超快激光场中双原子分子的定向和超阈值电离动力学理论研究
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摘要
本学位论文采用含时量子波包方法,从理论上研究了超短激光脉冲场中双原子分子的定向和超阈值电离动力学过程。主要工作包括以下几个方面：
首先,我们以LiH原子为研究对象,提出了三种利用激光场自身特性或激光场的组合来控制分子场后定向的理论方案。它们是：
(1)提出了利用三个完全相同的半周期太赫兹激光脉冲链来控制分子场后定向的理论方案。同单个半周期太赫兹脉冲的结果相比,利用三个相同的半周期太赫兹脉冲能激发更多的振转布居跃迁,明显增强分子定向。通过合理调整场强幅值、脉冲之间的延迟时间等激光场参数,可以获得最大定向度为0.798的分子场后定向。
(2)提出了在一束调制的双色激光脉冲之后,再加上一束半周期太赫兹脉冲来增强分子定向的理论方案。在本方案中,半周期太赫兹脉冲用来定向分子,调制的双色激光脉冲则用于控制分子的振转激发和提高分子的定向度。我们详细讨论了调制双色激光场的包络相位Φ和包络周期Tp对目标态布居以及定向效果的影响。结果表明：通过改变双色调制激光场的参数,可以有效控制目标态的布居,并且能够明显增强分子的定向。此外,我们还讨论了温度对定向的影响。结果显示本方案在温度小于50K的条件下依然有效。
(3)提出了一个获得高效、长寿命的分子场后定向的理论控制方案。我们将两束有合适延迟时间的双色调制周期量级太赫兹脉冲叠加成一个激光场来控制分子场后定向。分别研究了调制周期量级太赫兹脉冲的总包络周期、中心频率以及包络相位对分子定向度以及定向持续时间的影响。同时也讨论了温度的影响。结果表明：通过合理调节这些激光场参数,可以兼顾分子的定向度与持续时间,得到定向度比较高,持续时间比较长的长寿命分子场后定向。计算中所用到的激光场参数都是目前实验室能够获得的,所以本方案为实验上获得长寿命的分子场后定向提供了一个新思路。
此外,我们还以NaK分子为研究对象,研究了周期量级激光场中极性分子的超阈值电离过程。通过计算分子的左、右超阈值电离谱,我们发现：左右超阈值电离谱是不对称的,并且这种不对称性强烈依赖于分子的定向以及激光场的载波包络相位。通过改变分子的初始转动态,我们还分别计算了J=3、5和7时的左、右超阈值电离谱和激发态布居分布,揭示转动温度对超阈值电离谱的左右不对称性的影响。
The works in this thesis are based upon the time-dependent quantum wave packet method. to study the orientation and above threshold ionization dynamics of diatomic molecules in ultrashort laser field. The main works are as follows.
With the LiH molecule as an example, we propose three new schemes to control the field-free molecular orientation by utilizing the characters of the external laser fields and dif-ferent combination of several fields.
(1) A theoretical scenario used for achieving efficient field-free molecular orientation with a few half-cycle pulses (HCPs) is proposed, with the LiH molecule as an example. Compared with a single HCP. three HCPs can excite more rovibrational transitions and obviously en-hance the degree of molecular orientation. By optimizing the field amplitude and the delay time of laser field, a maximum value of0.798for the degree of molecular orientation is ob-tained.
(2) Using the two-dimension time-dependent quantum wave packet method, we investi-gate theoretically the field-free molecular orientation driven by a modulated two-color laser pulse together with a delayed half-cycle THz pulse. In our control scheme. the half-cycle THz pulse is used to orient molecules, and the modulated two-color laser pulse is utilized to control the rovibrational excitation and enhance the molecular orientation degree. The effects of the phase of envelope (?) and the period Tp of the modulated two-color laser field on the molecular orientation and the population of the target state are discussed in detail. It is shown that more molecules are populated to the target state and more efficient molecular orientation is achieved by adjusting these parameters of the modulated two-color laser pulse. The molecular orientation is comparatively robust towards thermal averaging in the region of T<50K.
(3) Considering the effect of the polarizability. we present a theoretical scheme used for achieving an efficient long-lived field-free molecular orientation by utilizing two modulated few-cycle THz pulses with an appropriate delay time. The exact numerical calculations are performed by solving the time-dependent Schrodinger equation including the vibrational and rotational degrees of freedom. The results indicate that the orientation degree and the orien- tation duration are strongly related to the period of envelope. the central frequency and the phase of envelope of the modulated few-cycle THz pulses. Taking a compromise. a long-lived and efficient field-free molecular orientation can be realized by adjusting these laser param-eters which is available in the current experiment. The effect of temperature on molecular orientation is also discussed.
We also investigate theoretically the above-threshold ionization (ATI) of the polar NaK molecule exposed in few-cycle laser field. The left and right ATI spectra are calculated by integrating the ionization continuum wave function over the left and the right half spheres along the laser polarization. We find that the left and right ATI spectra are asymmetric, and this asymmetry depends strongly on the molecular orientation and the carrier-envelope phase (CEP) of the laser pulse. Moreover, we also perform the calculation for different ini-tially rotational states to study the effect of rotational temperature on the ATI danamics.
首先,我们以LiH原子为研究对象,提出了三种利用激光场自身特性或激光场的组合来控制分子场后定向的理论方案。它们是：
(1)提出了利用三个完全相同的半周期太赫兹激光脉冲链来控制分子场后定向的理论方案。同单个半周期太赫兹脉冲的结果相比,利用三个相同的半周期太赫兹脉冲能激发更多的振转布居跃迁,明显增强分子定向。通过合理调整场强幅值、脉冲之间的延迟时间等激光场参数,可以获得最大定向度为0.798的分子场后定向。
(2)提出了在一束调制的双色激光脉冲之后,再加上一束半周期太赫兹脉冲来增强分子定向的理论方案。在本方案中,半周期太赫兹脉冲用来定向分子,调制的双色激光脉冲则用于控制分子的振转激发和提高分子的定向度。我们详细讨论了调制双色激光场的包络相位Φ和包络周期Tp对目标态布居以及定向效果的影响。结果表明：通过改变双色调制激光场的参数,可以有效控制目标态的布居,并且能够明显增强分子的定向。此外,我们还讨论了温度对定向的影响。结果显示本方案在温度小于50K的条件下依然有效。
(3)提出了一个获得高效、长寿命的分子场后定向的理论控制方案。我们将两束有合适延迟时间的双色调制周期量级太赫兹脉冲叠加成一个激光场来控制分子场后定向。分别研究了调制周期量级太赫兹脉冲的总包络周期、中心频率以及包络相位对分子定向度以及定向持续时间的影响。同时也讨论了温度的影响。结果表明：通过合理调节这些激光场参数,可以兼顾分子的定向度与持续时间,得到定向度比较高,持续时间比较长的长寿命分子场后定向。计算中所用到的激光场参数都是目前实验室能够获得的,所以本方案为实验上获得长寿命的分子场后定向提供了一个新思路。
此外,我们还以NaK分子为研究对象,研究了周期量级激光场中极性分子的超阈值电离过程。通过计算分子的左、右超阈值电离谱,我们发现：左右超阈值电离谱是不对称的,并且这种不对称性强烈依赖于分子的定向以及激光场的载波包络相位。通过改变分子的初始转动态,我们还分别计算了J=3、5和7时的左、右超阈值电离谱和激发态布居分布,揭示转动温度对超阈值电离谱的左右不对称性的影响。
The works in this thesis are based upon the time-dependent quantum wave packet method. to study the orientation and above threshold ionization dynamics of diatomic molecules in ultrashort laser field. The main works are as follows.
With the LiH molecule as an example, we propose three new schemes to control the field-free molecular orientation by utilizing the characters of the external laser fields and dif-ferent combination of several fields.
(1) A theoretical scenario used for achieving efficient field-free molecular orientation with a few half-cycle pulses (HCPs) is proposed, with the LiH molecule as an example. Compared with a single HCP. three HCPs can excite more rovibrational transitions and obviously en-hance the degree of molecular orientation. By optimizing the field amplitude and the delay time of laser field, a maximum value of0.798for the degree of molecular orientation is ob-tained.
(2) Using the two-dimension time-dependent quantum wave packet method, we investi-gate theoretically the field-free molecular orientation driven by a modulated two-color laser pulse together with a delayed half-cycle THz pulse. In our control scheme. the half-cycle THz pulse is used to orient molecules, and the modulated two-color laser pulse is utilized to control the rovibrational excitation and enhance the molecular orientation degree. The effects of the phase of envelope (?) and the period Tp of the modulated two-color laser field on the molecular orientation and the population of the target state are discussed in detail. It is shown that more molecules are populated to the target state and more efficient molecular orientation is achieved by adjusting these parameters of the modulated two-color laser pulse. The molecular orientation is comparatively robust towards thermal averaging in the region of T<50K.
(3) Considering the effect of the polarizability. we present a theoretical scheme used for achieving an efficient long-lived field-free molecular orientation by utilizing two modulated few-cycle THz pulses with an appropriate delay time. The exact numerical calculations are performed by solving the time-dependent Schrodinger equation including the vibrational and rotational degrees of freedom. The results indicate that the orientation degree and the orien- tation duration are strongly related to the period of envelope. the central frequency and the phase of envelope of the modulated few-cycle THz pulses. Taking a compromise. a long-lived and efficient field-free molecular orientation can be realized by adjusting these laser param-eters which is available in the current experiment. The effect of temperature on molecular orientation is also discussed.
We also investigate theoretically the above-threshold ionization (ATI) of the polar NaK molecule exposed in few-cycle laser field. The left and right ATI spectra are calculated by integrating the ionization continuum wave function over the left and the right half spheres along the laser polarization. We find that the left and right ATI spectra are asymmetric, and this asymmetry depends strongly on the molecular orientation and the carrier-envelope phase (CEP) of the laser pulse. Moreover, we also perform the calculation for different ini-tially rotational states to study the effect of rotational temperature on the ATI danamics.
引文
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