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arXiv 2010.06017physics.opticsphysics.app-phphysics.atm-clus
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共振和非共振相干非线性光学过程的一维和二维相关谱分析

One- and two-dimensional correlation spectroscopy analyses for resonant and non-resonant coherent nonlinear optical processes

Supriya Nagpal, Bryan Semon, Gombojav O. Ariunbold

摘要:

三色相干反斯托克斯喇曼散射代表了非简并四波混频过程,包括非共振和共振两个过程,其贡献取决于输入激光脉冲如何激发分子振动模。非简并四波混频过程很复杂,理解这些过程需要严格的数据分析工具,而这在该研究领域仍然缺乏。在这项工作中,我们引入了一个新的变量(例如,探测脉冲延迟)和新的扰动参数(例如,探测脉冲线宽)。特别是,对角线投影在这里被定义为一种工具,以减少同步和异步的二维相关光谱分析到一维分析,揭示有价值的分析信息。详细的分析使用全高斯相干拉曼散射的封闭形式的解决方案和有代表性的实验数据的共振和非共振过程,并进行了比较。这种强度-强度相关分析工具在解决和可视化定量无标记物种特异性非线性光谱和显微镜的共振与非共振四波混频过程中具有很好的潜力。

英文摘要:

Three-color coherent anti-Stokes Raman scattering represents non-degenerate four wave mixing process that includes both a non-resonant and resonant processes, the contributions of which depend on how the molecular vibrational modes are being excited by the input laser pulses. Non-degenerate four wave mixing processes are complex and understanding these processes requires rigorous data analytical tools, which still lack in this research field. In this work, we introduce one- and two-dimensional intensity-intensity correlation functions in terms of a new variable (e.g., probe pulse delay) and new perturbation parameter (e.g., probe pulse linewidth). In particular, diagonal projections are defined here as a tool to reduce both synchronous and asynchronous two-dimensional correlation spectroscopy analyses down to one-dimensional analysis, revealing valuable analytical information. Detailed analyses using the all Gaussian coherent Raman scattering closed-form solutions and the representative experimental data for resonant and non-resonant processes are presented and compared. This intensity-intensity correlation analytical tool holds a promising potential in resolving and visualizing resonant versus non-resonant four wave mixing processes for quantitative label-free species-specific nonlinear spectroscopy and microscopy.

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