Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities,ACS Nano

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Quantum Mechanical Description of Raman Scattering from Molecules in Plasmonic Cavities
ACS Nano ( IF 15.8 ) Pub Date : 2016-05-31 00:00:00 , DOI: 10.1021/acsnano.6b02484
Mikolaj K. Schmidt _{1,

2} , Ruben Esteban ₂ , Alejandro González-Tudela ₃ , Geza Giedke _{2,

4} , Javier Aizpurua _{1,

2}

Affiliation

Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of phonon-stimulated Raman scattering and a counterintuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this QED framework opens a venue to analyze the correlations of photons emitted from a plasmonic cavity.

中文翻译：

等离子体腔中分子从拉曼散射的量子力学描述

等离子体增强的拉曼散射可以使单分子振动光谱学超越经典电动力学可解决的范围。我们采用等离激元和分子振动相干相互作用的量子电动力学（QED）描述，揭示了系统非弹性响应中非线性的出现。对于现实情况，我们预测了声子激发的拉曼散射的发生以及反斯托克斯发射对激发频率的反直觉依赖性。我们进一步表明，该QED框架为分析等离子体腔发出的光子的相关性开辟了场所。

更新日期：2016-05-31

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