35 research outputs found

    Structure Dependence of Kinetic and Thermodynamic Parameters in Singlet Fission Processes

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    Singlet fission—whereby one absorbed photon generates two coupled triplet excitons—is a key process for increasing the efficiency of optoelectronic devices by overcoming the Shockley–Queisser limit. A crucial parameter is the rate of dissociation of the coupled triplets, as this limits the number of free triplets subsequently available for harvesting and ultimately the overall efficiency of the device. Here we present an analysis of the thermodynamic and kinetic parameters for this process in parallel and herringbone dimers measured by electron paramagnetic resonance spectroscopy in coevaporated films of pentacene in p-terphenyl. The rate of dissociation is higher for parallel dimers than for their herringbone counterparts, as is the rate of recombination to the ground state. DFT calculations, which provide the magnitude of the electronic coupling as well as the distribution of molecular orbitals for each geometry, suggest that weaker triplet coupling in the parallel dimer is the driving force for faster dissociation. Conversely, localization of the molecular orbitals and a stronger triplet–triplet interaction result in slower dissociation and recombination. The identification and understanding of how the intermolecular geometry promotes efficient triplet dissociation provide the basis for control of triplet coupling and thereby the optimization of one important parameter of device performance

    Maser threshold characterization by resonator Q-factor tuning

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    Whereas the laser is nowadays an ubiquitous technology, applications for its microwave analog, the maser, remain highly specialized, despite the excellent low-noise microwave amplification properties. The widespread application of masers is typically limited by the need of cryogenic temperatures. The recent realization of a continuous-wave room-temperature maser, using NV− centers in diamond, is a first step towards establishing the maser as a potential platform for microwave research and development, yet its design is far from optimal. Here, we design and construct an optimized setup able to characterize the operating space of a maser using NV− centers. We focus on the interplay of two key parameters for emission of microwave photons: the quality factor of the microwave resonator and the degree of spin level-inversion. We characterize the performance of the maser as a function of these two parameters, identifying the parameter space of operation and highlighting the requirements for maximal continuous microwave emission

    Towards high performance dielectric microwave resonators for X-band EPR spectroscopy

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    Microwave (MW) resonators in Electron Paramagnetic Resonance (EPR) spectroscopy concentrate the MW magnetic field (B1) at the sample and separate the MW electric field from the sample. There are numerous experimental methods in EPR spectroscopy which all impose different requirements on MW resonators (e.g. high or low quality factor, MW conversion, and B1-field homogeneity). Although commercial spectrometers offer standardized MW resonators for a broad application range, newly emerging and highly-specialized research fields push these spectrometers to or beyond their sensitivity limits. Optimizing the MW resonator offers one direct approach to improve the sensitivity. Here we present three low-cost optimization approaches for a commercially available X-band (9–10 GHz) MW resonator for three experimental purposes (continuous-wave (CW), transient and pulse EPR). We obtain enhanced MW conversion factors for all three optimized resonators and higher quality factors for two optimized resonators. The latter is important for CW and transient EPR. Furthermore, we fabricated a resonator which features an extended area of homogeneous B1-field and, hence, improved pulse EPR performance. Our results demonstrate that small changes to a commercial MW resonator can enhance its performance in general or for specific applications

    Structure dependence of kinetic and thermodynamic parameters in singlet fission processes.

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    Singlet fission-whereby one absorbed photon generates two coupled triplet excitons-is a key process for increasing the efficiency of optoelectronic devices by overcoming the Shockley-Queisser limit. A crucial parameter is the rate of dissociation of the coupled triplets, as this limits the number of free triplets subsequently available for harvesting and ultimately the overall efficiency of the device. Here we present an analysis of the thermodynamic and kinetic parameters for this process in parallel and herringbone dimers measured by electron paramagnetic resonance spectroscopy in coevaporated films of pentacene in p-terphenyl. The rate of dissociation is higher for parallel dimers than for their herringbone counterparts, as is the rate of recombination to the ground state. DFT calculations, which provide the magnitude of the electronic coupling as well as the distribution of molecular orbitals for each geometry, suggest that weaker triplet coupling in the parallel dimer is the driving force for faster dissociation. Conversely, localization of the molecular orbitals and a stronger triplet-triplet interaction result in slower dissociation and recombination. The identification and understanding of how the intermolecular geometry promotes efficient triplet dissociation provide the basis for control of triplet coupling and thereby the optimization of one important parameter of device performance

    Zwischenstaatliche Kriege

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    Aus dem Blick der Risikobewertung und -bewältigung ist zwischenstaatlicher Krieg ein Schadensereignis mit regional unterschiedlicher Wahrscheinlichkeit bei großer Wirkung (varying probability/high impact). Dieser Beitrag diskutiert (1) die definitorische Abgrenzung des zwischenstaatlichen Krieges von anderen Formen des Krieges sowie (2) die Häufigkeit der Formen von Krieg in der Zeit seit 1946. Danach präsentiert er (3) eine Phänomenologie des Kriegsbeginns und fasst (4) die Resultate der Forschung zu den Ursachen von zwischenstaatlichen Kriegen zusammen. Es folgt (5) eine Systematik der sicherheitspolitischen Maßnahmen des Staates zur Kriegsprävention und abschließend (6) der Blick auf das völkerrechtliche Umfeld
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