A tunable XUV monochromatic light source based on the time preserving grating selection of high-order harmonic generation

We accomplish a laboratory facility for producing a femtosecond XUV coherent monochromatic radiation with a broad tunable spectral range of 20 eV-75 eV. It is based on spectral selected single-order harmonics from intense laser driven high harmonic generation in gas phase. The time preserving for the selected harmonic radiation is achieved by a Czerny-Turner type monochromator designed with a conical diffraction grating mount for minimizing the time broadening caused by grating diffraction and keeping a relatively high diffraction efficiency. Our measurement shows that the photon flux of the 23-order harmonic(H23) centered at 35.7 eV is 1×10~9 photons/s approximately with a resolving power E/?E ≈ 36.This source provides an ultrashort tunable monochromatic XUV beam for ultrafast studies of electronic and structural dynamics in a large variety of matters.     

椭圆偏振强激光场中准直的乙炔分子的高次谐波发射

We perform an experimental study on high-order harmonic generation (HHG) of aligned acetylene molecules induced by a 35-fs 800-nm strong laser field, by using a home-built HHG spectrometer. It is observed that the molecular HHG probability declines with increasing the laser ellipticity, which is in consistence with the deduction from the well-known tunneling-plus-rescattering scenario. By introducing a weak femtosecond laser pulse to nonadiabatically align the molecules, we investigated the molecular orbital effect on the HHG in both linearly and elliptically polarized driving laser fields. The results show that the harmonic intensity is maximum for the molecular axis aligned perpendicularly to the laser electric field. It indicates that both the highest occupied molecular orbitals (HOMO) and HOMO-1 contribute to the strong-field HHG of acetylene molecules. Our study should pave the way for understanding the interaction of molecules with ultrafast strong laser fields.     

Minimum structure of high-harmonic spectrafrom aligned O2 and N2 molecules

We experimentally investigated the high-order harmonic generation (HHG) from aligned O₂ and N₂ molecules in a linearly polarized laser field, and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle. The minimum position of HHG of O₂ varies with changing the laser intensity, which is caused by multi-orbital interference. However, the location of the observed minimum structure in N₂ harmonic spectrum remained unchanged upon changing the laser intensity. The mechanism of the spectral minimum for N₂ case is regarded as a Cooper-like minimum in HHG associated with the molecular electronic structure. This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.     

基于高次谐波产生的极紫外偏振涡旋光

突破传统涡旋光场束缚,发展短波极紫外涡旋光场是实现阿秒脉冲偏振控制的有效途径.本研究利用自制的平场光栅光谱仪和超快时间保持的单色仪,以800 nm,35 fs高斯或具有偏振奇点的涡旋光脉冲驱动诱导氩原子产生高次谐波,分别获得相应的高次谐波光谱以及谐波谱单阶光源的分布.实验结果表明,基于高次谐波产生实现近红外波段的涡旋光束特性转移到极紫外波段,优化后的极紫外涡旋可以实现每秒108光子数输出.同时发现极紫外波段的涡旋场和高斯场高次谐波产生具有相似相位匹配机制.基于高次谐波产生的极紫外波段的偏振涡旋光为探究和操控原子分子量子态的含时演化动力学以及形成阿秒矢量光束提供了重要的方法和技术手段.     

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

By using a heated molecular beam in combination with a time-of-flight mass spectrometer, we experimentally study the ionization of vibrational-hot carbon disulfide(CS_2) molecules irradiated by a linearly polarized 800-nm 50-fs strong laser field. The ion yields are measured in a laser intensity range of 7.0 × 10~(12) W/cm~2–1.5 × 10~(14) W/cm~2 at different molecular temperatures of up to 1400 K. Enhanced ionization yield is observed for vibrationally excited CS_2 molecules.The results show that the enhancement decreases as the laser intensity increases, and exhibits non-monotonical dependence on the molecular temperature. According to the calculated potential energy curves of the neutral and ionic electronic states of CS_2, as well as the theoretical models of molecular strong-field ionization available in the literature, we discuss the mechanism of the enhanced ionization of vibrational-hot molecules. It is indicated that the enhanced ionization could be attributed to both the reduced ionization potential with vibrational excitation and the Frank–Condon factors between the neutral and ionic electronic states. Our study paves the way to understanding the effect of nuclear motion on the strongfield ionization of molecules, which would give a further insight into theoretical and experimental investigations on the interaction of polyatomic molecules with strong laser fields.