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荧光团到单壁碳纳米管的能量转移。

Excitation energy transfer from a fluorophore to single-walled carbon nanotubes.

机构信息

Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012, India.

出版信息

J Chem Phys. 2010 Mar 14;132(10):104502. doi: 10.1063/1.3351844.

Abstract

We study the process of electronic excitation energy transfer from a fluorophore to the electronic energy levels of a single-walled carbon nanotube. The matrix element for the energy transfer involves the Coulombic interaction between the transition densities on the donor and the acceptor. In the Forster approach, this is approximated as the interaction between the corresponding transition dipoles. For energy transfer from a dye to a nanotube, one can use the dipole approximation for the dye, but not for the nanotube. We have therefore calculated the rate using an approach that avoids the dipole approximation for the nanotube. We find that for the metallic nanotubes, the rate has an exponential dependence if the energy that is to be transferred, variant Planck's over 2piOmega is less than a threshold and a d(-5) dependence otherwise. The threshold is the minimum energy required for a transition other than the k(i, perpendicular)=0 and l=0 transition. Our numerical evaluation of the rate of energy transfer from the dye pyrene to a (5,5) carbon nanotube, which is metallic leads to a distance of approximately 165 A up to which energy transfer is appreciable. For the case of transfer to semiconducting carbon nanotubes, apart from the process of transfer to the electronic energy levels within the one electron picture, we also consider the possibility of energy transfer to the lowest possible excitonic state. Transfer to semiconducting carbon nanotubes is possible only if variant Planck's over 2piOmega > or = epsilon(g)-epsilon(b). The long range behavior of the rate of transfer has been found to have a d(-5) dependence if variant Planck's over 2piOmega > or = epsilon(g). But, when the emission energy of the fluorophore is in the range epsilon(g) > variant Planck's over 2piOmega > or = epsilon(g)-epsilon(b), the rate has an exponential dependence on the distance. For the case of transfer from pyrene to the semiconducting (6,4) carbon nanotube, energy transfer is found to be appreciable up to a distance of approximately 175 A.

摘要

我们研究了从荧光团到单壁碳纳米管的电子激发能量转移过程。能量转移的矩阵元涉及供体和受体的跃迁密度之间的库仑相互作用。在福斯特方法中,这被近似为相应跃迁偶极子之间的相互作用。对于从染料到纳米管的能量转移,可以对染料使用偶极近似,但对纳米管不能使用。因此,我们使用避免纳米管偶极近似的方法来计算速率。我们发现,对于金属纳米管,当要转移的能量小于阈值且小于 d(-5)时,速率具有指数依赖性。阈值是除了 k(i,perpendicular)=0 和 l=0 跃迁之外的跃迁所需的最小能量。我们对从染料芘到(5,5)碳纳米管(金属)的能量转移速率的数值评估导致在大约 165 A 的距离内能量转移是可观的。对于转移到半导体碳纳米管的情况,除了在单电子图像内转移到电子能级的过程之外,我们还考虑了能量转移到最低可能激子态的可能性。只有当 variant Planck's over 2piOmega > or = epsilon(g)-epsilon(b)时,才能向半导体碳纳米管转移能量。转移到半导体碳纳米管的长程行为具有 d(-5)依赖性,如果 variant Planck's over 2piOmega > or = epsilon(g)。但是,当荧光团的发射能量处于 epsilon(g) > variant Planck's over 2piOmega > or = epsilon(g)-epsilon(b)范围内时,速率与距离呈指数关系。对于从芘到半导体(6,4)碳纳米管的转移情况,发现能量转移在大约 175 A 的距离内是可观的。

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