含氚氢分子T $_2$，DT，HT振动基频的精密测量
Precision measurement of the fundamental vibrational frequencies of tritium-bearing hydrogen molecules: T$_2$, DT, HT
摘要：
利用高分辨相干拉曼光谱测量了三种含氚氢同位素T-$_2$、DT和HT的基态电子态基本Q-分支（$v=0 \rightarrow 1, ΔJ = 0$）跃迁频率，测量精度为$0.0005$ cm $^{-1}$ .一个超过百倍的改进，在以前的实验精度允许与最新的从头计算的框架内的非绝热微扰理论，包括非相对论，相对论和QED的贡献进行比较。实验和理论之间的良好协议，从而提供了一个验证的有效性的NAPT框架，这些氚化物种。在对跃迁频率进行ac-Stark位移校正的同时，定量研究了非共振背景的贡献以及非线性光谱中共振特征之间的量子干涉效应，并对跃迁频率进行了校正。饱和CARS与兰姆倾角的观察，以及使用连续波辐射的斯托克斯频率的方法进行了探讨，这可能为未来更高精度的CARS测量铺平道路。
英文摘要：
High-resolution coherent Raman spectroscopic measurements of all three tritium-containing molecular hydrogen isotopologues T$_2$, DT and HT were performed to determine the ground electronic state fundamental Q-branch ($v=0 \rightarrow 1, ΔJ = 0$) transition frequencies at accuracies of $0.0005$ cm$^{-1}$. An over hundred-fold improvement in accuracy over previous experiments allows the comparison with the latest ab initio calculations in the framework of Non-Adiabatic Perturbation Theory including nonrelativisitic, relativisitic and QED contributions. Excellent agreement is found between experiment and theory, thus providing a verification of the validity of the NAPT-framework for these tritiated species. While the transition frequencies were corrected for ac-Stark shifts, the contributions of non-resonant background as well as quantum interference effects between resonant features in the nonlinear spectroscopy were quantitatively investigated, also leading to corrections to the transition frequencies. Methods of saturated CARS with the observation of Lamb dips, as well as the use of continuous-wave radiation for the Stokes frequency were explored, that might pave the way for future higher-accuracy CARS measurements.
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