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Spectroscopic sensing enhanced by quantum molecular coherence and by plasmonic nanoantennas

机译:量子分子相干性和等离子体纳米环增强的光谱传感

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Raman scattering is a powerful instrument for spectroscopic sensing, which o ers superb selectivity but typicallyat the expense of low signal and long collection times. In this paper we discuss mechanisms for signalenhancement that dramatically improve the performance of Raman spectroscopic systems. Several approaches,as well as their combinations are considered. One approach is to produce Raman coherence; other approachesexploit the advantages of nanosized antenna-like structures, or employ wavefront shaping of the applied laserbeams. Combining these techniques in one system leads to multiplicative signal enhancement and results in anunprecedented sensitivity. In a sequence of steps toward this goal, we show that the automated feedback-basedwavefront shaping algorithm is capable of improving coherent cascaded Raman scattering in crystals. In addition,we utilize the fact that specially designed nanoantennas, placed in the vicinity of the target molecule, cansigni cantly increase the probability of exciting dipole-forbidden electronic transitions. Nanostructure-enhancedspectroscopy with shaped beams will allow for an increase in spectroscopic sensitivity and e cient detection ofmagnetic dipole and electric quadrupole transitions induced in molecules. The ultimate goal for developing thesetechniques is to achieve single-molecule sensitivity in spectroscopy, combined with atomic spatial resolution,study the layout and chemical bonds of the molecular structure and extract information relevant to chirality.
机译:拉曼散射是一种强大的光谱传感仪器,哪种仪器均匀的选择性,但通常以低信号和长收集时间为代价。在本文中,我们讨论了信号的机制提高显着改善拉曼光谱系统性能的性能。几种方法,以及他们的组合被考虑。一种方法是产生拉曼一致性;其他方法利用纳米天线结构的优点,或采用应用激光的波前整形梁。在一个系统中结合这些技术导致乘法信号增强和结果前所未有的敏感性。在朝着这一目标的一系列步骤中,我们表明基于自动化反馈波前塑形算法能够改善晶体中的相干级联拉曼散射。此外,我们利用特殊设计的纳米环绕的事实,置于目标分子附近,可以Signi显着提高了令人兴奋的偶极禁止电子转换的可能性。纳米结构增强具有成形光束的光谱将允许增加光谱敏感性和e CIER检测分子中诱导的磁性偶极子和电动四极转变。发展这些的最终目标技术是在光谱学中实现单分子敏感性,结合原子空间分辨率,研究分子结构的布局和化学键,提取与手性相关的提取信息。

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