冷分子囚禁新方案的理论研究与CH自由基的实验制备及光谱研究
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摘要
冷分子在科学领域有很多非常重要的应用,例如：高分辨光谱的研究、冷化学与冷碰撞的研究、量子计算与信息处理、基本物理常数的测量等。本文首先介绍了冷分子的制备方法、囚禁及其应用；然后提出了极性分子静电囚禁的两种新方案；接着介绍了一种可用于静电Stark减速与操控的重要分子(CH自由基分子),以及本实验采用的两种制备方法：直流脉冲放电和五倍频YAG激光器光解；最后对本文的研究工作进行了总结和展望。
本文提出了用两个带电金属环和一个接地金属板实现一种可操控的、光学通道开放的、芯片表面的冷极性分子静电储存环。笔者数值计算了空间电场的分布情况,然后详细分析了势阱中心距离芯片表面高度与实验参数的关系,并以OH分子为例,采用经典蒙特卡洛方法模拟了分子在储存环中的运动情况。随后,我们分析了系统参数、分子束的初始分布等对分子的平动温度、囚禁效率的影响。模拟结果表明通过引入聚束功能可以显著提高分子波包在储存环中运行的圈数。
我们提出了利用三个带电金属环和两个绝缘介质板来实现一种高效、可控的冷极性分子静电表面囚禁的新方案。作者计算了电场和重氨分子的|J,KM>=|1,-1>态的囚禁势,分析了有效阱深与系统参量的关系。蒙特卡洛数值模拟表明：该方案的冷分子装载效率高达90%,最后得到的分子波包平动温度为14mK左右。通过降低阱深我们数值模拟了绝热冷却过程。结果表明通过绝热冷却,被囚禁的分子的温度从34.5mK降低到5.8mK。
我们开展了利用直流脉冲放电产生CH自由基的实验研究。通过将实验数据和LIFBASE软件模拟结果进行比对,给出了所产生的激发态CH(A2△)的振动和转动温度。我们进一步研究了CH(A2△)发射光谱强度和一些实验参量的关系,例如：放电持续时间、脉冲阀的触发与放电之间延迟时间以及放电电压等。利用共振增强多光子电离探测手段,我们获得了CH自由基的共振增强多光子电离谱线。
最后,我们采用五倍频YAG激光器多光子解离四种不同样品((CH3)2CO,CH3NO2,CH2Br2和CHBr3)来分别产生CH(A2△)自由基分子。我们获得了CH(A2△→X2Π)的发射荧光光谱,并进行了分析。通过对荧光强度与激光单脉冲能量依赖关系的测量,分析了可能的解离渠道。我们研究了荧光强度和其他实验参数的关系,例如：束源温度、束源气压、脉冲阀的触发与激光器之间延迟时间等,并分析了载气在光解实验中所扮演的角色。通过实验数据和LIFBASE软件模拟结果的比对,我们获得了CH(A2△)的振动和转动温度。
Cold molecules have many important applications in the field of science, such as high-resolution spectrum, cold chemistry, cold collision, quantum computation, quantum information processing and the measurement of fundamental physical constants. In this thesis, methods of preparing cold molecules and trapping of neutral molecules are first reviewed, the applications of cold molecules are also introduced. Then two new schemes of trapping cold polar molecules are proposed. After that, an important molecule(CH radical) which can be used for Stark deceleration and manipulation is introduced. Two methods for CH radical production are used:the DC pulse discharge and the photodissociation using the fifth harmonic YAG laser. Summary and outlook are given in the end.
Using two charged stainless steel rings and a grounded metal plate, an optically accessible and controllable electrostatic surface storage ring for cold polar molecules can be formed on a chip. The spatial distribution of the electrostatic fields is numerically calculated. Relationships between the height of the trap center above the chip surface and the setup parameters are investgated in detail. The motion of the molecules in the storage ring is numerically simulated with OH radical molecules as a tester. Dependencies of molecular translational temperature and their trapping efficiency on parameters of the trap setup and the initial distribution of cold molecules are analyzed. Numerical simulations indicate that the number of round trips a trapped molecular packet makes can be improved significantly by incorporating bunching function into the scheme.
Another scheme of a controllable high-efficient electrostatic surface trap for cold polar molecules on a chip is also studied, which consists of three charged rings and two insulating substrates. The electric fields and corresponding trapping potential for ND3molecules of J, K M>=|1,-1> state are calculated. The dependence of the effective well depth on the system parameters is analyzed. Monte-Carlo simulation shows that the loading efficiency of molecules into the trap can as high as-90%with a translational temperature of cold molecules being-14mK. Adiabatic cooling is numerically simulated by decreasing the trap depth and the temperature of the trapped molecules drops from34.5mK to5.8mK.
Experimental study of production of CH radicals is performed using the method of DC pulse discharge. Experimental data are compared to the simulated ones given by the LIFBASE software and the vibrational and rotational temperatures of CH(A2△) product are obtained. The relationships between the CH(A2Λ) emission spectrum intensity and the experimental parameters are studied, such as the discharge duration, the time delay between the trigger of the pulse valve and the discharge and the voltage of discharge.Using the tool of resonance enhanced multiphoton ionization(REMPI), we study the REMPI of CH radical.
Finally, The fifth harmonic YAG laser is used to produce CH (A2△) by multiphoton dissociation of (CH3)2CO, CH3NO2, CH2Br2and CHBr3respectively. The emission spectrum of CH (A2△) is acquired and analyzed. The dependence of fluorescence intensity on pulse energy of the laser is studied and the probable dissociation channels are analyzed. The relationships between the fluorescence intensity and some parameters are studied, such as the temperature of the beam source, stagnation pressure and the delay between the trigger of pulse valve and the laser. The role that the carrier gases play during the photodissociation is analyzed. The vibrational and rotational temperatures of CH(A2△) are obtained by comparing experimental data to simulated ones from the LIFBASE program.
本文提出了用两个带电金属环和一个接地金属板实现一种可操控的、光学通道开放的、芯片表面的冷极性分子静电储存环。笔者数值计算了空间电场的分布情况,然后详细分析了势阱中心距离芯片表面高度与实验参数的关系,并以OH分子为例,采用经典蒙特卡洛方法模拟了分子在储存环中的运动情况。随后,我们分析了系统参数、分子束的初始分布等对分子的平动温度、囚禁效率的影响。模拟结果表明通过引入聚束功能可以显著提高分子波包在储存环中运行的圈数。
我们提出了利用三个带电金属环和两个绝缘介质板来实现一种高效、可控的冷极性分子静电表面囚禁的新方案。作者计算了电场和重氨分子的|J,KM>=|1,-1>态的囚禁势,分析了有效阱深与系统参量的关系。蒙特卡洛数值模拟表明：该方案的冷分子装载效率高达90%,最后得到的分子波包平动温度为14mK左右。通过降低阱深我们数值模拟了绝热冷却过程。结果表明通过绝热冷却,被囚禁的分子的温度从34.5mK降低到5.8mK。
我们开展了利用直流脉冲放电产生CH自由基的实验研究。通过将实验数据和LIFBASE软件模拟结果进行比对,给出了所产生的激发态CH(A2△)的振动和转动温度。我们进一步研究了CH(A2△)发射光谱强度和一些实验参量的关系,例如：放电持续时间、脉冲阀的触发与放电之间延迟时间以及放电电压等。利用共振增强多光子电离探测手段,我们获得了CH自由基的共振增强多光子电离谱线。
最后,我们采用五倍频YAG激光器多光子解离四种不同样品((CH3)2CO,CH3NO2,CH2Br2和CHBr3)来分别产生CH(A2△)自由基分子。我们获得了CH(A2△→X2Π)的发射荧光光谱,并进行了分析。通过对荧光强度与激光单脉冲能量依赖关系的测量,分析了可能的解离渠道。我们研究了荧光强度和其他实验参数的关系,例如：束源温度、束源气压、脉冲阀的触发与激光器之间延迟时间等,并分析了载气在光解实验中所扮演的角色。通过实验数据和LIFBASE软件模拟结果的比对,我们获得了CH(A2△)的振动和转动温度。
Cold molecules have many important applications in the field of science, such as high-resolution spectrum, cold chemistry, cold collision, quantum computation, quantum information processing and the measurement of fundamental physical constants. In this thesis, methods of preparing cold molecules and trapping of neutral molecules are first reviewed, the applications of cold molecules are also introduced. Then two new schemes of trapping cold polar molecules are proposed. After that, an important molecule(CH radical) which can be used for Stark deceleration and manipulation is introduced. Two methods for CH radical production are used:the DC pulse discharge and the photodissociation using the fifth harmonic YAG laser. Summary and outlook are given in the end.
Using two charged stainless steel rings and a grounded metal plate, an optically accessible and controllable electrostatic surface storage ring for cold polar molecules can be formed on a chip. The spatial distribution of the electrostatic fields is numerically calculated. Relationships between the height of the trap center above the chip surface and the setup parameters are investgated in detail. The motion of the molecules in the storage ring is numerically simulated with OH radical molecules as a tester. Dependencies of molecular translational temperature and their trapping efficiency on parameters of the trap setup and the initial distribution of cold molecules are analyzed. Numerical simulations indicate that the number of round trips a trapped molecular packet makes can be improved significantly by incorporating bunching function into the scheme.
Another scheme of a controllable high-efficient electrostatic surface trap for cold polar molecules on a chip is also studied, which consists of three charged rings and two insulating substrates. The electric fields and corresponding trapping potential for ND3molecules of J, K M>=|1,-1> state are calculated. The dependence of the effective well depth on the system parameters is analyzed. Monte-Carlo simulation shows that the loading efficiency of molecules into the trap can as high as-90%with a translational temperature of cold molecules being-14mK. Adiabatic cooling is numerically simulated by decreasing the trap depth and the temperature of the trapped molecules drops from34.5mK to5.8mK.
Experimental study of production of CH radicals is performed using the method of DC pulse discharge. Experimental data are compared to the simulated ones given by the LIFBASE software and the vibrational and rotational temperatures of CH(A2△) product are obtained. The relationships between the CH(A2Λ) emission spectrum intensity and the experimental parameters are studied, such as the discharge duration, the time delay between the trigger of the pulse valve and the discharge and the voltage of discharge.Using the tool of resonance enhanced multiphoton ionization(REMPI), we study the REMPI of CH radical.
Finally, The fifth harmonic YAG laser is used to produce CH (A2△) by multiphoton dissociation of (CH3)2CO, CH3NO2, CH2Br2and CHBr3respectively. The emission spectrum of CH (A2△) is acquired and analyzed. The dependence of fluorescence intensity on pulse energy of the laser is studied and the probable dissociation channels are analyzed. The relationships between the fluorescence intensity and some parameters are studied, such as the temperature of the beam source, stagnation pressure and the delay between the trigger of pulse valve and the laser. The role that the carrier gases play during the photodissociation is analyzed. The vibrational and rotational temperatures of CH(A2△) are obtained by comparing experimental data to simulated ones from the LIFBASE program.
引文
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