Dynamics of polar polarizable rotors acted upon by unipolar electromagnetic pulses: From the sudden to the adiabatic regime.

Dynamics of polar polarizable rotors acted upon by unipolar electromagnetic pulses: From the sudden to the adiabatic regime.
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DOI:
10.1063/1.5051591
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发表时间:
2018-06
期刊:
The Journal of chemical physics
影响因子:
--
通讯作者:
M. Mirahmadi;B. Schmidt;Mallikarjun Karra;B. Friedrich
M. Mirahmadi;B. Schmidt;Mallikarjun Karra;B. Friedrich
中科院分区:
其他
文献类型:
--
作者:
M. Mirahmadi;B. Schmidt;Mallikarjun Karra;B. Friedrich

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我们从解析和数值两方面研究了极化型刚性转子与单极变长电磁脉冲Δτ相互作用时相对于转子转动周期τr的动力学行为。在突然的非绝热极限Δτ≪τr下,我们导出了转子波函数、动能以及取向和取向的无场演化的解析表达式。我们通过数值求解相应的含时薛定谔方程来验证解析结果,并将所考虑的相互作用的时间范围一直扩展到绝热极限Δτ>τr,其中超出无场情况的一般解析解不再可用。取向和排列相互作用以及它们的组合对旋转态的后脉冲布居的影响被可视化为关于布居棉被的定向和排列踢力的函数。封装了旋转波包演化的量子地毯提供了由此产生的动力学的时空肖像。种群被子和量子地毯揭示了纯定向、纯对齐或平衡-破坏的组合相互作用,每个都表现出独特的动力学。在中间时间区域,我们发现波包作为定向和排列踢强度的函数显示出与脉冲持续时间的特定值下的动能减小相对应的共振。
We study, analytically as well as numerically, the dynamics that arises from the interaction of a polar polarizable rigid rotor with single unipolar electromagnetic pulses of varying length, Δτ, with respect to the rotational period of the rotor, τ r . In the sudden, non-adiabatic limit, Δτ ≪ τ r , we derive analytic expressions for the rotor's wavefunctions, kinetic energies, and field-free evolution of orientation and alignment. We verify the analytic results by solving the corresponding time-dependent Schrödinger equation numerically and extend the temporal range of the interactions considered all the way to the adiabatic limit, Δτ > τ r , where general analytic solutions beyond the field-free case are no longer available. The effects of the orienting and aligning interactions as well as of their combination on the post-pulse populations of the rotational states are visualized as functions of the orienting and aligning kick strengths in terms of population quilts. Quantum carpets that encapsulate the evolution of the rotational wavepackets provide the space-time portraits of the resulting dynamics. The population quilts and quantum carpets reveal that purely orienting, purely aligning, or even-break combined interactions each exhibit sui generis dynamics. In the intermediate temporal regime, we find that the wavepackets as functions of the orienting and aligning kick strengths show resonances that correspond to diminished kinetic energies at particular values of the pulse duration.