基于中红外飞秒激光场的原子分子电离行为若干问题的研究
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摘要
超短强激光与物质的相互作用,超越了传统微扰论框架内的非线性光学的范畴,进入了极端非线性光学区域,成为当代物理学研究的重要前沿。在该区域内,超短强激光与原子分子相互作用,呈现出一系列有趣且新颖的高度非线性物理现象,如阈上电离、非顺序双电离、高次谐波辐射产生、库仑爆炸等。强激光场中原子分子电离过程是理解这些极端非线性过程的基础,对它的研究不仅有助于在原子级时间和空间尺度上理解电子动力学,还将推动分子结构及动力学超快成像技术的发展,从而为观测和控制分子化学反应过程奠定基础。
然而,长期以来,受限于超短强激光技术,绝大多数强场电离实验研究都局限于飞秒钛宝石激光输出的波段(800nm附近)。近几年,基于光参量放大技术的可调谐中红外超短激光脉冲的出现和发展,开辟了强场物理领域中迄今很少探索到的参量空间,使强场电离研究更容易深入到隧穿电离甚至深隧穿电离区域,为完整的强场电离物理图像的形成创造了可能性。
本论文系统地开展了稀有气体原子以及同核双原子分子与中红外波段超短强激光相互作用引起的电离实验研究,通过测量原子分子在不同激光参数(如激光波长和强度)条件下的电离离子产量以及光电子能量和角分布,观察到了强场电离过程中的一些重要新现象和新效应。结合合适理论模型,阐明了这些现象和效应的物理起因,揭示出原子实库仑势以及分子基态结构等对强场电离过程的重要影响。主要工作和创新性成果如下：
1实验上系统研究了中红外波长下稀有气体原子(Ar, Kr和Xe)和双原子分子气体(N2和O2)的阈上电离行为。首次观测到在中红外波长下阈上电离光电子能谱中出现的两个新奇低能结构,即非常低能结构(Very Low-Energy Structure, VLES)和较高低能结构(High Low-Energy Structure, HLES)。这两个结构在所有研究气体中均出现,但呈现出不同的激光参数依赖关系。结合半经典理论模型,从电子能谱,二维动量分布以及初始相位分布等方面分析了这两结构的形成机制,揭示出原子实库仑势与出射电子之间的长程库仑相互作用是这两个结构形成的物理起因。
2基于半经典理论模型,引入库仑势软化参数进一步甄别原子实库仑势对VLES和HLES的具体影响。研究发现,虽然这两个结构的形成都来自于电子与原子实库仑势的相互作用,但是它们的形成对应不同的物理机制,即VLES源于电子与原子实在较短距离内的相互作用,而HLES可归结于较远距离内的相互作用。
3实验上研究并比较了不同中红外波长下同核双原子分子(N2和O2)与电离势相近的对照原子(Xe和Ar)之间电离行为的差异。首次观察到,与近红外波长下的实验结果相比,在中红外波长下O2分子相对于Xe原子发生了与光强和波长皆有关系的电离抑制现象；而N2分子的电离率与其对照原子Ar基本一样,并且不随着光强和波长改变而变化,其行为类似于无结构的原子。结合散射矩阵理论计算,我们很好地重复了实验结果并揭示出由于O2分子基态波函数具有反键对称性,来自不同氧原子核的电离电子波包间会发生相消干涉,该干涉效应引起的分子电离抑制随着激光波长和强度的减小而逐渐增强,从而产生了实验观察到的电离抑制对波长和光强的强烈依赖现象。我们的研究澄清了长期以来对双原子分子(02)在强场中出现奇特电离抑制现象背后物理机制的争议。
Ultrashort intense laser-matter interactions, which have broken up the framework of the traditional nonlinear optics, have reached the realm of extreme nonlinear optics and become an important frontier research field in modern physics. In this realm, the interactions of ultrafast intense laser with atoms and molecules lead in a series of interesting and novel highly nonlinear phenomena, such as above threshold ionization (ATI), nonsequential double ionization(NSDI), high-order harmonic generation (HHG) and Coulomb explosion. Research on the strong field ionization of atoms and molecules, which is a fundamental process, not only provides ways for understanding the dynamics of electrons in atomic time and spatial scales, but also greatly prompts the development of ultrafast imaging of the molecular structure and dynamics, opening a new avenue for monitoring and controlling the chemical reaction of molecules.
However, limited by the ultrafast laser technology, most studies on strong field ionization of atoms and molecules have been practically confined to Ti:Sapphire laser wavelength (i.e., around800nm). Until recently, with the rapid advancement of the optical parametric amplification (OPA) technique, intense wavelength-tunable mid-infrared femtosecond laser pulses becomes available, opening new avenues for research in the strong field atomic and molecular physics. Intense laser with long wavelengths offers a convenient experimental knob to push the ionization regime into the unprecedented deep tunneling limits and facilitate a comprehensive understanding of the strong field ionization.
In this dissertation, by virtue of the intense wavelength-tunable mid-infrared femtosecond laser, we perform a systematic experimental investigation on the ionization process of various noble gas atoms and homonuclear diatomic molecules under different laser parameters, i.e., wavelength and intensity, and have discovered several novel strong field atomic phenomena and effects. The underlying physical mechanisms behind these findings are uncovered by comparing the experimental data with appropriate theoretical simulations. Our works reveal an important influence of the atomic and molecular structure and the molecular orbital symmetry on the strong field ionization. The major achievements and innovations are listed as follows:
1. We have performed a systematic investigation on the ATI process of the noble gas atoms (Ar, Kr and Xe) and the diatomic molecules (N2and O2) exposed to the intense mid-infrared laser fields. The low-energy part of the measured ATI photoelectron spectra exhibits two unexpected peak-like structures with different energies, i.e., the very low-energy structure (VLES) and the high low-energy structure (HLES). The two structures were observed in all atomic and molecular species investigated and thus seemed to be universal. Moreover, it is found that VLES and HLES exhibit different dependences of laser parameters. These experimental features have been well reproduced by a semiclassical model simulation. By analyzing in detail the calculated photoelectron energy spectra, two-dimensional electron momentum distributions and the initial tunnel ionization phase distributions, we are able to ascribe the production of the low-energy structure to the long-range Coulomb interaction between the parent ionic Coulomb potential and the outgoing electron.
2. Resorting to a semiclassical model including a Coulomb potential (CP) softened by different softening parameters, we further reveal that though the very low-energy structure (VLES) and the high low-energy structure (HLES) are both due to the interaction between the ionic CP and the electron, the two structures have different physical mechanisms:the VLES can be attributed to the electron-parent ion Coulomb interaction at a rather small distance and the HLES is more likely to be ascribed to the electron-parent ion Coulomb interaction at large distance.
3. We have performed a comparison study of the ionization process of molecules (N2and O2) and their companion atoms (Ar and Xe) with mid-infrared laser wavelengths. Experimental data recorded at a mid-infrared laser wavelength and its comparison with that at a near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O2with respect to its companion atom of Xe, while N2behaves like a structureless atom. It is found that the S-matrix theory calculation can reproduce well the experimental observations and unambiguously identifies that the ionization suppression of O2is due to the effect of destructive interference between ionizing wave packets emitted from the two atomic centers of O2with an antibonding molecular ground state. Our results clarify the underlying physical mechanism of the peculiar ionization suppression behavior of molecule O2, which has been a hot topic of debate for decades.
然而,长期以来,受限于超短强激光技术,绝大多数强场电离实验研究都局限于飞秒钛宝石激光输出的波段(800nm附近)。近几年,基于光参量放大技术的可调谐中红外超短激光脉冲的出现和发展,开辟了强场物理领域中迄今很少探索到的参量空间,使强场电离研究更容易深入到隧穿电离甚至深隧穿电离区域,为完整的强场电离物理图像的形成创造了可能性。
本论文系统地开展了稀有气体原子以及同核双原子分子与中红外波段超短强激光相互作用引起的电离实验研究,通过测量原子分子在不同激光参数(如激光波长和强度)条件下的电离离子产量以及光电子能量和角分布,观察到了强场电离过程中的一些重要新现象和新效应。结合合适理论模型,阐明了这些现象和效应的物理起因,揭示出原子实库仑势以及分子基态结构等对强场电离过程的重要影响。主要工作和创新性成果如下：
1实验上系统研究了中红外波长下稀有气体原子(Ar, Kr和Xe)和双原子分子气体(N2和O2)的阈上电离行为。首次观测到在中红外波长下阈上电离光电子能谱中出现的两个新奇低能结构,即非常低能结构(Very Low-Energy Structure, VLES)和较高低能结构(High Low-Energy Structure, HLES)。这两个结构在所有研究气体中均出现,但呈现出不同的激光参数依赖关系。结合半经典理论模型,从电子能谱,二维动量分布以及初始相位分布等方面分析了这两结构的形成机制,揭示出原子实库仑势与出射电子之间的长程库仑相互作用是这两个结构形成的物理起因。
2基于半经典理论模型,引入库仑势软化参数进一步甄别原子实库仑势对VLES和HLES的具体影响。研究发现,虽然这两个结构的形成都来自于电子与原子实库仑势的相互作用,但是它们的形成对应不同的物理机制,即VLES源于电子与原子实在较短距离内的相互作用,而HLES可归结于较远距离内的相互作用。
3实验上研究并比较了不同中红外波长下同核双原子分子(N2和O2)与电离势相近的对照原子(Xe和Ar)之间电离行为的差异。首次观察到,与近红外波长下的实验结果相比,在中红外波长下O2分子相对于Xe原子发生了与光强和波长皆有关系的电离抑制现象；而N2分子的电离率与其对照原子Ar基本一样,并且不随着光强和波长改变而变化,其行为类似于无结构的原子。结合散射矩阵理论计算,我们很好地重复了实验结果并揭示出由于O2分子基态波函数具有反键对称性,来自不同氧原子核的电离电子波包间会发生相消干涉,该干涉效应引起的分子电离抑制随着激光波长和强度的减小而逐渐增强,从而产生了实验观察到的电离抑制对波长和光强的强烈依赖现象。我们的研究澄清了长期以来对双原子分子(02)在强场中出现奇特电离抑制现象背后物理机制的争议。
Ultrashort intense laser-matter interactions, which have broken up the framework of the traditional nonlinear optics, have reached the realm of extreme nonlinear optics and become an important frontier research field in modern physics. In this realm, the interactions of ultrafast intense laser with atoms and molecules lead in a series of interesting and novel highly nonlinear phenomena, such as above threshold ionization (ATI), nonsequential double ionization(NSDI), high-order harmonic generation (HHG) and Coulomb explosion. Research on the strong field ionization of atoms and molecules, which is a fundamental process, not only provides ways for understanding the dynamics of electrons in atomic time and spatial scales, but also greatly prompts the development of ultrafast imaging of the molecular structure and dynamics, opening a new avenue for monitoring and controlling the chemical reaction of molecules.
However, limited by the ultrafast laser technology, most studies on strong field ionization of atoms and molecules have been practically confined to Ti:Sapphire laser wavelength (i.e., around800nm). Until recently, with the rapid advancement of the optical parametric amplification (OPA) technique, intense wavelength-tunable mid-infrared femtosecond laser pulses becomes available, opening new avenues for research in the strong field atomic and molecular physics. Intense laser with long wavelengths offers a convenient experimental knob to push the ionization regime into the unprecedented deep tunneling limits and facilitate a comprehensive understanding of the strong field ionization.
In this dissertation, by virtue of the intense wavelength-tunable mid-infrared femtosecond laser, we perform a systematic experimental investigation on the ionization process of various noble gas atoms and homonuclear diatomic molecules under different laser parameters, i.e., wavelength and intensity, and have discovered several novel strong field atomic phenomena and effects. The underlying physical mechanisms behind these findings are uncovered by comparing the experimental data with appropriate theoretical simulations. Our works reveal an important influence of the atomic and molecular structure and the molecular orbital symmetry on the strong field ionization. The major achievements and innovations are listed as follows:
1. We have performed a systematic investigation on the ATI process of the noble gas atoms (Ar, Kr and Xe) and the diatomic molecules (N2and O2) exposed to the intense mid-infrared laser fields. The low-energy part of the measured ATI photoelectron spectra exhibits two unexpected peak-like structures with different energies, i.e., the very low-energy structure (VLES) and the high low-energy structure (HLES). The two structures were observed in all atomic and molecular species investigated and thus seemed to be universal. Moreover, it is found that VLES and HLES exhibit different dependences of laser parameters. These experimental features have been well reproduced by a semiclassical model simulation. By analyzing in detail the calculated photoelectron energy spectra, two-dimensional electron momentum distributions and the initial tunnel ionization phase distributions, we are able to ascribe the production of the low-energy structure to the long-range Coulomb interaction between the parent ionic Coulomb potential and the outgoing electron.
2. Resorting to a semiclassical model including a Coulomb potential (CP) softened by different softening parameters, we further reveal that though the very low-energy structure (VLES) and the high low-energy structure (HLES) are both due to the interaction between the ionic CP and the electron, the two structures have different physical mechanisms:the VLES can be attributed to the electron-parent ion Coulomb interaction at a rather small distance and the HLES is more likely to be ascribed to the electron-parent ion Coulomb interaction at large distance.
3. We have performed a comparison study of the ionization process of molecules (N2and O2) and their companion atoms (Ar and Xe) with mid-infrared laser wavelengths. Experimental data recorded at a mid-infrared laser wavelength and its comparison with that at a near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O2with respect to its companion atom of Xe, while N2behaves like a structureless atom. It is found that the S-matrix theory calculation can reproduce well the experimental observations and unambiguously identifies that the ionization suppression of O2is due to the effect of destructive interference between ionizing wave packets emitted from the two atomic centers of O2with an antibonding molecular ground state. Our results clarify the underlying physical mechanism of the peculiar ionization suppression behavior of molecule O2, which has been a hot topic of debate for decades.
引文
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