460 research outputs found

    Accessing dark states optically through excitation-ferrying states

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    The efficiency of solar energy harvesting systems is largely determined by their ability to transfer excitations from the antenna to the energy trapping center before recombination. Dark state protection, achieved by coherent coupling between subunits in the antenna structure, can significantly reduce radiative recombination and enhance the efficiency of energy trapping. Because the dark states cannot be populated by optical transitions from the ground state, they are usually accessed through phononic relaxation from the bright states. In this study, we explore a novel way of connecting the dark states and the bright states via optical transitions. In a ring-like chromophore system inspired by natural photosynthetic antennae, the single-excitation bright state can be optically connected to the lowest energy single-excitation dark state through certain double-excitation states. We call such double-excitation states the ferry states and show that they are the result of accidental degeneracy between two categories of double-excitation states. We then mathematically prove that the ferry states are only available when N, the number of subunits on the ring, satisfies N=4l+2 (l being an integer). Numerical calculations confirm that the ferry states enhance the energy transfer power of our model, showing a significant energy transfer power spike at N=6 compared with smaller N values, even without phononic relaxation. The proposed mathematical theory for the ferry states is not restricted to this one particular system or numerical model. In fact, it is potentially applicable to any coherent optical system that adopts a ring-shaped chromophore arrangement. Beyond the ideal case, the ferry state mechanism also demonstrates robustness under weak phononic dissipation, weak site energy disorder, and large coupling strength disorder

    Optical resonance imaging: An optical analog to MRI with sub-diffraction-limited capabilities

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    We propose here optical resonance imaging (ORI), a direct optical analog to magnetic resonance imaging (MRI). The proposed pulse sequence for ORI maps space to time and recovers an image from a heterodyne-detected third-order nonlinear photon echo measurement. As opposed to traditional photon echo measurements, the third pulse in the ORI pulse sequence has significant pulse-front tilt that acts as a temporal gradient. This gradient couples space to time by stimulating the emission of a photon echo signal from different lateral spatial locations of a sample at different times, providing a widefield ultrafast microscopy. We circumvent the diffraction limit of the optics by mapping the lateral spatial coordinate of the sample with the emission time of the signal, which can be measured to high precision using interferometric heterodyne detection. This technique is thus an optical analog of MRI, where magnetic-field gradients are used to localize the spin-echo emission to a point below the diffraction limit of the radio-frequency wave used. We calculate the expected ORI signal using 15 fs pulses and 87° of pulse-front tilt, collected using f/2 optics and find a two-point resolution 275 nm using 800 nm light that satisfies the Rayleigh criterion. We also derive a general equation for resolution in optical resonance imaging that indicates that there is a possibility of superresolution imaging using this technique. The photon echo sequence also enables spectroscopic determination of the input and output energy. The technique thus correlates the input energy with the final position and energy of the exciton

    Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides

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    Light harvesting in photosynthetic organisms involves efficient transfer of energy from peripheral antenna complexes to core antenna complexes, and ultimately to the reaction center where charge separation drives downstream photosynthetic processes. Antenna complexes contain many strongly coupled chromophores, which complicates analysis of their electronic structure. Two-dimensional electronic spectroscopy (2DES) provides information on energetic coupling and ultrafast energy transfer dynamics, making the technique well suited for the study of photosynthetic antennae. Here, we present 2DES results on excited state properties and dynamics of a core antenna complex, light harvesting complex 1 (LH1), embedded in the photosynthetic membrane of Rhodobacter sphaeroides. The experiment reveals weakly allowed higher-lying excited states in LH1 at 770 nm, which transfer energy to the strongly allowed states at 875 nm with a lifetime of 40 fs. The presence of higher-lying excited states is in agreement with effective Hamiltonians constructed using parameters from crystal structures and atomic force microscopy (AFM) studies. The energy transfer dynamics between the higher- and lower-lying excited states agree with Redfield theory calculations

    Proteomic analysis of Plasmodium falciparum histone deacetylase 1 complex proteins

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    Plasmodium falciparum histone deacetylases (PfHDACs) are an important class of epigenetic regulators that alter protein lysine acetylation, contributing to regulation of gene expression and normal parasite growth and development. PfHDACs are therefore under investigation as drug targets for malaria. Despite this, our understanding of the biological roles of these enzymes is only just beginning to emerge. In higher eukaryotes, HDACs function as part of multi-protein complexes and act on both histone and non-histone substrates. Here, we present a proteomics analysis of PfHDAC1 immunoprecipitates, identifying 26 putative P. falciparum complex proteins in trophozoite-stage asexual intraerythrocytic parasites. The co-migration of two of these (P. falciparum heat shock proteins 70-1 and 90) with PfHDAC1 was validated using Blue Native PAGE combined with Western blot. These data provide a snapshot of possible PfHDAC1 interactions and a starting point for future studies focused on elucidating the broader function of PfHDACs in Plasmodium parasites

    Fanny Copeland and the geographical imagination

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    Raised in Scotland, married and divorced in the English south, an adopted Slovene, Fanny Copeland (1872 – 1970) occupied the intersection of a number of complex spatial and temporal conjunctures. A Slavophile, she played a part in the formation of what subsequently became the Kingdom of Yugoslavia that emerged from the First World War. Living in Ljubljana, she facilitated the first ‘foreign visit’ (in 1932) of the newly formed Le Play Society (a precursor of the Institute of British Geographers) and guided its studies of Solčava (a then ‘remote’ Alpine valley system) which, led by Dudley Stamp and commended by Halford Mackinder, were subsequently hailed as a model for regional studies elsewhere. Arrested by the Gestapo and interned in Italy during the Second World War, she eventually returned to a socialist Yugoslavia, a celebrated figure. An accomplished musician, linguist, and mountaineer, she became an authority on (and populist for) the Julian Alps and was instrumental in the establishment of the Triglav National Park. Copeland’s role as participant observer (and protagonist) enriches our understanding of the particularities of her time and place and illuminates some inter-war relationships within G/geography, inside and outside the academy, suggesting their relative autonomy in the production of geographical knowledge

    Diverse Contexts of Zoonotic Transmission of Simian Foamy Viruses in Asia

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    In Asia, contact between persons and nonhuman primates is widespread in multiple occupational and nonoccupational contexts. Simian foamy viruses (SFVs) are retroviruses that are prevalent in all species of nonhuman primates. To determine SFV prevalence in humans, we tested 305 persons who lived or worked around nonhuman primates in several South and Southeast Asian countries; 8 (2.6%) were confirmed SFV positive by Western blot and, for some, by PCR. The interspecies interactions that likely resulted in virus transmission were diverse; 5 macaque taxa were implicated as the source of infection. Phylogenetic analysis showed that SFV from 3 infected persons was similar to that from the nonhuman primate populations with which the infected persons reported contact. Thus, SFV infections are likely to be prevalent among persons who live or work near nonhuman primates in Asia
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