potential by relying on hydrogen bonding and conventional van der Waals interactions. Here, the capacity to access novel LD perovskite structures that uniquely assemble through unorthodox S‐mediated interactions is explored by incorporating benzothiadiazole‐based moieties. The formation of S‐mediated LD structures is demonstrated, including one‐dimensional (1D) and layered two‐dimensional (2D) perovskite phases assembled via chalcogen bonding and S–π interactions, through a combination of techniques, such as single crystal and thin film X‐ray diffraction, as well as solid‐state NMR spectroscopy, complemented by molecular dynamics simulations, density functional theory calculations, and optoelectronic characterization, revealing superior conductivities of S‐mediated LD perovskites. The resulting materials are applied in n‐i‐p and p‐i‐n perovskite solar cells, demonstrating enhancements in performance and operational stability that reveal a versatile supramolecular strategy in photovoltaics

    From Chalcogen Bonding to S–π Interactions in Hybrid Perovskite Photovoltaics

    Get PDF
    The stability of hybrid organic–inorganic halide perovskite semiconductors remains a significant obstacle to their application in photovoltaics. To this end, the use of low‐dimensional (LD) perovskites, which incorporate hydrophobic organic moieties, provides an effective strategy to improve their stability, yet often at the expense of their performance. To address this limitation, supramolecular engineering of noncovalent interactions between organic and inorganic components has shown potential by relying on hydrogen bonding and conventional van der Waals interactions. Here, the capacity to access novel LD perovskite structures that uniquely assemble through unorthodox S‐mediated interactions is explored by incorporating benzothiadiazole‐based moieties. The formation of S‐mediated LD structures is demonstrated, including one‐dimensional (1D) and layered two‐dimensional (2D) perovskite phases assembled via chalcogen bonding and S–π interactions, through a combination of techniques, such as single crystal and thin film X‐ray diffraction, as well as solid‐state NMR spectroscopy, complemented by molecular dynamics simulations, density functional theory calculations, and optoelectronic characterization, revealing superior conductivities of S‐mediated LD perovskites. The resulting materials are applied in n‐i‐p and p‐i‐n perovskite solar cells, demonstrating enhancements in performance and operational stability that reveal a versatile supramolecular strategy in photovoltaics

    Deconinck, Marielle

    No full text

    Effects of sub-picosecond direct laser interference patterning on the optoelectronic properties of fluorine-doped tin oxide thin films

    No full text
    Micropatterning of metal oxides is of high interest for structuring electrodes in optoelectronic devices. In this work, the impact of infrared (IR) sub-picosecond Direct Laser Interference Patterning (DLIP) on the surface morphology, surface chemistry, optical and electrical properties of Fluorine-doped Tin Oxide (FTO) is studied. The topography characterization reveals periodic microchannels with an average height between 15 and 600 nm, depending on the applied laser fluence, decorated with Laser-Induced Periodic Surface Structures (LIPSS). The doping by aliovalent Sn atoms induced by non-linear IR absorption were revealed by X-ray Photoemission Spectroscopy (XPS) analysis. An increase in the average diffuse optical transmittance up to 730% was obtained in the spectral range 400-1000 nm as a consequence of the interaction of white light with the periodic micro- and nanostructures. The one-dimensionality of the microstructures caused a significant anisotropic electrical behavior, and an enhancement of the conductivity of up to 50% was obtained following the direction of the microchannels of the patterned films as compared to the unstructured material. Our results demonstrate that DLIP is a powerful technique for future application in structuring electrodes for highly efficient optoelectronic devices and sensors.Fil: Heffner, Herman. Consejo Nacional de Investigaciones CientĂ­ficas y TĂ©cnicas. Centro CientĂ­fico TecnolĂłgico Conicet - BahĂ­a Blanca. Instituto de QuĂ­mica del Sur. Universidad Nacional del Sur. Departamento de QuĂ­mica. Instituto de QuĂ­mica del Sur; Argentina. Technische UniversitĂ€t Dresden; AlemaniaFil: Soldera, Marcos. Technische UniversitĂ€t Dresden; AlemaniaFil: Schell, Frederic. Fraunhofer-Institut fĂŒr Werkstoff und Strahltechnik Dresden ; AlemaniaFil: Deconinck, Marielle. Technische UniversitĂ€t Dresden; AlemaniaFil: Vaynzof, Yana. Technische UniversitĂ€t Dresden; AlemaniaFil: Mulko, Lucinda. Technische UniversitĂ€t Dresden; AlemaniaFil: Lasagni, AndrĂ©s FabiĂĄn. Technische UniversitĂ€t Dresden; Alemani

    Bright electrically controllable quantum-dot-molecule devices fabricated by in situ electron-beam lithography

    No full text
    Self-organized semiconductor quantum dots represent almost ideal two-level systems, which have strong potential to applications in photonic quantum technologies. For instance, they can act as emitters in close-to-ideal quantum light sources. Coupled quantum dot systems with significantly increased functionality are potentially of even stronger interest since they can be used to host ultra-stable singlet-triplet spin qubits for efficient spin-photon interfaces and for deterministic photonic 2D cluster-state generation. An advanced quantum dot molecule (QDM) device is realized and excellent optical properties are demonstrated. The device includes electrically controllable QDMs based on stacked quantum dots in a pin-diode structure. The QDMs are deterministically integrated into a photonic structure with a circular Bragg grating using in situ electron beam lithography. A photon extraction efficiency of up to (24 ± 4)% is measured in good agreement with numerical simulations. The coupling character of the QDMs is clearly demonstrated by bias voltage dependent spectroscopy that also controls the orbital couplings of the QDMs and their charge state in quantitative agreement with theory. The QDM devices show excellent single-photon emission properties with a multi-photon suppression of (2)(0)=(3.9±0.5)×10−3 . These metrics make the developed QDM devices attractive building blocks for use in future photonic quantum networks using advanced nanophotonic hardware.BMBF, 13N14876, Quantenkommunikations-Systeme auf Basis von Einzelphotonenquellen (QuSecure

    Controlled Coherent Coupling in a Quantum Dot Molecule Revealed by Ultrafast Four-Wave Mixing Spectroscopy

    No full text
    International audienceSemiconductor quantum dot molecules are considered as promising candidates for quantum technological applications due to their wide tunability of optical properties and coverage of different energy scales associated with charge and spin physics. While previous works have studied the tunnel-coupling of the different excitonic charge complexes shared by the two quantum dots by conventional optical spectroscopy, we here report on the first demonstration of a coherently controlled inter-dot tunnel-coupling focusing on the quantum coherence of the optically active trion transitions. We employ ultrafast four-wave mixing spectroscopy to resonantly generate a quantum coherence in one trion complex, transfer it to and probe it in another trion configuration. With the help of theoretical modelling on different levels of complexity we give an instructive explanation of the underlying coupling mechanism and dynamical processes

    Le Mal et ses masques

    No full text
    Le « mal », impensĂ© collectif, prend corps au grĂ© de diverses reprĂ©sentations mythiques, poĂ©tiques, graphiques, musicales. SorciĂšres, guĂ©risseuses, Machiavels, AntĂ©christs, voire bestiaire infernal, incarnent au thĂ©Ăątre ou dans la littĂ©rature pamphlĂ©taire des xvie et xviie siĂšcles ces « agents du diable » censĂ©s rendre visibles les dangers de l'invisible, mais que seuls leurs masques permettent de dĂ©masquer. La « diabolisation » de l'adversaire politique autorise une «chasse aux sorciĂšres» qui n'a rien de mĂ©taphorique, mais au thĂ©Ăątre comme sur la scĂšne politique, elle permet aussi la mise en Ă©vidence des jeux pervers du discours, le mal aux prises avec les mots, masque de l' « Ă©quivoque » qui ne parle pas seulement par la voix des sorciĂšres comme dans Macbeth, mais inscrit l'ambivalence, menace de dĂ©votement, comme mal au cƓur de tout discours. L'ambivalence contient en elle la parodie, qui ne retient de l'invisible que le risible, mais elle permet aussi toutes les ruses de l'imaginaire pour surmonter les traumatismes du corps et de l'esprit, comme chez Graves ou Coleridge. Le thĂ©Ăątre lyrique, « chant des Enfers », tĂ©moigne aussi de cette « double voix ». Divertissement entre Ă©thique et esthĂ©tique avec Purcell, ou affrontement idĂ©ologique entre choeurs des opprimĂ©s et chƓurs des oppresseurs chez Haendel, il peut aussi prendre le relais du tragique : l'amalgame sensationnel, « thĂ©Ăątral », entre les monstres des enfers paĂŻens et l'enfer chrĂ©tien prive ce lieu par excellence du mal de toute rĂ©fĂ©rence mĂ©taphysique, pour mieux isoler comme nouveau « mal » le seul malheur de la passion trop humaine. L'enfer traditionnel se rĂ©duit Ă  ses propres reprĂ©sentations parodiques, combien moins angoissantes que l'ontologie infernale proposĂ©e dans le Faust de Marlowe, Ă©gale Ă  la contingence de l'ĂȘtre-lĂ  sans lieu ni durĂ©e dĂ©finis

    Increased risk of severe COVID-19 in hospitalized patients with SARS-CoV-2 Alpha variant infection: a multicentre matched cohort study

    No full text
    International audienceBackground: The impact of the variant of concern (VOC) Alpha on the severity of COVID-19 has been debated. We report our analysis in France.Methods: We conducted an exposed/unexposed cohort study with retrospective data collection, comparing patients infected by VOC Alpha to contemporaneous patients infected by historical lineages. Participants were matched on age (± 2.5 years), sex and region of hospitalization. The primary endpoint was the proportion of hospitalized participants with severe COVID-19, defined as a WHO-scale > 5 or by the need of a non-rebreather mask, occurring up to day 29 after admission. We used a logistic regression model stratified on each matched pair and accounting for factors known to be associated with the severity of the disease.Results: We included 650 pairs of patients hospitalized between Jan 1, 2021, and Feb 28, 2021, in 47 hospitals. Median age was 70 years and 61.3% of participants were male. The proportion of participants with comorbidities was high in both groups (85.0% vs 90%, p = 0.004). Infection by VOC Alpha was associated with a higher odds of severe COVID-19 (41.7% vs 38.5%-aOR = 1.33 95% CI [1.03-1.72]).Conclusion: Infection by the VOC Alpha was associated with a higher odds of severe COVID-19
    corecore