论文标题
2d-terahertz-terahertz-raman光谱学中的总和信号
Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy
论文作者
论文摘要
我们证明，卤代甲烷2d-terahertz Terahertz拉曼（2D-TTR）光谱由沿$ f_1 $的仪器响应函数（IRF）的复杂结构和沿$ f_2 $的分子相干确定。实验改进有助于增加测量的分辨率和动态范围，包括准确的THZ脉冲形状表征。发现与IRF卷积的总频激发可定量再现2D-TTR信号。一个新的还原密度矩阵模型，该模型结合了总和频率途径，线性和谐波操作员完全支持对2D-TTR光谱的（重新）解释。
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.
