91 research outputs found

    Exciton Dynamics in the J-Aggregates of a Carbocyanine Dye

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    We report on the exciton dynamics in the J-aggregating dye 5,5',6,6'-tetrachloro-1,1'-diethyl-3,3'-di(4-sulfobutyl)-benzimidazolocarbocyanine, which is known readily to form J-aggregates, even at room temperature and at a low concentration. We performed a series of time-correlated single-photon-counting experiments at different emission wavelengths and at different temperatures in the range between 1.5 and 125 K. Additionally, the temperature dependence of the relative fluorescence quantum yield was determined

    Linear optical properties of one-dimensional Frenkel exciton systems with intersite energy correlations

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    We analyze the effects of intersite energy correlations on the linear optical properties of one-dimensional disordered Frenkel exciton systems. The absorption line width and the factor of radiative rate enhancement are studied as a function of the correlation length of the disorder. The absorption line width monotonously approaches the seeding degree of disorder on increasing the correlation length. On the contrary, the factor of radiative rate enhancement shows a non-monotonous trend, indicating a complicated scenario of the exciton localization in correlated systems. The concept of coherently bound molecules is exploited to explain the numerical results, showing good agreement with theory. Some recent experiments are discussed in the light of the present theory.Comment: 18 pages, 3 figues, REVTeX, to appear in Physical Review

    Impact of Penny Brohn UK’s Living Well course on informal caregivers of people with cancer

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    Objectives: This study evaluated the change in the concerns, wellbeing and lifestyle behaviours of informal caregivers of people with cancer attending Penny Brohn UK’s Living Well Course (LWC), a self-management education intervention. Design: A pre-post-course design collected self-reported quantitative and qualitative data from informal caregivers attending a LWC. Setting/Location: Penny Brohn UK is a UK based charity (not-for-profit) providing specialist integrative, whole person support, free of charge, to people affected by cancer. Subjects: Informal caregivers taking part in a Penny Brohn UK LWC between June 2014 and May 2016 attending alongside the person with cancer. Intervention: The LWC is a structured 15 hour, multi-modal group self-management educational course, designed to help people affected by cancer learn tools and techniques to help build resilience. Trained facilitators deliver LWCs to around 12 people with various types and stages of cancer, and their informal caregivers. Outcome measures: MYCaW (Measure Yourself Concern and Wellbeing) completed pre-course and at 6 weeks post-course; and bespoke 6 week follow up Patient Reported Experience Measure (PREM). Results: 480 informal caregivers attended a LWC June 2014 to May 2016. 118 completed a 6 week follow up MYCaW: MYCaW Concerns 1 and 2 showed statistically significant improvements (p<.0001), there was no significant improvement in wellbeing. Informal caregivers’ most reported concerns relating to themselves were psychological and emotional issues (59%). The primary concern of the caregiver for the care recipient was related to the physical health of the person with cancer (40%). 87% of responding informal caregivers stated the LWC enabled health self-management. Conclusions: The LWC was followed by an improvement in informal caregivers’ concerns, and increased self-management of their own health needs. More studies, with larger sample size, are needed to explore if better self-management by informal caregivers may also lead to improvements in patients’ health and wellbeing

    Synthesis And Characterization Of Zno And Zno:ga Films And Their Application In Dye-sensitized Solar Cells

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    Highly crystalline ZnO and Ga-modified zinc oxide (ZnO:Ga) nanoparticles containing 1, 3 and 5 atom% of Ga 3+ were prepared by precipitation method at low temperature. The films were characterized by XRD, BET, XPS and SEM. No evidence of zinc gallate formation (ZnGa 2O 4), even in the samples containing 5 atom% of gallium, was detected by XRD. XPS data revealed that Ga is present into the ZnO matrix as Ga 3+, according to the characteristic binding energies. The particle size decreased as the gallium level was increased as observed by SEM, which might be related to a faster hydrolysis reaction rate. The smaller particle size provided films with higher porosity and surface area, enabling a higher dye loading. When these films were applied to dye-sensitized solar cells (DSSCs) as photoelectrodes, the device based on ZnO:Ga 5 atom% presented an overall conversion efficiency of 6% (at 10 mW cm -2), a three-fold increase compared to the ZnO-based DSSCs under the same conditions. To our knowledge, this is one of the highest efficiencies reported so far for ZnO-based DSSCs. Transient absorption (TAS) study of the photoinduced dynamics of dye-sensitized ZnO:Ga films showed that the higher the gallium content, the higher the amount of dye cation formed, while no significant change on the recombination dynamics was observed. The study indicates that Ga-modification of nanocrystalline ZnO leads to an improvement of photocurrent and overall efficiency in the corresponding device. © 2008 The Royal Society of Chemistry.1114871491O'Regan, B., Gratzel, M., (1991) Nature, 353, p. 737. , -740Kroon, J.M., Bakker, N.J., Smit, H.J.P., Liska, P., Thampi, K.R., Wang, P., Zakeeruddin, S.M., Tulloch, G.E., (2007) Prog. Photovoltaics, 15, p. 1. , -18Ma, T., Akiyama, M., Abe, E., Imai, I., (2005) Nano Lett., 5, p. 2543. , -2547Ko, K.H., Lee, Y.C., Jung, Y.J., (2005) J. Colloid Interface Sci., 283, p. 482. , -487Kakiuchi, K., Hosono, E., Fujihara, S., (2006) J. Photochem. Photobiol., A, 179, p. 81. , -86Keis, K., Magnusson, E., Lindstrom, H., Lindquist, S.-E., Hagfeldt, A., (2002) Sol. Energy Mater. Sol. Cells, 73, p. 51. , -58Horiuchi, H., Katoh, R., Hara, K., Yanagida, M., Murata, S., Arakawa, H., Tachiya, M., (2003) J. Phys. Chem. B, 107, p. 2570. , -2574Katoh, R., Furube, A., Tamaki, Y., Yoshihara, T., Murai, M., Hara, K., Murata, S., Tachiya, M., (2004) J. Photochem. Photobiol., A, 166, p. 69. , -74Keis, K., Vayssieres, L., Rensmo, H., Lindquist, S.-E., Hagfeldt, A., (2001) J. Electrochem. Soc., 148, p. 149. , -A155Rensmo, H., Keis, K., Lindstrom, H., Sodergren, S., Solbrand, A., Hagfeldt, A., Lindquist, S.E., Muhammed, M., (1997) J. Phys. Chem. B, 101, p. 2598. , -2601Minami, T., Sato, H., Nanto, H., Takata, S., (1985) Jpn. J. Appl. Phys., 24, p. 781. , -L784Park, S.-M., Ikegami, T., Ebihara, K., (2006) Thin Solid Films, 513, p. 90. , -94Nonaka, M., Matsushima, S., Mizuno, M., Kobayashi, K., (2002) Chem. Lett., p. 580. , -581Ohkita, H., Cook, S., Ford, T.A., Greenham, N.C., Durrant, J.R., (2006) J. Photochem. Photobiol., A, 182, p. 225. , -230Haque, S.A., Tachibana, Y., Willis, R.L., Moser, J.E., Gratzel, M., Klug, D.R., Durrant, J.R., (2000) J. Phys. Chem. B, 104, p. 538. , -547Haque, S.A., Tachibana, Y., Klug, D.R., Durrant, J.R., (1998) J. Phys. Chem. B, 102, p. 1745. , -1749Gonçalves, A.S., Lima, S.A.M., Davolos, M.R., Antônio, S.G., Paiva-Santos, C.O., (2006) J. Solid State Chem., 179, p. 1330. , -1334Roberts, N., Wang, R.P., Sleight, A.W., Warren, W.W., (1998) Phys. Rev. B, 57, p. 5734Wang, R., Sleight, A.W., Cleary, D., (1996) Chem. Mater., 8, p. 433. , -439Passlack, M., Schubert, E.F., Hobson, W.S., Hong, M., Moriya, N., Chu, S.N.G., Konstadinidis, K., Zydzik, G.J., (1995) J. Appl. Phys., 77, p. 686. , -693Bhosle, V., Tiwari, A., Narayan, J., (2006) J. Appl. Phys., 100, p. 033713. , -033716Nazeeruddin, M.K., Kay, A., Rodicio, I., Humphrybaker, R., Muller, E., Liska, P., Vlachopoulos, N., Gratzel, M., (1993) J. Am. Chem. Soc., 115, p. 6382. , -6390Imai, Y., Watanabe, A., (2005) J. Mater. Sci., 15, p. 743. , -749Willis, R.L., Olson, C., O'Regan, B., Lutz, T., Nelson, J., Durrant, J.R., (2002) J. Phys. Chem. B, 106, p. 7605. , -7613Green, A.N.M., Palomares, E., Haque, S.A., Kroon, J.M., Durrant, J.R., (2005) J. Phys. Chem. B, 109, p. 12525. , -1253

    The PHENIX Experiment at RHIC

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    The physics emphases of the PHENIX collaboration and the design and current status of the PHENIX detector are discussed. The plan of the collaboration for making the most effective use of the available luminosity in the first years of RHIC operation is also presented.Comment: 5 pages, 1 figure. Further details of the PHENIX physics program available at http://www.rhic.bnl.gov/phenix

    Multihole water oxidation catalysis on haematite photoanodes revealed by operando spectroelectrochemistry and DFT

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    Water oxidation is the key kinetic bottleneck of photoelectrochemical devices for fuel synthesis. Despite advances in the identification of intermediates, elucidating the catalytic mechanism of this multi redox reaction on metal oxide photoanodes remains a significant experimental and theoretical challenge. Here, we report an experimental analysis of water oxidation kinetics on four widely studied metal oxides, focusing particularly on haematite. We observe that haematite is able to access a reaction mechanism that is third order in surface hole density, which is assigned to equilibration between three surface holes and M OH O M OH sites. This reaction exhibits low activation energy Ea amp; 8201; amp; 8776; amp; 8201;60 amp; 8201;meV . Density functional theory is used to determine the energetics of charge accumulation and O O bond formation on a model haematite 110 surface. The proposed mechanism shows parallels with the function of the oxygen evolving complex of photosystem II, and provides new insights into the mechanism of heterogeneous water oxidation on a metal oxide surfac

    Impact of interface energetic alignment and mobile ions on charge carrier accumulation and extraction in p‐i‐n perovskite solar cells

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    Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement of real-time PL spectra during current–voltage (J–V) scans under 1-sun equivalent illumination, with the results of drift-diffusion simulations. This operando PL analysis allows direct comparison between the internal performance (recombination currents and quasi-Fermi-level-splitting (QFLS)) and the external performance (J–V) of a PSC during operation. Analyses of four PSCs with different electron transport materials (ETMs) quantify how a deeper ETM LUMO induces greater interfacial recombination, while a shallower LUMO impedes charge extraction. Furthermore, it is found that a low ETM mobility leads to charge accumulation in the perovskite under short-circuit conditions. However, thisalone cannot explain the remarkably high short-circuit QFLS of over 1 eV which is observed in all devices. Instead, drift-diffusion simulations allow this effect to be assigned to the presence of mobile ions which screen the internal electric field at short-circuit and lead to a reduction in the short-circuit current density by over 2 mA cm−2 in the best device
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