Stimulated Raman Spectroscopy with Entangled Light: Enhanced Resolution and Pathway Selection

Stimulated Raman Spectroscopy with Entangled Light: Enhanced Resolution and Pathway Selection
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DOI:
10.1021/jz501124a
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发表时间:
2014-08-21
影响因子:
5.7
通讯作者:
Mukamel, Shaul
Mukamel, Shaul
中科院分区:
化学2区
文献类型:
--
作者:
Dorfman, Konstantin E.;Schlawin, Frank;Mukamel, Shaul

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我们提出了一种新颖的飞秒受激拉曼光谱(FSRS)技术,该技术将纠缠光子与干涉检测相结合,以选择物质路径并提高分辨率。通过光化泵进行光激发后,测量使用一对宽带纠缠光子;一个(信号)与分子相互作用,并与第三个窄带脉冲一起引发拉曼过程。另一个(闲频)光子为符合测量提供参考。这种干涉光子符合计数检测允许人们单独测量拉曼增益和损耗信号,这是传统探针传输检测不可能实现的。纠缠光子进一步提供了独特的时间和光谱检测窗口,与经典和相关的光解纠缠态相比,可以更好地解析快速激发态动力学。
We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photoexcitation by an actinic pump, the measurement uses a pair of broad-band entangled photons; one (signal) interacts with the molecule and together with a third narrow-band pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon coincidence counting detection allows one to separately measure the Raman gain and loss signals, which is not possible with conventional probe transmission detection. Entangled photons further provide a unique temporal and spectral detection window that can better resolve fast excited-state dynamics compared to classical and correlated disentangled states of light.