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首页> 外文期刊>The Journal of Chemical Physics >STATE-SELECTIVE CONTROL FOR VIBRATIONAL EXCITATION AND DISSOCIATION OF DIATOMIC MOLECULES WITH SHAPED ULTRASHORT INFRARED LASER PULSES
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STATE-SELECTIVE CONTROL FOR VIBRATIONAL EXCITATION AND DISSOCIATION OF DIATOMIC MOLECULES WITH SHAPED ULTRASHORT INFRARED LASER PULSES

机译：超短脉冲红外激光脉动分子的振动激发和解离的状态选择控制

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Ultrafast state-selective dynamics of diatomic molecules in the electronic ground state under the control of infrared picosecond and femtosecond shaped laser pulses is investigated for the discrete vibrational bound states and for the dissociative continuum states. Quantum dynamics in a classical laser field is simulated for a one-dimensional nonrotating dissociative Morse oscillator, representing the local OH bond in the H2O and HOD molecules. Computer simulations are based on two approaches - exact treatment by the time-dependent Schrodinger equation and approximate treatment by integro-differential equations for the probability amplitudes of the bound states only. Combination of these two approaches is useful to reveal mechanisms underlying selective excitation of the continuum states and above-threshold dissociation in a single electronic state and for designing optimal laser fields to control selective preparation of the high-lying bound states and the continuum states. Optimal laser fields can be designed to yield almost 100% selective preparation of any prescribed bound state, including those close to the dissociation threshold. State-selective preparation of the highest bound state may be accompanied by the appearance of a quasi-bound molecular state in the continuum with the kinetic energy of the fragments being close to zero. The respective above-threshold dissociation spectrum contains an additional, zero-order peak. The laser-induced dissociation from selectively prepared high-lying bound states is shown to be very efficient, with the dissociation probability approaching the maximal value. Flexible tools of state-selective laser control are developed which enable one to achieve selective control of the dissociation spectra resulting in time-selective and space-selective control of the dissociation fragments. (C) 1996 American Institute of Physics. [References: 81]
机译：研究了在红外皮秒和飞秒形激光脉冲控制下，电子基态中双原子分子的超快状态选择动力学，用于离散的振动束缚态和解离的连续态。针对一维非旋转解离摩尔斯振荡器，模拟了经典激光场中的量子动力学，该动力学代表了H2O和HOD分子中的局部OH键。计算机仿真基于两种方法-仅对依赖于时间的Schrodinger方程进行精确处理，而对于积分态的概率幅度仅通过Integro-微分方程进行近似处理。这两种方法的组合可用于揭示在单个电子态中连续态的选择性激发和阈值以上解离的基础机理，以及设计最佳激光场以控制高结合态和连续态的选择性制备。可以设计最佳激光场，以对任何规定的结合状态（包括接近解离阈值的结合状态）进行几乎100％的选择性制备。最高结合态的状态选择性制备可能伴随着在连续体中出现准结合分子态，而片段的动能接近于零。各自的阈上解离谱包含一个附加的零阶峰。激光诱导的从选择性制备的高束缚态的离解被证明是非常有效的，其离解概率接近最大值。开发了状态选择激光控制的灵活工具，该工具使人们能够实现对解离光谱的选择性控制，从而实现对解离碎片的时间选择性和空间选择性控制。 （C）1996年美国物理研究所。 [参考：81]

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