199 research outputs found

    Model-independent determination of the carrier multiplication time constant in CdSe nanocrystals

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    The experimental determination of the carrier multiplication (CM) time constant is complicated by the fact that this process occurs within the initial few hundreds of femtoseconds after excitation and, in transient-absorption experiments, cannot be separated from the buildup time of the 1p-state population. This work provides an accurate theoretical determination of the electron relaxation lifetime during the last stage of the p-state buildup, in CdSe nanocrystals, in the presence of a single photogenerated hole (no CM) and of a hole plus an additional electron–hole pair (following CM). From the invariance of the 1p buildup time observed experimentally for excitations above and below the CM threshold producing hot carriers with the same average per-exciton excess energy, and the calculated corresponding variations in the electron decay time in the two cases, an estimate is obtained for the carrier multiplication time constant. Unlike previous estimates reported in the literature so far, this result is model-independent, i.e., is obtained without making any assumption on the nature of the mechanism governing carrier multiplication. It is then compared with the time constant calculated, as a function of the excitation energy, assuming an impact-ionization-like process for carrier multiplication (DCM). The two results are in good agreement and show that carrier multiplication can occur on timescales of the order of tens of femtoseconds at energies close to the observed onset. These findings, which are compatible with the fastest lifetime estimated experimentally, confirm the suitability of the impact-ionization model to explain carrier multiplication in CdSe nanocrystals

    Acrylamide acute neurotoxicity in adult zebrafish

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    Un articulo indexadoAcute exposure to acrylamide (ACR), a type-2 alkene, may lead to a ataxia, skeletal muscles weakness and numbness of the extremities in human and laboratory animals. In the present manuscript, ACR acute neurotoxicity has been characterized in adult zebrafish, a vertebrate model increasingly used in human neuropharmacology and toxicology research. At behavioral level, ACR-treated animals exhibited “depression-like” phenotype comorbid with anxiety behavior. At transcriptional level, ACR induced down-regulation of regeneration-associated genes and up-regulation of oligodendrocytes and reactive astrocytes markers, altering also the expression of genes involved in the presynaptic vesicle cycling. ACR induced also significant changes in zebrafish brain proteome and formed adducts with selected cysteine residues of specific proteins, some of them essential for the presynaptic function. Finally, the metabolomics analysis shows a depletion in the monoamine neurotransmitters, consistent with the comorbid depression and anxiety disorder, in the brain of the exposed fish.Conacy

    Ultrafast charge dynamics in trap-free and surface-trapping colloidal quantum dots

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    Ultrafast transient absorption spectroscopy is used to study subnanosecond charge dynamics in CdTe colloidal quantum dots. After treatment with chloride ions, these can become free of surface traps that produce nonradiative recombination. A comparison between these dots and the same dots before treatment enables new insights into the effect of surface trapping on ultrafast charge dynamics. The surface traps typically increase the rate of electron cooling by 70% and introduce a recombination pathway that depopulates the conduction band minimum of single excitons on a subnanosecond timescale, regardless of whether the sample is stirred or flowed. It is also shown that surface trapping significantly reduces the peak bleach obtained for a particular pump fluence, which has important implications for the interpretation of transient absorption data, including the estimation of absorption cross‐sections and multiple exciton generation yields

    A Minimal Model of Metabolism Based Chemotaxis

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    Since the pioneering work by Julius Adler in the 1960's, bacterial chemotaxis has been predominantly studied as metabolism-independent. All available simulation models of bacterial chemotaxis endorse this assumption. Recent studies have shown, however, that many metabolism-dependent chemotactic patterns occur in bacteria. We hereby present the simplest artificial protocell model capable of performing metabolism-based chemotaxis. The model serves as a proof of concept to show how even the simplest metabolism can sustain chemotactic patterns of varying sophistication. It also reproduces a set of phenomena that have recently attracted attention on bacterial chemotaxis and provides insights about alternative mechanisms that could instantiate them. We conclude that relaxing the metabolism-independent assumption provides important theoretical advances, forces us to rethink some established pre-conceptions and may help us better understand unexplored and poorly understood aspects of bacterial chemotaxis

    Investigation of effect of nutritional drink on chemotherapy-induced mucosal injury and tumor growth in an established animal model

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    Chemotherapy-induced mucositis represents a significant burden to quality of life and healthcare costs, and may be improved through enhanced nutritional status. We first determined the safety of two nutritional drinks (plus placebo), and then potential gut protection in tumor-bearing rats in a model of methotrexate-induced mucositis. In study 1, animals were fed one of two test diets (or placebo or control chow pellets) for a total of 60 days and were monitored daily. All diets were found to be safe to administer. In study 2, after seven days of receiving diets, a Dark Agouti Mammary Adenocarcinoma (DAMA) was transplanted subcutaneously. Ten days after starting diets, animals had 2 mg/kg intramuscular methotrexate administered on two consecutive days; after this time, all animals were given soaked chow. Animals were monitored daily for changes in bodyweight, tumor burden and general health. Animals were killed 10, 12 and 16 days after initially starting diets, and tissues were collected at necropsy. In study 1, animals receiving diets had gained 0.8% and 10.8% of their starting bodyweight after 60 days, placebo animals 4.4%, and animals fed on standard chow had gained 15.1%. In study 2, there was no significant influence of test diet on bodyweight, organ weight, tumor burden or biochemical parameters. Only animals treated with MTX exhibited diarrhea, although animals receiving Diet A and Diet C showed a non-significant increase in incidence of diarrhea. Administration of these nutritional drinks did not improve symptoms of mucositis.Emma Bateman, Joanne Bowen, Andrea Stringer, Bronwen Mayo, Erin Plews, Anthony Wignall, Norman Greenberg, Eduardo Schiffrin and Dorothy Keef

    Theory of multiexciton generation in semiconductor nanocrystals

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    We develop a generalized framework based on a Green's function formalism to calculate the efficiency of multiexciton gen-eration in nanocrystal quantum dots. The direct/indirect absorption and coherent/incoherent impact ionization mechanisms, often used to describe multiexciton generation in nanocrystals, are reviewed and rederived from the unified theory as certain approximations. In addition, two new limits are described systematically - the weak Coulomb coupling limit and the semi-wide band limit. We show that the description of multiexciton generation in nanocrystals can be described as incoherent process and we discuss the scaling of multiexciton generation with respect to the photon energy and nanocrystal size. Illustrations are given for three prototype systems: CdSe, InAs and silicon quantum dots.Comment: 9 pages, 5 figure

    Therapeutic potential of N-acetylcysteine in acrylamide acute neurotoxicity in adult zebrafish

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    Two essential key events in acrylamide (ACR) acute neurotoxicity are the formation of adducts with nucleophilic sulfhydryl groups on cysteine residues of selected proteins in the synaptic terminals and the depletion of the glutathione (GSx) stores in neural tissue. The use of N-acetylcysteine (NAC) has been recently proposed as a potential antidote against ACR neurotoxicity, as this chemical is not only a well-known precursor of the reduced form of glutathione (GSH), but also is an scavenger of soft electrophiles such as ACR. In this study, the suitability of 0.3 and 0.75 mM NAC to protect against the neurotoxic effect of 0.75 mM ACR has been tested in vivo in adult zebrafish. NAC provided only a mild to negligible protection against the changes induced by ACR in the motor function, behavior, transcriptome and proteome. The permeability of NAC to cross blood-brain barrier (BBB) was assessed, as well as the ACR-scavenging activity and the gamma-glutamyl-cysteine ligase (γ-GCL) and acylase I activities. The results show that ACR not only depletes GSx levels but also inhibits it synthesis from NAC/cysteine, having a dramatic effect over the glutathione system. Moreover, results indicate a very low NAC uptake to the brain, probably by a combination of low BBB permeability and high deacylation of NAC during the intestinal absorption. These results strongly suggest that the use of NAC is not indicated in ACR acute neurotoxicity treatment.This work was supported by the NATO SfP project MD.SFPP 984777 (D.R.) and the Spanish Government (CTM2017-83242-R; D.R.). M.F acknowledges financial support from the Beatriu de Pinós programme (Grant No. 2016 BP 00233) provided by the Secretariat of Universities and Research department of the Ministry for Business and Knowledge, Catalonia Government. Mention of specific products or trade names does not indicate endorsement by the US federal government.Peer reviewe

    Distribution of carrier multiplication rates in CdSe and InAs nanocrystals

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    The distribution of rates of carrier multiplication (CM) following photon absorption is calculated for semiconductor nanocrystals (NCs). The NC electronic structure is described using a screened pseudopotential method known to give reliable description of NC excitons. The rates of biexciton generation are calculated using the Fermi golden rule with all relevant Coulomb matrix elements, taking into account proper selection rules. In CdSe and InAs NCs we find a broad distribution biexciton generation rates depending strongly on the exciton energy and size of the NC. The process becomes inefficient for NC exceeding 3 nm in diameter in the photon energy range of 2-3 times the band gap.Comment: 4 pages 3 fi
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