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arXiv 2001.05521physics.optics
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等离子体波导中的单分子非线性

Single Molecule Nonlinearity in a Plasmonic Waveguide

Christian Schörner, Markus Lippitz

摘要:

等离子体波导提供了将光限制在远低于衍射极限的独特可能性。耦合到这种波导的单量子发射器的过去的室温实验主要集中在线性光激发之后将自发发射有效地引导到波导模式中。然而,只有发射体与多个等离子体激元场的同时相互作用才会导致等离子体激元电路中的功能。在这里,我们展示了一个单一的分子和传播等离子体激元的非线性光学相互作用。一个单独的三萘嵌苯二酰亚胺(TDI)分子被放置在两个单晶银纳米线之间的纳米间隙中。可见波长泵浦脉冲和红移耗尽脉冲沿波导传播,导致观察到的荧光中的受激发射耗尽(STED)。与远场激励相比,效率提高了50倍。因此,我们的研究表明远程非线性四波混频在一个单一的分子与传播等离子体激元。它为功能化量子等离子体电路和改进的非线性单分子光谱学铺平了道路。

英文摘要:

Plasmonic waveguides offer the unique possibility to confine light far below the diffraction limit. Past room temperature experiments of single quantum emitters coupled to such waveguides have mainly focused on efficient channelling of the spontaneous emission into waveguide modes after a linear optical excitation. However, only the simultaneous interaction of the emitter with multiple plasmonic fields would lead to functionality in a plasmonic circuit. Here, we demonstrate the nonlinear optical interaction of a single molecule and propagating plasmons. An individual terrylene diimide (TDI) molecule is placed in the nanogap between two single-crystalline silver nanowires. A visible wavelength pump pulse and a red-shifted depletion pulse travel along the waveguide, leading to stimulated emission depletion (STED) in the observed fluorescence. The efficiency increases by up to a factor of 50 compared to far-field excitation. Our study thus demonstrates remote nonlinear four-wave mixing at a single molecule with propagating plasmons. It paves the way towards functional quantum plasmonic circuits and improved nonlinear single-molecule spectroscopy.

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