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首页> 外文期刊>The Journal of Chemical Physics >A theoretical investigation of the influence of gold nanosphere size on the decay and energy transfer rates and efficiencies of quantum emitters
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A theoretical investigation of the influence of gold nanosphere size on the decay and energy transfer rates and efficiencies of quantum emitters

机译：金纳米尺寸对量子发射器衰变和能量转移率和效率影响的理论研究

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We present in this contribution a comprehensive investigation of the effect of the size of gold nanospheres on the decay and energy transfer rates of quantum systems placed close to these nanospheres. These phenomena have been investigated before, theoretically and experimentally, but no comprehensive study of the influence of the nanoparticle size on important dependences of the decay and energy transfer rates, such as the dependence on the donor-acceptor spectral overlap and the relative positions of the donor, acceptor, and nanoparticle, exists. As such, different accounts of the energy transfer mechanism have been presented in the literature. We perform an investigation of the energy transfer mechanisms between emitters and gold nanospheres and between donor-acceptor pairs in the presence of the gold nanospheres using a Green's tensor formalism, experimentally verified in our lab. We find that the energy transfer rate to small nanospheres is greatly enhanced, leading to a strong quenching of the emission of the emitter. When the nanosphere size is increased, it acts as an antenna, increasing the emission of the emitter. We also investigate the emission wavelength and intrinsic quantum yield dependence of the energy transfer to the nanosphere. As evidenced from the literature, the energy transfer process between the quantum system and the nanosphere can have a complicated distance dependence, with a r(-6) regime, characteristic of the Forster energy transfer mechanism, but also exhibiting other distance dependences. In the case of a donor-acceptor pair of quantum systems in the presence of a gold nanosphere, when the donor couples strongly to the nanosphere, acting as an enhanced dipole; the donor-acceptor energy transfer rate then follows a Forster trend, with an increased Forster radius. The coupling of the acceptor to the nanosphere has a different distance dependence. The angular dependence of the energy transfer efficiency between donor and acceptor exhibits a strong focusing effect and the same enhanced donor-dipole character in different angular arrangements. The spectral overlap of the donor emission and acceptor absorption spectra shows that the energy transfer follows the near-field scattering efficiency, with a red-shift from the localized surface plasmon peak for small sphere sizes. (C) 2016 AIP Publishing LLC.
机译：我们在这一贡献中展示了对金纳米球的大小对靠近这些纳米球的衰变和能量转移率的综合调查。这些现象已经在理论上和实验之前进行了调查，但没有对纳米粒子尺寸对衰减和能量转移率的重要依赖性的影响，例如对施主 - 受体光谱重叠的依赖性以及相对位置的影响存在供体，受体和纳米粒子。因此，在文献中呈现了能量转移机制的不同账户。我们在使用绿色的张量形式主义的情况下，在金纳米纳米球的存在下进行发射器和金纳米球之间的能量转移机制以及供体 - 受体对进行研究。我们发现，小纳米球的能量转移率大大提高，导致发射器发射的强烈淬火。当纳米距尺寸增加时，它充当天线，增加发射器的发射。我们还研究了发射波长和固有量子产量依赖于能量转移到纳米圈的依赖性。如文献所证明的，量子系统和纳米之间的能量转移过程可以具有复杂的距离依赖性，具有R（-6）个体，福斯特能力转移机制的特征，但也表现出其他距离依赖性。在纳米球存在下的供体受体对量子系统的情况下，当供体耦合到纳米末端的供体耦合时，作用为增强偶极子;随后供体接受者能量转移率随后用增加的福斯特半径而遵循福尔斯特趋势。受体对纳米片的耦合具有不同的距离依赖性。供体和受体之间的能量转移效率的角度依赖性表现出强烈的聚焦效果和不同角度布置中的相同增强的供体 - 偶极性特征。供体发射和受体吸收光谱的光谱重叠表明，能量传递遵循近场散射效率，从局部表面等离子体峰值进行近场散射效率，用于小球体尺寸。 （c）2016 AIP发布LLC。

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