2D THz-THz-Raman Photon-Echo Spectroscopy of Molecular Vibrations in Liquid Bromoform,The Journal of Physical Chemistry Letters

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2D THz-THz-Raman Photon-Echo Spectroscopy of Molecular Vibrations in Liquid Bromoform
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-09-13 00:00:00 , DOI: 10.1021/acs.jpclett.7b02106
Ian A. Finneran ₁ , Ralph Welsch ₁ , Marco A. Allodi ₁ , Thomas F. Miller ₁ , Geoffrey A. Blake _{1,

2}

Affiliation

Fundamental properties of molecular liquids are governed by long-range interactions that most prominently manifest at terahertz (THz) frequencies. Here we report the detection of nonlinear THz photon-echo (rephasing) signals in liquid bromoform using THz-THz-Raman spectroscopy. Together, the many observed signatures span frequencies from 0.5 to 8.5 THz and result from couplings between thermally populated ladders of vibrational states. The strongest peaks in the spectrum are found to be multiquantum dipole and 1-quantum polarizability transitions and may arise from nonlinearities in the intramolecular dipole moment surface driven by intermolecular interactions.

中文翻译：

液体溴仿中分子振动的二维THz-THz-拉曼光子-回波光谱

分子液体的基本特性由在太赫兹（THz）频率上最显着表现出来的远程相互作用所控制。在这里，我们报告使用THz-THz-拉曼光谱检测液态溴仿中的非线性THz光子回波（重定）信号。总之，许多观察到的信号跨度介于0.5到8.5 THz之间，这是由振动状态的热填充梯子之间的耦合引起的。光谱中最强的峰是多量子偶极和1量子极化率跃迁，可能是由分子间相互作用驱动的分子内偶极矩表面的非线性引起的。

更新日期：2017-09-14

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