有机卟啉树枝状大分子中的纠缠光子吸收

Entangled photon absorption in an organic porphyrin dendrimer.

作者信息

Lee Dong-Ik, Goodson Theodore

机构信息

Department of Chemistry and Applied Physics, University of Michigan, Ann Arbor, Michigan 48109.

出版信息

J Phys Chem B. 2006 Dec 28;110(51):25582-5. doi: 10.1021/jp066767g.

Abstract

Two-photon absorption spectroscopy is an intensity dependent nonlinear effect related to the excitation of virtual intermediate states. The classical two-photon absorption has an extremely low efficiency which is quantified by its cross-section (delta approximately 10(-48) cm4 s at 800 nm). To overcome this limitation, we demonstrate a novel effect of the two-photon absorption method utilizing the high degree of quantum optical correlation between photon pairs created by the process of spontaneous parametric downconversion. A large entangled two-photon absorption cross-section (delta(e) approximately 10(-17) cm2 at 800 nm) was measured in an organic porphyrin dendrimer. We also discuss the nonmonotonic behavior of variation of the entangled two-photon absorption cross-section by controlling the entanglement time. This novel effect may open new avenues for ultrasensitive detection in chemical and biological systems. TPA spectroscopy has been considered as a powerful tool in physics, chemistry, and biology. The inherent nonlinear process of the classical TPA is distinguishable from the single photon absorption (SPA) linear process. Although the benefits of greater penetration depth and better control and reduction of scattering, the TPA spectroscopy has been restricted by the necessity of a high power optical source due to the low efficiency of the TPA effect. The use of entangled photons from a correlated source for the purpose of the two-photon effect is promising in this regard as one may obtain two-photon effects with very small numbers of photons.

摘要

双光子吸收光谱是一种与虚拟中间态激发相关的强度依赖型非线性效应。经典的双光子吸收效率极低,其通过截面来量化(在800纳米处,δ约为10^(-48) 平方厘米每秒)。为克服这一限制,我们展示了一种利用自发参量下转换过程产生的光子对之间高度量子光学相关性的双光子吸收方法的新效应。在一种有机卟啉树枝状大分子中测量到了较大的纠缠双光子吸收截面(在800纳米处,δ(e)约为10^(-17) 平方厘米)。我们还讨论了通过控制纠缠时间来改变纠缠双光子吸收截面的非单调行为。这种新效应可能为化学和生物系统中的超灵敏检测开辟新途径。双光子吸收光谱已被视为物理、化学和生物学中的一种强大工具。经典双光子吸收的固有非线性过程与单光子吸收(SPA)的线性过程不同。尽管双光子吸收光谱具有更大穿透深度以及更好地控制和减少散射等优点,但由于双光子吸收效应效率低,一直受到高功率光源需求的限制。在这方面,使用来自相关源的纠缠光子实现双光子效应很有前景,因为人们可以用非常少量的光子获得双光子效应。

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