311 research outputs found

    Reversible Modulation of Surface Plasmons in Gold Nanoparticles Enabled by Surface Redox Chemistry

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    This is the peer reviewed version of the following article: “Reversible modulation of surface plasmons in gold nanoparticles enabled by surface redox chemistry” Z. Li*, J. J. Foley IV*, S. Peng, C.-J. Sun, Y. Ren, G. P. Wiederrecht, S. K. Gray, Y. Sun, Angew. Chemie 127, 9076-9079 (2015), which has been published in final form at https://doi.org/10.1002/anie.201502012. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.Switchable surface redox chemistry is demonstrated in gold@iron/iron oxide core–shell nanoparticles with ambient oxidation and plasmon-mediated reduction to modulate the oxidation state of shell layers. The iron shell can be oxidized to iron oxide through ambient oxidation, leading to an enhance- ment and red-shift of the gold surface plasmon resonance (SPR). This enhanced gold SPR can drive reduction of the iron oxide shell under broadband illumination to reversibly blue- shift and significantly dampen gold SPR absorption. The observed phenomena provide a unique mechanism for con- trolling the plasmonic properties and surface chemistry of small metal nanoparticles.Accepted Manuscript (AM

    Paranoia and irony in the Anglophone dectective narrative and the novels of Umberto Eco

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    The thesis provides a reading of Umberto Eco's three novels, The Name of the Rose, Foucault's Pendulum, and The Island of the Day Before, that, while it acknowledges the importance of the Italian literary tradition in which they stand, also seeks to explain why their author appeals so frequently to literary models outside Italy, and in particular the Anglo-American detective genre. Chapter One explains Eco's relationship to the development of Italian literature through his lifetime. It is noted that Eco is beginning, both in his semiotics and his fiction, from a position where post-structuralism has been extensively explored by neo-avant-gardew riters. Eco positions himself alongsides uchw riters as Italo Calvino and Jorge Luis Borges, who wish to explore the ludic possibilities of working within structures, while all the time acknowledging the epistemological limitations of so doing. Eco's chosen structure, more often than not, is the highly defined genre of the detective story. From here, the following chapters engage in close readings of the three novels, with particular emphasis on The Name of the Rose and Foucault's Pendulum, demonstrating that they explore problems of interpretation central to the detective narrative. In doing this, they display an intimate knowledge of generic developments within the detective tradition, and of the philosophical and aesthetic uses made of the genre by other writers. The embedding of intertextual references to other detective narratives within Eco's novels is an important factor, as they come together to form a narrative of epistemological inquiry that itself follows Eco's philosophical progress through the years. In short, the novels, inter alia, map a systematic inquiry into the possibility of systematic inquiry. They reserve the space to engage in such an ironic and self-referential project precisely through their fictionality

    An advanced LED-based setup enabling characterization of full-size modules at different temperatures and spectra

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    Standard IV characterization of solar cells and modules is typically performed with Xe-, W- and/or metalhalide-based systems. These are either built around a flash or a steady-state illumination. However, there is a growing trend towards LED-based systems, which allows both flash and steady-state white-light illumination, as well as spectrally-tuned irradiance, broadening the scope of measurements from IV to also include spectral dependencies [1]. In this paper we introduce an advanced LED-based setup for modules and investigate its potential for spectrally-tuned measurements as a function of temperature. While the impact of temperature in measured currents and resulting extraction of accurate EQE requires further fine-tuning of the equipment, some applications with comparative measurements are elaborated to demonstrate the approach and capabilities at its current stage.The work in this paper was partially funded by the Kuwait Foundation for the Advancement of Sciences under project number P115-15EE-01, by the Flemish government within the projects SolsThore, LenoPV and ICONTWILL-BIPV, and by the partners in the imec SiPV industrial affiliation programme. Additionally, we also want to acknowledge Geert, Luc and Reinoud from our technical team for their support in the installation, maintenance and improvement of the new facilities and equipment with all its challenges, that is instrumental for obtaining these results and further progress in our research. Finally, we also want to acknowledge Soltech for the supply of printed glass.Govaerts, J (corresponding author), IMEC, EnergyVille, Thorpk 8320, B-3600 Genk, Belgium. [email protected]

    WPTherml: Pioneering the design of materials for harvesting heat.

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    WPTherml stands for William Paterson University’s tool for Thermal Energy and Radiation management with Multi Layer nanostructures. The vision of this software package is to provide an easy-to-use platform for the design of materials with tailored optical and thermal properties for the vast number of energy applications where control of absorption and emission of radiation, or conversion of heat to radiation or vice versa, is paramount. The optical properties are treated within classical electrodynamics, and the current version uses the Transfer Matrix Method to rigorously solve Maxwell’s equations for layered isotropic media. WPTherml was conceived and developed by the Foley Lab at William Paterson University.WPTherml is a Python package for the design of materials with tailored optical and thermal properties for the vast number of energy applications where control of absorption and emission of radiation, or conversion of heat to radiation or vice versa, is paramount. The optical properties are treated within classical electrodynamics via the Transfer Matrix Method which rigorously solve Maxwell's equations for layered isotropic media. A flexible multilayer class connects rigorous electrodynamics properties to figures of merit for a variety of thermal applications, and facilitates extensions to other applications for greater reuse potential. WPTherml can be accessed at https://github.com/FoleyLab/wptherml

    Cage versus Prism: Electronic Energies of the Water Hexamer

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    This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry A, copyright © 2013 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://doi.org/10.1021/jp405739d.Recent experiments show that the cage isomer of the water hexamer is lower in energy than the prism isomer near 0 K, and yet state-of-the-art electronic structure calculations predict the prism to be lower in energy than the cage at 0 K. Here we study the relative energies of the water hexamers from the parametric 2-electron reduced-density-matrix (2-RDM) method in which the 2-RDM rather than the wavefunction is the basic variable of the calculations. In agreement with experiment and in contrast with traditional wavefunction methods, the 2-RDM calculations predict the cage to be more stable than the prism after vibrational zero-point correction. Multiple configurations from the hydrogen bonding are captured by the method. More generally, the results are consistent with our previous 2-RDM applications in that they reveal how multireference correlation in molecular systems is important for resolving small energy differences from hydrogen bonding as well as other types of intermolecular forces, even in systems that are not conventionally considered strongly correlated.D.A.M. gratefully acknowledges the NSF under Grant No. CHE-1152425, the ARO under Grant No. W91 INF-1 1-504 1-0085, the Keck Foundation, and Microsoft Corporation for their support.Accepted Manuscript (AM

    Unique Hot Carrier Distributions from Scattering-Mediated Absorption

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    Light-initiated generation of energetic carriers has attracted considerable attention as a paradigm for photocatalysis and solar energy conversion, and the use of noble metal nanoparticles that support localized surface plasmon resonances has been widely explored as a medium for realizing this paradigm. It was recently shown that composite nanostructures enabling the interplay between dielectric scattering resonances and broadband absorption in small metal nanostructures, a phenomenon termed scattering-mediated absorption, can be used to mediate energetic carrier transfer and selective photochemistry with low-intensity light while completely circumventing plasmon resonance. In this work, we develop a multiscale modeling approach for elucidating the hot carrier dynamics initiated by scattering-mediated absorption. Our calculations reveal that unique hot carrier distributions and dynamics arise from scattering-mediated absorption as compared to plasmon excitation and also suggest that in a variety of circumstances scattering-mediated absorption may lead to more efficient hot carrier generation compared to plasmon resonance under the same external illumination conditions. These results are an important first step in understanding the phenomena of scattering-mediated hot carrier generation, which has potential for expanding the palette of materials that can be utilized for hot carrier mediated photochemistry beyond plasmonic metals and for enabling unique pathways for photocatalytic transformations

    Design of emitter structures based on resonant perfect absorption for thermophotovoltaic applications

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    We report a class of thermophotovoltaic emitter structures built upon planar films that support resonant modes, known as perfectly absorbing modes, that facilitate an exceptional optical response for selective emission. These planar structures have several key advantages over previously-proposed designs for TPV applications: they are simple to fabricate, are stable across a range of temperatures and conditions, and are capable of achieving some of the highest spectral efficiencies reported of any class of emitter structure. Utilization of these emitters leads to exceptionally high device efficiencies under low operating temperature conditions, which should open new opportunities for waste heat management. We present a theoretical framework for understanding this performance, and show that this framework can be leveraged as a search algorithm for promising candidate structures. In addition to providing an efficient theoretical methodology for identifying high-performance emitter structures, our methodology provides new insight into underlying design principles and should pave way for future design of structures that are simple to fabricate, temperature stable, and possess exceptional optical properties.Version of Recor
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