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      Nonequilibrium Energy Transfer at Nanoscale: A Unified Theory from Weak to Strong Coupling

      research-article
      1 , 2 , 3 , a , 1 , 4 , b , 1 , 2
      Scientific Reports
      Nature Publishing Group

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          Abstract

          Unraveling the microscopic mechanism of quantum energy transfer across two-level systems provides crucial insights to the optimal design and potential applications of low-dimensional nanodevices. Here, we study the non-equilibrium spin-boson model as a minimal prototype and develop a fluctuation-decoupled quantum master equation approach that is valid ranging from the weak to the strong system-bath coupling regime. The exact expression of energy flux is analytically established, which dissects the energy transfer as multiple boson processes with even and odd parity. Our analysis provides a unified interpretation of several observations, including coherence-enhanced heat flux and negative differential thermal conductance. The results will have broad implications for the fine control of energy transfer in nano-structural devices.

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          Most cited references16

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          Opportunities and challenges for a sustainable energy future.

          Access to clean, affordable and reliable energy has been a cornerstone of the world's increasing prosperity and economic growth since the beginning of the industrial revolution. Our use of energy in the twenty-first century must also be sustainable. Solar and water-based energy generation, and engineering of microbes to produce biofuels are a few examples of the alternatives. This Perspective puts these opportunities into a larger context by relating them to a number of aspects in the transportation and electricity generation sectors. It also provides a snapshot of the current energy landscape and discusses several research and development opportunities and pathways that could lead to a prosperous, sustainable and secure energy future for the world.
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            Electron transport in molecular wire junctions.

            Molecular conductance junctions are structures in which single molecules or small groups of molecules conduct electrical current between two electrodes. In such junctions, the connection between the molecule and the electrodes greatly affects the current-voltage characteristics. Despite several experimental and theoretical advances, including the understanding of simple systems, there is still limited correspondence between experimental and theoretical studies of these systems.
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              Optimization of exciton trapping in energy transfer processes.

              In this paper, we establish optimal conditions for maximal energy transfer efficiency using solutions for multilevel systems and interpret these analytical solutions with more intuitive kinetic networks resulting from a systematic mapping procedure. The mapping procedure defines an effective hopping rate as the leading order picture and nonlocal kinetic couplings as the quantum correction, hence leading to a rigorous separation of thermal hopping and coherent transfer useful for visualizing pathway connectivity and interference in quantum networks. As a result of these calculations, the dissipative effects of the surrounding environments can be optimized to yield the maximal efficiency, and modulation of the efficiency can be achieved using the cumulative quantum phase along any closed loops. The optimal coupling of the system and its environments is interpreted with the generic mechanisms: (i) balancing localized trapping and delocalized coherence, (ii) reducing the effective detuning via homogeneous line-broadening, (iii) suppressing the destructive interference in nonlinear network configurations, and (iv) controlling phase modulation in closed loop configurations. Though these results are obtained for simple model systems, the physics thus derived provides insights into the working of light harvesting systems, and the approaches thus developed apply to large-scale computation.
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                Author and article information

                Journal
                Sci Rep
                Sci Rep
                Scientific Reports
                Nature Publishing Group
                2045-2322
                08 July 2015
                2015
                : 5
                : 11787
                Affiliations
                [1 ]Department of Chemistry, Massachusetts Institute of Technology , 77 Massachusetts Avenue, Cambridge, MA 02139, USA
                [2 ]Singapore-MIT Alliance for Research and Technology , 1 CREATE Way, Singapore 138602, Singapore
                [3 ]Department of Physics, Hangzhou Dianzi University , Hangzhou, Zhejiang 310018, China
                [4 ]Center for Phononics and Thermal Energy Science, School of Physics Science and Engineering, Tongji University , 200092 Shanghai, P. R. China
                Author notes
                Article
                srep11787
                10.1038/srep11787
                4495559
                26152705
                c45066cc-9e07-423e-b515-4b6777c63e94
                Copyright © 2015, Macmillan Publishers Limited

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 18 February 2015
                : 02 June 2015
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