High-resolution Spectroscopy Combined with Laser, Molecular Beam and Magnetic or Electric Field, and Dynamics of Excited Molecules

我们构建了一个工作在紫外-可见-近红外区域的单模自动扫描激光系统。利用主动稳定的标准子测量激光线的绝对波数，获得了优于0.0001cm^<-1>的精度。通过将激光腔锁定在稳定的外腔内，减小了扫描激光器的频率抖动，使线宽减小到0.00002cm^<-1>。我们把激光、分子束和外部磁场或电场结合起来，发展了新的实验方法。我们利用超高分辨率光谱技术研究了激发态分子的结构和动力学。我们在预离解中发现了一种新的干涉效应，即光解中的量子效应。它显示了与化学反应有关的波函数相的重要性。我们扩展了CS_2、乙二醛和吡嗪等多原子分子的高分辨率光谱。我们测量了乙二醛的无多普勒多o光子吸收光谱。光谱被完全分配，分子常数被确定。精度比以往的研究提高了100倍以上，即使在5高斯的情况下，我们也可以研究微小的扰动和磁场的影响。这些研究开辟了利用强度和能量转移的光谱学的新领域。Cs_2分子被激发到单能级D^1SIGMA^+_ (v=46， J=54)，预解离成Cs(6s^2S_<1/2>) + Cs（6p^2P_<3/2>）原子。磁场中Cs（8s^2S_<1/2, m'j>, *6p^2P_<2/3, mj>）跃迁的m_j分辨激发谱。这是关于m_j分辨多普勒线形状的第一份报告。在超第一光谱中，许多能级同时被激发，但在高分辨率光谱中，我们可以得到单个能级的寿命或预解离率。我们测量了预离解水平的旋转分辨线形状，并利用时间分辨光谱和高分辨光谱的补充结果对预离解进行了研究。少

We have constructed a single mode auto-scan laser system which works in UV-Visible-NearIR region. An actively stabilized etalon is used to measure the absolute wavenumber of laser line, and the accuracy better than 0.0001cm^<-1> is obtained. The jitters of frequency of the scanning laser is reduced by locking the laser cavity to a stabilized external cavity, and the line width is reduced to 0.00002cm^<-1>. We developed new experimental methods by combining the laser, a molecular beam, and the external magnetic or electric field.1. We have studied the structure and the dynamics of excited molecules by using techniques of ultra-high resolution spectroscopy. We found a new interference effect in predissociation which is a quantum effect in photodissociation. It shows the importance of phases of wave functions whose levels concerns a chemical reaction.2. We extended the high-resolution spectroscopy for polyatomic molecules, such as CS_2, glyoxal, and pyrazine. We measured a Doppler-free tw … More o-photon absorption apectrum of glyoxal. The spectrum is completely assigned and the molecular constants are determined. With accuracy better than 100 times than previous studies, we could study small perturbations and the effect of magnetic field even at 5 gauss. These studies opened a new field of spectroscopy which uses the intensity and energy shift.3. Cs_2 molecules were excited to the single level D^1SIGMA^+_ (v=46, J=54), which predissociated to Cs (6s^2S_<1/2>) + Cs(6p^2P_<3/2>) atoms. The m_j-resolved excitation spectra of the Cs(8s^2S_<1/2, m'j>, *6p^2P_<2/3, mj>) transition in a magnetic field. This is the first report concerning the m_j-resolved Doppler line shape.4. Many levels are excited simultaneously in a ultra-first spectroscopy, but we can get lifetime or predissociation rate of a single level in a high-resolution spectroscopy. We measured the rotationally resolved line shapes of predissociating levels, and the predissociation was studied by using supplementaly the results of time-resolved spectroscopy and high-resolution spectroscopy. Less