88 research outputs found

    Ultrafast charge carrier separation in Potassium-intercalated endohedral metallofullerene Sc3_3N@C80_{80} thin films

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    Molecular materials have emerged as highly tunable materials for photovoltaic and light-harvesting applications. The most severe challenge of this class of materials is the trapping of charge carriers in bound electron-hole pairs, which severely limits the free charge carrier generation. Here, we demonstrate a significant modification of the exciton dynamics of thin films of endohedral metallofullerene complexes upon alkali metal intercalation. For the exemplary case of Sc3_3N@C80_{80} thin films, we show that potassium intercalation results in an additional relaxation channel for the optically excited charge-transfer excitons that prevents the trapping of excitons in a long-lived Frenkel exciton-like state. Instead, K intercalation leads to an ultrafast exciton dissociation coinciding most likely with the generation of free charge carriers. In this way, we propose alkali metal doping of molecular films as a novel approach to enhance the light to-charge carrier conversion efficiency in photovoltaic materials

    Strong modification of the transport level alignment in organic materials after optical excitation

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    Organic photovoltaic devices operate by absorbing light and generating current. These two processes are governed by the optical and transport properties of the organic semiconductor. Despite their common microscopic origin—the electronic structure—disclosing their dynamical interplay is far from trivial. Here we address this issue by time-resolved photoemission to directly investigate the correlation between the optical and transport response in organic materials. We reveal that optical generation of non-interacting excitons in a fullerene film results in a substantial redistribution of all transport levels (within 0.4eV) of the non-excited molecules. As all observed dynamics evolve on identical timescales, we conclude that optical and transport properties are completely interlinked. This finding paves the way for developing novel concepts for transport level engineering on ultrafast time scales that could lead to novel functional optoelectronic devices

    A case study for the formation of stanene on a metal surface

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    The discovery and realization of graphene as an ideal two-dimensional (2D) material has triggered extensive efforts to create similar 2D materials with exciting spin-dependent properties. Here, we report on a novel Sn 2D superstructure on Au(111) that shows similarities and differences to the expected electronic features of ideal stanene. Using spin- and angle-resolved photoemission spectroscopy, we find that a particular Sn/Au superstructure reveals a linearly dispersing band centered at the Γ-point and below the Fermi level with antiparallel spin polarization and a Fermi velocity of vF ≈ 1×106 m/s, the same value as for graphene. We attribute the origin of the band structure to the hybridization between the Sn and the Au orbitals at the 2D Sn-Au interface. Considering that free-standing stanene simply cannot exist, our investigated structure is an important step towards the search of useful stanene-like overstructures for future technological applications

    Autonomic modulation and antiarrhythmic therapy in a model of long QT syndrome type 3

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    AIMS: Clinical observations in patients with long QT syndrome carrying sodium channel mutations (LQT3) suggest that bradycardia caused by parasympathetic stimulation may provoke torsades de pointes (TdP). beta-Adrenoceptor blockers appear less effective in LQT3 than in other forms of the disease. METHODS AND RESULTS: We studied effects of autonomic modulation on arrhythmias in vivo and in vitro and quantified sympathetic innervation by autoradiography in heterozygous mice with a knock-in deletion (DeltaKPQ) in the Scn5a gene coding for the cardiac sodium channel and increased late sodium current (LQT3 mice). Cholinergic stimulation by carbachol provoked bigemini and TdP in freely roaming LQT3 mice. No arrhythmias were provoked by physical stress, mental stress, isoproterenol, or atropine. In isolated, beating hearts, carbachol did not prolong action potentials per se, but caused bradycardia and rate-dependent action potential prolongation. The muscarinic inhibitor AFDX116 prevented effects of carbachol on heart rate and arrhythmias. beta-Adrenoceptor stimulation suppressed arrhythmias, shortened rate-corrected action potential duration, increased rate, and minimized difference in late sodium current between genotypes. beta-Adrenoceptor density was reduced in LQT3 hearts. Acute beta-adrenoceptor blockade by esmolol, propranolol or chronic propranolol in vivo did not suppress arrhythmias. Chronic flecainide pre-treatment prevented arrhythmias (all P < 0.05). CONCLUSION: Cholinergic stimulation provokes arrhythmias in this model of LQT3 by triggering bradycardia. beta-Adrenoceptor density is reduced, and beta-adrenoceptor blockade does not prevent arrhythmias. Sodium channel blockade and beta-adrenoceptor stimulation suppress arrhythmias by shortening repolarization and minimizing difference in late sodium current.status: publishe

    Abundance, Distribution, and Activity of Fe(II)-Oxidizing and Fe(III)-Reducing Microorganisms in Hypersaline Sediments of Lake Kasin, Southern Russia

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    The extreme osmotic conditions prevailing in hypersaline environments result in decreasing metabolic diversity with increasing salinity. Various microbial metabolisms have been shown to occur even at high salinity, including photosynthesis as well as sulfate and nitrate reduction. However, information about anaerobic microbial iron metabolism in hypersaline environments is scarce. We studied the phylogenetic diversity, distribution, and metabolic activity of iron(II)-oxidizing and iron(III)-reducing Bacteria and Archaea in pH-neutral, iron-rich salt lake sediments (Lake Kasin, southern Russia; salinity, 348.6 g liter-1) using a combination of culture-dependent and -independent techniques. 16S rRNA gene clone libraries for Bacteria and Archaea revealed a microbial community composition typical for hypersaline sediments. Most-probable-number counts confirmed the presence of 4.26&times;102 to 8.32&times;103 iron(II)-oxidizing Bacteria and 4.16&times;102 to 2.13&times;103 iron(III)-reducing microorganisms per gram dry sediment. Microbial iron(III) reduction was detected in the presence of 5 M NaCl, extending the natural habitat boundaries for this important microbial process. Quantitative real-time PCR showed that 16S rRNA gene copy numbers of total Bacteria, total Archaea, and species dominating the iron(III)-reducing enrichment cultures (relatives of Halobaculum gomorrense, Desulfosporosinus lacus, and members of the Bacilli) were highest in an iron oxide-rich sediment layer. Combined with the presented geochemical and mineralogical data, our findings suggest the presence of an active microbial iron cycle at salt concentrations close to the solubility limit of NaCl
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