二维太赫兹拉曼光谱中的和频信号
Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy
摘要：
我们证明了卤代甲烷的2D-TTR光谱是由沿$f_1$的仪器响应函数（IRF）的复杂结构和沿$f_2$的分子相干性决定的。实验改进有助于提高测量的分辨率和动态范围，包括精确的THz脉冲形状表征。和频激励卷积的IRF被发现定量再现的2D-TTR信号。一个新的减少密度矩阵模型，其中包括和频路径，与线性和谐波算子完全支持这种（重新）解释的二维TTR光谱。
英文摘要：
We demonstrate that halogenated methane 2D-Terahertz Terahertz Raman (2D-TTR) spectra are determined by the complicated structure of the instrument response function (IRF) along $f_1$ and by the molecular coherences along $f_2$. Experimental improvements have helped increase the resolution and dynamic range of the measurements, including accurate THz pulse shape characterization. Sum-frequency excitations convolved with the IRF are found to quantitatively reproduce the 2D-TTR signal. A new Reduced Density Matrix model which incorporates sum-frequency pathways, with linear and harmonic operators fully supports this (re)interpretation of the 2D-TTR spectra.
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